@article{StefancuNanZhuetal.2022,
author = {Stefancu, Andrei and Nan, Lin and Zhu, Li and Chis, Vasile and Bald, Ilko and Liu, Min and Leopold, Nicolae and Maier, Stefan A. and Cortes, Emiliano},
title = {Controlling plasmonic chemistry pathways through specific ion effects},
series = {Advanced optical materials},
volume = {10},
journal = {Advanced optical materials},
number = {14},
publisher = {Wiley-VCH},
address = {Weinheim},
issn = {2195-1071},
doi = {10.1002/adom.202200397},
pages = {10},
year = {2022},
abstract = {Plasmon-driven dehalogenation of brominated purines has been recently explored as a model system to understand fundamental aspects of plasmon-assisted chemical reactions. Here, it is shown that divalent Ca2+ ions strongly bridge the adsorption of bromoadenine (Br-Ade) to Ag surfaces. Such ion-mediated binding increases the molecule's adsorption energy leading to an overlap of the metal energy states and the molecular states, enabling the chemical interface damping (CID) of the plasmon modes of the Ag nanostructures (i.e., direct electron transfer from the metal to Br-Ade). Consequently, the conversion of Br-Ade to adenine almost doubles following the addition of Ca2+. These experimental results, supported by theoretical calculations of the local density of states of the Ag/Br-Ade complex, indicate a change of the charge transfer pathway driving the dehalogenation reaction, from Landau damping (in the lack of Ca2+ ions) to CID (after the addition of Ca2+). The results show that the surface dynamics of chemical species (including water molecules) play an essential role in charge transfer at plasmonic interfaces and cannot be ignored. It is envisioned that these results will help in designing more efficient nanoreactors, harnessing the full potential of plasmon-assisted chemistry.},
language = {en}
}
@article{ZhaoOpitzEljarratetal.2021,
author = {Zhao, Yuhang and Opitz, Andreas and Eljarrat, Alberto and Kochovski, Zdravko and Koch, Christoph and Koch, Norbert and Lu, Yan},
title = {Kinetic study on the adsorption of 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane on Ag nanoparticles in chloroform},
series = {ACS applied nano materials},
volume = {4},
journal = {ACS applied nano materials},
number = {11},
publisher = {American Chemical Society},
address = {Washington},
issn = {2574-0970},
doi = {10.1021/acsanm.1c02153},
pages = {11625 -- 11635},
year = {2021},
abstract = {In this study, the kinetics of the adsorption of 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F(4)TCNQ) on the surface of Ag nanoparticles (Ag NPs) in chloroform has been intensively investigated, as molecular doping is known to play a crucial role in organic electronic devices. Based on the results obtained from UV-visible (vis)-near-infrared (NIR) absorption spectroscopy, cryogenic transmission electron microscopy, scanning nanobeam electron diffraction, and electron energy loss spectroscopy, a two-step interaction kinetics has been proposed for the Ag NPs and F(4)TCNQ molecules, which includes the first step of electron transfer from Ag NPs to F(4)TCNQ indicated by the ionization of F(4)TCNQ and the second step of the formation of a Ag-F(4)TCNQ complex. The whole process has been followed via UV-vis-NIR absorption spectroscopy, which reveals distinct kinetics at two stages: the instantaneous ionization and the long-term complex formation. The kinetics and the influence of the molar ratio of Ag NPs/F(4)TCNQ molecules on the interaction between Ag NPs and F(4)TCNQ molecules in an organic solution are reported herein for the first time. Furthermore, the control experiment with silica-coated Ag NPs manifests that the charge transfer at the surface between Ag NPs and F(4)TCNQ molecules is prohibited by a silica layer of 18 nm.},
language = {en}
}
@article{ZhouXuMaetal.2021,
author = {Zhou, Shuo and Xu, Xun and Ma, Nan and Jung, Friedrich and Lendlein, Andreas},
title = {Influence of sterilization conditions on sulfate-functionalized polyGGE},
series = {Clinical hemorheology and microcirculation : blood flow and vessels},
volume = {79},
journal = {Clinical hemorheology and microcirculation : blood flow and vessels},
number = {4},
publisher = {IOS Press},
address = {Amsterdam},
issn = {1386-0291},
doi = {10.3233/CH-211241},
pages = {597 -- 608},
year = {2021},
abstract = {Sulfated biomolecules are known to influence numerous biological processes in all living organisms. Particularly, they contribute to prevent and inhibit the hypercoagulation condition. The failure of polymeric implants and blood contacting devices is often related to hypercoagulation and microbial contamination. Here, bioactive sulfated biomacromolecules are mimicked by sulfation of poly(glycerol glycidyl ether) (polyGGE) films. Autoclaving, gamma-ray irradiation and ethylene oxide (EtO) gas sterilization techniques were applied to functionalized materials. The sulfate group density and hydrophilicity of sulfated polymers were decreased while chain mobility and thermal degradation were enhanced post autoclaving when compared to those after EtO sterilization. These results suggest that a quality control after sterilization is mandatory to ensure the amount and functionality of functionalized groups are retained.},
language = {en}
}
@phdthesis{Mostafa2024,
author = {Mostafa, Amr},
title = {DNA origami nanoforks: A platform for cytochrome c single molecule surface enhanced Raman spectroscopy},
doi = {10.25932/publishup-63548},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-635482},
school = {Universit{\"a}t Potsdam},
pages = {xi, 90, x},
year = {2024},
abstract = {This thesis presents a comprehensive exploration of the application of DNA origami nanofork antennas (DONAs) in the field of spectroscopy, with a particular focus on the structural analysis of Cytochrome C (CytC) at the single-molecule level. The research encapsulates the design, optimization, and application of DONAs in enhancing the sensitivity and specificity of Raman spectroscopy, thereby offering new insights into protein structures and interactions. The initial phase of the study involved the meticulous optimization of DNA origami structures. This process was pivotal in developing nanoscale tools that could significantly enhance the capabilities of Raman spectroscopy. The optimized DNA origami nanoforks, in both dimer and aggregate forms, demonstrated an enhanced ability to detect and analyze molecular vibrations, contributing to a more nuanced understanding of protein dynamics. A key aspect of this research was the comparative analysis between the dimer and aggregate forms of DONAs. This comparison revealed that while both configurations effectively identified oxidation and spin states of CytC, the aggregate form offered a broader range of detectable molecular states due to its prolonged signal emission and increased number of molecules. This extended duration of signal emission in the aggregates was attributed to the collective hotspot area, enhancing overall signal stability and sensitivity. Furthermore, the study delved into the analysis of the Amide III band using the DONA system. Observations included a transient shift in the Amide III band's frequency, suggesting dynamic alterations in the secondary structure of CytC. These shifts, indicative of transitions between different protein structures, were crucial in understanding the protein's functional mechanisms and interactions. The research presented in this thesis not only contributes significantly to the field of spectroscopy but also illustrates the potential of interdisciplinary approaches in biosensing. The use of DNA origami-based systems in spectroscopy has opened new avenues for research, offering a detailed and comprehensive understanding of protein structures and interactions. The insights gained from this research are expected to have lasting implications in scientific fields ranging from drug development to the study of complex biochemical pathways. This thesis thus stands as a testament to the power of integrating nanotechnology, biochemistry, and spectroscopic techniques in addressing complex scientific questions.},
language = {en}
}
@article{MichaelisAengenheisterTuchtenhagenetal.2022,
author = {Michaelis, Vivien and Aengenheister, Leonie and Tuchtenhagen, Max and Rinklebe, J{\"o}rg and Ebert, Franziska and Schwerdtle, Tanja and Buerki-Thurnherr, Tina and Bornhorst, Julia},
title = {Differences and interactions in placental manganese and iron transfer across an in vitro model of human villous trophoblasts},
series = {International journal of molecular sciences},
volume = {23},
journal = {International journal of molecular sciences},
number = {6},
publisher = {MDPI},
address = {Basel},
issn = {1422-0067},
doi = {10.3390/ijms23063296},
pages = {18},
year = {2022},
abstract = {Manganese (Mn) as well as iron (Fe) are essential trace elements (TE) important for the maintenance of physiological functions including fetal development. However, in the case of Mn, evidence suggests that excess levels of intrauterine Mn are associated with adverse pregnancy outcomes. Although Mn is known to cross the placenta, the fundamentals of Mn transfer kinetics and mechanisms are largely unknown. Moreover, exposure to combinations of TEs should be considered in mechanistic transfer studies, in particular for TEs expected to share similar transfer pathways. Here, we performed a mechanistic in vitro study on the placental transfer of Mn across a BeWo b30 trophoblast layer. Our data revealed distinct differences in the placental transfer of Mn and Fe. While placental permeability to Fe showed a clear inverse dose-dependency, Mn transfer was largely independent of the applied doses. Concurrent exposure of Mn and Fe revealed transfer interactions of Fe and Mn, indicating that they share common transfer mechanisms. In general, mRNA and protein expression of discussed transporters like DMT1, TfR, or FPN were only marginally altered in BeWo cells despite the different exposure scenarios highlighting that Mn transfer across the trophoblast layer likely involves a combination of active and passive transport processes.},
language = {en}
}
@misc{BandeGonzalezKlamrothetal.2022,
author = {Bande, Annika and Gonz{\´a}lez, Leticia and Klamroth, Tillmann and Tremblay, Jean Christophe},
title = {Theoretical chemistry and quantum dynamics at interfaces},
series = {Chemical physics : a journal devoted to experimental and theoretical research involving problems of both a chemical and physical nature},
volume = {558},
journal = {Chemical physics : a journal devoted to experimental and theoretical research involving problems of both a chemical and physical nature},
publisher = {Elsevier Science},
address = {Amsterdam [u.a.]},
issn = {0301-0104},
doi = {10.1016/j.chemphys.2022.111509},
pages = {3},
year = {2022},
language = {en}
}
@article{CrovettoKojdaYietal.2022,
author = {Crovetto, Andrea and Kojda, Danny and Yi, Feng and Heinselman, Karen N. and LaVan, David A. and Habicht, Klaus and Unold, Thomas and Zakutayev, Andriy},
title = {Crystallize It before It diffuses},
series = {Journal of the american chemical society},
volume = {144},
journal = {Journal of the american chemical society},
number = {29},
publisher = {American Chemical Society},
address = {Washington},
issn = {0002-7863},
doi = {10.1021/jacs.2c04868},
pages = {13334 -- 13343},
year = {2022},
abstract = {Numerous phosphorus-rich metal phosphides containing both P-P bonds and metal-P bonds are known from the solid-state chemistry literature. A method to grow these materials in thin-film form would be desirable, as thin films are required in many applications and they are an ideal platform for high-throughput studies. In addition, the high density and smooth surfaces achievable in thin films are a significant advantage for characterization of transport and optical properties. Despite these benefits, there is hardly any published work on even the simplest binary phosphorus-rich phosphide films. Here, we demonstrate growth of single-phase CuP2 films by a two-step process involving reactive sputtering of amorphous CuP2+x and rapid annealing in an inert atmosphere. At the crystallization temperature, CuP2 is thermodynamically unstable with respect to Cu3P and P-4. However, CuP2 can be stabilized if the amorphous precursors are mixed on the atomic scale and are sufficiently close to the desired composition (neither too P poor nor too P rich). Fast formation of polycrystalline CuP2, combined with a short annealing time, makes it possible to bypass the diffusion processes responsible for decomposition. We find that thin-film CuP2 is a 1.5 eV band gap semiconductor with interesting properties, such as a high optical absorption coefficient (above 10(5) cm(-1)), low thermal conductivity (1.1 W/(K m)), and composition-insensitive electrical conductivity (around 1 S/cm). We anticipate that our processing route can be extended to other phosphorus-rich phosphides that are still awaiting thin-film synthesis and will lead to a more complete understanding of these materials and of their potential applications.},
language = {en}
}
@article{TungMaringXuetal.2022,
author = {Tung, Wing Tai and Maring, Janita A. and Xu, Xun and Liu, Yue and Becker, Matthias and Somesh, Dipthi Bachamanda and Klose, Kristin and Wang, Weiwei and Sun, Xianlei and Ullah, Imran and Kratz, Karl and Neffe, Axel T. and Stamm, Christof and Ma, Nan and Lendlein, Andreas},
title = {In vivo performance of a cell and factor free multifunctional fiber mesh modulating postinfarct myocardial remodeling},
series = {Advanced Functional Materials},
volume = {32},
journal = {Advanced Functional Materials},
number = {31},
publisher = {Wiley},
address = {Weinheim},
issn = {1616-301X},
doi = {10.1002/adfm.202110179},
pages = {17},
year = {2022},
abstract = {Guidance of postinfarct myocardial remodeling processes by an epicardial patch system may alleviate the consequences of ischemic heart disease. As macrophages are highly relevant in balancing immune response and regenerative processes their suitable instruction would ensure therapeutic success. A polymeric mesh capable of attracting and instructing monocytes by purely physical cues and accelerating implant degradation at the cell/implant interface is designed. In a murine model for myocardial infarction the meshes are compared to those either coated with extracellular matrix or loaded with induced cardiomyocyte progenitor cells. All implants promote macrophage infiltration and polarization in the epicardium, which is verified by in vitro experiments. 6 weeks post-MI, especially the implantation of the mesh attenuates left ventricular adverse remodeling processes as shown by reduced infarct size (14.7\% vs 28-32\%) and increased wall thickness (854 mu m vs 400-600 mu m), enhanced angiogenesis/arteriogenesis (more than 50\% increase compared to controls and other groups), and improved heart function (ejection fraction = 36.8\% compared to 12.7-31.3\%). Upscaling as well as process controls is comprehensively considered in the presented mesh fabrication scheme to warrant further progression from bench to bedside.},
language = {en}
}
@article{BreternitzSchorr2021,
author = {Breternitz, Joachim and Schorr, Susan},
title = {Symmetry relations in wurtzite nitrides and oxide nitrides and the curious case of Pmc2(1)},
series = {Acta crystallographica / International Union of Crystallography. Section A, Foundations and advances},
volume = {77},
journal = {Acta crystallographica / International Union of Crystallography. Section A, Foundations and advances},
number = {3},
publisher = {Blackwell},
address = {Oxford [u.a.]},
issn = {2053-2733},
doi = {10.1107/S2053273320015971},
pages = {208 -- 216},
year = {2021},
abstract = {Binary III-V nitrides such as AlN, GaN and InN in the wurtzite-type structure have long been considered as potent semiconducting materials because of their optoelectronic properties, amongst others. With rising concerns over the utilization of scarce elements, a replacement of the trivalent cations by others in ternary and multinary nitrides has led to the development of different variants of nitrides and oxide nitrides crystallizing in lower-symmetry variants of wurtzite. This work presents the symmetry relationships between these structural types specific to nitrides and oxide nitrides and updates some prior work on this matter. The non-existence of compounds crystallizing in Pmc2(1), formally the highest subgroup of the wurtzite type fulfilling Pauling's rules for 1:1:2 stoichiometries, has been puzzling scientists for a while; a rationalization is given, from a crystallographic basis, of why this space group is unlikely to be adopted.},
language = {en}
}
@article{MeiSiebertXuetal.2022,
author = {Mei, Shilin and Siebert, Andreas and Xu, Yaolin and Quan, Ting and Garcia-Diez, Raul and B{\"a}r, Marcus and H{\"a}rtel, Paul and Abendroth, Thomas and D{\"o}rfler, Susanne and Kaskel, Stefan and Lu, Yan},
title = {Large-Scale Synthesis of Nanostructured Carbon-Ti4O7 Hollow Particles as Efficient Sulfur Host Materials for Multilayer Lithium-Sulfur Pouch Cells},
series = {Batteries \& supercaps},
volume = {5},
journal = {Batteries \& supercaps},
number = {6},
publisher = {Wiley-VCH},
address = {Weinheim},
issn = {2566-6223},
doi = {10.1002/batt.202100398},
pages = {11},
year = {2022},
abstract = {Applications of advanced cathode materials with well-designed chemical components and/or optimized nanostructures promoting the sulfur redox kinetics and suppressing the shuttle effect of polysulfides are highly valued. However, in the case of actual lithium-sulfur (Li-S) batteries under practical working conditions, one long-term obstacle still exists, which is mainly due to the difficulties in massive synthesis of such nanomaterials with low cost and ease of control on the nanostructure. Herein, we develop a facile synthesis of carbon coated Ti4O7 hollow nanoparticles (Ti4O7) using spherical polymer electrolyte brush as soft template, which is scalable via utilizing a minipilot reactor. The C Ti4O7 hollow nanoparticles provide strong chemical adsorption to polysulfides through the large polar surface and additional physical confinement by rich micro- \& mesopores and have successfully been employed as an efficient sulfur host for multilayer pouch cells. Besides, the sluggish kinetics of the sulfur and lithium sulfide redox mechanism can be improved by the highly conductive Ti4O7 via catalyzation of the conversion of polysulfides. Consequently, the C-Ti4O7 based pouch cell endows a high discharge capacity of 1003 mAhg(-1) at 0.05 C, a high-capacity retention of 83.7\% after 100 cycles at 0.1 C, and a high Coulombic efficiency of 97.5\% at the 100th cycle. This work proposes an effective approach to transfer the synthesis of hollow Ti4O7 nanoparticles from lab- to large-scale production, paving the way to explore a wide range of advanced nanomaterials for multilayer Li-S pouch cells.},
language = {en}
}
@article{LepreHeskeNowakowskietal.2022,
author = {Lepre, Enrico and Heske, Julian and Nowakowski, Michal and Scoppola, Ernesto and Zizak, Ivo and Heil, Tobias and K{\"u}hne, Thomas D. and Antonietti, Markus and Lopez-Salas, Nieves and Albero, Josep},
title = {Ni-based electrocatalysts for unconventional CO2 reduction reaction to formic acid},
series = {Nano energy},
volume = {97},
journal = {Nano energy},
publisher = {Elsevier},
address = {Amsterdam},
issn = {2211-2855},
doi = {10.1016/j.nanoen.2022.107191},
pages = {12},
year = {2022},
abstract = {Electrochemical reduction stands as an alternative to revalorize CO2. Among the different alternatives, Ni single atoms supported on carbonaceous materials are an appealing catalytic solution due to the low cost and versatility of the support and the optimal usage of Ni and its predicted selectivity and efficiency (ca. 100\% towards CO). Herein, we have used noble carbonaceous support derived from cytosine to load Ni subnanometric sites. The large heteroatom content of the support allows the stabilization of up to 11 wt\% of Ni without the formation of nanoparticles through a simple impregnation plus calcination approach, where nickel promotes the stabilization of C3NOx frameworks and the oxidative support promotes a high oxidation state of nickel. EXAFS analysis points at nickel single atoms or subnanometric clusters coordinated by oxygen in the material surface. Unlike the wellknown N-coordinated Ni single sites selectivity towards CO2 reduction, O-coordinated-Ni single sites (ca. 7 wt\% of Ni) reduced CO2 to CO, but subnanometric clusters (11 wt\% of Ni) foster the unprecedented formation of HCOOH with 27\% Faradaic efficiency at - 1.4 V. Larger Ni amounts ended up on the formation of NiO nanoparticles and almost 100\% selectivity towards hydrogen evolution.},
language = {en}
}
@article{HaubitzDrobotTsushimaetal.2021,
author = {Haubitz, Toni and Drobot, Bj{\"o}rn and Tsushima, Satoru and Steudtner, Robin and Stumpf, Thorsten and Kumke, Michael Uwe},
title = {Quenching mechanism of uranyl(VI) by chloride and bromide in aqueous and non-aqueous solutions},
series = {The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment \& general theory},
volume = {125},
journal = {The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment \& general theory},
number = {20},
publisher = {American Chemical Society},
address = {Washington},
issn = {1089-5639},
doi = {10.1021/acs.jpca.1c02487},
pages = {4380 -- 4389},
year = {2021},
abstract = {A major hindrance in utilizing uranyl(VI) luminescence as a standard analytical tool, for example, in environmental monitoring or nuclear industries, is quenching by other ions such as halide ions, which are present in many relevant matrices of uranyl(VI) speciation. Here, we demonstrate through a combination of time-resolved laser-induced fluorescence spectroscopy, transient absorption spectroscopy, and quantum chemistry that coordinating solvent molecules play a crucial role in U(VI) halide luminescence quenching. We show that our previously suggested quenching mechanism based on an internal redox reaction of the 1:2-uranyl-halide-complex holds also true for bromide-induced quenching of uranyl(VI). By adopting specific organic solvents, we were able to suppress the separation of the oxidized halide ligand X-2(center dot-) and the formed uranyl(V) into fully solvated ions, thereby "reigniting" U(VI) luminescence. Time-dependent density functional theory calculations show that quenching occurs through the outer-sphere complex of U(VI) and halide in water, while the ligand-to-metal charge transfer is strongly reduced in acetonitrile.},
language = {en}
}
@article{PhamQuanMeietal.2022,
author = {Pham, Duong Tung and Quan, Ting and Mei, Shilin and Lu, Yan},
title = {Colloidal metal sulfide nanoparticles for high performance electrochemical energy storage systems},
series = {Current opinion in green and sustainable chemistry},
volume = {34},
journal = {Current opinion in green and sustainable chemistry},
publisher = {Elsevier},
address = {Amsterdam},
issn = {2452-2236},
doi = {10.1016/j.cogsc.2022.100596},
pages = {11},
year = {2022},
abstract = {Transition metal sulfides have emerged as excellent replacement candidates of traditional insertion electrode materials based on their conversion or alloying mechanisms, facilitating high specific capacity and rate ability. However, parasitic reactions such as massive volume change during the discharge/ charge processes, intermediate polysulfide dissolution, and passivating solid electrolyte interface formation have led to poor cyclability, hindering their feasibility and applicability in energy storage systems. Colloidal metal sulfide nanoparticles, a special class that integrates the intrinsic chemical properties of metal sulfides and their specified structural features, have fairly enlarged their contribution due to the synergistic effect. This review highlights the latest synthetic approaches based on colloidal process. Their corresponding electrochemical outcomes will also be discussed, which are thoroughly updated along with their insight scientific standpoints.},
language = {en}
}
@article{ReitenbachGeigerWangetal.2023,
author = {Reitenbach, Julija and Geiger, Christina and Wang, Peixi and Vagias, Apostolos N. and Cubitt, Robert and Schanzenbach, Dirk and Laschewsky, Andr{\´e} and Papadakis, Christine M. and M{\"u}ller-Buschbaum, Peter},
title = {Effect of magnesium salts with chaotropic anions on the swelling behavior of PNIPMAM thin films},
series = {Macromolecules : a publication of the American Chemical Society},
volume = {56},
journal = {Macromolecules : a publication of the American Chemical Society},
number = {2},
publisher = {American Chemical Society},
address = {Washington},
issn = {0024-9297},
doi = {10.1021/acs.macromol.2c02282},
pages = {567 -- 577},
year = {2023},
abstract = {Poly(N-isopropylmethacrylamide) (PNIPMAM) is a stimuli responsive polymer, which in thin film geometry exhibits a volume-phase transition upon temperature increase in water vapor. The swelling behavior of PNIPMAM thin films containing magnesium salts in water vapor is investigated in view of their potential application as nanodevices. Both the extent and the kinetics of the swelling ratio as well as the water content are probed with in situ time-of-flight neutron reflectometry. Additionally, in situ Fourier-transform infrared (FTIR) spectroscopy provides information about the local solvation of the specific functional groups, while two-dimensional FTIR correlation analysis further elucidates the temporal sequence of solvation events. The addition of Mg(ClO4)2 or Mg(NO3)2 enhances the sensitivity of the polymer and therefore the responsiveness of switches and sensors based on PNIPMAM thin films. It is found that Mg(NO3)2 leads to a higher relative water uptake and therefore achieves the highest thickness gain in the swollen state.},
language = {en}
}
@inproceedings{BreternitzSchorr2021,
author = {Breternitz, Joachim and Schorr, Susan},
title = {Halide perovskites},
series = {Acta crystallographica / International Union of Crystallography. Section A, Foundations and advances},
volume = {77},
booktitle = {Acta crystallographica / International Union of Crystallography. Section A, Foundations and advances},
number = {Suppl.},
publisher = {Blackwell},
address = {Oxford [u.a.]},
issn = {2053-2733},
pages = {C750 -- C750},
year = {2021},
language = {en}
}
@article{NchiozemNgnitedemSperlichMatietaetal.2023,
author = {Nchiozem-Ngnitedem, Vaderament-Alexe and Sperlich, Eric and Matieta, Valaire Yemene and Kuete, Jenifer Reine Ngnouzouba and Kuete, Victor and Omer, Ejlal A. A. and Efferth, Thomas and Schmidt, Bernd},
title = {Synthesis and bioactivity of isoflavones from ficus carica and some non-natural analogues},
series = {Journal of natural products : Lloydia},
volume = {86},
journal = {Journal of natural products : Lloydia},
number = {6},
publisher = {American Chemical Society},
address = {Washington, DC},
issn = {0163-3864},
doi = {10.1021/acs.jnatprod.3c00219},
pages = {1520 -- 1528},
year = {2023},
abstract = {FicucariconeD (1) and its 4 '-demethyl congener 2 are isoflavones isolated from fruits of Ficus carica that share a 5,7-dimethoxy-6-prenyl-substituted A-ring. Both naturalproducts were, for the first time, obtained by chemical synthesisin six steps, starting from 2,4,6-trihydroxyacetophenone. Key stepsare a microwave-promoted tandem sequence of Claisen- and Cope-rearrangementsto install the 6-prenyl substituent and a Suzuki-Miyaura crosscoupling for installing the B-ring. By using various boronic acids,non-natural analogues become conveniently available. All compoundswere tested for cytotoxicity against drug-sensitive and drug-resistanthuman leukemia cell lines, but were found to be inactive. The compoundswere also tested for antimicrobial activities against a panel of eightGram-negative and two Gram-positive bacterial strains. Addition ofthe efflux pump inhibitor phenylalanine-arginine-beta-naphthylamide(PA beta N) significantly improved the antibiotic activity in mostcases, with MIC values as low as 2.5 mu M and activity improvementfactors as high as 128-fold.},
language = {en}
}
@article{GeigerReitenbachHenscheletal.2021,
author = {Geiger, Christina and Reitenbach, Julija and Henschel, Cristiane and Kreuzer, Lucas and Widmann, Tobias and Wang, Peixi and Mangiapia, Gaetano and Moulin, Jean-Fran{\c{c}}ois and Papadakis, Christine M. and Laschewsky, Andr{\´e} and M{\"u}ller-Buschbaum, Peter},
title = {Ternary nanoswitches realized with multiresponsive PMMA-b-PNIPMAM films in mixed water/acetone vapor atmospheres},
series = {Advanced engineering materials},
volume = {23},
journal = {Advanced engineering materials},
number = {11},
publisher = {Wiley-VCH},
address = {Weinheim},
issn = {1438-1656},
doi = {10.1002/adem.202100191},
pages = {12},
year = {2021},
abstract = {To systematically add functionality to nanoscale polymer switches, an understanding of their responsive behavior is crucial. Herein, solvent vapor stimuli are applied to thin films of a diblock copolymer consisting of a short poly(methyl methacrylate) (PMMA) block and a long poly(N-isopropylmethacrylamide) (PNIPMAM) block for realizing ternary nanoswitches. Three significantly distinct film states are successfully implemented by the combination of amphiphilicity and co-nonsolvency effect. The exposure of the thin films to nitrogen, pure water vapor, and mixed water/acetone (90 vol\%/10 vol\%) vapor switches the films from a dried to a hydrated (solvated and swollen) and a water/acetone-exchanged (solvated and contracted) equilibrium state. These three states have distinctly different film thicknesses and solvent contents, which act as switch positions "off," "on," and "standby." For understanding the switching process, time-of-flight neutron reflectometry (ToF-NR) and spectral reflectance (SR) studies of the swelling and dehydration process are complemented by information on the local solvation of functional groups probed with Fourier-transform infrared (FTIR) spectroscopy. An accelerated responsive behavior beyond a minimum hydration/solvation level is attributed to the fast build-up and depletion of the hydration shell of PNIPMAM, caused by its hydrophobic moieties promoting a cooperative hydration character.},
language = {en}
}
@article{MelaniNagataSaalfrank2021,
author = {Melani, Giacomo and Nagata, Yuki and Saalfrank, Peter},
title = {Vibrational energy relaxation of interfacial OH on a water-covered alpha-Al2O3(0001) surface},
series = {Physical chemistry, chemical physics : PCCP ; a journal of European chemical societies},
volume = {23},
journal = {Physical chemistry, chemical physics : PCCP ; a journal of European chemical societies},
number = {13},
publisher = {Royal Society of Chemistry},
address = {Cambridge},
issn = {1463-9076},
doi = {10.1039/d0cp03777j},
pages = {7714 -- 7723},
year = {2021},
abstract = {Vibrational relaxation of adsorbates is a sensitive tool to probe energy transfer at gas/solid and liquid/solid interfaces. The most direct way to study relaxation dynamics uses time-resolved spectroscopy. Here we report on a non-equilibrium ab initio molecular dynamics (NE-AIMD) methodology to model vibrational relaxation of OH vibrations on a hydroxylated, water-covered alpha-Al2O3(0001) surface. In our NE-AIMD approach, after exciting selected O-H bonds their coupling to surface phonons and to the water adlayer is analyzed in detail, by following both the energy flow in time, as well as the time-evolution of Vibrational Density of States (VDOS) curves. The latter are obtained from Time-dependent Correlation Functions (TCFs) and serve as prototypical, generic representatives of time-resolved vibrational spectra. As most important results, (i) we find a few-picosecond lifetime of the excited modes and (ii) identify both hydrogen-bonded aluminols and water molecules in the adsorbed water layer as main dissipative channels, while the direct coupling to Al2O3 surface phonons is of minor importance on the timescales of interest. Our NE-AIMD/TCF methodology is powerful for complex adsorbate systems, in principle even reacting ones, and opens a way towards time-resolved vibrational spectroscopy.},
language = {en}
}
@article{WangFritschBerendtsetal.2021,
author = {Wang, Zhenyu and Fritsch, Daniel and Berendts, Stefan and Lerch, Martin and Breternitz, Joachim and Schorr, Susan},
title = {Elucidation of the reaction mechanism for the synthesis of ZnGeN2 through Zn2GeO4 ammonolysis},
series = {Chemical science / RSC, Royal Society of Chemistry},
volume = {12},
journal = {Chemical science / RSC, Royal Society of Chemistry},
number = {24},
publisher = {Royal Society of Chemistry},
address = {Cambridge},
issn = {2041-6539},
doi = {10.1039/d1sc00328c},
pages = {8493 -- 8500},
year = {2021},
abstract = {Ternary II-IV-N-2 materials have been considered as a promising class of materials that combine photovoltaic performance with earth-abundance and low toxicity. When switching from binary III-V materials to ternary II-IV-N-2 materials, further structural complexity is added to the system that may influence its optoelectronic properties. Herein, we present a systematic study of the reaction of Zn2GeO4 with NH3 that produces zinc germanium oxide nitrides, and ultimately approach stoichiometric ZnGeN2, using a combination of chemical analyses, X-ray powder diffraction and DFT calculations. Elucidating the reaction mechanism as being dominated by Zn and O extrusion at the later reaction stages, we give an insight into studying structure-property relationships in this emerging class of materials.},
language = {en}
}
@article{SaeediGarakaniXieKhorsandKheirabadetal.2021,
author = {Saeedi Garakani, Sadaf and Xie, Dongjiu and Khorsand Kheirabad, Atefeh and Lu, Yan and Yuan, Jiayin},
title = {Template-synthesis of a poly(ionic liquid)-derived Fe1-xS/nitrogen-doped porous carbon membrane and its electrode application in lithium-sulfur batteries},
series = {Materials advances},
volume = {2},
journal = {Materials advances},
number = {15},
publisher = {Royal Society of Chemistry},
address = {Cambridge},
issn = {2633-5409},
doi = {10.1039/d1ma00441g},
pages = {5203 -- 5212},
year = {2021},
abstract = {This study deals with the facile synthesis of Fe1-xS nanoparticle-containing nitrogen-doped porous carbon membranes (denoted as Fe1-xS/N-PCMs) via vacuum carbonization of hybrid porous poly(ionic liquid) (PIL) membranes, and their successful use as a sulfur host material to mitigate the shuttle effect in lithium-sulfur (Li-S) batteries. The hybrid porous PIL membranes as the sacrificial template were prepared via ionic crosslinking of a cationic PIL with base-neutralized 1,1 '-ferrocenedicarboxylic acid, so that the iron source was molecularly incorporated into the template. The carbonization process was investigated in detail at different temperatures, and the chemical and porous structures of the carbon products were comprehensively analyzed. The Fe1-xS/N-PCMs prepared at 900 degrees C have a multimodal pore size distribution with a satisfactorily high surface area and well-dispersed iron sulfide nanoparticles to physically and chemically confine the LiPSs. The sulfur/Fe1-xS/N-PCM composites were then tested as electrodes in Li-S batteries, showing much improved capacity, rate performance and cycle stability, in comparison to iron sulfide-free, nitrogen-doped porous carbon membranes.},
language = {en}
}
@article{XuNieWangetal.2021,
author = {Xu, Xun and Nie, Yan and Wang, Weiwei and Ma, Nan and Lendlein, Andreas},
title = {Periodic thermomechanical modulation of toll-like receptor expression and distribution in mesenchymal stromal cells},
series = {MRS communications / a publication of the Materials Research Society},
volume = {11},
journal = {MRS communications / a publication of the Materials Research Society},
number = {4},
publisher = {Springer},
address = {Berlin},
issn = {2159-6859},
doi = {10.1557/s43579-021-00049-5},
pages = {425 -- 431},
year = {2021},
abstract = {Toll-like receptor (TLR) can trigger an immune response against virus including SARS-CoV-2. TLR expression/distribution is varying in mesenchymal stromal cells (MSCs) depending on their culture environments. Here, to explore the effect of periodic thermomechanical cues on TLRs, thermally controlled shape-memory polymer sheets with programmable actuation capacity were created. The proportion of MSCs expressing SARS-CoV-2-associated TLRs was increased upon stimulation. The TLR4/7 colocalization was promoted and retained in the endoplasmic reticula. The TLR redistribution was driven by myosin-mediated F-actin assembly. These results highlight the potential of boosting the immunity for combating COVID-19 via thermomechanical preconditioning of MSCs.},
language = {en}
}
@article{SchulzeKoetz2017,
author = {Schulze, Nicole and Koetz, Joachim},
title = {Kinetically controlled growth of gold nanotriangles in a vesicular template phase by adding a strongly alternating polyampholyte},
series = {Journal of dispersion science and technology},
volume = {38},
journal = {Journal of dispersion science and technology},
number = {8},
publisher = {Taylor \& Francis},
address = {Philadelphia},
issn = {0193-2691},
doi = {10.1080/01932691.2016.1220318},
pages = {1073 -- 1078},
year = {2017},
abstract = {This paper is focused on the temperature-dependent synthesis of gold nanotriangles in a vesicular template phase, containing phosphatidylcholine and AOT, by adding the strongly alternating polyampholyte PalPhBisCarb. UV-vis absorption spectra in combination with TEM micrographs show that flat gold nanoplatelets are formed predominantly in the presence of the polyampholyte at 45°C. The formation of triangular and hexagonal nanoplatelets can be directly influenced by the kinetic approach, i.e., by varying the polyampholyte dosage rate at 45°C. Corresponding zeta potential measurements indicate that a temperature-dependent adsorption of the polyampholyte on the {111} faces will induce the symmetry breaking effect, which is responsible for the kinetically controlled hindered vertical and preferred lateral growth of the nanoplatelets.},
language = {en}
}
@phdthesis{Margraf2023,
author = {Margraf, Johannes T.},
title = {Science-driven chemical machine learning},
school = {Universit{\"a}t Potsdam},
pages = {413},
year = {2023},
language = {en}
}
@article{DengWangXuetal.2021,
author = {Deng, Zijun and Wang, Weiwei and Xu, Xun and Ma, Nan and Lendlein, Andreas},
title = {Polydopamine-based biofunctional substrate coating promotes mesenchymal stem cell migration},
series = {MRS advances : a journal of the Materials Research Society (MRS)},
volume = {6},
journal = {MRS advances : a journal of the Materials Research Society (MRS)},
number = {31},
publisher = {Springer Nature Switzerland AG},
address = {Cham},
issn = {2059-8521},
doi = {10.1557/s43580-021-00091-4},
pages = {739 -- 744},
year = {2021},
abstract = {Rapid migration of mesenchymal stem cells (MSCs) on device surfaces could support in vivo tissue integration and might facilitate in vitro organoid formation. Here, polydopamine (PDA) is explored as a biofunctional coating to effectively promote MSC motility. It is hypothesized that PDA stimulates fibronectin deposition and in this way enhances integrin-mediated migration capability. The random and directional cell migration was investigated by time-lapse microscopy and gap closure assay respectively, and analysed with softwares as computational tools. A higher amount of deposited fibronectin was observed on PDA substrate, compared to the non-coated substrate. The integrin beta 1 activation and focal adhesion kinase (FAK) phosphorylation at Y397 were enhanced on PDA substrate, but the F-actin cytoskeleton was not altered, suggesting MSC migration on PDA was regulated by integrin initiated FAK signalling. This study strengthens the biofunctionality of PDA coating for regulating stem cells and offering a way of facilitating tissue integration of devices.},
language = {en}
}
@article{MachatschekSaretiaLendlein2021,
author = {Machatschek, Rainhard Gabriel and Saretia, Shivam and Lendlein, Andreas},
title = {Assessing the influence of temperature-memory creation on the degradation of copolyesterurethanes in ultrathin films},
series = {Advanced materials interfaces},
volume = {8},
journal = {Advanced materials interfaces},
number = {6},
publisher = {Wiley-VCH},
address = {Weinheim},
issn = {2196-7350},
doi = {10.1002/admi.202001926},
pages = {8},
year = {2021},
abstract = {Copolyesterurethanes (PDLCLs) based on oligo(epsilon-caprolactone) (OCL) and oligo(omega-pentadecalactone) (OPDL) segments are biodegradable thermoplastic temperature-memory polymers. The temperature-memory capability in these polymers with crystallizable control units is implemented by a thermomechanical programming process causing alterations in the crystallite arrangement and chain organization. These morphological changes can potentially affect degradation. Initial observations on the macroscopic level inspire the hypothesis that switching of the controlling units causes an accelerated degradation of the material, resulting in programmable degradation by sequential coupling of functions. Hence, detailed degradation studies on Langmuir films of a PDLCL with 40 wt\% OPDL content are carried out under enzymatic catalysis. The temperature-memory creation procedure is mimicked by compression at different temperatures. The evolution of the chain organization and mechanical properties during the degradation process is investigated by means of polarization-modulated infrared reflection absorption spectroscopy, interfacial rheology and to some extend by X-ray reflectivity. The experiments on PDLCL Langmuir films imply that degradability is not enhanced by thermal switching, as the former depends on the temperature during cold programming. Nevertheless, the thin film experiments show that the leaching of OCL segments does not induce further crystallization of the OPDL segments, which is beneficial for a controlled and predictable degradation.},
language = {en}
}
@article{SperlichKoeckerling2023,
author = {Sperlich, Eric and K{\"o}ckerling, Martin},
title = {The double cluster compound [Nb6Cl14(MeCN)(4)] [Nb6Cl14(pyz)(4)].6MeCN (Me: methyl, pyz: pyrazine) with a layered structure resulting from weak intermolecular interactions},
series = {Zeitschrift f{\"u}r Naturforschung},
volume = {78},
journal = {Zeitschrift f{\"u}r Naturforschung},
number = {5},
publisher = {De Gruyter},
address = {Berlin},
issn = {0932-0776},
doi = {10.1515/znb-2023-0001},
pages = {279 -- 283},
year = {2023},
abstract = {The synthesis and the crystal structure of the double cluster compound [Nb6Cl14(MeCN)(4)][Nb6Cl14(pyz)(4)]middot6CH(3)CN are described. The synthesis is based on a partial ligand exchange reaction, which proceeds upon dissolving [Nb6Cl14(pyz)(4)]middot2CH(2)Cl(2) in acetonitrile. The compound is built up of two discrete neutral cluster units, which consist of octahedra of Nb-6 atoms coordinated by 12 edge-bridging chlorido and two terminal chlorido ligands, and four acetonitrile ligands on one and four pyrazine ligands on the other cluster unit. Co-crystallized acetonitrile molecules are also present. The single-crystal structure determination has revealed a cluster arrangement in which the [Nb6Cl14(pyz)(4)] units are connected by (halogen) lone-pair-(pyrazine) pi interactions. These lead to chains of [Nb6Cl14(pyz)(4)] clusters. These chains are further connected to cluster layers by (nitrile-halogen) dipole-dipole interactions, in which the [Nb6Cl14(MeCN)(4)] and co-crystallized MeCN molecules are also involved. These cluster layers are arranged parallel to the crystallographic {011} plane.},
language = {en}
}
@article{KreuzerWidmannGeigeretal.2021,
author = {Kreuzer, Lucas and Widmann, Tobias and Geiger, Christina and Wang, Peixi and Vagias, Apostolos N. and Heger, Julian Eliah and Haese, Martin and Hildebrand, Viet and Laschewsky, Andr{\´e} and Papadakis, Christine M. and M{\"u}ller-Buschbaum, Peter},
title = {Salt-dependent phase transition behavior of doubly thermoresponsive poly(sulfobetaine)-based diblock copolymer thin films},
series = {Langmuir : the ACS journal of surfaces and colloids / American Chemical Society},
volume = {37},
journal = {Langmuir : the ACS journal of surfaces and colloids / American Chemical Society},
number = {30},
publisher = {American Chemical Society},
address = {Washington},
issn = {0743-7463},
doi = {10.1021/acs.langmuir.1c01342},
pages = {9179 -- 9191},
year = {2021},
abstract = {The water vapor-induced swelling, as well as subsequent phase-transition kinetics, of thin films of a diblock copolymer (DBC) loaded with different amounts of the salt NaBr, is investigated in situ. In dilute aqueous solution, the DBC features an orthogonally thermoresponsive behavior. It consists of a zwitterionic poly(sulfobetaine) block, namely, poly(4-(N-(3'-methacrylamidopropyl)-N, N-dimethylammonio) butane-1-sulfonate) (PSBP), showing an upper critical solution temperature, and a nonionic block, namely, poly(N-isopropylmethacrylamide) (PNIPMAM), exhibiting a lower critical solution temperature. The swelling kinetics in D2O vapor at 15 degrees C and the phase transition kinetics upon heating the swollen film to 60 degrees C and cooling back to 15 degrees C are followed with simultaneous time-of-flight neutron reflectometry and spectral reflectance measurements. These are complemented by Fourier transform infrared spectroscopy. The collapse temperature of PNIPMAM and the swelling temperature of PSBP are found at lower temperatures than in aqueous solution, which is attributed to the high polymer concentration in the thin-film geometry. Upon inclusion of sub-stoichiometric amounts (relative to the monomer units) of NaBr in the films, the water incorporation is significantly increased. This increase is mainly attributed to a salting-in effect on the zwitterionic PSBP block. Whereas the addition of NaBr notably shifts the swelling temperature of PSBP to lower temperatures, the collapse temperature of PNIPMAM remains unaffected by the presence of salt in the films.},
language = {en}
}
@article{PessanhaPaschoalinoDerocoetal.2022,
author = {Pessanha, Tatiana and Paschoalino, Waldemir J. and Deroco, Patricia B. and Kogikoski Junior, Sergio and Moraes, Ana C. M. de and Carvalho Castro de Silva, Cecilia de and Kubota, Lauro T.},
title = {Interfacial capacitance of graphene oxide films electrodes},
series = {Electroanalysis : an internatinal journal devoted to electroanalysis, sensors and bioelectronic devices},
volume = {34},
journal = {Electroanalysis : an internatinal journal devoted to electroanalysis, sensors and bioelectronic devices},
number = {4},
publisher = {Wiley-VCH},
address = {Weinheim},
issn = {1521-4109},
doi = {10.1002/elan.202100220},
pages = {692 -- 700},
year = {2022},
abstract = {The understanding of bidimensional materials dynamics and its electrolyte interface equilibrium, such as graphene oxide (GO), is critical for the development of a capacitive biosensing platform. The interfacial capacitance (C-i) of graphene-based materials may be tuned by experimental conditions such as pH optimization and cation size playing key roles at the enhancement of their capacitive properties allowing their application as novel capacitive biosensors. Here we reported a systematic study of C-i of multilayer GO films in different aqueous electrolytes employing electrochemical impedance spectroscopy for the application in a capacitive detection system. We demonstrated that the presence of ionizable oxygen-containing functional groups within multilayer GO film favors the interactions and the accumulation of cations in the structure of the electrodes enhancing the GO C-i in aqueous solutions, where at pH 7.0 (the best condition) the C-i was 340 mu F mg(-1) at -0.01 V vs Ag/AgCl. We also established that the hydrated cation radius affects the mobility and interaction with GO functional groups and it plays a critical role in the Ci, as demonstrated in the presence of different cations Na+=640 mu F mg(-1), Li+=575 mu F mg(-1) and TMA(+)=477 mu F mg(-1). As a proof-of-concept, the capacitive behaviour of GO was explored as biosensing platform for standard streptavidin-biotin systems. For this system, the C-i varied linearly with the log of the concentration of the targeting analyte in the range from 10 pg mL(-1) to 100 ng mL(-1), showing the promising applicability of capacitive GO based sensors for label-free biosensing.},
language = {en}
}
@phdthesis{Savatieiev2023,
author = {Savatieiev, Oleksandr},
title = {Carbon nitride semiconductors: properties and application as photocatalysts in organic synthesis},
school = {Universit{\"a}t Potsdam},
pages = {272},
year = {2023},
abstract = {Graphitic carbon nitrides (g-CNs) are represented by melon-type g-CN, poly(heptazine imides) (PHIs), triazine-based g-CN and poly(triazine imide) with intercalated LiCl (PTI/Li+Cl‒). These materials are composed of sp2-hybridized carbon and nitrogen atoms; C:N ratio is close to 3:4; the building unit is 1,3,5-triazine or tri-s-triazine; the building units are interconnected covalently via sp2-hybridized nitrogen atoms or NH-moieties; the layers are assembled into a stack via weak van der Waals forces as in graphite. Due to medium band gap (~2.7 eV) g-CNs, such as melon-type g-CN and PHIs, are excited by photons with wavelength ≤ 460 nm. Since 2009 g-CNs have been actively studied as photocatalysts in evolution of hydrogen and oxygen - two half-reactions of full water splitting, by employing corresponding sacrificial agents. At the same time application of g-CNs as photocatalysts in organic synthesis has been remaining limited to few reactions only. Cumulative Habilitation summarizes research work conducted by the group 'Innovative Heterogeneous Photocatalysis' between 2017-2023 in the field of carbon nitride organic photocatalysis, which is led by Dr. Oleksandr Savatieiev. g-CN photocatalysts activate molecules, i.e. generate their more reactive open-shell intermediates, via three modes: i) Photoinduced electron transfer (PET); ii) Excited state proton-coupled electron transfer (ES-PCET) or direct hydrogen atom transfer (dHAT); iii) Energy transfer (EnT). The scope of reactions that proceed via oxidative PET, i.e. one-electron oxidation of a substrate to the corresponding radical cation, are represented by synthesis of sulfonylchlorides from S-acetylthiophenols. The scope of reactions that proceed via reductive PET, i.e. one-electron reduction of a substrate to the corresponding radical anion, are represented by synthesis of γ,γ-dichloroketones from the enones and chloroform. Due to abundance of sp2-hybridized nitrogen atoms in the structure of g-CN materials, they are able to cleave X-H bonds in organic molecules and store temporary hydrogen atom. ES-PCET or dHAT mode of organic molecules activation to the corresponding radicals is implemented for substrates featuring relatively acidic X-H bonds and those that are characterized by low bond dissociation energy, such as C-H bond next to the heteroelements. On the other hand, reductively quenched g-CN carrying hydrogen atom reduces a carbonyl compound to the ketyl radical via PCET that is thermodynamically more favorable pathway compared to the electron transfer. The scope of these reactions is represented by cyclodimerization of α,β-unsaturated ketones to cyclopentanoles. g-CN excited state demonstrates complex dynamics with the initial formation of singlet excited state, which upon intersystem crossing produces triplet excited state that is characterized by the lifetime > 2 μs. Due to long lifetime, g-CN activate organic molecules via EnT. For example, g-CN sensitizes singlet oxygen, which is the key intermediate in the dehydrogenation of aldoximes to nitrileoxides. The transient nitrileoxide undergoes [3+2]-cycloaddition to nitriles and gives oxadiazoles-1,2,4. PET, ES-PCET and EnT are fundamental phenomena that are applied beyond organic photocatalysis. Hybrid composite is formed by combining conductive polymers, such as poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) with potassium poly(heptazine imide) (K-PHI). Upon PET, K-PHI modulated population of polarons and therefore conductivity of PEDOT:PSS. The initial state of PEDOT:PSS is recovered upon material exposure to O2. K-PHI:PEDOT:PSS may be applied in O2 sensing. In the presence of electron donors, such as tertiary amines and alcohols, and irradiation with light, K-PHI undergoes photocharging - the g-CN material accumulates electrons and charge-compensating cations. Such photocharged state is stable under anaerobic conditions for weeks, but at the same time it is a strong reductant. This feature allows decoupling in time light harvesting and energy storage in the form of electron-proton couples from utilization in organic synthesis. The photocharged state of K-PHI reduces nitrobenzene to aniline, and enables dimerization of α,β-unsaturated ketones to hexadienones in dark.},
language = {en}
}
@misc{HechenbichlerLaschewskyGradzielski2020,
author = {Hechenbichler, Michelle and Laschewsky, Andre and Gradzielski, Michael},
title = {Poly(N,N-bis(2-methoxyethyl)acrylamide), a thermoresponsive non-ionic polymer combining the amide and the ethyleneglycolether motifs},
series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
volume = {299},
journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
number = {2},
publisher = {Springer},
address = {Berlin; Heidelberg},
issn = {0303-402X},
doi = {10.25932/publishup-59837},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-598378},
pages = {17},
year = {2020},
abstract = {Poly(N,N-bis(2-methoxyethyl)acrylamide) (PbMOEAm) featuring two classical chemical motifs from non-ionic water-soluble polymers, namely, the amide and ethyleneglycolether moieties, was synthesized by reversible addition fragmentation transfer (RAFT) polymerization. This tertiary polyacrylamide is thermoresponsive exhibiting a lower critical solution temperature (LCST)-type phase transition. A series of homo- and block copolymers with varying molar masses but low dispersities and different end groups were prepared. Their thermoresponsive behavior in aqueous solution was analyzed via turbidimetry and dynamic light scattering (DLS). The cloud points (CP) increased with increasing molar masses, converging to 46 degrees C for 1 wt\% solutions. This rise is attributed to the polymers' hydrophobic end groups incorporated via the RAFT agents. When a surfactant-like strongly hydrophobic end group was attached using a functional RAFT agent, CP was lowered to 42 degrees C, i.e., closer to human body temperature. Also, the effect of added salts, in particular, the role of the Hofmeister series, on the phase transition of PbMOEAm was investigated, exemplified for the kosmotropic fluoride, intermediate chloride, and chaotropic thiocyanate anions. A pronounced shift of the cloud point of about 10 degrees C to lower or higher temperatures was observed for 0.2 M fluoride and thiocyanate, respectively. When PbMOEAm was attached to a long hydrophilic block of poly(N,N-dimethylacrylamide) (PDMAm), the cloud points of these block copolymers were strongly shifted towards higher temperatures. While no phase transition was observed for PDMAm-b-pbMOEAm with short thermoresponsive blocks, block copolymers with about equally sized PbMOEAm and PDMAm blocks underwent the coil-to-globule transition around 60 degrees C.},
language = {en}
}
@phdthesis{Hussein2024,
author = {Hussein, Mahmoud},
title = {Solvent engineering for highly-efficiency lead-free perovskite solar cells},
doi = {10.25932/publishup-63037},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-630375},
school = {Universit{\"a}t Potsdam},
pages = {137},
year = {2024},
abstract = {Global warming, driven primarily by the excessive emission of greenhouse gases such as carbon dioxide into the atmosphere, has led to severe and detrimental environmental impacts. Rising global temperatures have triggered a cascade of adverse effects, including melting glaciers and polar ice caps, more frequent and intense heat waves disrupted weather patterns, and the acidification of oceans. These changes adversely affect ecosystems, biodiversity, and human societies, threatening food security, water availability, and livelihoods. One promising solution to mitigate the harmful effects of global warming is the widespread adoption of solar cells, also known as photovoltaic cells. Solar cells harness sunlight to generate electricity without emitting greenhouse gases or other pollutants. By replacing fossil fuel-based energy sources, solar cells can significantly reduce CO2 emissions, a significant contributor to global warming. This transition to clean, renewable energy can help curb the increasing concentration of greenhouse gases in the atmosphere, thereby slowing down the rate of global temperature rise. Solar energy's positive impact extends beyond emission reduction. As solar panels become more efficient and affordable, they empower individuals, communities, and even entire nations to generate electricity and become less dependent on fossil fuels. This decentralized energy generation can enhance resilience in the face of climate-related challenges. Moreover, implementing solar cells creates green jobs and stimulates technological innovation, further promoting sustainable economic growth. As solar technology advances, its integration with energy storage systems and smart grids can ensure a stable and reliable energy supply, reducing the need for backup fossil fuel power plants that exacerbate environmental degradation. The market-dominant solar cell technology is silicon-based, highly matured technology with a highly systematic production procedure. However, it suffers from several drawbacks, such as: 1) Cost: still relatively high due to high energy consumption due to the need to melt and purify silicon, and the use of silver as an electrode, which hinders their widespread availability, especially in low-income countries. 2) Efficiency: theoretically, it should deliver around 29\%; however, the efficiency of most of the commercially available silicon-based solar cells ranges from 18 - 22\%. 3) Temperature sensitivity: The efficiency decreases with the increase in the temperature, affecting their output. 4) Resource constraints: silicon as a raw material is unavailable in all countries, creating supply chain challenges. Perovskite solar cells arose in 2011 and matured very rapidly in the last decade as a highly efficient and versatile solar cell technology. With an efficiency of 26\%, high absorption coefficients, solution processability, and tunable band gap, it attracted the attention of the solar cells community. It represented a hope for cheap, efficient, and easily processable next-generation solar cells. However, lead toxicity might be the block stone hindering perovskite solar cells' market reach. Lead is a heavy and bioavailable element that makes perovskite solar cells environmentally unfriendly technology. As a result, scientists try to replace lead with a more environmentally friendly element. Among several possible alternatives, tin was the most suitable element due to its electronic and atomic structure similarity to lead. Tin perovskites were developed to alleviate the challenge of lead toxicity. Theoretically, it shows very high absorption coefficients, an optimum band gap of 1.35 eV for FASnI3, and a very high short circuit current, which nominates it to deliver the highest possible efficiency of a single junction solar cell, which is around 30.1\% according to Schockly-Quisser limit. However, tin perovskites' efficiency still lags below 15\% and is irreproducible, especially from lab to lab. This humble performance could be attributed to three reasons: 1) Tin (II) oxidation to tin (IV), which would happen due to oxygen, water, or even by the effect of the solvent, as was discovered recently. 2) fast crystallization dynamics, which occurs due to the lateral exposure of the P-orbitals of the tin atom, which enhances its reactivity and increases the crystallization pace. 3) Energy band misalignment: The energy bands at the interfaces between the perovskite absorber material and the charge selective layers are not aligned, leading to high interfacial charge recombination, which devastates the photovoltaic performance. To solve these issues, we implemented several techniques and approaches that enhanced the efficiency of tin halide perovskites, providing new chemically safe solvents and antisolvents. In addition, we studied the energy band alignment between the charge transport layers and the tin perovskite absorber. Recent research has shown that the principal source of tin oxidation is the solvent known as dimethylsulfoxide, which also happens to be one of the most effective solvents for processing perovskite. The search for a stable solvent might prove to be the factor that makes all the difference in the stability of tin-based perovskites. We started with a database of over 2,000 solvents and narrowed it down to a series of 12 new solvents that are suitable for processing FASnI3 experimentally. This was accomplished by looking into 1) the solubility of the precursor chemicals FAI and SnI2, 2) the thermal stability of the precursor solution, and 3) the potential to form perovskite. Finally, we show that it is possible to manufacture solar cells using a novel solvent system that outperforms those produced using DMSO. The results of our research give some suggestions that may be used in the search for novel solvents or mixes of solvents that can be used to manufacture stable tin-based perovskites. Due to the quick crystallization of tin, it is more difficult to deposit tin-based perovskite films from a solution than manufacturing lead-based perovskite films since lead perovskite is more often utilized. The most efficient way to get high efficiencies is to deposit perovskite from dimethyl sulfoxide (DMSO), which slows down the quick construction of the tin-iodine network that is responsible for perovskite synthesis. This is the most successful approach for achieving high efficiencies. Dimethyl sulfoxide, which is used in the processing, is responsible for the oxidation of tin, which is a disadvantage of this method. This research presents a potentially fruitful alternative in which 4-(tert-butyl) pyridine can substitute dimethyl sulfoxide in the process of regulating crystallization without causing tin oxidation to take place. Perovskite films that have been formed from pyridine have been shown to have a much-reduced defect density. This has resulted in increased charge mobility and better photovoltaic performance, making pyridine a desirable alternative for use in the deposition of tin perovskite films. The precise control of perovskite precursor crystallization inside a thin film is of utmost importance for optimizing the efficiency and manufacturing of solar cells. The deposition process of tin-based perovskite films from a solution presents difficulties due to the quick crystallization of tin compared to the more often employed lead perovskite. The optimal approach for attaining elevated efficiencies entails using dimethyl sulfoxide (DMSO) as a medium for depositing perovskite. This choice of solvent impedes the tin-iodine network's fast aggregation, which plays a crucial role in the production of perovskite. Nevertheless, this methodology is limited since the utilization of dimethyl sulfoxide leads to the oxidation of tin throughout the processing stage. In this thesis, we present a potentially advantageous alternative approach wherein 4-(tert-butyl) pyridine is proposed as a substitute for dimethyl sulfoxide in regulating crystallization processes while avoiding the undesired consequence of tin oxidation. Films of perovskite formed using pyridine as a solvent have a notably reduced density of defects, resulting in higher mobility of charges and improved performance in solar applications. Consequently, the utilization of pyridine for the deposition of tin perovskite films is considered advantageous. Tin perovskites are suffering from an apparent energy band misalignment. However, the band diagrams published in the current body of research display contradictions, resulting in a dearth of unanimity. Moreover, comprehensive information about the dynamics connected with charge extraction is lacking. This thesis aims to ascertain the energy band locations of tin perovskites by employing the kelvin probe and Photoelectron yield spectroscopy methods. This thesis aims to construct a precise band diagram for the often-utilized device stack. Moreover, a comprehensive analysis is performed to assess the energy deficits inherent in the current energetic structure of tin halide perovskites. In addition, we investigate the influence of BCP on the improvement of electron extraction in C60/BCP systems, with a specific emphasis on the energy factors involved. Furthermore, transient surface photovoltage was utilized to investigate the charge extraction kinetics of frequently studied charge transport layers, such as NiOx and PEDOT as hole transport layers and C60, ICBA, and PCBM as electron transport layers. The Hall effect, KP, and TRPL approaches accurately ascertain the p-doping concentration in FASnI3. The results consistently demonstrated a value of 1.5 * 1017 cm-3. Our research findings highlight the imperative nature of autonomously constructing the charge extraction layers for tin halide perovskites, apart from those used for lead perovskites. The crystallization of perovskite precursors relies mainly on the utilization of two solvents. The first one dissolves the perovskite powder to form the precursor solution, usually called the solvent. The second one precipitates the perovskite precursor, forming the wet film, which is a supersaturated solution of perovskite precursor and in the remains of the solvent and the antisolvent. Later, this wet film crystallizes upon annealing into a full perovskite crystallized film. In our research context, we proposed new solvents to dissolve FASnI3, but when we tried to form a film, most of them did not crystallize. This is attributed to the high coordination strength between the metal halide and the solvent molecules, which is unbreakable by the traditionally used antisolvents such as Toluene and Chlorobenzene. To solve this issue, we introduce a high-throughput antisolvent screening in which we screened around 73 selected antisolvents against 15 solvents that can form a 1M FASnI3 solution. We used for the first time in tin perovskites machine learning algorithm to understand and predict the effect of an antisolvent on the crystallization of a precursor solution in a particular solvent. We relied on film darkness as a primary criterion to judge the efficacy of a solvent-antisolvent pair. We found that the relative polarity between solvent and antisolvent is the primary factor that affects the solvent-antisolvent interaction. Based on our findings, we prepared several high-quality tin perovskite films free from DMSO and achieved an efficiency of 9\%, which is the highest DMSO tin perovskite device so far.},
language = {en}
}
@article{WangGeigerKreuzeretal.2022,
author = {Wang, Peixi and Geiger, Christina and Kreuzer, Lucas and Widmann, Tobias and Reitenbach, Julija and Liang, Suzhe and Cubitt, Robert and Henschel, Cristiane and Laschewsky, Andr{\´e} and Papadakis, Christine M. and M{\"u}ller-Buschbaum, Peter},
title = {Poly(sulfobetaine)-based diblock copolymer thin films in water/acetone atmosphere: modulation of water hydration and co-nonsolvency-triggered film contraction},
series = {Langmuir : the ACS journal of surfaces and colloids},
volume = {38},
journal = {Langmuir : the ACS journal of surfaces and colloids},
number = {22},
publisher = {American Chemical Society},
address = {Washington},
issn = {0743-7463},
doi = {10.1021/acs.langmuir.2c00451},
pages = {6934 -- 6948},
year = {2022},
abstract = {The water swelling and subsequent solvent exchange including co-nonsolvency behavior of thin films of a doubly thermo-responsive diblock copolymer (DBC) are studied viaspectral reflectance, time-of-flight neutron reflectometry, and Fourier transform infrared spectroscopy. The DBC consists of a thermo-responsive zwitterionic (poly(4-((3-methacrylamidopropyl) dimethylammonio) butane-1-sulfonate)) (PSBP) block, featuring an upper critical solution temperature transition in aqueous media but being insoluble in acetone, and a nonionic poly(N-isopropylmethacrylamide) (PNIPMAM) block, featuring a lower critical solution temperature transition in water, while being soluble in acetone. Homogeneous DBC films of 50-100 nm thickness are first swollen in saturated water vapor (H2OorD2O), before they are subjected to a contraction process by exposure to mixed saturated water/acetone vapor (H2OorD2O/acetone-d6 = 9:1 v/v). The affinity of the DBC film toward H2O is stronger than for D2O, as inferred from the higher film thickness in the swollen state and the higher absorbed water content, thus revealing a pronounced isotope sensitivity. During the co-solvent-induced switching by mixed water/acetone vapor, a two-step film contraction is observed, which is attributed to the delayed expulsion of water molecules and uptake of acetone molecules. The swelling kinetics are compared for both mixed vapors (H2O/acetone-d6 and D2O/acetone-d6) and with those of the related homopolymer films. Moreover, the concomitant variations of the local environment around the hydrophilic groups located in the PSBP and PNIPMAM blocks are followed. The first contraction step turns out to be dominated by the behavior of the PSBP block, where as the second one is dominated by the PNIPMAM block. The unusual swelling and contraction behavior of the latter block is attributed to its co-nonsolvency behavior. Furthermore, we observe cooperative hydration effects in the DBC films, that is, both polymer blocks influence each other's solvation behavior.},
language = {en}
}
@article{KuntzeViljakkaTitovetal.2022,
author = {Kuntze, Kim and Viljakka, Jani and Titov, Evgenii and Ahmed, Zafar and Kalenius, Elina and Saalfrank, Peter and Priimagi, Arri},
title = {Towards low-energy-light-driven bistable photoswitches},
series = {Photochemical \& photobiological sciences / European Society for Photobiology},
volume = {21},
journal = {Photochemical \& photobiological sciences / European Society for Photobiology},
number = {2},
publisher = {Springer},
address = {Heidelberg},
issn = {1474-905X},
doi = {10.1007/s43630-021-00145-4},
pages = {159 -- 173},
year = {2022},
abstract = {Thermally stable photoswitches that are driven with low-energy light are rare, yet crucial for extending the applicability of photoresponsive molecules and materials towards, e.g., living systems. Combined ortho-fluorination and -amination couples high visible light absorptivity of o-aminoazobenzenes with the extraordinary bistability of o-fluoroazobenzenes. Herein, we report a library of easily accessible o-aminofluoroazobenzenes and establish structure-property relationships regarding spectral qualities, visible light isomerization efficiency and thermal stability of the cis-isomer with respect to the degree of o-substitution and choice of amino substituent. We rationalize the experimental results with quantum chemical calculations, revealing the nature of low-lying excited states and providing insight into thermal isomerization. The synthesized azobenzenes absorb at up to 600 nm and their thermal cis-lifetimes range from milliseconds to months. The most unique example can be driven from trans to cis with any wavelength from UV up to 595 nm, while still exhibiting a thermal cis-lifetime of 81 days.
[GRAPHICS]
.},
language = {en}
}
@article{XieXuWangetal.2022,
author = {Xie, Dongjiu and Xu, Yaolin and Wang, Yonglei and Pan, Xuefeng and H{\"a}rk, Eneli and Kochovski, Zdravko and Eljarrat, Alberto and M{\"u}ller, Johannes and Koch, Christoph T. and Yuan, Jiayin and Lu, Yan},
title = {Poly(ionic liquid) nanovesicle-templated carbon nanocapsules functionalized with uniform iron nitride nanoparticles as catalytic sulfur host for Li-S batteries},
series = {ACS nano},
volume = {16},
journal = {ACS nano},
number = {7},
publisher = {American Chemical Society},
address = {Washington},
issn = {1936-0851},
doi = {10.1021/acsnano.2c01992},
pages = {10554 -- 10565},
year = {2022},
abstract = {Poly(ionic liquid)s (PIL) are common precursors for heteroatom-doped carbon materials. Despite a relatively higher carbonization yield, the PIL-to-carbon conversion process faces challenges in preserving morphological and structural motifs on the nanoscale. Assisted by a thin polydopamine coating route and ion exchange, imidazoliumbased PIL nanovesicles were successfully applied in morphology-maintaining carbonization to prepare carbon composite nanocapsules. Extending this strategy further to their composites, we demonstrate the synthesis of carbon composite nanocapsules functionalized with iron nitride nanoparticles of an ultrafine, uniform size of 3-5 nm (termed "FexN@C "). Due to its unique nanostructure, the sulfur-loaded FexN@C electrode was tested to efficiently mitigate the notorious shuttle effect of lithium polysulfides (LiPSs) in Li-S batteries. The cavity of the carbon nanocapsules was spotted to better the loading content of sulfur. The well-dispersed iron nitride nanoparticles effectively catalyze the conversion of LiPSs to Li2S, owing to their high electronic conductivity and strong binding power to LiPSs. Benefiting from this well-crafted composite nanostructure, the constructed FexN@C/S cathode demonstrated a fairly high discharge capacity of 1085 mAh g(-1) at 0.5 C initially, and a remaining value of 930 mAh g(-1 )after 200 cycles. In addition, it exhibits an excellent rate capability with a high initial discharge capacity of 889.8 mAh g(-1) at 2 C. This facile PIL-to-nanocarbon synthetic approach is applicable for the exquisite design of complex hybrid carbon nanostructures with potential use in electrochemical energy storage and conversion.},
language = {en}
}
@article{NeffeLoewenbergJulichGruneretal.2021,
author = {Neffe, Axel T. and L{\"o}wenberg, Candy and Julich-Gruner, Konstanze K. and Behl, Marc and Lendlein, Andreas},
title = {Thermally-induced shape-memory behavior of degradable gelatin-based networks},
series = {International journal of molecular sciences},
volume = {22},
journal = {International journal of molecular sciences},
number = {11},
publisher = {Molecular Diversity Preservation International},
address = {Basel},
issn = {1422-0067},
doi = {10.3390/ijms22115892},
pages = {15},
year = {2021},
abstract = {Shape-memory hydrogels (SMH) are multifunctional, actively-moving polymers of interest in biomedicine. In loosely crosslinked polymer networks, gelatin chains may form triple helices, which can act as temporary net points in SMH, depending on the presence of salts. Here, we show programming and initiation of the shape-memory effect of such networks based on a thermomechanical process compatible with the physiological environment. The SMH were synthesized by reaction of glycidylmethacrylated gelatin with oligo(ethylene glycol) (OEG) alpha,omega-dithiols of varying crosslinker length and amount. Triple helicalization of gelatin chains is shown directly by wide-angle X-ray scattering and indirectly via the mechanical behavior at different temperatures. The ability to form triple helices increased with the molar mass of the crosslinker. Hydrogels had storage moduli of 0.27-23 kPa and Young's moduli of 215-360 kPa at 4 degrees C. The hydrogels were hydrolytically degradable, with full degradation to water-soluble products within one week at 37 degrees C and pH = 7.4. A thermally-induced shape-memory effect is demonstrated in bending as well as in compression tests, in which shape recovery with excellent shape-recovery rates R-r close to 100\% were observed. In the future, the material presented here could be applied, e.g., as self-anchoring devices mechanically resembling the extracellular matrix.},
language = {en}
}
@article{BochoveGrijpmaLendleinetal.2021,
author = {Bochove, Bas van and Grijpma, Dirk W. and Lendlein, Andreas and Sepp{\"a}l{\"a}, Jukka},
title = {Designing advanced functional polymers for medicine},
series = {European polymer journal : EPJ},
volume = {155},
journal = {European polymer journal : EPJ},
publisher = {Elsevier},
address = {Oxford},
issn = {0014-3057},
doi = {10.1016/j.eurpolymj.2021.110573},
pages = {2},
year = {2021},
language = {en}
}
@article{HwangZhangYouketal.2021,
author = {Hwang, Jinyeon and Zhang, Wuyong and Youk, Sol and Schutjajew, Konstantin and Oschatz, Martin},
title = {Understanding structure-property relationships under experimental conditions for the optimization of lithium-ion capacitor anodes based on all-carbon-composite materials},
series = {Energy technology : generation, conversion, storage, distribution},
volume = {9},
journal = {Energy technology : generation, conversion, storage, distribution},
number = {3},
publisher = {Wiley-VCH},
address = {Weinheim},
issn = {2194-4296},
doi = {10.1002/ente.202001054},
pages = {8},
year = {2021},
abstract = {The nanoscale combination of a conductive carbon and a carbon-based material with abundant heteroatoms for battery electrodes is a method to overcome the limitation that the latter has high affinity to alkali metal ions but low electronic conductivity. The synthetic protocol and the individual ratios and structures are important aspects influencing the properties of such multifunctional compounds. Their interplay is, herein, investigated by infiltration of a porous ZnO-templated carbon (ZTC) with nitrogen-rich carbon obtained by condensation of hexaazatriphenylene-hexacarbonitrile (HAT-CN) at 550-1000 degrees C. The density of lithiophilic sites can be controlled by HAT-CN content and condensation temperature. Lithium storage properties are significantly improved in comparison with those of the individual compounds and their physical mixtures. Depending on the uniformity of the formed composite, loading ratio and condensation temperature have different influence. Most stable operation at high capacity per used monomer is achieved with a slowly dried composite with an HAT-CN:ZTC mass ratio of 4:1, condensed at 550 degrees C, providing more than 400 mAh g(-1) discharge capacity at 0.1 A g(-1) and a capacity retention of 72\% after 100 cycles of operation at 0.5 A g(-1) due to the homogeneity of the composite and high content of lithiophilic sites.},
language = {en}
}
@article{PanSarhanKochovskietal.2022,
author = {Pan, Xuefeng and Sarhan, Radwan Mohamed and Kochovski, Zdravko and Chen, Guosong and Taubert, Andreas and Mei, Shilin and Lu, Yan},
title = {Template synthesis of dual-functional porous MoS2 nanoparticles with photothermal conversion and catalytic properties},
series = {Nanoscale},
volume = {14},
journal = {Nanoscale},
number = {18},
publisher = {RSC Publ. (Royal Society of Chemistry)},
address = {Cambridge},
issn = {2040-3372},
doi = {10.1039/d2nr01040b},
pages = {6888 -- 6901},
year = {2022},
abstract = {Advanced catalysis triggered by photothermal conversion effects has aroused increasing interest due to its huge potential in environmental purification. In this work, we developed a novel approach to the fast degradation of 4-nitrophenol (4-Nip) using porous MoS2 nanoparticles as catalysts, which integrate the intrinsic catalytic property of MoS2 with its photothermal conversion capability. Using assembled polystyrene-b-poly(2-vinylpyridine) block copolymers as soft templates, various MoS 2 particles were prepared, which exhibited tailored morphologies (e.g., pomegranate-like, hollow, and open porous structures). The photothermal conversion performance of these featured particles was compared under near-infrared (NIR) light irradiation. Intriguingly, when these porous MoS2 particles were further employed as catalysts for the reduction of 4-Nip, the reaction rate constant was increased by a factor of 1.5 under NIR illumination. We attribute this catalytic enhancement to the open porous architecture and light-to-heat conversion performance of the MoS2 particles. This contribution offers new opportunities for efficient photothermal-assisted catalysis.},
language = {en}
}
@article{ZhaoSarhanEljarratetal.2022,
author = {Zhao, Yuhang and Sarhan, Radwan Mohamed and Eljarrat, Alberto and Kochovski, Zdravko and Koch, Christoph and Schmidt, Bernd and Koopman, Wouter-Willem Adriaan and Lu, Yan},
title = {Surface-functionalized Au-Pd nanorods with enhanced photothermal conversion and catalytic performance},
series = {ACS applied materials \& interfaces},
volume = {14},
journal = {ACS applied materials \& interfaces},
number = {15},
publisher = {American Chemical Society},
address = {Washington, DC},
issn = {1944-8244},
doi = {10.1021/acsami.2c00221},
pages = {17259 -- 17272},
year = {2022},
abstract = {Bimetallic nanostructures comprising plasmonic and catalytic components have recently emerged as a promising approach to generate a new type of photo-enhanced nanoreactors. Most designs however concentrate on plasmon-induced charge separation, leaving photo-generated heat as a side product. This work presents a photoreactor based on Au-Pd nanorods with an optimized photothermal conversion, which aims to effectively utilize the photo-generated heat to increase the rate of Pd-catalyzed reactions. Dumbbell-shaped Au nanorods were fabricated via a seed-mediated growth method using binary surfactants. Pd clusters were selectively grown at the tips of the Au nanorods, using the zeta potential as a new synthetic parameter to indicate the surfactant remaining on the nanorod surface. The photothermal conversion of the Au-Pd nanorods was improved with a thin layer of polydopamine (PDA) or TiO2. As a result, a 60\% higher temperature increment of the dispersion compared to that for bare Au rods at the same light intensity and particle density could be achieved. The catalytic performance of the coated particles was then tested using the reduction of 4-nitrophenol as the model reaction. Under light, the PDA-coated Au-Pd nanorods exhibited an improved catalytic activity, increasing the reaction rate by a factor 3. An analysis of the activation energy confirmed the photoheating effect to be the dominant mechanism accelerating the reaction. Thus, the increased photothermal heating is responsible for the reaction acceleration. Interestingly, the same analysis shows a roughly 10\% higher reaction rate for particles under illumination compared to under dark heating, possibly implying a crucial role of localized heat gradients at the particle surface. Finally, the coating thickness was identified as an essential parameter determining the photothermal conversion efficiency and the reaction acceleration.},
language = {en}
}
@article{FloydSongHapeshietal.2022,
author = {Floyd, Thomas G. and Song, Ji-Inn and Hapeshi, Alexia and Laroque, Sophie and Hartlieb, Matthias and Perrier, Sebastien},
title = {Bottlebrush copolymers for gene delivery: influence of architecture, charge density, and backbone length on transfection efficiency},
series = {Journal of materials chemistry : B, materials for biology and medicine},
volume = {10},
journal = {Journal of materials chemistry : B, materials for biology and medicine},
number = {19},
publisher = {Royal Society of Chemistry},
address = {London [u.a.]},
issn = {2050-750X},
doi = {10.1039/d2tb00490a},
pages = {3696 -- 3704},
year = {2022},
abstract = {The influence of polymer architecture of polycations on their ability to transfect mammalian cells is probed. Polymer bottle brushes with grafts made from partially hydrolysed poly(2-ethyl-2-oxazoline) are used while varying the length of the polymer backbone as well as the degree of hydrolysis (cationic charge content). Polyplex formation is investigated via gel electrophoresis, dye-displacement and dynamic light scattering. Bottle brushes show a superior ability to complex pDNA when compared to linear copolymers. Also, nucleic acid release was found to be improved by a graft architecture. Polyplexes based on bottle brush copolymers showed an elongated shape in transmission electron microscopy images. The cytotoxicity against mammalian cells is drastically reduced when a graft architecture is used instead of linear copolymers. Moreover, the best-performing bottle brush copolymer showed a transfection ability comparable with that of linear poly(ethylenimine), the gold standard of polymeric transfection agents, which is used as positive control. In combination with their markedly lowered cytotoxicity, cationic bottle brush copolymers are therefore shown to be a highly promising class of gene delivery vectors.},
language = {en}
}
@misc{PerovicZeiningerOschatz2020,
author = {Perovic, Milena and Zeininger, Lukas and Oschatz, Martin},
title = {Immobilization of gold-on-carbon catalysts onto perfluorocarbon emulsion droplets to promote oxygen delivery in aqueous phase (D)-glucose oxidation},
series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
number = {1},
issn = {1867-3880},
doi = {10.25932/publishup-56947},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-569471},
pages = {8},
year = {2020},
abstract = {The catalytic activity of metal nanoparticles (NPs) supported on porous supports can be controlled by various factors, such as NPs size, shape, or dispersivity, as well as their interaction with the support or the properties of the support material itself. However, these intrinsic properties are not solely responsible for the catalytic behavior of the overall reaction system, as the local environment and surface coverage of the catalyst with reactants, products, intermediates and other invloved species often play a crucial role in catalytic processes as well. Their contribution can be particularly critical in liquid-phase reactions with gaseous reactants that often suffer from low solubiltiy. One example is (D)-glucose oxidation with molecular oxygen over gold nanoparticles supported on porous carbons. The possibility to promote oxygen delivery in such aqueous phase oxidation reactions via the immobilization of heterogenous catalysts onto the interface of perfluorocarbon emulsion droplets is reported here. Gold-on-carbon catalyst particles can stabilize perfluorocarbon droplets in the aqueous phase and the local concentration of the oxidant in the surroundings of the gold nanoparticles accelerates the rate-limiting step of the reaction. Consequently, the reaction rate of a system with the optimal volume fraction of fluorocarbon is higher than a reference emulsion system without fluorocarbon, and the effect is observed even without additional oxygen supply.},
language = {en}
}
@article{AbbasiXuKhezrietal.2022,
author = {Abbasi, Ali and Xu, Yaolin and Khezri, Ramin and Etesami, Mohammad and Lin, C. and Kheawhom, Soorathep and Lu, Yan},
title = {Advances in characteristics improvement of polymeric membranes/separators for zinc-air batteries},
series = {Materials Today Sustainability},
volume = {18},
journal = {Materials Today Sustainability},
publisher = {Elsevier},
address = {Amsterdam},
issn = {2589-2347},
doi = {10.1016/j.mtsust.2022.100126},
pages = {17},
year = {2022},
abstract = {Zinc-air batteries (ZABs) are gaining popularity for a wide range of applications due to their high energy density, excellent safety, and environmental friendliness. A membrane/separator is a critical component of ZABs, with substantial implications for battery performance and stability, particularly in the case of a battery in solid state format, which has captured increased attention in recent years. In this review, recent advances as well as insight into the architecture of polymeric membrane/separators for ZABs including porous polymer separators (PPSs), gel polymer electrolytes (GPEs), solid polymer electrolytes (SPEs) and anion exchange membranes (AEMs) are discussed. The paper puts forward strategies to enhance stability, ionic conductivity, ionic selectivity, electrolyte storage capacity and mechanical properties for each type of polymeric membrane. In addition, the remaining major obstacles as well as the most potential avenues for future research are examined in detail.},
language = {en}
}
@misc{RauschBrockmeyerSchwerdtle2021,
author = {Rausch, Ann-Kristin and Brockmeyer, Robert and Schwerdtle, Tanja},
title = {Development, validation, and application of a multi-method for the determination of mycotoxins, plant growth regulators, tropane alkaloids, and pesticides in cereals by two-dimensional liquid chromatography tandem mass spectrometry},
series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
number = {143},
issn = {1866-8372},
doi = {10.25932/publishup-51479},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-514795},
pages = {16},
year = {2021},
abstract = {Mycotoxins and pesticides regularly co-occur in agricultural products worldwide. Thus, humans can be exposed to both toxic contaminants and pesticides simultaneously, and multi-methods assessing the occurrence of various food contaminants and residues in a single method are necessary. A two-dimensional high performance liquid chromatography tandem mass spectrometry method for the analysis of 40 (modified) mycotoxins, two plant growth regulators, two tropane alkaloids, and 334 pesticides in cereals was developed. After an acetonitrile/water/formic acid (79:20:1, v/v/v) multi-analyte extraction procedure, extracts were injected into the two-dimensional setup, and an online clean-up was performed. The method was validated according to Commission Decision (EC) no. 657/2002 and document N° SANTE/12682/2019. Good linearity (R2 > 0.96), recovery data between 70-120\%, repeatability and reproducibility values < 20\%, and expanded measurement uncertainties < 50\% were obtained for a wide range of analytes, including very polar substances like deoxynivalenol-3-glucoside and methamidophos. However, results for fumonisins, zearalenone-14,16-disulfate, acid-labile pesticides, and carbamates were unsatisfying. Limits of quantification meeting maximum (residue) limits were achieved for most analytes. Matrix effects varied highly (-85 to +1574\%) and were mainly observed for analytes eluting in the first dimension and early-eluting analytes in the second dimension. The application of the method demonstrated the co-occurrence of different types of cereals with 28 toxins and pesticides. Overall, 86\% of the samples showed positive findings with at least one mycotoxin, plant growth regulator, or pesticide.},
language = {en}
}
@misc{IlicTsoukaPerovicetal.2020,
author = {Ilic, Ivan K. and Tsouka, Alexandra and Perovic, Milena and Hwang, Jinyeon and Heil, Tobias and L{\"o}ffler, Felix and Oschatz, Martin and Antonietti, Markus and Liedel, Clemens},
title = {Sustainable cathodes for Lithium-ion energy storage devices based on tannic acid-toward ecofriendly energy storage},
series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
number = {1},
issn = {1866-8372},
doi = {10.25932/publishup-57056},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-570560},
pages = {10},
year = {2020},
abstract = {The use of organic materials with reversible redox activity holds enormous potential for next-generation Li-ion energy storage devices. Yet, most candidates are not truly sustainable, i.e., not derived from renewable feedstock or made in benign reactions. Here an attempt is reported to resolve this issue by synthesizing an organic cathode material from tannic acid and microporous carbon derived from biomass. All constituents, including the redox-active material and conductive carbon additive, are made from renewable resources. Using a simple, sustainable fabrication method, a hybrid material is formed. The low cost and ecofriendly material shows outstanding performance with a capacity of 108 mAh g(-1) at 0.1 A g(-1) and low capacity fading, retaining approximately 80\% of the maximum capacity after 90 cycles. With approximately 3.4 V versus Li+/Li, the cells also feature one of the highest reversible redox potentials reported for biomolecular cathodes. Finally, the quinone-catecholate redox mechanism responsible for the high capacity of tannic acid is confirmed by electrochemical characterization of a model compound similar to tannic acid but without catecholic groups.},
language = {en}
}
@misc{FarhanChaudharyNoecheletal.2020,
author = {Farhan, Muhammad and Chaudhary, Deeptangshu and N{\"o}chel, Ulrich and Behl, Marc and Kratz, Karl and Lendlein, Andreas},
title = {Electrical actuation of coated and composite fibers based on poly[ethylene-co-(vinyl acetate)]},
series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
number = {2},
issn = {1866-8372},
doi = {10.25932/publishup-57167},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-571679},
pages = {10},
year = {2020},
abstract = {Robots are typically controlled by electrical signals. Resistive heating is an option to electrically trigger actuation in thermosensitive polymer systems. In this study electrically triggerable poly[ethylene-co-(vinyl acetate)] (PEVA)-based fiber actuators are realized as composite fibers as well as polymer fibers with conductive coatings. In the coated fibers, the core consists of crosslinked PEVA (cPEVA), while the conductive coating shell is achieved via a dip coating procedure with a coating thickness between 10 and 140 mu m. The conductivity of coated fibers sigma = 300-550 S m(-1) is much higher than that of the composite fibers sigma = 5.5 S m(-1). A voltage (U) of 110 V is required to heat 30 cm of coated fiber to a targeted temperature of approximate to 65 degrees C for switching in less than a minute. Cyclic electrical actuation investigations reveal epsilon '(rev) = 5 +/- 1\% reversible change in length for coated fibers. The fabrication of such electro-conductive polymeric actuators is suitable for upscaling so that their application potential as artificial muscles can be explored in future studies.},
language = {en}
}
@article{MayerPicconiRobinsonetal.2022,
author = {Mayer, Dennis and Picconi, David and Robinson, Matthew S. and G{\"u}hr, Markus},
title = {Experimental and theoretical gas-phase absorption spectra of thionated uracils},
series = {Chemical physics : a journal devoted to experimental and theoretical research involving problems of both a chemical and physical nature},
volume = {558},
journal = {Chemical physics : a journal devoted to experimental and theoretical research involving problems of both a chemical and physical nature},
publisher = {Elsevier},
address = {Amsterdam},
issn = {0301-0104},
doi = {10.1016/j.chemphys.2022.111500},
pages = {9},
year = {2022},
abstract = {We present a comparative study of the gas-phase UV spectra of uracil and its thionated counterparts (2-thiouracil, 4-thiouracil and 2,4-dithiouracil), closely supported by time-dependent density functional theory calculations to assign the transitions observed. We systematically discuss pure gas-phase spectra for the (thio)uracils in the range of 200-400 nm (similar to 3.2-6.4 eV), and examine the spectra of all four species with a single theoretical approach. We note that specific vibrational modelling is needed to accurately determine the spectra across the examined wavelength range, and systematically model the transitions that appear at wavelengths shorter than 250 nm. Additionally, we find in the cases of 2-thiouracil and 2,4-dithiouracil, that the gas-phase spectra deviate significantly from some previously published solution-phase spectra, especially those collected in basic environments.},
language = {en}
}
@article{ZimmermannStompsSchulteOsseilietal.2020,
author = {Zimmermann, Marc and Stomps, Benjamin Ren{\´e} Harald and Schulte-Osseili, Christine and Grigoriev, Dmitry and Ewen, Dirk and Morgan, Andrew and B{\"o}ker, Alexander},
title = {Organic dye anchor peptide conjugates as an advanced coloring agent for polypropylene yarn},
series = {Textile Research Journal},
volume = {91},
journal = {Textile Research Journal},
number = {1-2},
publisher = {Sage Publ.},
address = {London},
issn = {0040-5175},
doi = {10.1177/0040517520932231},
pages = {28 -- 39},
year = {2020},
abstract = {Polypropylene as one of the world's top commodity polymers is also widely used in the textile industry. However, its non-polar nature and partially crystalline structure significantly complicate the process of industrial coloring of polypropylene. Currently, textiles made of polypropylene or with a significant proportion of polypropylene are dyed under quite harsh conditions, including the use of high pressures and temperatures, which makes this process energy intensive. This research presents a three-step synthesis of coloring agents, capable of adhering onto synthetic polypropylene yarns without harsh energy-consuming conditions. This is possible by encapsulation of organic pigments using trimethoxyphenylsilane, introduction of surface double bonds via modification of the silica shell with trimethoxysilylpropylmethacrylate and final attachment of highly adhesive anchor peptides using thiol-ene chemistry. We demonstrate the applicability of this approach by dyeing polypropylene yarns in a simple process under ambient conditions after giving a step-by-step guide for the synthesis of these new dyeing agents. Finally, the successful dyeing of the yarns is visualized, and its practicability is discussed.},
language = {en}
}
@misc{ZimmermannStompsSchulteOsseilietal.2020,
author = {Zimmermann, Marc and Stomps, Benjamin Ren{\´e} Harald and Schulte-Osseili, Christine and Grigoriev, Dmitry and Ewen, Dirk and Morgan, Andrew and B{\"o}ker, Alexander},
title = {Organic dye anchor peptide conjugates as an advanced coloring agent for polypropylene yarn},
series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
number = {1-2},
issn = {1866-8372},
doi = {10.25932/publishup-54891},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-548913},
pages = {14},
year = {2020},
abstract = {Polypropylene as one of the world's top commodity polymers is also widely used in the textile industry. However, its non-polar nature and partially crystalline structure significantly complicate the process of industrial coloring of polypropylene. Currently, textiles made of polypropylene or with a significant proportion of polypropylene are dyed under quite harsh conditions, including the use of high pressures and temperatures, which makes this process energy intensive. This research presents a three-step synthesis of coloring agents, capable of adhering onto synthetic polypropylene yarns without harsh energy-consuming conditions. This is possible by encapsulation of organic pigments using trimethoxyphenylsilane, introduction of surface double bonds via modification of the silica shell with trimethoxysilylpropylmethacrylate and final attachment of highly adhesive anchor peptides using thiol-ene chemistry. We demonstrate the applicability of this approach by dyeing polypropylene yarns in a simple process under ambient conditions after giving a step-by-step guide for the synthesis of these new dyeing agents. Finally, the successful dyeing of the yarns is visualized, and its practicability is discussed.},
language = {en}
}
@misc{WessigJohnSperlichetal.2020,
author = {Wessig, Pablo and John, Leonard and Sperlich, Eric and Kelling, Alexandra},
title = {Sulfur tuning of [1,3]-dioxolo[4.5-f]benzodioxole (DBD) fluorescent dyes},
series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
number = {3},
issn = {1866-8372},
doi = {10.25932/publishup-56624},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-566241},
pages = {15},
year = {2020},
abstract = {The replacement of oxygen by sulfur atoms of [1,3]-dioxolo[4.5-f]benzodioxole (DBD) fluorescent dyes is an efficient way to adjust the photophysical properties (sulfur tuning). While previously developed S-4-DBD dyes exhibit considerably red-shifted absorption and emission wavelength, the heavy atom effect of four sulfur atoms cause low fluorescence quantum yields and short fluorescence lifetimes. Herein, we demonstrate that the replacement of less than four sulfur atoms (S-1-DBD, 1,2-S-2-DBD, and 1,4-S-2-DBD dyes) permits a fine-tuning of the photophysical properties. In some cases, a similar influence on the wavelength without the detrimental effect on the quantum yields and lifetimes is observed. Furthermore, the synthetic accessibility of S-1- and S-2-DBD dyes is improved, compared with S-4-DBD dyes. For coupling with biomolecules a series of reactive derivatives of the new dyes were developed (azides, OSu esters, alkynes, maleimides).},
language = {en}
}
@misc{BourgatTierschKoetzetal.2020,
author = {Bourgat, Yannick and Tiersch, Brigitte and Koetz, Joachim and Menzel, Henning},
title = {Enzyme degradable polymersomes from chitosan-g-[poly-l-lysine-block-epsilon-caprolactone] copolymer},
series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe},
number = {1},
issn = {1866-8372},
doi = {10.25932/publishup-56658},
url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-566584},
pages = {11},
year = {2020},
abstract = {The scope of this study includes the synthesis of chitosan-g-[peptide-poly-epsilon-caprolactone] and its self-assembly into polymeric vesicles employing the solvent shift method. In this way, well-defined core-shell structures suitable for encapsulation of drugs are generated. The hydrophobic polycaprolactone side-chain and the hydrophilic chitosan backbone are linked via an enzyme-cleavable peptide. The synthetic route involves the functionalization of chitosan with maleimide groups and the preparation of polycaprolactone with alkyne end-groups. A peptide functionalized with a thiol group on one side and an azide group on the other side is prepared. Thiol-ene click-chemistry and azide-alkyne Huisgen cycloaddition are then used to link the chitosan and poly-epsilon-caprolactone chains, respectively, with this peptide. For a preliminary study, poly-l-lysin is a readily available and cleavable peptide that is introduced to investigate the feasibility of the system. The size and shape of the polymersomes are studied by dynamic light scattering and cryo-scanning electron microscopy. Furthermore, degradability is studied by incubating the polymersomes with two enzymes, trypsin and chitosanase. A dispersion of polymersomes is used to coat titanium plates and to further test the stability against enzymatic degradation.},
language = {en}
}