@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} } @article{YangHuDingetal.2018, author = {Yang, Guang and Hu, Rongting and Ding, Hong-ming and Kochovski, Zdravko and Mei, Shilin and Lu, Yan and Ma, Yu-qiang and Chen, Guosong and Jiang, Ming}, title = {CO2-switchable response of protein microtubules}, series = {Materials chemistry frontiers}, volume = {2}, journal = {Materials chemistry frontiers}, number = {9}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {2052-1537}, doi = {10.1039/c8qm00245b}, pages = {1642 -- 1646}, year = {2018}, abstract = {Recently, we proposed a small molecular inducing ligand strategy to assemble proteins into highly-ordered structures via dual non-covalent interactions, i.e. carbohydrate-protein interaction and dimerization of Rhodamine B. Using this approach, artificial protein microtubules were successfully constructed. In this study, we find that these microtubules exhibit a perfect CO2 responsiveness; assembly and disassembly of these microtubules were nicely controlled by the alternative passage of CO2 and N-2. Upon the injection of CO2, a negative net-charged SBA turns into a neutral or positive net-charged SBA, which elongated, to some extent, the effective distance between SBA and Rhodamine B, resulting in the disassociation of the Rhodamine B dimer. Further experimental and simulation results reveal that the CO2-responsive mechanism differs from that of solubility change of the previously reported CO2-responsive synthetic materials.}, 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{JiaFriebeSchubertetal.2019, author = {Jia, He and Friebe, Christian and Schubert, Ulrich S. and Zhang, Xiaozhe and Quan, Ting and Lu, Yan and Gohy, Jean-Francois}, title = {Core-Shell Nanoparticles with a Redox Polymer Core and a Silica Porous Shell as High-Performance Cathode Material for Lithium-Ion Batteries}, series = {Energy technology : generation, conversion, storage, distribution}, volume = {8}, journal = {Energy technology : generation, conversion, storage, distribution}, number = {3}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2194-4288}, doi = {10.1002/ente.201901040}, pages = {8}, year = {2019}, abstract = {A facile and novel method for the fabrication of core-shell nanoparticles (PTMA@SiO2) based on a poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl methacrylate) (PTMA) core and a porous SiO2 shell is reported. The core-shell nanoparticles are further self-assembled with negatively charged multi-walled carbon nanotubes (MWCNTs), which results in the formation of a free-standing cathode electrode. The porous SiO2 shell not only effectively improves the stability of the linear PTMA redox polymer with low molar mass in organic electrolytes but also leads to the uniform dispersion of PTMA active units in the MWCNTs conductive network. The PTMA@SiO2@MWCNT composite electrode exhibits a specific capacity as high as 73.8 mAh g at 1 C and only 0.11\% capacity loss per cycle at a rate of 2 C.}, language = {en} } @article{JiaQuanLiuetal.2019, author = {Jia, He and Quan, Ting and Liu, Xuelian and Bai, Lu and Wang, Jiande and Boujioui, Fadoi and Ye, Ran and Vald, Alexandru and Lu, Yan and Gohy, Jean-Francois}, title = {Core-shell nanostructured organic redox polymer cathodes with superior performance}, series = {Nano Energy}, volume = {64}, journal = {Nano Energy}, publisher = {Elsevier}, address = {Amsterdam}, issn = {2211-2855}, doi = {10.1016/j.nanoen.2019.103949}, pages = {9}, year = {2019}, abstract = {Core-shell nanoparticles stabilized by a cationic surfactant are prepared from the poly(2,2,6,6-tetra-methylpiperidinyloxy-4-yl methacrylate) redox polymer. The nanoparticles are further self-assembled with negatively charged reduced graphene oxide nanosheets and negatively charged mull-walled carbon nanotubes. This results in the formation of a free-standing cathode with a layered nanostructure and a high content of redox polymer that exhibits 100\% utilization of the active substance with a measured capacity as high as 105 mAh/g based on the whole weight of the electrode.}, language = {en} } @article{SunOsenbergDongetal.2018, author = {Sun, Fu and Osenberg, Markus and Dong, Kang and Zhou, Dong and Hilger, Andre and Jafta, Charl J. and Risse, Sebastian and Lu, Yan and Markoetter, Henning and Manke, Ingo}, title = {Correlating Morphological Evolution of Li Electrodes with Degrading Electrochemical Performance of Li/LiCoO2 and Li/S Battery Systems}, series = {ACS energy letters / American Chemical Society}, volume = {3}, journal = {ACS energy letters / American Chemical Society}, number = {2}, publisher = {American Chemical Society}, address = {Washington}, issn = {2380-8195}, doi = {10.1021/acsenergylett.7b01254}, pages = {356 -- 365}, year = {2018}, abstract = {Efficient Li utilization is generally considered to be a prerequisite for developing next-generation energy storage systems (ESSs). However, uncontrolled growth of Li microstructures (LmSs) during electrochemical cycling has prevented its practical commercialization. Herein, we attempt to understand the correlation of morphological evolution of Li electrodes with degrading electrochemical performances of Li/LiCoO2 and Li/S systems by synchrotron X-ray phase contrast tomography technique. It was found that the continuous transformation of the initial dense Li bulk to a porous lithium interface (PL1) structure intimately correlates with the gradually degrading overall cell performance of these two systems. Additionally, the formation mechanism of the PLI and its correlation with previously reported inwardly growing LmS and the lithium-reacted region have been intensively discussed. The information that we gain herein is complementary to previous investigations and may provide general insights into understanding of degradation mechanisms of Li metal anodes and also provide highly needed guidelines for effective design of reliable next-generation Li metal-based ESSs.}, language = {en} } @article{KochovskiChenYuanetal.2020, author = {Kochovski, Zdravko and Chen, Guosong and Yuan, Jiayin and Lu, Yan}, title = {Cryo-Electron microscopy for the study of self-assembled poly(ionic liquid) nanoparticles and protein supramolecular structures}, series = {Colloid and polymer science : official journal of the Kolloid-Gesellschaft}, volume = {298}, journal = {Colloid and polymer science : official journal of the Kolloid-Gesellschaft}, number = {7}, publisher = {Springer}, address = {New York}, issn = {0303-402X}, doi = {10.1007/s00396-020-04657-w}, pages = {707 -- 717}, year = {2020}, abstract = {Cryo-electron microscopy (cryo-EM) is a powerful structure determination technique that is well-suited to the study of protein and polymer self-assembly in solution. In contrast to conventional transmission electron microscopy (TEM) sample preparation, which often times involves drying and staining, the frozen-hydrated sample preparation allows the specimens to be kept and imaged in a state closest to their native one. Here, we give a short overview of the basic principles of Cryo-EM and review our results on applying it to the study of different protein and polymer self-assembled nanostructures. More specifically, we show how we have applied cryo-electron tomography (cryo-ET) to visualize the internal morphology of self-assembled poly(ionic liquid) nanoparticles and cryo-EM single particle analysis (SPA) to determine the three-dimensional (3D) structures of artificial protein microtubules.}, language = {en} } @article{JiaGaoMeietal.2018, author = {Jia, He and Gao, Haitao and Mei, Shilin and Kneer, Janosch and Lin, Xianzhong and Ran, Qidi and Wang, Fuxian and Palzer, Stefan and Lu, Yan}, title = {Cu2O@PNIPAM core-shell microgels as novel inkjet materials for the preparation of CuO hollow porous nanocubes gas sensing layers}, series = {Journal of materials chemistry : C, Materials for optical and electronic devices}, volume = {6}, journal = {Journal of materials chemistry : C, Materials for optical and electronic devices}, number = {27}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {2050-7526}, doi = {10.1039/c8tc01995a}, pages = {7249 -- 7256}, year = {2018}, abstract = {There has been long-standing interest in developing metal oxide-based sensors with high sensitivity, selectivity, fast response and low material consumption. Here we report for the first time the utilization of Cu2O@PNIPAM core-shell microgels with a nanocube-shaped core structure for construction of novel CuO gas sensing layers. The hybrid microgels show significant improvement in colloidal stability as compared to native Cu2O nanocubes. Consequently, a homogeneous thin film of Cu2O@PNIPAM nanoparticles can be engineered in a quite low solid content (1.5 wt\%) by inkjet printing of the dispersion at an optimized viscosity and surface tension. Most importantly, thermal treatment of the Cu2O@PNIPAM microgels forms porous CuO nanocubes, which show much faster response to relevant trace NO2 gases than sensors produced from bare Cu2O nanocubes. This outcome is due to the fact that the PNIPAM shell can successfully hinder the aggregation of CuO nanoparticles during pyrolysis, which enables full utilization of the sensor layers and better access of the gas to active sites. These results point out great potential of such an innovative system as gas sensors with low cost, fast response and high sensitivity.}, language = {en} } @article{YuantenBrummelhuisJungingeretal.2011, author = {Yuan, Jiayin and ten Brummelhuis, Niels and Junginger, Mathias and Xie, Zailai and Lu, Yan and Taubert, Andreas and Schlaad, Helmut}, title = {Diversified applications of chemically modified 1,2-Polybutadiene}, series = {Macromolecular rapid communications}, volume = {32}, journal = {Macromolecular rapid communications}, number = {15}, publisher = {Wiley-Blackwell}, address = {Malden}, issn = {1022-1336}, doi = {10.1002/marc.201100254}, pages = {1157 -- 1162}, year = {2011}, abstract = {Commercially available 1,2-PB was transformed into a well-defined reactive intermediate by quantitative bromination. The brominated polymer was used as a polyfunctional macroinitiator for the cationic ring-opening polymerization of 2-ethyl-2-oxazoline to yield a water-soluble brush polymer. Nucleophilic substitution of bromide by 1-methyl imidazole resulted in the formation of polyelectrolyte copolymers consisting of mixed units of imidazolium, bromo, and double bond. These copolymers, which were soluble in water without forming aggregates, were used as stabilizers in the heterophase polymerization of styrene and were also studied for their ionic conducting properties.}, language = {en} } @article{YangZhengTaoetal.2019, author = {Yang, Guang and Zheng, Wei and Tao, Guoqing and Wu, Libin and Zhou, Qi-Feng and Kochovski, Zdravko and Ji, Tan and Chen, Huaijun and Li, Xiaopeng and Lu, Yan and Ding, Hong-ming and Yang, Hai-Bo and Chen, Guosong and Jiang, Ming}, title = {Diversiform and Transformable Glyco-Nanostructures Constructed from Amphiphilic Supramolecular Metallocarbohydrates through Hierarchical Self-Assembly: The Balance between Metallacycles and Saccharides}, series = {ACS nano}, volume = {13}, journal = {ACS nano}, number = {11}, publisher = {American Chemical Society}, address = {Washington}, issn = {1936-0851}, doi = {10.1021/acsnano.9b07134}, pages = {13474 -- 13485}, year = {2019}, abstract = {During the past decade, self-assembly of saccharide-containing amphiphilic molecules toward bioinspired functional glycomaterials has attracted continuous attention due to their various applications in fundamental and practical areas. However, it still remains a great challenge to prepare hierarchical glycoassemblies with controllable and diversiform structures because of the complexity of saccharide structures and carbohydrate-carbohydrate interactions. Herein, through hierarchical self-assembly of modulated amphiphilic supramolecular metallocarbohydrates, we successfully prepared various well-defined glyco-nanostructures in aqueous solution, including vesicles, solid spheres, and opened vesicles depending on the molecular structures of metallocarbohydrates. More attractively, these glyco-nanostructures can further transform into other morphological structures in aqueous solutions such as worm-like micelles, tubules, and even tupanvirus-like vesicles (TVVs). It is worth mentioning that distinctive anisotropic structures including the opened vesicles (OVs) and TVVs were rarely reported in glycobased nano-objects. This intriguing diversity was mainly controlled by the subtle structural trade-off of the two major components of the amphiphiles, i.e., the saccharides and metallacycles. To further understand this precise structural control, molecular simulations provided deep physical insights on the morphology evolution and balancing of the contributions from saccharides and metallacycles. Moreover, the multivalency of glyco-nanostructures with different shapes and sizes was demonstrated by agglutination with a diversity of sugarbinding protein receptors such as the plant lectins Concanavalin A (ConA). This modular synthesis strategy provides access to systematic tuning of molecular structure and self-assembled architecture, which undoubtedly will broaden our horizons on the controllable fabrication of biomimetic glycomaterials such as biological membranes and supramolecular lectin inhibitors.}, language = {en} } @article{XieMeiXuetal.2021, author = {Xie, Dongjiu and Mei, Shilin and Xu, Yaolin and Quan, Ting and Haerk, Eneli and Kochovski, Zdravko and Lu, Yan}, title = {Efficient sulfur host based on yolk-shell iron oxide/sulfide-carbon nanospindles for lithium-sulfur batteries}, series = {ChemSusChem : chemistry, sustainability, energy, materials}, volume = {14}, journal = {ChemSusChem : chemistry, sustainability, energy, materials}, number = {5}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1864-5631}, doi = {10.1002/cssc.202002731}, pages = {1404 -- 1413}, year = {2021}, abstract = {Numerous nanostructured materials have been reported as efficient sulfur hosts to suppress the problematic "shuttling" of lithium polysulfides (LiPSs) in lithium-sulfur (Li-S) batteries. However, direct comparison of these materials in their efficiency of suppressing LiPSs shuttling is challenging, owing to the structural and morphological differences between individual materials. This study introduces a simple route to synthesize a series of sulfur host materials with the same yolk-shell nanospindle morphology but tunable compositions (Fe3O4, FeS, or FeS2), which allows for a systematic investigation into the specific effect of chemical composition on the electrochemical performances of Li-S batteries. Among them, the S/FeS2-C electrode exhibits the best performance and delivers an initial capacity of 877.6 mAh g(-1) at 0.5 C with a retention ratio of 86.7 \% after 350 cycles. This approach can also be extended to the optimization of materials for other functionalities and applications.}, language = {en} } @article{MeiKochovskiRoaetal.2019, author = {Mei, Shilin and Kochovski, Zdravko and Roa, Rafael and Gu, Sasa and Xu, Xiaohui and Yu, Hongtao and Dzubiella, Joachim and Ballauff, Matthias and Lu, Yan}, title = {Enhanced Catalytic Activity of Gold@Polydopamine Nanoreactors with Multi-compartment Structure Under NIR Irradiation}, series = {Nano-Micro Letters}, volume = {11}, journal = {Nano-Micro Letters}, number = {1}, publisher = {Shanghai JIAO TONG univ press}, address = {Shanghai}, issn = {2311-6706}, doi = {10.1007/s40820-019-0314-9}, pages = {16}, year = {2019}, abstract = {Photothermal conversion (PTC) nanostructures have great potential for applications in many fields, and therefore, they have attracted tremendous attention. However, the construction of a PTC nanoreactor with multi-compartment structure to achieve the combination of unique chemical properties and structural feature is still challenging due to the synthetic difficulties. Herein, we designed and synthesized a catalytically active, PTC gold (Au)@polydopamine (PDA) nanoreactor driven by infrared irradiation using assembled PS-b-P2VP nanosphere as soft template. The particles exhibit multi-compartment structure which is revealed by 3D electron tomography characterization technique. They feature permeable shells with tunable shell thickness. Full kinetics for the reduction reaction of 4-nitrophenol has been investigated using these particles as nanoreactors and compared with other reported systems. Notably, a remarkable acceleration of the catalytic reaction upon near-infrared irradiation is demonstrated, which reveals for the first time the importance of the synergistic effect of photothermal conversion and complex inner structure to the kinetics of the catalytic reduction. The ease of synthesis and fresh insights into catalysis will promote a new platform for novel nanoreactor studies.}, language = {en} } @article{SungKochovskiZhangetal.2017, author = {Sung, Jian-Ke and Kochovski, Zdravko and Zhang, Wei-Yi and Kirmse, Holm and Lu, Yan and Antonietti, Markus and Yuan, Jiayin}, title = {General Synthetic Route toward Highly Dispersed Metal Clusters Enabled by Poly(ionic liquid)s}, series = {Journal of the American Chemical Society}, volume = {139}, journal = {Journal of the American Chemical Society}, publisher = {American Chemical Society}, address = {Washington}, issn = {0002-7863}, doi = {10.1021/jacs.7b03357}, pages = {8971 -- 8976}, year = {2017}, abstract = {The ability to synthesize a broad spectrum of metal clusters (MCs) with their size controllable on a subnanometer scale presents an enticing prospect for exploring nanosize-dependent properties. Here we report an innovative design of a capping agent from a polytriazolium poly(ionic liquid) (PIL) in a vesicular form in solution that allows for crafting a variety of MCs including transition metals, noble metals, and their bimetallic alloy with precisely controlled sizes (similar to 1 nm) and record-high catalytic performance. The ultrastrong stabilization power is a result of an unusual synergy between the conventional binding sites in the heterocyclic cations in PIL and an in situ generated polycarbene structure induced simultaneously to the reduction reaction.}, language = {en} } @article{QuanGoubardBretescheHaerketal.2019, author = {Quan, Ting and Goubard-Bretesche, Nicolas and Haerk, Eneli and Kochovski, Zdravko and Mei, Shilin and Pinna, Nicola and Ballauff, Matthias and Lu, Yan}, title = {Highly Dispersible Hexagonal Carbon-MoS2-Carbon Nanoplates with Hollow Sandwich Structures for Supercapacitors}, series = {Chemistry - a European journal}, volume = {25}, journal = {Chemistry - a European journal}, number = {18}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {0947-6539}, doi = {10.1002/chem.201806060}, pages = {4757 -- 4766}, year = {2019}, abstract = {MoS2, a typical layered transition-metal dichalcogenide, is promising as an electrode material in supercapacitors. However, its low electrical conductivity could lead to limited capacitance if applied in electrochemical devices. Herein, a new nanostructure composed of hollow carbon-MoS2-carbon was successfully synthesized through an L-cysteine-assisted hydrothermal method by using gibbsite as a template and polydopamine as a carbon precursor. After calcination and etching of the gibbsite template, uniform hollow platelets, which were made of a sandwich-like assembly of partial graphitic carbon and two-dimensional layered MoS2 flakes, were obtained. The platelets showed excellent dispersibility and stability in water, and good electrical conductivity due to carbon provided by the calcination of polydopamine coatings. The hollow nanoplate morphology of the material provided a high specific surface area of 543 m(2) g(-1), a total pore volume of 0.677 cm(3) g(-1), and fairly small mesopores (approximate to 5.3 nm). The material was applied in a symmetric supercapacitor and exhibited a specific capacitance of 248 F g(-1) (0.12 F cm(-2)) at a constant current density of 0.1 Ag-1; thus suggesting that hollow carbon-MoS2 carbon nanoplates are promising candidate materials for supercapacitors.}, language = {en} } @article{YangDingKochovskietal.2017, author = {Yang, Guang and Ding, Hong-ming and Kochovski, Zdravko and Hu, Rongting and Lu, Yan and Ma, Yu-qiang and Chen, Guosong and Jiang, Ming}, title = {Highly Ordered Self-Assembly of Native Proteins into 1D, 2D, and 3D Structures Modulated by the Tether Length of Assembly-Inducing Ligands}, series = {Angewandte Chemie : a journal of the Gesellschaft Deutscher Chemiker ; International edition}, volume = {56}, journal = {Angewandte Chemie : a journal of the Gesellschaft Deutscher Chemiker ; International edition}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1433-7851}, doi = {10.1002/anie.201703052}, pages = {10691 -- 10695}, year = {2017}, abstract = {In nature, proteins self-assemble into various structures with different dimensions. To construct these nanostructures in laboratories, normally proteins with different symmetries are selected. However, most of these approaches are engineering-intensive and highly dependent on the accuracy of the protein design. Herein, we report that a simple native protein LecA assembles into one-dimensional nanoribbons and nanowires, two-dimensional nanosheets, and three-dimensional layered structures controlled mainly by small-molecule assembly-inducing ligands RnG (n = 1, 2, 3, 4, 5) with varying numbers of ethylene oxide repeating units. To understand the formation mechanism of the different morphologies controlled by the small-molecule structure, molecular simulations were performed from microscopic and mesoscopic view, which presented a clear relationship between the molecular structure of the ligands and the assembled patterns. These results introduce an easy strategy to control the assembly structure and dimension, which could shed light on controlled protein assembly.}, language = {en} } @article{XuAngiolettiUbertiLuetal.2018, author = {Xu, Xiao and Angioletti-Uberti, Stefano and Lu, Yan and Dzubiella, Joachim and Ballauff, Matthias}, title = {Interaction of Proteins with Polyelectrolytes}, series = {Langmuir}, volume = {35}, journal = {Langmuir}, number = {16}, publisher = {American Chemical Society}, address = {Washington}, issn = {0743-7463}, doi = {10.1021/acs.langmuir.8b01802}, pages = {5373 -- 5391}, year = {2018}, abstract = {We discuss recent investigations of the interaction of polyelectrolytes with proteins. In particular, we review our recent studies on the interaction of simple proteins such as human serum albumin (HSA) and lysozyme with linear polyelectrolytes, charged dendrimers, charged networks, and polyelectrolyte brushes. In all cases discussed here, we combined experimental work with molecular dynamics (MD) simulations and mean-field theories. In particular, isothermal titration calorimetry (ITC) has been employed to obtain the respective binding constants K-b and the Gibbs free energy of binding. MD simulations with explicit counterions but implicit water demonstrate that counterion release is the main driving force for the binding of proteins to strongly charged polyelectrolytes: patches of positive charges located on the surface of the protein become multivalent counterions of the polyelectrolyte, thereby releasing a number of counterions condensed on the polyelectrolyte. The binding Gibbs free energy due to counterion release is predicted to scale with the logarithm of the salt concentration in the system, which is verified by both simulations and experiment. In several cases, namely, for the interaction of proteins with linear polyelectrolytes and highly charged hydrophilic dendrimers, the binding constant could be calculated from simulations to very good approximation. This finding demonstrated that in these cases explicit hydration effects do not contribute to the Gibbs free energy of binding. The Gibbs free energy can also be used to predict the kinetics of protein uptake by microgels for a given system by applying dynamic density functional theory. The entire discussion demonstrates that the direct comparison of theory with experiments can lead to a full understanding of the interaction of proteins with charged polymers. Possible implications for applications, such as drug design, are discussed.}, language = {en} } @article{ZhangKochovskiLeeetal.2019, author = {Zhang, Su-Yun and Kochovski, Zdravko and Lee, Hui-Chun and Lu, Yan and Zhang, Hemin and Zhang, Jie and Sun, Jian-Ke and Yuan, Jiayin}, title = {Ionic organic cage-encapsulating phase-transferable metal clusters}, series = {Chemical science}, volume = {10}, journal = {Chemical science}, number = {5}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {2041-6520}, doi = {10.1039/c8sc04375b}, pages = {1450 -- 1456}, year = {2019}, abstract = {Exploration of metal clusters (MCs) adaptive to both aqueous and oil phases without disturbing their size is promising for a broad scope of applications. The state-of-the-art approach via ligand-binding may perturb MCs' size due to varied metal-ligand binding strength when shuttling between solvents of different polarity. Herein, we applied physical confinement of a series of small noble MCs (<1 nm) inside ionic organic cages (I-Cages), which by means of anion exchange enables reversible transfer of MCs between aqueous and hydrophobic solutions without varying their ultrasmall size. Moreover, the MCs@I-Cage hybrid serves as a recyclable, reaction-switchable catalyst featuring high activity in liquid-phase NH3BH3 (AB) hydrolysis reaction with a turnover frequency (TOF) of 115 min-1.}, 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{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{GuRisseLuetal.2019, author = {Gu, Sasa and Risse, Sebastian and Lu, Yan and Ballauff, Matthias}, title = {Mechanism of the oxidation of 3,3′,5,5′-tetramethylbenzidine catalyzed by peroxidase-like Pt nanoparticles immobilized in spherical polyelectrolyte brushes}, series = {ChemPhysChem}, volume = {21}, journal = {ChemPhysChem}, number = {5}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1439-4235}, doi = {10.1002/cphc.201901087}, pages = {450 -- 458}, year = {2019}, abstract = {Experimental and kinetic modelling studies are presented to investigate the mechanism of 3,3 ',5,5 '-tetramethylbenzidine (TMB) oxidation by hydrogen peroxide (H2O2) catalyzed by peroxidase-like Pt nanoparticles immobilized in spherical polyelectrolyte brushes (SPB-Pt). Due to the high stability of SPB-Pt colloidal, this reaction can be monitored precisely in situ by UV/VIS spectroscopy. The time-dependent concentration of the blue-colored oxidation product of TMB expressed by different kinetic models was used to simulate the experimental data by a genetic fitting algorithm. After falsifying the models with abundant experimental data, it is found that both H2O2 and TMB adsorb on the surface of Pt nanoparticles to react, indicating that the reaction follows the Langmuir-Hinshelwood mechanism. A true rate constant k, characterizing the rate-determining step of the reaction and which is independent on the amount of catalysts used, is obtained for the first time. Furthermore, it is found that the product adsorbes strongly on the surface of nanoparticles, thus inhibiting the reaction. The entire analysis provides a new perspective to study the catalytic mechanism and evaluate the catalytic activity of the peroxidase-like nanoparticles.}, language = {en} }