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Chirality‐Assisted Ring‐Like Aggregation of Aβ(1–40) at Liquid–Solid Interfaces: A Stereoselective Two‐Step Assembly Process†

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Angewandte Chemie 2014年第7期127卷

作者： Guanbin Gao Mingxi Zhang Pei Lu Guanlun Guo Dong Wang Taolei Sun State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 (PR China) Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences Beijing 100190 (PR China) Hubei Key Laboratory of Advanced Technology of Automotive Components Wuhan University of Technology Wuhan 430070 (PR China) School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology Wuhan 430070 (PR China)

Molecular chirality is introduced at liquid–solid interfaces. A ring‐like aggregation of amyloid Aβ(1–40) on N ‐isobutyryl‐ L ‐cysteine ( L ‐NIBC)‐modified gold substrate occurs at low Aβ(1–40) concentration, while D ‐NIBC modification only results in rod‐like aggregation. Utilizing atomic force microscope controlled tip‐enhanced Raman scattering, we directly observe the secondary structure information for Aβ(1–40) assembly in situ at the nanoscale. D ‐ or L ‐NIBC on the surface can guide parallel or nonparallel alignment of β‐hairpins through a two‐step process based on electrostatic‐interaction‐enhanced adsorption and subsequent stereoselective recognition. Possible electrostatic interaction sites (R5 and K16) and a chiral recognition site (H14) of Aβ(1–40) are proposed, which may provide insight into the understanding of this effect.

关键词： Adsorption Amyloide Chiralität Oberflächenchemie Stereoselektivität

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Eutectic Electrolyte with Unique Solvation Structure for High-Performance Zinc-Ion Batteries

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Angewandte Chemie 2022年第31期134卷

作者： Lishan Geng Dr. Jiashen Meng Dr. Xuanpeng Wang Dr. Chunhua Han Kang Han Zhitong Xiao Meng Huang Peng Xu Dr. Lei Zhang Prof. Liang Zhou Prof. Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Department of Physical Science & Technology School of Science Wuhan University of Technology Wuhan 430070 P. R. China Hubei Longzhong Laboratory Xiangyang 441000 P. R. Hubei China

Zinc-ion batteries (ZIB) present great potential in energy storage due to low cost and high safety. However, the poor stability, dendrite growth, and narrow electrochemical window limit their practical application. Herein, we develop a new eutectic electrolyte consisting of ethylene glycol (EG) and ZnCl 2 for dendrite-free and long-lifespan ZIBs. The EG molecules participate in the Zn 2+ solvation via coordination and hydrogen-bond interactions. Optimizing the ZnCl 2 /EG molar ratio (1 : 4) can strengthen intermolecular interactions to form [ZnCl(EG)] + and [ZnCl(EG) 2 ] + cations. The dissociation–reduction of these complex cations enables the formation of a Cl-rich organic–inorganic hybrid solid electrolyte interphase film on a Zn anode, realizing highly reversible Zn plating/stripping with long-term stability of ≈3200 h. Furthermore, the polyaniline||Zn cell manifests decent cycling performance with ≈78 % capacity retention after 10 000 cycles, and the assembled pouch cell demonstrates high safety and stable capacity. This work opens an avenue for developing eutectic electrolytes for high-safety and practical ZIBs.

关键词： Deep Eutectic Solvents Dendrite-Free Zn Anodes Eutectic Electrolytes Solvation Structure Zinc-Ion Batteries

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Work-function-induced Interfacial Built-in Electric Fields in Os-OsSe2Heterostructures for Active Acidic and Alkaline Hydrogen Evolution

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Angewandte Chemie 2022年第36期134卷

作者： Ding Chen Ruihu Lu Ruohan Yu Yuhang Dai Hongyu Zhao Dulan Wu Pengyan Wang Jiawei Zhu Dr. Zonghua Pu Lei Chen Jun Yu Prof. Shichun Mu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen Valley Foshan 528200 P. R. China NRC (Nanostructure Research Centre) Wuhan University of Technology Wuhan 430070 P. R. China

Theoretical calculations unveil that the formation of Os-OsSe 2 heterostructures with neutralized work function (WF) perfectly balances the electronic state between strong (Os) and weak (OsSe 2 ) adsorbents and bidirectionally optimizes the hydrogen evolution reaction (HER) activity of Os sites, significantly reducing thermodynamic energy barrier and accelerating kinetics process. Then, heterostructural Os-OsSe 2 is constructed for the first time by a molten salt method and confirmed by in-depth structural characterization. Impressively, due to highly active sites endowed by the charge balance effect, Os-OsSe 2 exhibits ultra-low overpotentials for HER in both acidic (26 mV @ 10 mA cm −2 ) and alkaline (23 mV @ 10 mA cm −2 ) media, surpassing commercial Pt catalysts. Moreover, the solar-to-hydrogen device assembled with Os-OsSe 2 further highlights its potential application prospects. Profoundly, this special heterostructure provides a new model for rational selection of heterocomponents.

关键词： Charge Balance Effect DFT Calculation Heterostructure Engineering Hydrogen Evolution Os-Based Electrocatalyst Electrocatalysis

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A Bifunctional CdS/MoO2/MoS2Catalyst Enhances Photocatalytic H2Evolution and Pyruvic Acid synthesis

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Angewandte Chemie 2022年第44期134卷

作者： Dr. Chuanbiao Bie Dr. Bicheng Zhu Dr. Linxi Wang Prof. Huogen Yu Dr. Chenhui Jiang Prof. Tao Chen Prof. Jiaguo Yu Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 430074 Wuhan P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 430070 Wuhan P. R. China Hefei National Laboratory for Physical Sciences at Microscale CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering University of Science and Technology of China 230026 Hefei P. R. China

The best use of photogenerated electrons and holes is crucial to boosting photocatalytic activity. Herein, a bifunctional dual-cocatalyst-modified photocatalyst is constructed based on CdS/MoO 2 /MoS 2 hollow spheres for hydrogen evolution coupled with selective pyruvic acid (PA) production from lactic acid (LA) oxidation. MoS 2 and MoO 2 are simultaneously obtained from the conversion of CdMoO 4 in one step. In a photocatalytic process, the MoS 2 and MoO 2 function as the reduction and oxidation centers on which photogenerated electrons and holes accumulate and are used for hydrogen evolution reaction (HER) and PA synthesis, respectively. By monitoring the intermediates, a two-step single-electron route for PA production is proposed, initiated by the cleavage of the α-C(sp 3 )−H bond in the LA. The conversion of LA and the selectivity of PA can reach ca . 29 % and 95 % after a five-hour reaction, respectively.

关键词： CdS Dual Cocatalysts Hollow Sphere Hydrogen Evolution Organic synthesis

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Sodium‐Ion Batteries: Superior Electrochemical Performance and Storage Mechanism of Na3V2(PO4)3Cathode for Room‐Temperature Sodium‐Ion Batteries (Adv. Energy Mater. 2/2013)

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advanced Energy materials 2013年第2期3卷

作者： Zelang Jian Wenze Han Xia Lu Huaixin Yang Yong‐Sheng Hu Jing Zhou Zhibin Zhou Jianqi Li Wen Chen Dongfeng Chen Liquan Chen Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and Devices Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China China Institute of Atomic Energy Beijing 102413 China School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 China

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Macromol. Rapid Commun. 5/2018

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Macromolecular Rapid Communications 2018年第5期39卷

作者： Zhengbang Wang Cong Liang Haolin Tang Sylvain Grosjean Artak Shahnas Joerg Lahann Stefan Bräse Christof Wöll Institute of Functional Interfaces Karlsruhe Institute of Technology Hermann‐von‐Helmholtz‐Platz 1 76344 Eggenstein‐Leopoldshafen Germany Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Key Laboratory for the Green Preparation and Application of Functional Materials Ministry‐of‐Education Hubei Key Laboratory of Polymer Materials Hubei University Wuhan 430062 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China China Automotive Technology and Research Center Tianjin 300300 China Institute for Organic Chemistry (IOC) Karlsruhe Institute of Technology (KIT) Fritz‐Haber‐Weg 6 76131 Karlsruhe Germany

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MoB/g‐C3N4Interface materials as a Schottky Catalyst to Boost Hydrogen Evolution

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Angewandte Chemie 2017年第2期130卷

作者： Zechao Zhuang Yong Li Zilan Li Fan Lv Zhiquan Lang Kangning Zhao Liang Zhou Lyudmila Moskaleva Shaojun Guo Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology Universität Bremen 28359 Bremen Germany Department of Materials Science and Engineering College of Engineering Peking University Beijing 100871 China Department of Chemistry University of California Berkeley CA 94720 USA

Proton adsorption on metallic catalysts is a prerequisite for efficient hydrogen evolution reaction (HER). However, tuning proton adsorption without perturbing metallicity remains a challenge. A Schottky catalyst based on metal–semiconductor junction principles is presented. With metallic MoB, the introduction of n‐type semiconductive g‐C 3 N 4 induces a vigorous charge transfer across the MoB/g‐C 3 N 4 Schottky junction, and increases the local electron density in MoB surface, confirmed by multiple spectroscopic techniques. This Schottky catalyst exhibits a superior HER activity with a low Tafel slope of 46 mV dec −1 and a high exchange current density of 17 μA cm −2 , which is far better than that of pristine MoB. First‐principle calculations reveal that the Schottky contact dramatically lowers the kinetic barriers of both proton adsorption and reduction coordinates, therefore benefiting surface hydrogen generation.

关键词： Elektrokatalyse Graphitische Kohlenstoffnitride Molybdänborid Schottky-Kontakt Wasserstoffentwicklung

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High-Entropy Lithium Argyrodite Solid Electrolytes Enabling Stable All-Solid-state Batteries

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Angewandte Chemie 2023年第50期135卷

作者： Shenghao Li Jing Lin Mareen Schaller Sylvio Indris Xin Zhang Torsten Brezesinski Ce-Wen Nan Shuo Wang Florian Strauss Center of Smart Materials and Devices State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Material Science and Engineering Wuhan University of Technology Wuhan 430070 China Institute of Nanotechnology Karlsruhe Institute of Technology (KIT) Hermann-von-Helmholtz-Platz 1 76344 Eggenstein-Leopoldshafen Germany Institute for Applied Materials-Energy Storage Systems (IAM-ESS) Karlsruhe Institute of Technology (KIT) Hermann-von-Helmholtz-Platz 1 76344 Eggenstein-Leopoldshafen Germany State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China Foshan (Southern China) Institute for New Materials Foshan 528200 China

Superionic solid electrolytes (SEs) are essential for bulk-type solid-state battery (SSB) applications. Multicomponent SEs are recently attracting attention for their favorable charge-transport properties, however a thorough understanding of how configurational entropy (Δ S conf ) affects ionic conductivity is lacking. Here, we successfully synthesized a series of halogen-rich lithium argyrodites with the general formula Li 5.5 PS 4.5 Cl x Br 1.5- x (0≤ x ≤1.5). Using neutron powder diffraction and 31 P magic-angle spinning nuclear magnetic resonance spectroscopy, the S 2− /Cl − /Br − occupancy on the anion sublattice was quantitatively analyzed. We show that disorder positively affects Li-ion dynamics, leading to a room-temperature ionic conductivity of 22.7 mS cm −1 (9.6 mS cm −1 in cold-pressed state) for Li 5.5 PS 4.5 Cl 0.8 Br 0.7 (Δ S conf =1.98 R ). To the best of our knowledge, this is the first experimental evidence that configurational entropy of the anion sublattice correlates with ion mobility. Our results indicate the possibility of improving ionic conductivity in ceramic ion conductors by tailoring the degree of compositional complexity. Moreover, the Li 5.5 PS 4.5 Cl 0.8 Br 0.7 SE allowed for stable cycling of single-crystal LiNi 0.9 Co 0.06 Mn 0.04 O 2 (s-NCM90) composite cathodes in SSB cells, emphasizing that dual-substituted lithium argyrodites hold great promise in enabling high-performance electrochemical energy storage.

关键词： Argyrodite High-Entropy materials Solid Electrolyte Solid-state Batteries

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Hierarchical Structuring: Phases Hybriding and Hierarchical Structuring of Mesoporous TiO2Nanowire Bundles for High-Rate and High-Capacity Lithium Batteries (Adv. Sci. 7/2015)

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advanced Science 2015年第7期2卷 n/a-n/a页

作者： Jun Jin Shao-Zhuan Huang Jing Liu Yu Li Li-Hua Chen Yong Yu Hong-En Wang Clare P. Grey Bao-Lian Su Laboratory of Living Materials at the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China Department of Chemistry University of Cambridge Lensfeild Road Cambridge CB2 1EW UK Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles B-5000 Namur Belgium

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Bifunctional o-CoSe 2 /c-CoSe 2 /MoSe 2 heterostructures for enhanced electrocatalytic and photoelectrochemical hydrogen evolution reaction

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materials Today Chemistry 2022年 23卷

作者： Y. Ji W. Luo Y. Liu Z. He N. Cheng Z. Zhang X. Qi J. Zhong L. Ren Hunan Key Laboratory of Micro-Nano Energy Materials and Devices Laboratory for Quantum Engineering and Micro-Nano Energy Technology Faculty of Materials and Optoelectronic Physics Xiangtan University Hunan 411105 PR China Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Institutes of Physical Science and Information Technology Anhui University Hefei 230601 PR China Department of Materials Science and Engineering and Shenzhen Key Laboratory of Hydrogen Energy Southern University of Science and Technology Shenzhen 518055 PR China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 PR China

The bottleneck of alkaline hydrogen evolution reaction lies in the kinetically sluggish brought from multistep reaction processes involving water adsorption and dissociation, as well as hydrogen adsorption. In this work, we successfully synthesized o-CoSe 2 /c-CoSe 2 heterostructures anchored on MoSe 2 nanosheets to powerfully promote reaction processes. As an electrocatalyst, it exhibits a low overpotential of 112 mV at 10 mA/cm 2 and a Tafel slope of 96.9 mV/dec for an alkaline hydrogen evolution reaction. Moreover, the as-prepared catalyst can behave as both cathode and anode for overall water splitting, which only requires 1.61 V cell voltage at 10 mA/cm 2 . Significantly, the cell voltage can be further reduced to 1.53 V at 10 mA/cm 2 for water electrolysis under the simulated solar irradiation owing to such a semiconductor-based heterostructure that facilitates the separation of photogenerated charges. Here, the improving overall performance of this ternary electrocatalyst is attributed to the multifunctionality and synergistic interaction of different components in this heterogeneous material. The work provides a novel strategy to design active catalysts simultaneously using electric energy and solar energy for effective water splitting.

关键词： Transition-metal dichalcogenides Ternary hybrids Alkaline hydrogen evolution Photoelectrochemical water splitting

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