TY  - JOUR
A1  - Rothe, Martin
A1  - Zhao, Yuhang
A1  - Müller, Johannes
A1  - Kewes, Günter
A1  - Koch, Christoph T.
A1  - Lu, Yan
A1  - Benson, Oliver
T1  - Self-assembly of plasmonic nanoantenna-waveguide structures for subdiffractional chiral sensing
JF  - ACS nano
N2  - Spin-momentum locking is a peculiar effect in the near-field of guided optical or plasmonic modes. It can be utilized to map the spinning or handedness of electromagnetic fields onto the propagation direction. This motivates a method to probe the circular dichroism of an illuminated chiral object. In this work, we demonstrate local, subdiffraction limited chiral coupling of light and propagating surface plasmon polaritons in a self-assembled system of a gold nanoantenna and a silver nanowire. A thin silica shell around the nanowire provides precise distance control and also serves as a host for fluorescent molecules, which indicate the direction of plasmon propagation. We characterize our nanoantenna-nanowire systems comprehensively through correlated electron microscopy, energy-dispersive X-ray spectroscopy, dark-field, and fluorescence imaging. Three-dimensional numerical simulations support the experimental findings. Besides our measurement of far-field polarization, we estimate sensing capabilities and derive not only a sensitivity of 1 mdeg for the ellipticity of the light field, but also find 10(3) deg cm(2)/dmol for the circular dichroism of an analyte locally introduced in the hot spot of the antenna-wire system. Thorough modeling of a prototypical design predicts on-chip sensing of chiral analytes. This introduces our system as an ultracompact sensor for chiral response far below the diffraction limit.
KW  - plasmonics
KW  - nanoparticle assemblies
KW  - core-shell
KW  - spin-orbit coupling
KW  - chirality
KW  - circular dichroism
KW  - nano-optics
Y1  - 2021
U6  - https://doi.org/10.1021/acsnano.0c05240
SN  - 1936-0851
SN  - 1936-086X
VL  - 15
IS  - 1
SP  - 351
EP  - 361
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Lau, Skadi
A1  - Liu, Yue
A1  - Maier, Anna
A1  - Braune, Steffen
A1  - Gossen, Manfred
A1  - Neffe, Axel T.
A1  - Lendlein, Andreas
T1  - Establishment of an in vitro thrombogenicity test system with cyclic olefin copolymer substrate for endothelial layer formation
JF  - MRS communications / a publication of the Materials Research Society
N2  - In vitro thrombogenicity test systems require co-cultivation of endothelial cells and platelets under blood flow-like conditions. Here, a commercially available perfusion system is explored using plasma-treated cyclic olefin copolymer (COC) as a substrate for the endothelial cell layer. COC was characterized prior to endothelialization and co-cultivation with platelets under static or flow conditions. COC exhibits a low roughness and a moderate hydrophilicity. Flow promoted endothelial cell growth and prevented platelet adherence. These findings show the suitability of COC as substrate and the importance of blood flow-like conditions for the assessment of the thrombogenic risk of drugs or cardiovascular implant materials.
Y1  - 2021
U6  - https://doi.org/10.1557/s43579-021-00072-6
SN  - 2159-6867
VL  - 11
IS  - 5
SP  - 559
EP  - 567
PB  - Springer
CY  - Berlin
ER  - 
TY  - JOUR
A1  - Tung, Wing Tai
A1  - Sun, Xianlei
A1  - Wang, Weiwei
A1  - Xu, Xun
A1  - Ma, Nan
A1  - Lendlein, Andreas
T1  - Structure, mechanical properties and degradation behavior of electrospun PEEU fiber meshes and films
JF  - MRS advances : a journal of the Materials Research Society (MRS)
N2  - The capability of a degradable implant to provide mechanical support depends on its degradation behavior. Hydrolytic degradation was studied for a polyesteretherurethane (PEEU70), which consists of poly(p-dioxanone) (PPDO) and poly(epsilon-caprolactone) (PCL) segments with a weight ratio of 70:30 linked by diurethane junction units. PEEU70 samples prepared in the form of meshes with average fiber diameters of 1.5 mu m (mesh1.5) and 1.2 mu m (mesh1.2), and films were sterilized and incubated in PBS at 37 degrees C with 5 vol% CO2 supply for 1 to 6 weeks. Degradation features, such as cracks or wrinkles, became apparent from week 4 for all samples. Mass loss was found to be 11 wt%, 6 wt%, and 4 wt% for mesh1.2, mesh1.5, and films at week 6. The elongation at break decreased to under 20% in two weeks for mesh1.2. In case of the other two samples, this level of degradation was achieved after 4 weeks. The weight average molecular weight of both PEEU70 mesh and film samples decreased to below 30 kg/mol when elongation at break dropped below 20%. The time period of sustained mechanical stability of PEEU70-based meshes depends on the fiber diameter and molecular weight.
Y1  - 2021
U6  - https://doi.org/10.1557/s43580-020-00001-0
SN  - 2059-8521
VL  - 6
IS  - 10
SP  - 276
EP  - 282
PB  - Springer Nature Switzerland AG
CY  - Cham
ER  - 
TY  - JOUR
A1  - Zhao, Yuhang
A1  - Opitz, Andreas
A1  - Eljarrat, Alberto
A1  - Kochovski, Zdravko
A1  - Koch, Christoph
A1  - Koch, Norbert
A1  - Lu, Yan
T1  - Kinetic study on the adsorption of 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane on Ag nanoparticles in chloroform
BT  - implications for the charge transfer complex of Ag-F(4)TCNQ
JF  - ACS applied nano materials
N2  - 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.
KW  - Ag nanoparticles
KW  - F(4)TCNQ
KW  - phase transfer
KW  - kinetics
KW  - electron transfer
KW  - surface interaction
Y1  - 2021
U6  - https://doi.org/10.1021/acsanm.1c02153
SN  - 2574-0970
VL  - 4
IS  - 11
SP  - 11625
EP  - 11635
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Zhou, Shuo
A1  - Xu, Xun
A1  - Ma, Nan
A1  - Jung, Friedrich
A1  - Lendlein, Andreas
T1  - Influence of sterilization conditions on sulfate-functionalized polyGGE
JF  - Clinical hemorheology and microcirculation : blood flow and vessels
N2  - 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.
KW  - Sulfated polymer
KW  - sulfation
KW  - sterilization
KW  - ethylene oxide
Y1  - 2021
U6  - https://doi.org/10.3233/CH-211241
SN  - 1386-0291
SN  - 1875-8622
VL  - 79
IS  - 4
SP  - 597
EP  - 608
PB  - IOS Press
CY  - Amsterdam
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  - 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  - 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
U6  - https://doi.org/10.1107/S0108767321089479
SN  - 2053-2733
VL  - 77
IS  - Suppl.
SP  - C750
EP  - C750
PB  - Blackwell
CY  - Oxford [u.a.]
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  - 2159-6867
VL  - 11
IS  - 4
SP  - 425
EP  - 431
PB  - Springer
CY  - Berlin
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  - 
TY  - JOUR
A1  - Kreuzer, Lucas
A1  - Widmann, Tobias
A1  - Geiger, Christina
A1  - Wang, Peixi
A1  - Vagias, Apostolos N.
A1  - Heger, Julian Eliah
A1  - Haese, Martin
A1  - Hildebrand, Viet
A1  - Laschewsky, André
A1  - Papadakis, Christine M.
A1  - Müller-Buschbaum, Peter
T1  - Salt-dependent phase transition behavior of doubly thermoresponsive poly(sulfobetaine)-based diblock copolymer thin films
JF  - Langmuir : the ACS journal of surfaces and colloids / American Chemical Society
N2  - 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.
Y1  - 2021
U6  - https://doi.org/10.1021/acs.langmuir.1c01342
SN  - 0743-7463
SN  - 1520-5827
VL  - 37
IS  - 30
SP  - 9179
EP  - 9191
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Neffe, Axel T.
A1  - Löwenberg, Candy
A1  - Julich-Gruner, Konstanze K.
A1  - Behl, Marc
A1  - Lendlein, Andreas
T1  - Thermally-induced shape-memory behavior of degradable gelatin-based networks
JF  - International journal of molecular sciences
N2  - 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.
KW  - shape-memory hydrogel
KW  - active polymer
KW  - biopolymer
KW  - mechanical
KW  - properties
KW  - degradation
Y1  - 2021
U6  - https://doi.org/10.3390/ijms22115892
SN  - 1422-0067
SN  - 1661-6596
VL  - 22
IS  - 11
PB  - Molecular Diversity Preservation International
CY  - Basel
ER  - 
TY  - JOUR
A1  - Bochove, Bas van
A1  - Grijpma, Dirk W.
A1  - Lendlein, Andreas
A1  - Seppälä, Jukka
T1  - Designing advanced functional polymers for medicine
JF  - European polymer journal : EPJ
Y1  - 2021
U6  - https://doi.org/10.1016/j.eurpolymj.2021.110573
SN  - 0014-3057
VL  - 155
PB  - Elsevier
CY  - Oxford
ER  - 
TY  - JOUR
A1  - Hwang, Jinyeon
A1  - Zhang, Wuyong
A1  - Youk, Sol
A1  - Schutjajew, Konstantin
A1  - Oschatz, Martin
T1  - Understanding structure-property relationships under experimental conditions for the optimization of lithium-ion capacitor anodes based on all-carbon-composite materials
JF  - Energy technology : generation, conversion, storage, distribution
N2  - 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.
KW  - anodes
KW  - hybrid materials
KW  - nitrogen-doped carbon
KW  - porous carbon
KW  - lithium-ion capacitors
Y1  - 2021
U6  - https://doi.org/10.1002/ente.202001054
SN  - 2194-4296
VL  - 9
IS  - 3
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - GEN
A1  - Rausch, Ann-Kristin
A1  - Brockmeyer, Robert
A1  - Schwerdtle, Tanja
T1  - 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
T2  - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe
N2  - 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.
T3  - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1365 
KW  - 2D-LC-MS/MS
KW  - Multi-method
KW  - Mycotoxins
KW  - Modified mycotoxins
KW  - Pesticides
KW  - Cereals
Y1  - 2021
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-514795
SN  - 1866-8372
IS  - 143
ER  -