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Polyolefin-Based Separator with Interfacial Chemistry Regulation for Robust Potassium Metal Batteries

Angewandte Chemie 2023年第35期135卷

作者： Long Tu Zhijia Zhang Zelin Zhao Xinyuan Xiang Prof. Bohua Deng Prof. Dan Liu Prof. Deyu Qu Prof. Haolin Tang Prof. Junsheng Li Prof. Jinping Liu School of Chemistry Chemical Engineering and Life Sciences Wuhan University of Technology Wuhan 430070 P. R. China Department of Physics and Astronomy University of Manchester Manchester M13 9PL UK State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Hubei Provincial Key Laboratory of Fuel Cell Wuhan University of Technology Wuhan 430070 P. R. China

Potassium metal batteries (KMBs) are ideal choices for high energy density storage system owing to the low electrochemical potential and low cost of K. However, the practical KMB applications suffer from intrinsically active K anode, which would bring serious safety concerns due to easier generation of dendrites. Herein, to explore a facile approach to tackle this issue, we propose to regulate K plating/stripping via interfacial chemistry engineering of commercial polyolefin-based separator using multiple functional units integrated in tailored metal organic framework. As a case study, the functional units of MIL-101(Cr) offer high elastic modulus, facilitate the dissociation of potassium salt, improve the K + transfer number and homogenize the K + flux at the electrode/electrolyte interface. Benefiting from these favorable features, uniform and stable K plating/stripping is realized with the regulated separator. Full battery assembled with the regulated separator showed ~19.9 % higher discharge capacity than that with glass fiber separator at 20 mA g −1 and much better cycling stability at high rates. The generality of our approach is validated with KMBs using different cathodes and electrolytes. We envision that the strategy to suppress dendrite formation by commercial separator surface engineering using tailor-designed functional units can be extended to other metal/metal ion batteries.

关键词： Elastic Modulus Ionic Transport Modification Potassium Metal Battery Separator

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Highly sensitive wearable sensor based on a flexible multi-layer graphene film antenna

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Science Bulletin 2018年第9期63卷 574-579页

作者： Danli Tang Qianlong Wang Zhe Wang Quantao Liu Bin Zhang Daping He Zhi Wu Shichun Mu Hubei Engineering Research Center of Rf-Microwave Technology and Application School of ScienceWuhan University of technologyWuhan 430070China Shenzhen Institute of Advanced Graphene Application and Technology(SIAGAT) Shenzhen 518106China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China

The use of advanced carbon nanomaterials for flexible antenna sensors has attracted great attention due to their outstanding electromechanical properties. However, carbon nanomaterial based composites have yet to overcome drawbacks, such as low conductivity and toughness. In this work, a flexible multi-layer graphene film(FGF) with a high conductivity of 10~6 S/m for antenna based wearable sensors is investigated. A 1.63 GHz FGF antenna sensor exhibits significantly high strain sensitivity of 9.8 for compressive bending and 9.36 for tensile bending, which is super than the copper antenna sensor(5.39 for compressive bending and 4.05 for tensile bending). Moreover, the FGF antenna sensor shows very good mechanical flexibility, reversible deformability and structure stability, and thus is well suited for applications like wearable devices and wireless strain sensing.

关键词： Multi-layer graphene film Flexibility Antenna based sensor High performance

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Isotope interface design for high-energy aqueous proton batteries

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Chem 2025年

作者： Cai, Hongwei Fu, Kai Chen, Ruixi Bao, Wenyuan Guan, Deyang Zhang, Xiangchen Deng, Zhaohui Wu, Xinfei Chen, Xingbao Gaumet, Jean-Jacques Luo, Wen Mai, Liqiang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China School of Physics and Mechanics Wuhan University of Technology Wuhan 430070 China School of Chemical Sciences University of Auckland Auckland 1010 New Zealand Laboratoire de Chimie et Physique: Approche Multi-échelles des Milieux Complexes (LCP-A2MC) Institut Jean Barriol Université de Lorraine Metz 57070 France Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang 441000 China

The stability of the electrode-electrolyte interface is crucial for the long-term operation of battery chemistries, particularly under harsh conditions with corrosive acidic/alkaline aqueous electrolytes. Here, we report the design of a H₂¹⁸O-H₂¹⁶O isotope interface to promote the formation of a protective electrode-electrolyte interphase, as demonstrated by a model investigation based on an aqueous proton battery (APB) utilizing strongly acidic aqueous electrolytes. This design enables the manganese-iron Prussian blue analog (MnFe-PBA), typically considered acid intolerant, to cycle stably over 10,000 cycles in corrosive H₃PO₄ electrolytes. This acid resistance is attributed to the isotope interface-governed in situ formation of interphases comprising hydrogen-bonded frameworks. With the high-energy MnFe-PBA cathode, the full battery attains a high voltage plateau (⁓1.2 V) and energy density (77.6 Wh kg⁻¹), both surpassing all previously reported APBs. Our findings provide a novel approach for enhancing the performance of aqueous batteries subject to extremely corrosive conditions and encourage the integration of isotopic science with battery technology. © 2025 Elsevier Inc.

关键词： aqueous battery corrosion resistance electrode-electrolyte interface high-energy proton battery isotope effect SDG7: Affordable and clean energy

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Dual Ion Co-Insertion Induced Spontaneous and Reversible Phase Conversion Chemistry for Unprecedented Zn2+Storage

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Angewandte Chemie 2024年第2期137卷

作者： Xikun Zhang Junwei Zhang Dr. Haoxiang Yu Dr. Thomas L. Madanu Maoting Xia Dr. Pengcheng Xing Prof. Alexandru Vlad Prof. Jie Shu Prof. Bao-Lian Su School of Materials Science and Chemical Engineering Ningbo University 818 Fenghua road Ningbo Zhejiang 315211 China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles Namur B-5000 Belgium Institute of Condensed Matter and Nanosciences Molecular Chemistry Materials and Catalysis Université Catholique de Louvain Louvain-la-Neuve B-1348 Belgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi road Wuhan Hubei 430070 China Clare Hall University of Cambridge Cambridge CB2 1EW UK

Prussian blue analogues are highly promising electrode materials due to their versatile electrochemical activity and low cost. However, they often suffer from severe structural damage caused by the Jahn–Teller distortion and dissolution of high-spin outer metal ions, resulting in poor cycle life. Material modification and electrolyte regulation have been the common approaches to address this issue, albeit with very limited success. We report here a novel and efficient strategy to preserve structural stability by co-inserting Co 2+ and Zn 2+ ions in KCo[Fe(CN) 6 ]. This co-insertion induced a spontaneous and reversible phase conversion by the replacement of low-spin inner ion (Fe 3+ ), which efficiently relieves structural damage caused by Jahn–Teller distortion and metal-ion dissolution, leading to an outstanding Zn 2+ storage capacity and an exceptional improvement of cycle life with a capacity retention of 97.7 % over 4400 cycles at 40 C. We also demonstrated the enhancement of co-intercalation on ion migration using a combined approach of experimental and density functional theory (DFT) calculations. This work provides an important progress to solve the cycle stability of Prussian blue analogues towards their practical application as electrode materials for aqueous batteries.

关键词： Prussian blue analogues Aqueous zinc ion battery Structural damage common ion effect Phase conversion

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Coordinating the Edge Defects of Bismuth with Sulfur for Enhanced CO2Electroreduction to Formate

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Angewandte Chemie 2023年第25期135卷

作者： Lei Lv Ruihu Lu Jiexin Zhu Ruohan Yu Dr. Wei Zhang Enhui Cui Xingbao Chen Yuhang Dai Lianmeng Cui Dr. Jiong Li Prof. Liang Zhou Prof. Wei Chen Dr. Ziyun Wang Prof. Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 430070 Wuhan Hubei P. R. China School of Chemical Sciences The University of Auckland 1010 Auckland New Zealand Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences 201210 Shanghai P. R. China Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) 441000 Xiangyang Hubei P. R. China

Bismuth-based materials have been recognized as promising catalysts for the electrocatalytic CO 2 reduction reaction (ECO 2 RR). However, they show poor selectivity due to competing hydrogen evolution reaction (HER). In this study, we have developed an edge defect modulation strategy for Bi by coordinating the edge defects of bismuth (Bi) with sulfur, to promote ECO 2 RR selectivity and inhibit the competing HER. The prepared catalysts demonstrate excellent product selectivity, with a high HCOO − Faraday efficiency of ≈95 % and an HCOO − partial current of ≈250 mA cm −2 under alkaline electrolytes. Density function theory calculations reveal that sulfur tends to bind to the Bi edge defects, reducing the coordination-unsaturated Bi sites (*H adsorption sites), and regulating the charge states of neighboring Bi sites to improve *OCHO adsorption. This work deepens our understanding of ECO 2 RR mechanism on bismuth-based catalysts, guiding for the design of advanced ECO 2 RR catalysts.

关键词： Carbon Dioxide Reduction Electrocatalysis Electrochemical Reconstruction S-Doping

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Hierarchically Structured Zeolites: From Design to Application

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Chemical reviews 2020年第20期120卷 11194-11294页

作者： Li-Hua Chen Ming-Hui Sun Zhao Wang Weimin Yang Zaiku Xie Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan China. Laboratory of Inorganic Materials Chemistry University of Namur 61 rue de Bruxelles B-5000 Namur Belgium. State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Shanghai Research Institute of Petrochemical Technology SINOPEC Shanghai 201208 China. Clare Hall University of Cambridge Cambridge CB2 1EW United Kingdom.

Hierarchical zeolites combine the intrinsic catalytic properties of microporous zeolites and the enhanced access and transport of the additional meso- and/or macroporous system. These materials are the most desirable catalysts and sorbents for industry and become a highly evolving field of important current interests. In addition to the enhanced mass transfer leading to high activity, selectivity, and cycle time, another essential merit of the hierarchical structure in zeolite materials is that it can significantly improve the utilization effectiveness of zeolite materials resulting in the minimum energy, time, and raw materials consumption. Substantial progress has been made in the synthesis, characterization, and application of hierarchical zeolites. Herein, we provide an overview of recent achievements in the field, highlighting the significant progress in the past decade on the development of novel and remarkable strategies to create an additional pore system in zeolites. The most innovative synthesis approaches are reviewed according to the principle, versatility, effectiveness, and degree of reality while establishing a firm link between the preparation route and the resultant hierarchical pore quality in zeolites. Zeolites with different hierarchically porous structures, i.e., micro-mesoporous structure, micro-macroporous structure, and micro-meso-macroporous structure, are then analyzed in detail with concrete examples to illustrate their benefits and their fabrications. The significantly improved performances in catalytic, environmental, and biological applications resulting from enhanced mass transport properties are discussed through a series of representative cases. In the concluding part, we envision the emergence of "material-properties-by-quantitative and real rational design" based on the "generalized Murray's Law" that enables the predictable and controlled productions of bioinspired hierarchically structured zeolites. This Review is expected to att

关键词： Crystallization Porosity Genetics Crystal structure Zeolites

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Light-Assisted Semi-Hydrogenation of 1,3-Butadiene with Water

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Angewandte Chemie 2022年第38期134卷

作者： Qi-Chen Wei Ya Chen Prof. Zhao Wang Da-Zhuang Yu Wei-Hao Wang Jian-Quan Li Prof. Li-Hua Chen Prof. Yu Li Prof. Bao-Lian Su Laboratory of Living Materials the State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Guangdong Laboratory Xianhu Hydrogen Valley Foshan 528200 P. R. China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles 5000 Namur Belgium

Sustainable processes for semi-hydrogenation of alkynes/alkadienes impurities in alkenes feedstocks are in great demand in industry as the utilization of excessive hydrogen, high temperature and unsatisfactory alkenes selectivity of the current thermo-catalytic route, however, their development is still challenging. Herein, we innovate a light-assisted semi-hydrogenation process in gas-feed fixed bed reactor, with water as hydrogen atom source by in situ photocatalysis. Using Pd/TiO 2 as model catalyst, this process shows an excellent catalytic performance for the semi-hydrogenation of 1,3-butadiene, with 100 % of butenes selectivity at ≈99 % of conversion over 180 h of reaction at ambient temperature driven by 66 mW cm −2 of irradiation intensity. This light-driven, H 2 -free, ambient temperature semi-hydrogenation process, with superior performance to that of thermocatalytic route, shows attractive to bring an evolution in industrial hydrogenation technology to an economical and safe way.

关键词： 1,3-Butadiene Pd/TiO2 Photocatalysis Semi-Hydrogenation Unsaturated Hydrocarbons

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Solvent-free synthesis of Co single atom and nanocluster decorated N-doped carbon for efficient oxygen reduction

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Chinese Chemical Letters 2024年

作者： Xinyuan Li Zhuozhu Li Wenzhong Huang Jiantao Li Wei Zhang Shihao Feng Hao Fan Zhuo Chen Sungsik Lee Congcong Cai Liang Zhou Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang 441000 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 United States X-ray Science Division Argonne National Laboratory Lemont IL 60439 United States Zhongyu Feima New Material Technology Innovation Center (Zhengzhou) Co. Ltd. High Technology Industrial Development Zone Zhengzhou 450001 China

The advancement of efficient, cheap, and durable catalysts for oxygen reduction reaction (ORR) to substitute Pt/C in metal-air batteries is of paramount importance. However, traditional solvent-based methods fall short in terms of environmental benign and scalab.lity. Herein, a solvent-free organic-inorganic self-assembly approach is explored to construct cobalt single atom and cobalt nanocluster decorated nitrogen-doped porous carbon spheres (Co-SA/NC@NCS). The solvent-free synthesis demonstrates an impressively high yield (282 g/L) and the resultant Co-SA/NC@NCS possesses a high N content (6.9 wt%). Density functional theory calculations disclose that the Co-SAs and Co-NCs are able to optimize the surface oxygen adsorption capability and enhance the conductivity of the NCS, thereby facilitating the ORR performance. The solvent-free synthesis is also feasible for the synthesis of other non-noble metal element (Fe, Ni, and Zn) decorated nitrogen-doped porous carbon spheres.

关键词： Organic-inorganic self-assembly Nitrogen-doped carbon Oxygen reduction reaction Single atom catalyst Zn-air battery

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Flexible [email protected] PVDF hybrid membrane as advanced anode for lithium storage

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Chemical Engineering Journal 2019年 370卷 547-555页

作者： Xuan Zheng Yuhuan Zheng Huijun Zhang Quanling Yang Chuanxi Xiong State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China State Key Laboratory of Pulp and Paper Engineering South China University of Technology Wushan Road 381 Guangzhou 510640 China

Design and fabrication of flexible free-standing electrode is crucial in the rapid advances of durable/flexible electronic devices. Herein, a unique functional electrode made of hierarchical MoS 2 nanosheets anchored on electrospun poly (vinylidene difluoride) based fibrous membrane, has been developed through a facile hydrothermal method. When assessed as membrane electrodes in lithium-ion batteries, the as-prepared anodes exhibit a high capacity (854 mA h g −1 at 0.5 A g −1 and 513 mA h g −1 after 200 cycles at 2 A g −1 ), excellent rate capability, and long cycling life durability (332 mA h g −1 at 5 A g −1 after 1000 cycles). Grafting MoS 2 nanosheets onto 3D electrospun framework not only shortens the Li + diffusion path and increases their valid and accostable active surface area, but also invests it with flexible feature. Full membrane cells containing LiNi 0.5 Co 0.3 Mn 0.2 O 2 cathode also gain excellent capacity performance, distinctive cycling tolerance and a high capacity preservation of 92% after 250 cycles even in the 90° bending position, which are among those of the so far reported best-performing flexible lithium-ion batteries. This research offers a promising avenue for the exploitation of high-powered flexible lithium-ion batteries and other rechargeable batteries.

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[email protected] @SiO 2 microcapsules with controlled porosity for whole-cell based enantioselective biosynthesis of ( S )−1-phenylethanol

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Colloids and Surfaces B: Biointerfaces 2022年 214卷

作者： Li Wang Bo-Bo Zhang Xiao-Yu Yang Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Luoshi Road 122 Wuhan 430070 China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 Rue de Bruxelles Namur 5000 Belgium Guangdong Provincial Key Laboratory of Marine Biotechnology Institute of Marine Sciences Department of Biology College of Science Shantou University Shantou 515063 China

Whole-cell biocatalysis, owing to its high enantioselectivity, environment friendly and mild reaction condition, show a great prospect in chemical, pharmaceutical and fuel industry. However, several problems still limit its wide applications, mainly concerning the low productivity and poor stability. Although the biocatalyst encapsulated in the most-commonly-used alginate hydrogels demonstrate enhanced stability, it still suffers from low biocatalytic productivity, long-term reusability and poor mass diffusion control. In this work, hybrid [email protected] @SiO 2 microcapsules with controlled porosity are designed to encapsulate yeast cells for the asymmetric biosynthesis of ( S )− 1-phenylethonal from acetophenone. The hybrid microcapsules are formed by the ionic cross-linking of alginate, the polymerization of dopamine monomers and the protamine-assisted colloidal packing of uniform-sized silica nanoparticles. Alginate provides the encapsulated cells with highly biocompatible environment. Polydopamine enables to stimulate the biocatalytic productivity of the encapsulated yeast cells. Silica shells can not only regulate the mass diffusion in biocatalysis but also enhance the long-term mechanical and chemical stability of the microcapsules. The morphology, structure, chemical composition, stability and molecular accessibility of the hybrid microcapsules are investigated in detail. The viability and asymmetric bioreduction performance of the cells encapsulated in microcapsules are evaluated. The 24 h product yield of the cells encapsulated in the hybrid microcapsules shows 1.75 times higher than that of the cells encapsulated in pure alginate microcapsules. After 6 batches, the 24 h product yield of the cells encapsulated in the hybrid microcapsules is well maintained and 2 times higher than that of the cells encapsulated in pure alginate microcapsules. Therefore, the hybrid microcapsules designed in this study enable to enhance the asymmetric biocatalytic activity,

关键词： Hybrid hydrogel Surface coating Colloidal packing Ordered porosity Cell encapsulation Asymmetric bioreduction

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