可充电镁电池负极材料及界面化学的研究进展

doi:10.11900/0412.1961.2024.00357

金属学报

2025, Vol. 61

Issue (3): 437-454 DOI: 10.11900/0412.1961.2024.00357

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可充电镁电池负极材料及界面化学的研究进展

文恬恬¹^,², 岳继礼¹^,², 熊方宇¹^,², 袁媛¹^,², 黄光胜¹^,²(

), 王敬丰¹^,², 潘复生¹^,²

1 重庆大学材料科学与工程学院重庆 400044
2 重庆大学国家镁合金材料工程技术研究中心重庆 400044

Research Progress on Anode Materials and Interfacial Chemistry for Rechargeable Magnesium Batteries

WEN Tiantian¹^,², YUE Jili¹^,², XIONG Fangyu¹^,², YUAN Yuan¹^,², HUANG Guangsheng¹^,²(

), WANG Jingfeng¹^,², PAN Fusheng¹^,²

1 School of Materials Science and Engineering, Chongqing University, Chongqing 400044, China
2 National Engineering Research Center for Magnesium Alloys, Chongqing University, Chongqing 400044, China

引用本文:

文恬恬, 岳继礼, 熊方宇, 袁媛, 黄光胜, 王敬丰, 潘复生. 可充电镁电池负极材料及界面化学的研究进展[J]. 金属学报, 2025, 61(3): 437-454.
Tiantian WEN, Jili YUE, Fangyu XIONG, Yuan YUAN, Guangsheng HUANG, Jingfeng WANG, Fusheng PAN. Research Progress on Anode Materials and Interfacial Chemistry for Rechargeable Magnesium Batteries[J]. Acta Metall Sin, 2025, 61(3): 437-454.

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摘要:

可充电镁电池凭借其优异的电化学性能、镁资源的丰富性以及Mg均匀沉积的特性，已成为极具潜力的下一代电池之一。然而，其负极材料存在界面钝化、体积膨胀以及不均匀Mg剥离/沉积等问题，成为制约镁电池商业化进程的主要瓶颈。尽管在探索新型负极材料体系与界面化学调控策略上已取得了较多进展，但开发具有高能量密度、高功率密度、优异稳定性及长循环寿命等优势的负极材料仍面临着许多挑战。本文系统地回顾了可充电镁电池负极材料及界面调控领域的最新研究进展，深入剖析了材料组分、微观结构以及表面/界面结构对电化学性能的影响及其内在作用机制，并对未来负极材料的开发设计及界面调控进行了展望。

关键词 ：可充电镁电池, 负极材料, 负极-电解液界面, 调控策略

Abstract：

Rechargeable magnesium batteries have emerged as highly promising alternatives in the field of ion batteries, owing to their excellent electrochemical performance, abundance of magnesium resources, and uniform deposition of magnesium. However, challenges such as interface passivation, volume expansion, and uneven stripping/plating of anode materials persist in impeding the commercialization process of rechargeable magnesium batteries. Despite significant progress in exploring novel anode materials and interfacial chemical regulation strategies, developing anode materials that combine high energy density, high power density, excellent stability, and extremely long cycle life continues to pose numerous challenges. This study comprehensively and systematically reviewed the latest research on anode materials and interface regulations for rechargeable magnesium batteries. The influence of material composition, microstructure, and surface/interface structure on electrochemical properties and their underlying mechanisms were analyzed, along with the prospects for the future development and design of anode materials for magnesium batteries and interface regulation.

Key words： rechargeable magnesium battery anode material anode-electrolyte interface regulation strategy

收稿日期: 2024-10-25

ZTFLH:

TM911

基金资助:国家自然科学基金项目(U23A20555);重庆市技术创新与应用发展重点项目(揭榜挂帅)(2024TIAD-KPX0003)

通讯作者: 黄光胜，gshuang@cqu.edu.cn，主要从事镁电池关键材料与电池系统、镁合金的塑性机理与塑性加工技术研究

Corresponding author: HUANG Guangsheng, professor, Tel: (023)65102821, E-mail: gshuang@cqu.edu.cn

作者简介: 文恬恬，女，1995年生，博士

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图1 纯Mg负极的困境：钝化问题[19]；不均匀剥离/沉积问题[20,21]；加工难题[22,24]

图2 Mg-Ga合金负极的代表性研究：Mg-Ga体系的固-液相变机制及长循环稳定性[25]；还原氧化石墨烯(rGO)限域的Ga负极(Ga@rGO)充电前后的形貌[36]

图3 界面钝化：TFSI-、[Mg+-TFSI-]及[Mg2+-TFSI-]的解离能[41]；配位溶剂分子的不稳定性[42]；电解液溶剂化结构的结合能和电荷态[43]

图4 不均匀Mg沉积/剥离[55]：Mg沉积过程示意图及扩散限制理论和成核理论的标准参数(以全苯基络合物(APC)电解液为例)；扩散控制缓冲区示意图；10 mA/cm2电流密度下Mg在APC电解液中的沉积形貌；5 mA/cm2电流密度下Mg在玻璃纤维隔膜中的沉积行为

图5 Mg/黑磷复合负极(Mg@BP)[57]、Bi纳米管(Bi-NTs)纳米负极[34]、Bi-Sn多相合金负极[59]和InSb-10%C负极[64]的体积膨胀

图6 吸附能和扩散能的理论计算：Mg原子在不同Mg和MgIn晶面上的吸附能[65]；四氢呋喃(THF)、乙二醇二甲醚(DME)、二乙二醇二甲醚(G2)和2-甲氧基乙胺(MOEA)分子在Mg(0001)上的吸附模型和吸附能[51]；Mg在Mg3Sb2和MgCl2中的迁移能垒[66]；Mg2+在各种无机镁化合物中的扩散能垒[67]

图7 相场模拟及分子动力学模拟：通过相场模拟得出Li和Mg的沉积形貌[68]；Mg(OTf)2/DME/G2和Mg(OTf)2/DME/G2/MOEA电解质体系的溶剂化结构分析[44]；Mg(TFSI)2和Mg[B(Otfe)4]2电解质体系稳定性的从头计算分子动力学(AIMD)模拟[69]

图8 负极材料成分与结构设计：亲镁三维结构的材料[70]；AZ31镁合金负极[71]；纳米Mg负极(N-Mg)[72]；Mg-Gd镁合金负极[74]；Mg-Ce镁合金负极[76]

图9 负极固体电解质界面(SEI)膜改性：Mg2Ga5人工SEI膜[82]；Ga5Mg2-Mg人工SEI膜[80]；Bi/MgCl2/聚四氢呋喃(PTHF)杂化人工SEI膜[84]；MgMOF@Mg的作用机理[87]；无机沸石聚合物人工SEI膜[89]；植酸人工SEI膜[91]；Al3+增强型植酸人工SEI膜[92]

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