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Nature Chemical Engineering 2024年 542-551页

作者： Lun Li Huazhang Zhang Xin Zhao Daping He Wei Shu Zixin Zhang Yu Zhao Xingchuan Li Zongkui Kou Yong Xiao Francis Verpoort Liqiang Mai Jinlong Yang Rui Tan CheeTong John Low Cheng Li Yajun Zhang Hewu Wang Hubei Engineering Research Center of RF-Microwave Technology and Application School of Physics and Mechanics Wuhan University of Technology Wuhan China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing State Key Laboratory of Silicate Materials for Architectures School of Materials Science and Engineering Wuhan University of Technology Wuhan China Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering Shenzhen University Shenzhen China Department of Chemical Engineering Swansea University Swansea UK Warwick Electrochemical Engineering Group WMG Energy Innovation Centre University of Warwick Warwick UK School of Vehicle and Mobility Tsinghua University Beijing China

Thermal runaway, a major battery safety issue, is triggered when the local temperature exceeds a threshold value resulting from slower heat dissipation relative to heat generation inside the cell. However, improving internal heat transfer is challenged by the low thermal conductivity of metal current collectors (CCs) and challenges in manufacturing nonmetal CC foils at large scales. Here we report a rapid temperature-responsive nonmetallic CC that can substitute benchmark Al and Cu foils to enhance battery safety. The nonmetallic CC was fabricated through a continuous thermal pressing process to afford a highly oriented Gr foil on a hundred-meter scale. This Gr foil demonstrates a high thermal conductivity of 1,400.8 W m−1K−1, about one order of magnitude higher than those of Al and Cu foils. Importantly, LiNi0.8Co0.1Mn0.1O2||graphite cells integrated with these temperature-responsive foils show faster heat dissipation, eliminating the local heat concentration and circumventing the fast exothermic aluminothermic and hydrogen-evolution reactions, which are critical factors causing the thermal failure propagation of lithium-ion battery packs.

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The Role of the Molecular Encapsulation Effect in Stabilizing Hydrogen-Bond-Rich Gel-state Lithium Metal Batteries

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Angewandte Chemie 2024年第27期136卷

作者： Hantao Xu Wei Deng Lei Shi Juncai Long Yongcai Zhang Prof. Lin Xu Prof. Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 P.R. China School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225009 P.R. China Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang 441000 Hubei P.R. China Hainan Institute Wuhan University of Technology Sanya 572000 P.R. China

Gel-state polymer electrolytes with superior mechanical properties, self-healing abilities and high Li + transference numbers can be obtained by in situ polymerization of monomers with hydrogen-bonding moieties. However, it is overlooked that the active hydrogen atoms in hydrogen-bond donors experience displacement reactions with lithium metal in lithium metal batteries (LMBs), leading to corrosion of the lithium metal. Herein, it is discovered that the addition of hydrogen-bond acceptors to hydrogen-bond-rich gel-state electrolytes modulates the chemical activity of the active hydrogen atoms via the formation of hydrogen-bonded intermolecular interactions. The characterizations reveal that the added hydrogen-bond acceptors encapsulate the active hydrogen atoms to suppress the interfacial chemical corrosions of lithium metals, thereby enhancing the chemical stability of the polymer structure and interphase. With the employment of this strategy, a 1.1 Ah LiNi 0.8 Co 0.1 Mn 0.1 O 2 /Li metal pouch cell achieves stable cycling with 96.3 % capacity retention at 100 cycles. This new approach indicates a feasible path for achieving in situ polymerization of highly stable gel-state-based LMBs.

关键词： in situ polymerization molecular encapsulation effect interfaces lithium metal batteries gel-state polymer electrolytes

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Tailoring Zirconia Supported Intermetallic Platinum Alloy via Reactive Metal-Support Interactions for High-Performing Fuel Cells

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Angewandte Chemie 2024年第26期136卷

作者： Zijie Lin Nadaraj Sathishkumar Yu Xia Shenzhou Li Xuan Liu Jialun Mao Hao Shi Prof. Gang Lu Prof. Tanyuan Wang Prof. Hsing-Lin Wang Prof. Yunhui Huang Prof. Lior Elbaz Prof. Qing Li State Key Laboratory of Material Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology 430074 Wuhan China Department of Physics and Astronomy California State University Northridge 91330 Northridge CA USA Department of Materials Science and Engineering Southern University of Science and Technology 518055 Shenzhen China Department of Chemistry and the Institute of Nanotechnology and Advanced Materials Bar-Ilan University 5290002 Ramat-Gan Israel

Developing efficient and anti-corrosive oxygen reduction reaction (ORR) catalysts is of great importance for the applications of proton exchange membrane fuel cells (PEMFCs). Herein, we report a novel approach to prepare metal oxides supported intermetallic Pt alloy nanoparticles (NPs) via the reactive metal-support interaction (RMSI) as ORR catalysts, using Ni-doped cubic ZrO 2 (Ni/ZrO 2 ) supported L1 0 −PtNi NPs as a proof of concept. Benefiting from the Ni migration during RMSI, the oxygen vacancy concentrations in the support are increased, leading to an electron enrichment of Pt. The optimal L1 0 −PtNi−Ni/ZrO 2 −RMSI catalyst achieves remarkably low mass activity (MA) loss (17.8 %) after 400,000 accelerated durability test cycles in a half-cell and exceptional PEMFC performance (MA=0.76 A mg Pt −1 at 0.9 V, peak power density=1.52/0.92 W cm −2 in H 2 −O 2 /−air, and 18.4 % MA decay after 30,000 cycles), representing the best reported Pt-based ORR catalysts without carbon supports. Density functional theory (DFT) calculations reveal that L1 0 −PtNi−Ni/ZrO 2 −RMSI requires a lower energetic barrier for ORR than L1 0 −PtNi−Ni/ZrO 2 (direct loading), which is ascribed to a decreased Bader charge transfer between Pt and *OH, and the improved stability of L1 0 −PtNi−Ni/ZrO 2 −RMSI compared to L1 0 −PtNi−C can be contributed to the increased adhesion energy and Ni vacancy formation energy within the PtNi alloy.

关键词： oxygen reduction reaction zirconia reactive metal-support interaction intermetallics fuel cells

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Concerted Rattling in CsAg5Te3Leading to Ultralow Thermal Conductivity and High Thermoelectric Performance

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Angewandte Chemie 2016年第38期128卷

作者： Hua Lin Gangjian Tan Jin‐Ni Shen Shiqiang Hao Li‐Ming Wu Nicholas Calta Christos Malliakas Si Wang Ctirad Uher Christopher Wolverton Mercouri G. Kanatzidis Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 P.R. China Department of Chemistry Northwestern University Evanston IL 60208 USA Department of Materials Science and Engineering Northwestern University Evanston IL 60208 USA State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Department of Physics University of Michigan Ann Arbor MI 48109 USA

Thermoelectric (TE) materials convert heat energy directly into electricity, and introducing new materials with high conversion efficiency is a great challenge because of the rare combination of interdependent electrical and thermal transport properties required to be present in a single material. The TE efficiency is defined by the figure of merit ZT =( S 2 σ ) T / κ , where S is the Seebeck coefficient, σ is the electrical conductivity, κ is the total thermal conductivity, and T is the absolute temperature. A new p‐type thermoelectric material, CsAg 5 Te 3 , is presented that exhibits ultralow lattice thermal conductivity (ca. 0.18 Wm −1 K −1 ) and a high figure of merit of about 1.5 at 727 K. The lattice thermal conductivity is the lowest among state‐of‐the‐art thermoelectrics; it is attributed to a previously unrecognized phonon scattering mechanism that involves the concerted rattling of a group of Ag ions that strongly raises the Grüneisen parameters of the material.

关键词： CsAg5Te3 Konzertiertes Rasseln Thermoelektrika Tunnelstrukturen Wärmeleitfähigkeit

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Low-coordination Nanocrystalline Copper-based Catalysts through Theory-guided Electrochemical Restructuring for Selective CO2Reduction to Ethylene

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Angewandte Chemie 2024年第16期136卷

作者： Wensheng Fang Ruihu Lu Fu-Min Li Chaohui He Dan Wu Kaihang Yue Yu Mao Wei Guo Bo You Fei Song Tao Yao Ziyun Wang Prof. Bao Yu Xia School of Chemistry and Chemical Engineering State Key Laboratory of Materials Processing and Die & Mould Technology Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology (HUST) 1037 Luoyu Rd Wuhan 430074 China School of Chemical Sciences University of Auckland Auckland 1010 New Zealand National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230029 P. R. China CAS Key Laboratory of Materials for Energy Conversion Shanghai Institute of Ceramics Chinese Academy of Sciences (SICCAS) Shanghai 200050 China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201800 China

Revealing the dynamic reconstruction process and tailoring advanced copper (Cu) catalysts is of paramount significance for promoting the conversion of CO 2 into ethylene (C 2 H 4 ), paving the way for carbon neutralization and facilitating renewable energy storage. In this study, we initially employed density functional theory (DFT) and molecular dynamics (MD) simulations to elucidate the restructuring behavior of a catalyst under electrochemical conditions and delineated its restructuring patterns. Leveraging insights into this restructuring behavior, we devised an efficient, low-coordination copper-based catalyst. The resulting synthesized catalyst demonstrated an impressive Faradaic efficiency (FE) exceeding 70 % for ethylene generation at a current density of 800 mA cm −2 . Furthermore, it showed robust stability, maintaining consistent performance for 230 hours at a cell voltage of 3.5 V in a full-cell system. Our research not only deepens the understanding of the active sites involved in designing efficient carbon dioxide reduction reaction (CO 2 RR) catalysts but also advances CO 2 electrolysis technologies for industrial application.

关键词： Carbon dioxide reduction Restructuring behavior Cu catalyst Ethylene Low coordination number

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Appending Coronene Diimide with Carbon Nanohoops Allows for Rapid Intersystem Crossing in Neat Film

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Angewandte Chemie 2024年第18期136卷

作者： Jingjing Zhao Jingwen Xu Dr. Huaxi Huang Kangwei Wang Prof. Dr. Di Wu Prof. Dr. Ramesh Jasti Prof. Dr. Jianlong Xia State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Center of Smart Materials and Devices Wuhan University of Technology 430070 Wuhan China These authors contributed equally International School of Materials Science and Engineering Wuhan University of Technology 430070 Wuhan China School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology 430070 Wuhan China Department of Chemistry and Biochemistry Materials Science Institute University of Oregon 97403 Eugene Oregon USA

The development of innovative triplet materials plays a significant role in various applications. Although effective tuning of triplet formation by intersystem crossing (ISC) has been well established in solution, the modulation of ISC processes in the solid state remains a challenge due to the presence of other exciton decay channels through intermolecular interactions. The cyclic structure of cycloparaphenylenes (CPPs) offers a unique platform to tune the intermolecular packing, which leads to controllable exciton dynamics in the solid state. Herein, by integrating an electron deficient coronene diimide (CDI) unit into the CPP framework, a donor-acceptor type of conjugated macrocycle ( CDI-CPP ) featuring intramolecular charge-transfer (CT) interaction was designed and synthesized. Effective intermolecular CT interaction resulting from a slipped herringbone packing was confirmed by X-ray crystallography. Transient spectroscopy studies showed that CDI-CPP undergoes ISC in both solution and the film state, with triplet generation time constants of 4.5 ns and 238 ps, respectively. The rapid triplet formation through ISC in the film state can be ascribed to the cooperation between intra- and intermolecular charge-transfer interactions. Our results highlight that intermolecular CT interaction has a pronounced effect on the ISC process in the solid state, and shed light on the use of the characteristic structure of CPPs to manipulate intermolecular CT interactions.

关键词： cycloparaphenylenes rylene diimides triplet materials intersystem crossing

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Mussel‐Directed synthesis of Nitrogen‐Doped Anatase TiO2

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Angewandte Chemie 2016年第9期128卷

作者： Jingjing Xie Hao Xie Bao‐Lian Su Yi‐bing Cheng Xiaodong Du Hui Zeng Menghu Wang Weimin Wang Hao Wang Zhengyi Fu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P.R. China School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology Wuhan 430070 P.R. China Laboratory of Inorganic Materials Chemistry University of Namur B-5000 Namur Belgium Department of Materials Engineering Monash University Victoria 3800 Australia Department of Pearl Research Guangdong Ocean University Zhanjiang 524025 P.R. China

Structure‐forming processes leading to biominerals are well worth learning in pursuit of new synthetic techniques. Strategies that attempt to mimic nature in vitro cannot replace an entire complex natural organism, requiring ingenuity beyond chemists′ hands. A “bioprocess‐inspired synthesis” is demonstrated for fabrication of N‐doped TiO 2 materials at ambient temperature by direct implantation of precursor into living mussels. The amorphous precursor transforms into N‐doped anatase TiO 2 with a hierarchical nanostructure. Synthetic TiO 2 exhibits high phase stability and enhanced visible‐light photocatalytic activity as a result of modifications to its band gap during in vivo mineralization. Intracellular proteins were found to be involved in TiO 2 mineralization. Our findings may inspire material production by new synthetic techniques, especially under environmentally benign conditions.

关键词： Raumtemperatur Biologisch inspirierte Synthesen Intrazelluläre Proteine Organismen Stickstoffdotiertes TiO2

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Confinement Effects in Zeolite‐Confined Noble Metals

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Angewandte Chemie 2019年第36期131卷

作者： Si‐Ming Wu Xiao‐Yu Yang Christoph Janiak State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology (WHUT) Wuhan 430070 China Southern Marine Science and Engineering Guangdong Laboratory (Zhuhai)(SMSEGL) & School of Chemical Engineering and Technology Sun Yat-sen University (SYSU) Zhuhai 519082 China School of Engineering and Applied Sciences Harvard University (HU) Cambridge MA 02138 USA Institut für Anorganische Chemie und Strukturchemie Heinrich-Heine-Universität Düsseldorf 40204 Düsseldorf Germany

Confinement of noble nanometals in a zeolite matrix is a promising way to special types of catalysts that show significant advantages in size control, site adjustment, and nano‐architecture design. The beauty of zeolite‐confined noble metals lies in their unique confinement effects on a molecular scale, and thus enables spatially confined catalysis akin to enzyme catalysis. In this Minireview, the confined synthesis strategies of zeolite‐confined noble metals will be briefly discussed, showing the processes, advantages, features, and mechanisms. The confined catalysis carried on zeolite‐confined noble metals will be summarized, and great emphasis will be paid to the confinement effects involving size, encapsulation, recognition, and synergy. Great progress of atomic sites in the size effect, supercage stabilization in the encapsulation effect, site adsorption in the recognition effect, and cascade reaction in the synergy effect are highlighted. This Minireview is concluded with challenges and opportunities in terms of the synthesis of zeolite‐confined noble metals and their applications to design multifunctional catalysts with high catalytic activity, selectivity, and stability.

关键词： Confinement-Effekt Edelmetalle Heterogene Katalyse Kaskadenreaktionen Zeolithe

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A New 1D Mn(II) Coordination Polymer: synthesis, Crystal Structure, Hirshfeld Surface Analysis and Molecular Docking Studies

SSRN

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SSRN 2024年

作者： Gurbanov, Atash V. Firoozbakht, Fateme Pourshirband, Nafiseh Sharafi-Badr, Paria Hayati, Payam Souri, Bagher Eshghi, Fazlolah Kaminsky, Werner Mahmoudi, Ghodrat Verpoort, Francis Centro de Química Estrutural Institute of Molecular Sciences Instituto Superior Técnico Universidade de Lisboa Av. Rovisco Pais Lisboa1049-001 Portugal Department of Chemistry Baku State University Z. Khalilov Str. 23 AZ Baku1148 Azerbaijan Department of Chemistry University of Isfahan Isfahan81746-73441 Iran Department of Chemistry Shahreza Branch Islamic Azad University P.O. Box 311-86145 Isfahan Shahreza Iran Department of Pharmacognosy and Pharmaceutical Biotechnology School of Pharmacy Iran University of Medical Sciences Tehran Iran PO Box 16846-13114 Tehran Iran Department of Chemistry Faculty of Sciences University of Sistan and Baluchestan Zahedan Iran Department of Chemistry College of Sciences Shiraz University Shiraz Iran X-ray Crystallography Laboratory University of Washington United States Department of Chemistry Faculty of Science University of Maragheh P.O. Box 55136-83111 Maragheh Iran State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China

The synthesis of novel metal-organic coordination polymers (MOCP) with the chemical formula [Mn2L(SCN)2(OH)2]***3OH [L=1,5-bis(pyridine-4-ylmethylene) carbonohydrazide] {1} was accomplished using two different techniques: solvothermal and sonochemical ultrasonic-assisted. An investigation was carried out to examine the impact of various factors such as reaction time, sonication power, temperature, and reactant concentration on the morphology and size of the crystals. The results showed an inverse relationship between these parameters and the morphology and size of 1. Interestingly, it was found that sonication power and temperature did not affect the crystals’ morphology and size. To further analyze the prepared microcrystals of MOCPs, SEM was utilized to examine their surface morphology, and XRD, elemental evaluation composition. The identification of the functional groups present in the prepared Mn-MOCPs was accomplished through the utilization of FT-IR spectroscopy. Subsequently, the calcination of 1 in an air atmosphere at 650°C led to the formation of Mn3O4 nanoparticles. The geometric and electronic structure of the MOCPs was evaluated using density functional theory (DFT). The utilization of molecular docking methodologies demonstrated that the best cavity of the human androgen receptor possessed an interaction energy of -116.3 kJ mol−1. This energy encompassed a combination of both bonding and non-bonding interactions. © 2024, The Authors. All rights reserved.

关键词： Density functional theory

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Author Correction: Thermally activated delayed fluorescence (TADF) organic molecules for efficient X-ray scintillation and imaging

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Nature materials 2022年第7期21卷 836页

作者： Wenbo Ma Yirong Su Qisheng Zhang Chao Deng Luca Pasquali Wenjuan Zhu Yue Tian Peng Ran Zeng Chen Gaoyuan Yang Guijie Liang Tianyu Liu Haiming Zhu Peng Huang Haizheng Zhong Kangwei Wang Shaoqian Peng Jianlong Xia Huafeng Liu Xu Liu Yang Michael Yang State Key Laboratory of Modern Optical Instrumentation Institute for Advanced Photonics College of Optical Science and Engineering Zhejiang University Hangzhou China. Intelligent Optics & Photonics Research Center Jiaxing Institute of Zhejiang University Jiaxing China. MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou China. Dipartimento di Ingegneria E. Ferrari Università di Modena e Reggio Emilia Modena Italy. CNR-IOM Basovizza Trieste Italy. Department of Physics University of Johannesburg Auckland Park South Africa. State Key Laboratory of Modern Optical Instrumentation Key Laboratory of Excited-State Materials of Zhejiang Province Department of Chemistry Zhejiang University Hangzhou China. Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices Hubei University of Arts and Science Xiangyang China. MIIT Key Laboratory for Low Dimensional Quantum Structure and Devices School of Materials & Engineering Beijing Institute of Technology Beijing China. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Center of Smart Materials and Devices Wuhan University of Technology Wuhan China. State Key Laboratory of Modern Optical Instrumentation Institute for Advanced Photonics College of Optical Science and Engineering Zhejiang University Hangzhou China. yangyang15@***. Intelligent Optics & Photonics Research Center Jiaxing Institute of Zhejiang University Jiaxing China. yangyang15@***.

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