@article{62803, abstract = {{The aim to produce highly active, selective, and long-lived electrocatalysts by design drives major research efforts toward gaining fundamental understanding of the relationship between material properties and their catalytic performance. Surface characterization tools enable to assess atomic scale information on the complexity of electrocatalyst materials. Advancing electrochemical methodologies to adequately characterize such systems was less of a research focus point. In this Review, we shed light on the ability to gain fundamental insights into electrocatalysis from a complementary perspective and establish corresponding design strategies. These may rely on adopting the perceptions and models of other subareas of electrochemistry, such as corrosion, battery research, or electrodeposition. Concepts on how to account for and improve mass transport, manage gas bubble release, or exploit magnetic fields are highlighted in this respect. Particular attention is paid to deriving design strategies for nanoelectrocatalysts, which is often impeded, as structural and physical material properties are buried in electrochemical data of whole electrodes or even devices. Thus, a second major approach focuses on overcoming this difference in the considered level of complexity by methods of single-entity electrochemistry. The gained understanding of intrinsic catalyst performance may allow to rationally advance design concepts with increased complexity, such as three-dimensional electrode architectures. Many materials undergo structural changes upon formation of the working catalyst. Accordingly, developing “precatalysts” with low hindrance of the electrochemical transformation to the active catalyst is suggested as a final design strategy.}}, author = {{Linnemann, Julia and Kanokkanchana, Kannasoot and Tschulik, Kristina}}, issn = {{2155-5435}}, journal = {{ACS Catalysis}}, keywords = {{electrocatalysis}}, number = {{9}}, pages = {{5318--5346}}, publisher = {{American Chemical Society (ACS)}}, title = {{{Design Strategies for Electrocatalysts from an Electrochemist’s Perspective}}}, doi = {{10.1021/acscatal.0c04118}}, volume = {{11}}, year = {{2021}}, } @article{62806, abstract = {{The electrical double‐layer plays a key role in important interfacial electrochemical processes from catalysis to energy storage and corrosion. Therefore, understanding its structure is crucial for the progress of sustainable technologies. We extract new physico‐chemical information on the capacitance and structure of the electrical double‐layer of platinum and gold nanoparticles at the molecular level, employing single nanoparticle electrochemistry. The charge storage ability of the solid/liquid interface is larger by one order‐of‐magnitude than predicted by the traditional mean‐field models of the double‐layer such as the Gouy–Chapman–Stern model. Performing molecular dynamics simulations, we investigate the possible relationship between the measured high capacitance and adsorption strength of the water adlayer formed at the metal surface. These insights may launch the active tuning of solid–solvent and solvent–solvent interactions as an innovative design strategy to transform energy technologies towards superior performance and sustainability.}}, author = {{Azimzadeh Sani, Mahnaz and Pavlopoulos, Nicholas G. and Pezzotti, Simone and Serva, Alessandra and Cignoni, Paolo and Linnemann, Julia and Salanne, Mathieu and Gaigeot, Marie‐Pierre and Tschulik, Kristina}}, issn = {{1433-7851}}, journal = {{Angewandte Chemie International Edition}}, keywords = {{single-entity electrochemistry, electrical double layer, supercapacitor, nanoparticles}}, number = {{5}}, publisher = {{Wiley}}, title = {{{Unexpectedly High Capacitance of the Metal Nanoparticle/Water Interface: Molecular‐Level Insights into the Electrical Double Layer}}}, doi = {{10.1002/anie.202112679}}, volume = {{61}}, year = {{2021}}, } @article{62805, abstract = {{Single-entity electrochemistry allows for assessing electrocatalytic activities of individual material entities such as nanoparticles (NPs). Thus, it becomes possible to consider intrinsic electrochemical properties of nanocatalysts when researching how activity relates to physical and structural material properties. Conversely, conventional electrochemical techniques provide a normalized sum current referring to a huge ensemble of NPs constituting, along with additives (e.g., binders), a complete catalyst-coated electrode. Accordingly, recording electrocatalytic responses of single NPs avoids interferences of ensemble effects and reduces the complexity of electrocatalytic processes, thus enabling detailed description and modelling. Herein, we present insights into the oxygen evolution catalysis at individual cubic Co3O4 NPs impacting microelectrodes of different support materials. Simulating diffusion at supported nanocubes, measured step current signals can be analyzed, providing edge lengths, corresponding size distributions, and interference-free turnover frequencies. The provided nano-impact investigation of (electro-)catalyst-support effects contradicts assumptions on a low number of highly active sites.}}, author = {{Liu, Zhibin and Corva, Manuel and Amin, Hatem M. A. and Blanc, Niclas and Linnemann, Julia and Tschulik, Kristina}}, issn = {{1422-0067}}, journal = {{International Journal of Molecular Sciences}}, keywords = {{electrocatalysis, oxygen evolution reaction, cobalt spinel, single-entity electrochemistry}}, number = {{23}}, publisher = {{MDPI AG}}, title = {{{Single Co3O4 Nanocubes Electrocatalyzing the Oxygen Evolution Reaction: Nano-Impact Insights into Intrinsic Activity and Support Effects}}}, doi = {{10.3390/ijms222313137}}, volume = {{22}}, year = {{2021}}, } @article{62851, abstract = {{To reduce high-level radiotoxic waste generated by nuclear power plants, highly selective separation agents for minor actinides are mandatory. The mixed N,O-donor ligand N,N,N′,N′-tetrakis[(6-carboxypyridin-2-yl)methyl]ethylenediamine (H4TPAEN; 1) has shown good performance as a masking agent in Am3+/Eu3+ separation studies. Adjustments on the pyridyl backbone to raise the hydrophilicity led to a decrease in selectivity and a decrease in M3+–Nam interactions. An enhanced basicity of the pyridyl N-donors was given as a cause. In this work, we examine whether a decrease in O-donor basicity can promote the M3+–Nam interactions. Therefore, we replace the deprotonated “charged” carboxylic acid groups of TPAEN4– by neutral amide groups and introduce N,N,N′,N’-tetrakis[(6-N″,N′′-diethylcarbamoylpyridin-2-yl)methyl]ethylenediamine (TPAMEN; 2) as a new ligand. TPAMEN was crystallized with Eu(OTf)3 and Eu(NO3)3·6H2O to form positively charged 1:1 [Eu(TPAMEN)]3+ complexes in the solid state. Alterations in the M–O/N bond distances are compared to [Eu(TPAEN)]− and investigated by DFT calculations to expose the differences in charge/energy density distributions at europium(III) and the donor functionalities of the TPAEN4– and TPAMEN. On the basis of estimations of the bond orders, atomic charges spin populations, and density of states in the Eu and potential Am and Cm complexes, the specific contributions of the donor–metal interaction are analyzed. The prediction of complex formation energy differences for the [M(TPAEN)]− and [M(TPAMEN)]3+ (M3+ = Eu3+, Am3+) complexes provide an outlook on the potential performance of TPAMEN in Am3+/Eu3+ separation.}}, author = {{Schnaars, Kathleen and Kaneko, Masashi and Fujisawa, Kiyoshi}}, issn = {{0020-1669}}, journal = {{Inorganic Chemistry}}, number = {{4}}, pages = {{2477--2491}}, publisher = {{American Chemical Society (ACS)}}, title = {{{Effect of Oxygen-Donor Charge on Adjacent Nitrogen-Donor Interactions in Eu3+ Complexes of Mixed N,O-Donor Ligands Demonstrated on a 10-Fold [Eu(TPAMEN)]3+ Chelate Complex}}}, doi = {{10.1021/acs.inorgchem.0c03405}}, volume = {{60}}, year = {{2021}}, } @article{25301, author = {{Scherer, Beate and Kottenstedde, Ingo Leonard and Bremser, Wolfgang and Matysik, Frank-Michael}}, issn = {{0142-9418}}, journal = {{Polymer Testing}}, title = {{{Analytical characterization of polyamide 11 used in the context of selective laser sintering: Physico-chemical correlations}}}, doi = {{10.1016/j.polymertesting.2020.106786}}, year = {{2020}}, } @article{23599, abstract = {{Grazing-incidence wide-angle X-ray scattering (GIWAXS) has become an increasingly popular technique for quantitative structural characterization and comparison of thin films. For this purpose, accurate intensity normalization and peak position determination are crucial. At present, few tools exist to estimate the uncertainties of these measurements. Here, a simulation package is introduced called GIWAXS-SIIRkit, where SIIR stands for scattering intensity, indexing and refraction. The package contains several tools that are freely available for download and can be executed in MATLAB. The package includes three functionalities: estimation of the relative scattering intensity and the corresponding uncertainty based on experimental setup and sample dimensions; extraction and indexing of peak positions to approximate the crystal structure of organic materials starting from calibrated GIWAXS patterns; and analysis of the effects of refraction on peak positions. Each tool is based on a graphical user interface and designed to have a short learning curve. A user guide is provided with detailed usage instruction, tips for adding functionality and customization, and exemplary files.}}, author = {{Savikhin, Victoria and Steinrück, Hans-Georg and Liang, Ru-Ze and Collins, Brian A. and Oosterhout, Stefan D. and Beaujuge, Pierre M. and Toney, Michael F.}}, issn = {{1600-5767}}, journal = {{Journal of Applied Crystallography}}, pages = {{1108--1129}}, title = {{{GIWAXS-SIIRkit: scattering intensity, indexing and refraction calculation toolkit for grazing-incidence wide-angle X-ray scattering of organic materials}}}, doi = {{10.1107/s1600576720005476}}, volume = {{53}}, year = {{2020}}, } @article{23600, author = {{Gebers, Jan and Özen, Bilal and Hartmann, Lucia and Schaer, Michel and Suàrez, Stéphane and Bugnon, Philippe and Scopelliti, Rosario and Steinrück, Hans-Georg and Konovalov, Oleg and Magerl, Andreas and Brinkmann, Martin and Petraglia, Riccardo and Silva, Piotr and Corminboeuf, Clémence and Frauenrath, Holger}}, issn = {{0947-6539}}, journal = {{Chemistry – A European Journal}}, pages = {{10265--10275}}, title = {{{Crystallization and Organic Field‐Effect Transistor Performance of a Hydrogen‐Bonded Quaterthiophene}}}, doi = {{10.1002/chem.201904562}}, volume = {{26}}, year = {{2020}}, } @article{23601, author = {{Abdelsamie, Maged and Xu, Junwei and Bruening, Karsten and Tassone, Christopher J. and Steinrück, Hans-Georg and Toney, Michael F.}}, issn = {{1616-301X}}, journal = {{Advanced Functional Materials}}, pages = {{2001752}}, title = {{{Impact of Processing on Structural and Compositional Evolution in Mixed Metal Halide Perovskites during Film Formation}}}, doi = {{10.1002/adfm.202001752}}, volume = {{30}}, year = {{2020}}, } @article{23602, author = {{Tanim, Tanvir R. and Paul, Partha P. and Thampy, Vivek and Cao, Chuntian and Steinrück, Hans-Georg and Nelson Weker, Johanna and Toney, Michael F. and Dufek, Eric J. and Evans, Michael C. and Jansen, Andrew N. and Polzin, Bryant J. and Dunlop, Alison R. and Trask, Stephen E.}}, issn = {{2666-3864}}, journal = {{Cell Reports Physical Science}}, pages = {{100114}}, title = {{{Heterogeneous Behavior of Lithium Plating during Extreme Fast Charging}}}, doi = {{10.1016/j.xcrp.2020.100114}}, volume = {{1}}, year = {{2020}}, } @article{23603, author = {{Bone, Sharon E. and Steinrück, Hans-Georg and Toney, Michael F.}}, issn = {{2542-4351}}, journal = {{Joule}}, pages = {{1637--1659}}, title = {{{Advanced Characterization in Clean Water Technologies}}}, doi = {{10.1016/j.joule.2020.06.020}}, volume = {{4}}, year = {{2020}}, } @article{23604, abstract = {{

Investigation of the mechanisms underlying control of electrodeposited lithium metal morphology using electrolyte additives in lithium metal batteries.

}}, author = {{Kasse, Robert M. and Geise, Natalie R. and Ko, Jesse S. and Nelson Weker, Johanna and Steinrück, Hans-Georg and Toney, Michael F.}}, issn = {{2050-7488}}, journal = {{Journal of Materials Chemistry A}}, pages = {{16960--16972}}, title = {{{Understanding additive controlled lithium morphology in lithium metal batteries}}}, doi = {{10.1039/d0ta06020h}}, volume = {{8}}, year = {{2020}}, } @article{23605, author = {{Paulsen, Bryan D. and Wu, Ruiheng and Takacs, Christopher J. and Steinrück, Hans-Georg and Strzalka, Joseph and Zhang, Qingteng and Toney, Michael F. and Rivnay, Jonathan}}, issn = {{0935-9648}}, journal = {{Advanced Materials}}, pages = {{2003404}}, title = {{{Time‐Resolved Structural Kinetics of an Organic Mixed Ionic–Electronic Conductor}}}, doi = {{10.1002/adma.202003404}}, volume = {{32}}, year = {{2020}}, } @article{23606, author = {{Steinrück, Hans-Georg and Cao, Chuntian and Lukatskaya, Maria R. and Takacs, Christopher J. and Wan, Gang and Mackanic, David G. and Tsao, Yuchi and Zhao, Jingbo and Helms, Brett A. and Xu, Kang and Borodin, Oleg and Wishart, James F. and Toney, Michael F.}}, issn = {{1433-7851}}, journal = {{Angewandte Chemie International Edition}}, pages = {{23180--23187}}, title = {{{Interfacial Speciation Determines Interfacial Chemistry: X‐ray‐Induced Lithium Fluoride Formation from Water‐in‐salt Electrolytes on Solid Surfaces}}}, doi = {{10.1002/anie.202007745}}, volume = {{59}}, year = {{2020}}, } @article{23607, abstract = {{

Direct measurements of concentration and velocity profiles in a polymeric lithium-ion battery electrolyte provide insights into the transference number.

}}, author = {{Steinrück, Hans-Georg and Takacs, Christopher J. and Kim, Hong-Keun and Mackanic, David G. and Holladay, Benjamin and Cao, Chuntian and Narayanan, Suresh and Dufresne, Eric M. and Chushkin, Yuriy and Ruta, Beatrice and Zontone, Federico and Will, Johannes and Borodin, Oleg and Sinha, Sunil K. and Srinivasan, Venkat and Toney, Michael F.}}, issn = {{1754-5692}}, journal = {{Energy & Environmental Science}}, pages = {{4312--4321}}, title = {{{Concentration and velocity profiles in a polymeric lithium-ion battery electrolyte}}}, doi = {{10.1039/d0ee02193h}}, volume = {{13}}, year = {{2020}}, } @article{23608, author = {{Prihoda, Annemarie and Will, Johannes and Duchstein, Patrick and Becit, Bahanur and Lossin, Felix and Schindler, Torben and Berlinghof, Marvin and Steinrück, Hans-Georg and Bertram, Florian and Zahn, Dirk and Unruh, Tobias}}, issn = {{0743-7463}}, journal = {{Langmuir}}, pages = {{12077--12086}}, title = {{{Interface between Water–Solvent Mixtures and a Hydrophobic Surface}}}, doi = {{10.1021/acs.langmuir.0c02745}}, volume = {{36}}, year = {{2020}}, } @article{23617, author = {{Chen, Hao and Pei, Allen and Wan, Jiayu and Lin, Dingchang and Vilá, Rafael and Wang, Hongxia and Mackanic, David and Steinrück, Hans-Georg and Huang, William and Li, Yuzhang and Yang, Ankun and Xie, Jin and Wu, Yecun and Wang, Hansen and Cui, Yi}}, issn = {{2542-4351}}, journal = {{Joule}}, pages = {{938--952}}, title = {{{Tortuosity Effects in Lithium-Metal Host Anodes}}}, doi = {{10.1016/j.joule.2020.03.008}}, volume = {{4}}, year = {{2020}}, } @article{23618, author = {{Steinrück, Hans-Georg and Cao, Chuntian and Veith, Gabriel M. and Toney, Michael F.}}, issn = {{0021-9606}}, journal = {{The Journal of Chemical Physics}}, pages = {{084702}}, title = {{{Toward quantifying capacity losses due to solid electrolyte interphase evolution in silicon thin film batteries}}}, doi = {{10.1063/1.5142643}}, volume = {{152}}, year = {{2020}}, } @article{22644, abstract = {{The aggregation of human islet amyloid polypeptide (hIAPP) plays a major role in the pathogenesis of type 2 diabetes mellitus (T2DM), and numerous strategies for controlling hIAPP aggregation have been investigated so far. In particular, several organic and inorganic nanoparticles (NPs) have shown the potential to influence the aggregation of hIAPP and other amyloidogenic proteins and peptides. In addition to conventional NPs, DNA nanostructures are receiving more and more attention from the biomedical field. Therefore, in this work, we investigated the effects of two different DNA origami nanostructures on hIAPP aggregation. To this end, we employed in situ turbidity measurements and ex situ atomic force microscopy (AFM). The turbidity measurements revealed a retarding effect of the DNA nanostructures on hIAPP aggregation, while the AFM results showed the co-aggregation of hIAPP with the DNA origami nanostructures into hybrid peptide–DNA aggregates. We assume that this was caused by strong electrostatic interactions between the negatively charged DNA origami nanostructures and the positively charged peptide. Most intriguingly, the influence of the DNA origami nanostructures on hIAPP aggregation differed from that of genomic double-stranded DNA (dsDNA) and appeared to depend on DNA origami superstructure. DNA origami nanostructures may thus represent a novel route for modulating amyloid aggregation in vivo.}}, author = {{Hanke, Marcel and Gonzalez Orive, Alejandro and Grundmeier, Guido and Keller, Adrian}}, issn = {{2079-4991}}, journal = {{Nanomaterials}}, pages = {{2200}}, title = {{{Effect of DNA Origami Nanostructures on hIAPP Aggregation}}}, doi = {{10.3390/nano10112200}}, volume = {{10}}, year = {{2020}}, } @article{22645, abstract = {{Immobile Holliday junctions represent not only the most fundamental building block of structural DNA nanotechnology but are also of tremendous importance for the in vitro investigation of genetic recombination and epigenetics. Here, we present a detailed study on the room-temperature assembly of immobile Holliday junctions with the help of the single-strand annealing protein Redβ. Individual DNA single strands are initially coated with protein monomers and subsequently hybridized to form a rigid blunt-ended four-arm junction. We investigate the efficiency of this approach for different DNA/protein ratios, as well as for different DNA sequence lengths. Furthermore, we also evaluate the potential of Redβ to anneal sticky-end modified Holliday junctions into hierarchical assemblies. We demonstrate the Redβ-mediated annealing of Holliday junction dimers, multimers, and extended networks several microns in size. While these hybrid DNA–protein nanostructures may find applications in the crystallization of DNA–protein complexes, our work shows the great potential of Redβ to aid in the synthesis of functional DNA nanostructures under mild reaction conditions.}}, author = {{Ramakrishnan, Saminathan and Subramaniam, Sivaraman and Kielar, Charlotte and Grundmeier, Guido and Stewart, A. Francis and Keller, Adrian}}, issn = {{1420-3049}}, journal = {{Molecules}}, pages = {{5099}}, title = {{{Protein-Assisted Room-Temperature Assembly of Rigid, Immobile Holliday Junctions and Hierarchical DNA Nanostructures}}}, doi = {{10.3390/molecules25215099}}, volume = {{25}}, year = {{2020}}, } @article{22646, abstract = {{Abstract The surface-assisted hierarchical self-assembly of DNA origami lattices represents a versatile and straightforward method for the organization of functional nanoscale objects such as proteins and nanoparticles. Here, we demonstrate that controlling the binding and exchange of different monovalent and divalent cation species at the DNA-mica interface enables the self-assembly of highly ordered DNA origami lattices on mica surfaces. The development of lattice quality and order is quantified by a detailed topological analysis of high-speed atomic force microscopy (HS-AFM) images. We find that lattice formation and quality strongly depend on the monovalent cation species. Na+ is more effective than Li+ and K+ in facilitating the assembly of high-quality DNA origami lattices, because it is replacing the divalent cations at their binding sites in the DNA backbone more efficiently. With regard to divalent cations, Ca2+ can be displaced more easily from the backbone phosphates than Mg2+ and is thus superior in guiding lattice assembly. By independently adjusting incubation time, DNA origami concentration, and cation species, we thus obtain a highly ordered DNA origami lattice with an unprecedented normalized correlation length of 8.2. Beyond the correlation length, we use computer vision algorithms to compute the time course of different topological observables that, overall, demonstrate that replacing MgCl2 by CaCl2 enables the synthesis of DNA origami lattices with drastically increased lattice order.}}, author = {{Xin, Yang and Martinez Rivadeneira, Salvador and Grundmeier, Guido and Castro, Mario and Keller, Adrian}}, issn = {{1998-0124}}, journal = {{Nano Research}}, pages = {{3142--3150}}, title = {{{Self-assembly of highly ordered DNA origami lattices at solid-liquid interfaces by controlling cation binding and exchange}}}, doi = {{10.1007/s12274-020-2985-4}}, volume = {{13}}, year = {{2020}}, }