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Design Strategies for Aqueous Zinc Metal Batteries with High Zinc Utilization: From Metal Anodes to Anode-Free Structures

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Nano-Micro Letters 2024年第4期16卷 305-349页

作者： Xianfu Zhang Long Zhang Xinyuan Jia Wen Song Yongchang Liu School of materials science and Engineering University of Science and Technology Beijing30 College RoadBeijing 100083People’s Republic of China Beijing advanced Innovation Center for materials Genome Engineering Institute for Advanced Materials and TechnologyState Key Laboratory for Advanced Metals and MaterialsUniversity of Science and Technology BeijingBeijing 100083People’s Republic of China

Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage due to the excellent safety, environmental friendliness, natural abundance, high theoretical specific capacity, and low redox potential of zinc(Zn) metal. However,several issues such as dendrite formation, hydrogen evolution, corrosion, and passivation of Zn metal anodes cause irreversible loss of the active materials. To solve these issues, researchers often use large amounts of excess Zn to ensure a continuous supply of active materials for Zn anodes. This leads to the ultralow utilization of Zn anodes and squanders the high energy density of AZMBs. Herein, the design strategies for AZMBs with high Zn utilization are discussed in depth, from utilizing thinner Zn foils to constructing anode-free structures with theoretical Zn utilization of 100%, which provides comprehensive guidelines for further research. Representative methods for calculating the depth of discharge of Zn anodes with different structures are first summarized. The reasonable modification strategies of Zn foil anodes, current collectors with pre-deposited Zn, and anode-free aqueous Zn metal batteries(AF-AZMBs) to improve Zn utilization are then detailed. In particular, the working mechanism of AF-AZMBs is systematically introduced. Finally, the challenges and perspectives for constructing high-utilization Zn anodes are presented.

关键词： Aqueous zinc metal batteries Zinc anodes High zinc utilization Depth of discharge Anode-free structures

Negative enthalpy alloys and local chemical ordering:a concept and route leading to synergy of strength and ductility

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National science Review 2024年第4期11卷 172-184页

作者： Zibing An Tao Yang Caijuan Shi Shengcheng Mao Lihua Wang Ang Li Wei Li Xianmeng Xue Ming Sun Yifan Bai Yapeng He Fuzeng Ren Zhouguang Lu Ming Yan Yang Ren Chain-Tsuan Liu Ze Zhang Xiaodong Han Beijing Key Lab of Microstructure and Property of advanced materials College of Materials Science &Engineering Beijing University of Technology department of materials science and Engineering City University of Hong Kong Key Laboratory of Partial Acceleration Physics& Technology Institute of High Energy PhysicsChinese Academy of Sciences department of materials science &Engineering Southern University of Science and Technology department of Physics City University of Hong Kong State Key Laboratory of Silicon materials Department of Materials Science and Engineering Zhejiang University

Solid solutions are ubiquitous in metals and alloys. Local chemical ordering(LCO) is a fundamental sub-nano/nanoscale process that occurs in many solid solutions and can be used as a microstructure to optimize strength and ductility. However, the formation of LCO has not been fully elucidated, let alone how to provide efficient routes for designing LCO to achieve synergistic effects on both superb strength and ductility. Herein, we propose the formation and control of LCO in negative enthalpy alloys. With engineering negative enthalpy in solid solutions, genetic LCO components are formed in negative enthalpy refractory high-entropy alloys(RHEAs). In contrast to conventional ‘trial-and-error' approaches, the control of LCO by using engineering negative enthalpy in RHEAs is instructive and results in superior strength(1160 MPa) and uniform ductility(24.5%) under tension at ambient temperature, which are among the best reported so far. LCO can promote dislocation cross-slip, enhancing the interaction between dislocations and their accumulation at large tensile strains; sustainable strain hardening can thereby be attained to ensure high ductility of the alloy. This work paves the way for new research fields on negative enthalpy solid solutions and alloys for the synergy of strength and ductility as well as new functions.

关键词： negative enthalpy alloys local chemical ordering strength ductility dislocation

The dynamic surface evolution of halide perovskites induced by external energy stimulation

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National science Review 2024年第4期11卷 185-194页

作者： Feiyu Cheng Pengdong Wang Chenzhe Xu Qingliang Liao Suicai Zhang Haochun Sun Wenqiang Fan Guodong Liu Zhiyun Li Yaping Kong Li Wang Fangsen Li Zhuo Kang Yue Zhang Academy for advanced Interdisciplinary science and Technology State Key Laboratory for Advanced Metals and Materials University of Science and Technology Beijing Beijing Key Laboratory for advanced Energy materials and Technologies Key Laboratory of Advanced Materials and Devices for Post-Moore ChipsMinistry of EducationBeijing Advanced Innovation Center for Materials Genome Engineering School of Materials Science and EngineeringUniversity of Science and Technology Beijing Vacuum Interconnected Nanotech Workstation(Nano-X) Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of Sciences Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences

Tracking the dynamic surface evolution of metal halide perovskite is crucial for understanding the corresponding fundamental principles of photoelectric properties and intrinsic instability. However, due to the volatility elements and soft lattice nature of perovskites, several important dynamic behaviors remain unclear. Here, an ultra-high vacuum（UHV） interconnection system integrated by surface-sensitive probing techniques has been developed to investigate the freshly cleaved surface of CH3NH3PbBr3in situ under given energy stimulation. On this basis, the detailed three-step chemical decomposition pathway of perovskites has been clarified. Meanwhile, the evolution of crystal structure from cubic phase to tetragonal phase on the perovskite surface has been revealed under energy stimulation. Accompanied by chemical composition and crystal structure evolution, electronic structure changes including energy level position,hole effective mass, and Rashba splitting have also been accurately determined. These findings provide a clear perspective on the physical origin of optoelectronic properties and the decomposition mechanism of perovskites.

关键词： metal halide perovskite external energy stimulation surface dynamic evolution surface electronic structure ultra-high vacuum interconnection system

Design and tailoring of patterned ZnO nanostructures for perovskite light absorption modulation

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International Journal of Minerals,Metallurgy and materials 2024年第5期31卷 855-861页

作者： Haonan Si Xuan Zhao Qingliang Liao Yue Zhang Academy for advanced Interdisciplinary science and Technology Beijing Advanced Innovation Center for Materials Genome EngineeringUniversity of Science and Technology BeijingBeijing 100083China Key Laboratory of advanced materials and Devices for Post-Moore Chips Ministry of EducationBeijing Key Laboratory for Advanced Energy Materials and TechnologiesSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Lithography is a pivotal micro/nanomanufacturing technique,facilitating performance enhancements in an extensive array of devices,encompassing sensors,transistors,and photovoltaic devices.The key to creating highly precise,multiscale-distributed patterned structures is the precise control of the lithography process.Herein,high-quality patterned ZnO nanostructures are constructed by systematically tuning the exposure and development times during lithography.By optimizing these parameters,ZnO nanorod arrays with line/hole arrangements are successfully prepared.Patterned ZnO nanostructures with highly controllable morphology and structure possess discrete three-dimensional space structure,enlarged surface area,and improved light capture ability,which achieve highly efficient energy conversion in perovskite solar cells.The lithography process management for these patterned ZnO nanostructures provides important guidance for the design and construction of complex nanostructures and devices with excellent performance.

关键词： lithography patterned ZnO nanorod arrays light absorption perovskite solar cell

Phase field modeling of grain stability of nanocrystalline alloys by explicitly incorporating mismatch strain

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Rare Metals 2024年第7期43卷 3370-3382页

作者： Min Zhou Hong-Hui Wu Yuan Wu Hui Wang Xiong-Jun Liu Sui-He Jiang Xiao-Bin Zhang Zhao-Ping Lu Beijing advanced Innovation Center for materials Genome Engineering State Key Laboratory for Advanced Metals and MaterialsUniversity of Science and Technology Beijing Institute for Carbon Neutrality University of Science and Technology Institute of materials Intelligent Technology Liaoning Academy of Materials

Ab st ra ct Nanocrystalline materials exhibit unique properties due to their extremely high grain boundary(GB) density.However,this high-density characteristic induces grain coarsening at elevated temperatures,thereby limiting the widespread application of nanocrystalline materials.Recent experimental observations revealed that GB segregation and second-phase pinning effectively hinder GB migration,thereby improving the stability of nanocry stalline materials.In this study,a mouified phase-field model that integrates mismatch strain,solute segregation and precipitation was developed to evaluate the influence of lattice misfit on the thermal stability of nanocrystalline alloys.The simulation results indicated that introducing a suitable mismatch strain can effectively enhance the microstructural stability of nanocrystalline alloys.By synergizing precipitation with an appropriate lattice misfit,the formation of second-phase particles in the bulk grains can be suppressed,thereby facilitating solute segregation/precipitation at the GBs.This concentrated solute segregation and precipitation at the GBs effectively hinders grain migration,thereby preventing grain coarsening.These findings provide a new perspective on the design and regulation of nanocrystalline alloys with enhanced thermal stability.

关键词： Phase field model Mismatch strain Second-phase precipitation Grain boundary segregation Nanocrystalline alloys

Crystalline-amorphous M@MNx（M=Co,Fe,Ni）encapsulated in nitrogen-doped carbon for enhanced efficient and durable hydrogen evolution reaction

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Rare Metals 2024年第4期43卷 1547-1556页

作者： Yang Yang Xiao-Chuan Duan Shao-Hui Guo Xian-Ming Zhang College of materials science and Engineering College of ChemistryKey Laboratory of Interface Science and Engineering in Advanced MaterialsTaiyuan University of Technology

Developing earth-abundant electrocatalysts for hydrogen evolution reaction（HER） is important for the sustainable energy economy.Herein,efficient and stable heterocatalysts consisting of crystalline-amorphous M@MNx（M=Co,Fe,Ni） encapsulated in N-doped carbon layers supported with N-doped graphene sheets（denoted as M@MNx@NC-NG） are synthesized by facile hydrothermal reaction and nitridation process.During the nitriding process,metal ions in M（tzbc）2（H2O）4(tzbc=4-（1H-1,2,4-triazol-1-yl） benzoic acid) complexes are reduced to crystalline M cores,accompanied by the formation of amorphous MNxshells;the tzbc ligands are insitu carbonized to form outermost N-doped carbon（NC）layers that connect with inner MNxvia M-N-C motifs inherited from the complex precursors and inhibit the transition of MNxfrom amorphous to crystalline phase.The Co@CoNx@NC-NG catalyst exhibits excellent HER activity with small overpotentials of 45 and 64 mV at a cathode current density of 10 mA·cm-2and low Tafel slopes of 40 and 85 mV·dec-1in 0.5 mol·L-1H2SO4and1.0 mol·L-1KOH electrolytes,respectively.The Co@CoNx@NC-NG retains 97% of the initial overpotential after 100,000 s in both acidic and alkaline media.Such outstanding HER performance originates from the crystalline-amorphous Co@CoNxthat redistributes electrons around the heterointerfaces,facilitating the conversion process of H+/H2O to hydrogen and thereby promoting HER kinetics.The outermost NC layers serve as the armor of Co@CoNx,and graphene nanosheets act as carriers of egg-like Co@CoNx@NC and conduction paths for electron shuttles,ensuring stable and continuous electrocatalytic hydrogen production.

关键词： Hydrogen evolution reaction Electrocatalysts Iron group metals Heterojunction Crystalline-amorphous structure

Recent advances and perspectives in MXene-based cathodes for aqueous zinc-ion batteries

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International Journal of Minerals,Metallurgy and materials 2024年第7期31卷 1752-1765页

作者： Aiduo Wu Tianhao Wang Long Zhang Chen Chen Qiaomin Li Xuanhui Qu Yongchang Liu Beijing advanced Innovation Center for materials Genome Engineering Institute for Advanced Materials and TechnologyState Key Laboratory for Advanced Metals and MaterialsUniversity of Science and Technology BeijingBeijing 100083China School of materials science and Engineering University of Science and Technology BeijingBeijing 100083China School of Economics and Management University of Science and Technology BeijingBeijing 100083China

Aqueous zinc-ion batteries(AZIBs)show great potential for applications in grid-scale energy storage,given their intrinsic safety,cost effectiveness,environmental friendliness,and impressive electrochemical performance.However,strong electrostatic interactions exist between zinc ions and host materials,and they hinder the development of advanced cathode materials for efficient,rapid,and stable Zn-ion storage.MXenes and their derivatives possess a large interlayer spacing,excellent hydrophilicity,outstanding electronic conductivity,and high redox activity.These materials are considered“rising star”cathode candidates for AZIBs.This comprehensive review discusses recent advances in MXenes as AZIB cathodes from the perspectives of crystal structure,Zn-storage mechanism,surface modification,interlayer engineering,and conductive network design to elucidate the correlations among their composition,structure,and electrochemical performance.This work also outlines the remaining challenges faced by MXenes for aqueous Zn-ion storage,such as the urgent need for improved toxic preparation methods,exploration of potential novel MXene cathodes,and suppression of layered MXene restacking upon cycling,and introduces the prospects of MXene-based cathode materials for high-performance AZIBs.

关键词： aqueous zinc-ion batteries MXenes terminal groups interlayer engineering conductive network design

Modeling asymmetric fracture mechanics of Mg alloy wire in drawing process

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Journal of Magnesium and Alloys 2024年第5期12卷 2057-2069页

作者： Sunghoon Choi Jongwon Shin Joung Sik Suh Dongchoul Kim department of Mechanical Engineering Sogang University advanced Metals Division Korea Institute of Materials Science

In this study, a numerical analysis was conducted on the ductile fracture of a 2-mm diameter Mg-1Zn-0.5Mn-0.5Sr-0.1Ca alloy wire during drawing. The hexagonally close-packed crystal structure of Mg alloys causes asymmetric fracture behavior, especially in the compression region. The aim of this study is to develop a comprehensive damage model for Mg alloy wire that accurately predicts ductile fracture, with a focus on the compression region. A novel experimental method was introduced to measure the ductile fracture of Mg alloy wires under different stress states. The wire drawing process was simulated using the Generalized Incremental Stress-State dependent damage(GISSMO)Model and the Semi-Analytical Model for Polymers(SAMP) model. The damage model's prediction and the experimental results were found to be in excellent agreement, especially in determining crack initiation. Computational analysis established a safe zone diagram for die angle and reduction ratio, and experimental validation confirmed the feasibility of this approach. The proposed damage model can provide a practical and reliable analysis for optimizing the drawing process of Mg alloy wire.

关键词： Mg alloy Wire drawing Finite element method Damage model Safe zone diagram

Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li department of Chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State Key Laboratory of Surface Physics and department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable challenge.Herein,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as templates.The key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon matrix.The mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion lengths.This method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries