TY - GEN A1 - Bande, Annika A1 - González, Leticia A1 - Klamroth, Tillmann A1 - Tremblay, Jean Christophe T1 - Theoretical chemistry and quantum dynamics at interfaces BT - Celebrating the career of Peter Saalfrank on the occasion of his 60th birthday T2 - Chemical physics : a journal devoted to experimental and theoretical research involving problems of both a chemical and physical nature Y1 - 2022 U6 - https://doi.org/10.1016/j.chemphys.2022.111509 SN - 0301-0104 SN - 1873-4421 VL - 558 PB - Elsevier Science CY - Amsterdam [u.a.] ER - TY - JOUR A1 - Crovetto, Andrea A1 - Kojda, Danny A1 - Yi, Feng A1 - Heinselman, Karen N. A1 - LaVan, David A. A1 - Habicht, Klaus A1 - Unold, Thomas A1 - Zakutayev, Andriy T1 - Crystallize It before It diffuses BT - kinetic stabilization of thin-film phosphorus-rich semiconductor CuP2 JF - Journal of the american chemical society N2 - 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. Y1 - 2022 U6 - https://doi.org/10.1021/jacs.2c04868 SN - 0002-7863 SN - 1520-5126 VL - 144 IS - 29 SP - 13334 EP - 13343 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Tung, Wing Tai A1 - Maring, Janita A. A1 - Xu, Xun A1 - Liu, Yue A1 - Becker, Matthias A1 - Somesh, Dipthi Bachamanda A1 - Klose, Kristin A1 - Wang, Weiwei A1 - Sun, Xianlei A1 - Ullah, Imran A1 - Kratz, Karl A1 - Neffe, Axel T. A1 - Stamm, Christof A1 - Ma, Nan A1 - Lendlein, Andreas T1 - In vivo performance of a cell and factor free multifunctional fiber mesh modulating postinfarct myocardial remodeling JF - Advanced Functional Materials N2 - 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. KW - bioinstructive materials KW - cardiac regeneration KW - function by structure; KW - modulation of in vivo regeneration KW - multifunctional biomaterials Y1 - 2022 U6 - https://doi.org/10.1002/adfm.202110179 SN - 1616-301X SN - 1616-3028 VL - 32 IS - 31 PB - Wiley CY - Weinheim ER - TY - JOUR A1 - Breternitz, Joachim A1 - Schorr, Susan T1 - Symmetry relations in wurtzite nitrides and oxide nitrides and the curious case of Pmc2(1) JF - Acta crystallographica / International Union of Crystallography. Section A, Foundations and advances N2 - 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. KW - group-subgroup relationships KW - nitride materials KW - wurtzite type Y1 - 2021 U6 - https://doi.org/10.1107/S2053273320015971 SN - 2053-2733 VL - 77 IS - 3 SP - 208 EP - 216 PB - Blackwell CY - Oxford [u.a.] ER - TY - JOUR A1 - Mei, Shilin A1 - Siebert, Andreas A1 - Xu, Yaolin A1 - Quan, Ting A1 - Garcia-Diez, Raul A1 - Bär, Marcus A1 - Härtel, Paul A1 - Abendroth, Thomas A1 - Dörfler, Susanne A1 - Kaskel, Stefan A1 - Lu, Yan T1 - Large-Scale Synthesis of Nanostructured Carbon-Ti4O7 Hollow Particles as Efficient Sulfur Host Materials for Multilayer Lithium-Sulfur Pouch Cells JF - Batteries & supercaps N2 - 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. KW - lithium-sulfur batteries KW - pouch cell KW - spherical polyelectrolyte brushes (SPB) KW - Ti4O7 Y1 - 2022 U6 - https://doi.org/10.1002/batt.202100398 SN - 2566-6223 VL - 5 IS - 6 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Lepre, Enrico A1 - Heske, Julian A1 - Nowakowski, Michal A1 - Scoppola, Ernesto A1 - Zizak, Ivo A1 - Heil, Tobias A1 - Kühne, Thomas D. A1 - Antonietti, Markus A1 - Lopez-Salas, Nieves A1 - Albero, Josep T1 - Ni-based electrocatalysts for unconventional CO2 reduction reaction to formic acid JF - Nano energy N2 - 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. KW - CO 2 reduction reaction KW - Noble carbon KW - Ni-O4 electrocatalysts KW - Formic acid Y1 - 2022 U6 - https://doi.org/10.1016/j.nanoen.2022.107191 SN - 2211-2855 SN - 2211-3282 VL - 97 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Haubitz, Toni A1 - Drobot, Björn A1 - Tsushima, Satoru A1 - Steudtner, Robin A1 - Stumpf, Thorsten A1 - Kumke, Michael Uwe T1 - Quenching mechanism of uranyl(VI) by chloride and bromide in aqueous and non-aqueous solutions JF - The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment & general theory N2 - 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. Y1 - 2021 U6 - https://doi.org/10.1021/acs.jpca.1c02487 SN - 1089-5639 SN - 1520-5215 VL - 125 IS - 20 SP - 4380 EP - 4389 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Pham, Duong Tung A1 - Quan, Ting A1 - Mei, Shilin A1 - Lu, Yan T1 - Colloidal metal sulfide nanoparticles for high performance electrochemical energy storage systems JF - Current opinion in green and sustainable chemistry N2 - 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. Y1 - 2022 U6 - https://doi.org/10.1016/j.cogsc.2022.100596 SN - 2452-2236 VL - 34 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Reitenbach, Julija A1 - Geiger, Christina A1 - Wang, Peixi A1 - Vagias, Apostolos N. A1 - Cubitt, Robert A1 - Schanzenbach, Dirk A1 - Laschewsky, André A1 - Papadakis, Christine M. A1 - Müller-Buschbaum, Peter T1 - Effect of magnesium salts with chaotropic anions on the swelling behavior of PNIPMAM thin films JF - Macromolecules : a publication of the American Chemical Society N2 - 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. Y1 - 2023 U6 - https://doi.org/10.1021/acs.macromol.2c02282 SN - 0024-9297 SN - 1520-5835 VL - 56 IS - 2 SP - 567 EP - 577 PB - American Chemical Society CY - Washington ER - TY - CHAP A1 - Breternitz, Joachim A1 - Schorr, Susan T1 - Halide perovskites BT - structural systematisation and what we learn from it T2 - Acta crystallographica / International Union of Crystallography. Section A, Foundations and advances KW - halide perovskites KW - semiconductors KW - group-subgroup relations KW - twinning Y1 - 2021 SN - 2053-2733 SN - 1600-5724 SN - 1600-8596 SN - 0108-7673 SN - 0567-7394 VL - 77 IS - Suppl. SP - C750 EP - C750 PB - Blackwell CY - Oxford [u.a.] ER - TY - JOUR A1 - Nchiozem-Ngnitedem, Vaderament-Alexe A1 - Sperlich, Eric A1 - Matieta, Valaire Yemene A1 - Kuete, Jenifer Reine Ngnouzouba A1 - Kuete, Victor A1 - Omer, Ejlal A. A. A1 - Efferth, Thomas A1 - Schmidt, Bernd T1 - Synthesis and bioactivity of isoflavones from ficus carica and some non-natural analogues JF - Journal of natural products : Lloydia N2 - 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. KW - Antimicrobial activity KW - Bacteria KW - Ethers KW - Flavonoids KW - Mixtures Y1 - 2023 U6 - https://doi.org/10.1021/acs.jnatprod.3c00219 SN - 0163-3864 SN - 1520-6025 VL - 86 IS - 6 SP - 1520 EP - 1528 PB - American Chemical Society CY - Washington, DC ER - TY - JOUR A1 - Geiger, Christina A1 - Reitenbach, Julija A1 - Henschel, Cristiane A1 - Kreuzer, Lucas A1 - Widmann, Tobias A1 - Wang, Peixi A1 - Mangiapia, Gaetano A1 - Moulin, Jean-François A1 - Papadakis, Christine M. A1 - Laschewsky, André A1 - Müller-Buschbaum, Peter T1 - Ternary nanoswitches realized with multiresponsive PMMA-b-PNIPMAM films in mixed water/acetone vapor atmospheres JF - Advanced engineering materials N2 - 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. KW - co-nonsolvency KW - diblock copolymers KW - nanoswitches KW - neutron reflectometry KW - thin films Y1 - 2021 U6 - https://doi.org/10.1002/adem.202100191 SN - 1438-1656 SN - 1527-2648 VL - 23 IS - 11 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Melani, Giacomo A1 - Nagata, Yuki A1 - Saalfrank, Peter T1 - Vibrational energy relaxation of interfacial OH on a water-covered alpha-Al2O3(0001) surface BT - a non-equilibrium ab initio molecular dynamics study JF - Physical chemistry, chemical physics : PCCP ; a journal of European chemical societies N2 - 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. Y1 - 2021 U6 - https://doi.org/10.1039/d0cp03777j SN - 1463-9076 SN - 1463-9084 VL - 23 IS - 13 SP - 7714 EP - 7723 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Wang, Zhenyu A1 - Fritsch, Daniel A1 - Berendts, Stefan A1 - Lerch, Martin A1 - Breternitz, Joachim A1 - Schorr, Susan T1 - Elucidation of the reaction mechanism for the synthesis of ZnGeN2 through Zn2GeO4 ammonolysis JF - Chemical science / RSC, Royal Society of Chemistry N2 - 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. Y1 - 2021 U6 - https://doi.org/10.1039/d1sc00328c SN - 2041-6539 VL - 12 IS - 24 SP - 8493 EP - 8500 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Saeedi Garakani, Sadaf A1 - Xie, Dongjiu A1 - Khorsand Kheirabad, Atefeh A1 - Lu, Yan A1 - Yuan, Jiayin T1 - Template-synthesis of a poly(ionic liquid)-derived Fe1-xS/nitrogen-doped porous carbon membrane and its electrode application in lithium-sulfur batteries JF - Materials advances N2 - 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. Y1 - 2021 U6 - https://doi.org/10.1039/d1ma00441g SN - 2633-5409 VL - 2 IS - 15 SP - 5203 EP - 5212 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Xu, Xun A1 - Nie, Yan A1 - Wang, Weiwei A1 - Ma, Nan A1 - Lendlein, Andreas T1 - Periodic thermomechanical modulation of toll-like receptor expression and distribution in mesenchymal stromal cells JF - MRS communications / a publication of the Materials Research Society N2 - 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. KW - Actuation KW - Antiviral KW - Biomaterial KW - COVID-19 KW - Shape memory Y1 - 2021 U6 - https://doi.org/10.1557/s43579-021-00049-5 SN - 2159-6859 SN - 2159-6867 VL - 11 IS - 4 SP - 425 EP - 431 PB - Springer CY - Berlin ER - TY - JOUR A1 - Schulze, Nicole A1 - Koetz, Joachim T1 - Kinetically controlled growth of gold nanotriangles in a vesicular template phase by adding a strongly alternating polyampholyte JF - Journal of dispersion science and technology N2 - 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. KW - Kinetically controlled nanocrystal growth KW - nanotriangles KW - polyampholytes Y1 - 2016 U6 - https://doi.org/10.1080/01932691.2016.1220318 SN - 0193-2691 SN - 1532-2351 VL - 38 IS - 8 SP - 1073 EP - 1078 PB - Taylor & Francis CY - Philadelphia ER - TY - THES A1 - Margraf, Johannes T. T1 - Science-driven chemical machine learning Y1 - 2023 ER - TY - JOUR A1 - Deng, Zijun A1 - Wang, Weiwei A1 - Xu, Xun A1 - Ma, Nan A1 - Lendlein, Andreas T1 - Polydopamine-based biofunctional substrate coating promotes mesenchymal stem cell migration JF - MRS advances : a journal of the Materials Research Society (MRS) N2 - 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. Y1 - 2021 U6 - https://doi.org/10.1557/s43580-021-00091-4 SN - 2059-8521 VL - 6 IS - 31 SP - 739 EP - 744 PB - Springer Nature Switzerland AG CY - Cham ER - TY - JOUR A1 - Machatschek, Rainhard Gabriel A1 - Saretia, Shivam A1 - Lendlein, Andreas T1 - Assessing the influence of temperature-memory creation on the degradation of copolyesterurethanes in ultrathin films JF - Advanced materials interfaces N2 - 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. KW - block copolymers KW - degradation KW - Langmuir monolayers KW - rheology KW - temperature-memory polymers Y1 - 2021 U6 - https://doi.org/10.1002/admi.202001926 SN - 2196-7350 VL - 8 IS - 6 PB - Wiley-VCH CY - Weinheim ER -