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Design and application of copper/lithium composite anodes for advanced lithium metal batteries

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Abstract

Lithium (Li) is a promising candidate for next-generation battery anode due to its high theoretical specific capacity and low reduction potential. However, safety issues derived from the uncontrolled growth of Li dendrite and huge volume change of Li hinder its practical application. Constructing dendrite-free composite Li anodes can significantly alleviate the above problems. Copper (Cu)-based materials have been widely used as substrates of the composite electrodes due to their chemical stability, excellent conductivity, and good mechanical strength. Copper/lithium (Cu/Li) composite anodes significantly regulate the local current density and decrease Li nucleation overpotential, realizing the uniform and dendrite-free Li deposition. In this review, Cu/Li composite methods including electrodeposition, melting infusion, and mechanical rolling are systematically summarized and discussed. Additionally, design strategies of Cu-based current collectors for high performance Cu/Li composite anodes are illustrated. General challenges and future development for Cu/Li composite anodes are presented and postulated. We hope that this review can provide a comprehensive understanding of Cu/Li composite methods of the latest development of Li metal anode and stimulate more research in the future.

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摘要

金属锂具有超高的理论比容量 (3860 mAh·g–1) 和极低的电极电势 (− 3.04 V vs. 标准氢电极电势), 有望成为下一代电池负极材料。然而, 充放电过程中, 锂枝晶生长不可控和锂体积变化大导致的严重安全隐患和低效率问题阻碍了锂金属电池的商业化应用。通过构建无枝晶复合锂负极可以显著缓解上述问题。铜基材料因其化学稳定性、优良的导电性和良好的机械强度而被广泛应用于复合锂负极的基体。铜/锂 (Cu/Li) 复合阳极显著的调控了局部电流密度, 降低了锂形核过电位, 实现了均匀无枝晶的锂沉积。本文系统讨论了三种Cu/Li复合方法包括电沉积、热熔融浸润、机械辊压, 并总结了三种方法的优缺点。此外, 文章阐述了用于高性能Cu/Li复合负极的Cu基集流体的设计策略。提出了Cu/Li复合阳极所面临的挑战和未来的发展趋势。我们希望通过本文的综述可以全面了解Cu/Li复合方法在锂金属阳极方面的最新进展, 并激发未来更多的研究。

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Fig. 1
Fig. 2

Reproduced with permission from Ref. [34]. Copyright 2019, Wiley-VCH. d EBSD mappings for bare Cu foil (left), wCu foil (middle) and 100-wCu foil (right); surface morphologies of e bare Cu foil, f wCu foil and g 100-wCu foil after initial Li deposition. Reproduced with permission from Ref. [62]. Copyright 2021, Elsevier

Fig. 3

Reproduced with permission from Ref. [63]. Copyright 2019, Elsevier. i XRD patterns for 1 pristine Cu, 2 SF-Cu foils, 3 SF-Cu foil after 100 cycles and 4 SF-Cu foil after 200 cycles; j DFT simulation analysis of surface structure for SF-Cu foil; k CEs of cells with CuNW and SF-CuNW at 3 mA·cm−2 and 3 mAh·cm−2. Reproduced with permission from Ref. [33]. Copyright 2021, Wiley-VCH

Fig. 4

Reproduced with permission from Ref. [89]. Copyright 2022, Wiley-VCH. e Schematic diagram of Li plating/stripping for the dynamic intelligent porous Cu (DICu) CC; f schematic illustration of interaction between the Cu microparticles at pristine, low and high Li loading states. Reproduced with permission from Ref. [94]. Copyright 2020, American Chemical Society. g Schematic diagram of electric field distribution in planar Cu (P-Cu) and E-Cu; h simulated analysis of electric field distribution in E-Cu. Reproduced with permission from Ref. [96]. Copyright 2018, Springer Nature. i Simulated analysis of electrolyte and electrode current density of 2.5D micro/nanostructured Cu CC. Reproduced with permission from Ref. [65]. Copyright 2022, Wiley-VCH

Fig. 5

Reproduced with permission from Ref. [64]. Copyright 2019, American Chemical Society. b Schematic illustration of Li deposition behaviors on different CCs [39]. Copyright 2021, Elsevier. c Schematic diagram of synthesis process of CF@Cu2Mg; schematic illustration of Li plating behaviors on d bare CF and e CF@Cu2Mg; adsorption structures of single Li atom on f Cu(111) and g Cu2Mg(111) planes; h adsorption energies of single Li atom on Cu(111) and Cu2Mg(111) planes [40]. Copyright 2022, American Chemical Society

Fig. 6

Reproduced with permission from Ref. [29]. Copyright 2020, American Chemical Society. Schematic illustration of Li deposition behavior and simulated analysis of Li reaction flux for d Cu foil, e Cu mesh, and f conductivity gradient (CG) host. Reproduced with permission from Ref. [68]. Copyright 2020, Wiley-VCH. Schematic illustration of Li deposition behaviors on g Cu foam (CF) and h nickel–cobalt alloy and zinc oxide onto Cu foam (CNZ); simulation analysis of flow-field state vector of i CF and j CNZ. Reproduced with permission from Ref. [32]. Copyright 2022, Wiley-VCH. Simulation analysis of local current density distribution at k D-Cu@CuSe/electrolyte and l B-Cu/electrolyte interface; simulation analysis of Li-ions flux at m D-Cu@CuSe/electrolyte and n B-Cu/electrolyte interface. Reproduced with permission from Ref. [109]. Copyright 2022, Wiley-VCH

Fig. 7

Reproduced with permission from Ref. [53]. Copyright 2017, Elsevier. b Schematic illustration of fabrication process of 3D Li@Cu composite anode. The digital photographs of Li melting infusion into c 3D CuNW and d Cu foam over 20 s. Reproduced with permission from Ref. [54]. Copyright 2018, Elsevier. e Schematic illustration of fabrication process for LCC composite anode. Reproduced with permission from Ref. [117]. Copyright 2021, Wiley-VCH

Fig. 8

Reproduced with permission from Ref. [119]. Copyright 2022, Elsevier. d Schematic illustration of synthesis process of C-Li2O@CuNA/CF/Li and 3D Cu/CF. Reproduced with permission from Ref. [113]. Copyright 2020, Elsevier. e Schematic illustration of the different stages for self-propagating strategy during the thermal melting infusion process. Reproduced with permission from Ref. [118]. Copyright 2020, American Chemical Society

Fig. 9

Reproduced with permission from Ref. [23]. Copyright 2021, Wiley-VCH. e Schematics of synthetic process for Cu/Li3N rods/Li. Reproduced with permission from Ref. [47]. Copyright 2020, Elsevier. f Schematics of preparation process of Li@MIECS. Reproduced with permission from Ref. [19]. Copyright 2020, Wiley-VCH

Fig. 10

Reproduced with permission from Ref. [111]. Copyright 2020, American Chemical Society. i Gibbs free energy changes of reaction between ZnO and Li at different temperatures; j comparison of Gibbs free energy changes of different compounds at 300 °C. Reproduced with permission from Ref. [42]. Copyright 2020, Elsevier

Fig. 11

Reproduced with permission from Ref. [123]. Copyright 2022, Elsevier. Photographs of Li wettability of f Au/Cu and g pristine Cu CCs. Reproduced with permission from Ref. [116]. Copyright 2021, Wiley-VCH

Fig. 12

Reproduced with permission from Ref. [112]. Copyright 2020, Elsevier. h Schematic diagram of evolution process of Cu-Cu2Mg–Li. Reproduced with permission from Ref. [126]. Copyright 2021, American Chemical Society

Fig. 13

Reproduced with permission from Ref. [128]. Copyright 2017, Wiley-VCH. Schematic illustration of preparation process of e LiI@Cu foil and f LiI/Cu@Li foil electrode; contact angle of electrolyte on g bare Cu and h LiI/Cu@Cu; operando optical microscopy images of i bare Cu and j LiI/Cu during Li plating process. Reproduced with permission from Ref. [130]. Copyright 2022, American Chemical Society

Fig. 14

Reproduced with permission from Ref. [132]. Copyright 2019, Springer. c Schematics of preparation processes of vertically oriented Li-Cu-Li arrays; d elemental mapping for vertically oriented Li-Cu-Li arrays. Reproduced with permission from Ref. [21]. Copyright 2019, Wiley-VCH. e Schematic illustration of fabrication process of zeroVE-Li and Li plating behavior of zeroVE-Li and LiMg anodes; f cross-sectional SEM images of zeroVE-Li; g thickness change of different anodes during continuous plating/stripping; h cycling performance comparison of full batteries with LiMg and zeroVE-Li electrodes. Reproduced with permission from Ref. [22]. Copyright 2022, Wiley-VCH

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Acknowledgements

This study was financially supported by the National Key Research and Development Program of China (No. 2021YFB2500200), the National Natural Science Foundation of China (No. 52302243) and China Postdoctoral Science Foundation (Nos. 2022M721029 and 2022M721030)

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  1. Bin Zhang and Ji-Ping Ma have contributed equally to this work.

Authors and Affiliations

  1. School of Materials Science and Engineering, Henan University of Science and Technology, Luoyang, 471003, China

    Bin Zhang, Ji-Ping Ma, Yang Zhao, Zhan-Ling Zhang & Shi-Zhong Wei

  2. Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China

    Tong Li

  3. School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, 637371, Singapore

    Jin-Lin Yang

  4. Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China

    Guang-Min Zhou

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Zhang, B., Ma, JP., Zhao, Y. et al. Design and application of copper/lithium composite anodes for advanced lithium metal batteries. Rare Met. 43, 942–970 (2024). https://doi.org/10.1007/s12598-023-02477-9

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