水系镁离子电池研究进展

涂天成; 李龙燕; 代启航

doi:10.13801/j.cnki.fhclxb.20221206.001

水系镁离子电池研究进展

doi: 10.13801/j.cnki.fhclxb.20221206.001

南京信息工程大学　化学与材料学院，南京 210000

基金项目: 国家自然科学基金(21905139)

详细信息

通讯作者:
李龙燕，博士，副教授，硕士生导师，研究方向为储能、动力电池体系材料研究、电化学、功能性纳米材料、废旧动力电池资源化利用　E-mail: lilongyan@nuist.edu.cn

中图分类号: TQ152
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出版历程
- 收稿日期: 2022-10-12
- 修回日期: 2022-11-14
- 录用日期: 2022-11-30
- 网络出版日期: 2022-12-06
- 刊出日期: 2023-07-15

Research progress of aqueous magnesium ion battery

School of Chemistry and Materials Science, Nanjing University of Information Science and Technology, Nanjing 210000, China

Funds: National Natural Science Foundation of China (21905139)

摘要

摘要: 目的水系镁离子电池作为一种新兴的储能体系有着低成本、原料来源充足、高理论储能能力等优势。但水系电解液和镁自身带来的问题都极大地限制了水系镁离子电池的进一步发展。本文综述近年相关文献来对有关水系镁离子电池的最新研究进行总结并做出展望。方法综述有关水系镁离子电池的相关研究，从电解液、电极材料、新兴表征分析方法等方面总结存在的问题及相应研究成果，并对未来水系镁离子电池研究方向进行展望。结果目前水系镁离子电池尚未得到充分发展，其受限因素主要来自于水系电解液存在的电化学窗口窄、水分解产气等固有问题，正极材料匹配性问题，以及负极侧的枝晶、析氢等问题。电解液中电解质的种类及浓度对其性质有重要影响，在水系电池领域内有降低电解液游离水含量、引入chaotropic阴离子、构建多元阳离子体系、引入电解质添加剂等策略拓宽电解液电化学窗口、提高其工作电压、增强电池高低温极端条件下电化学性能。而“盐包水”等策略虽然能够拓宽水系电池的电化学稳定窗口，但其成本相对较高且镁离子迁移速率也并未得到提升。相较而言，在常规浓度电解液中构建混合阳离子补强和添加改变离子溶剂化结构的电解液添加剂等策略相对来说更加有发展前景。对于电极材料，如MgMnO、MgFeMnO和LiMnO•HO等正极材料来说，无论是单独作为正极材料还是与碳纳米管、石墨等材料制成复合材料，都已证明了他们在水系镁离子电池中的优越性。由于金属镁在水溶液中的不稳定性，可通过表面包覆改性、微合金化等方法提高镁金属及其合金直接作为水系电池负极的应用性。其它负极材料，如近年来新兴的聚合物负极材料，将传统的金属负极的溶解沉积的电化学过程替代为活性位点与离子反应过程，这将有效抑制枝晶等副反应的发生，也有助于提升水系镁离子电池的性能。除此之外也总结了一些计算手段、新兴的实验技术方法在水系镁离子电池体系中的应用。结论本文总结了目前水系镁离子电池受限因素和相应的策略，电解液中电解质的种类及浓度对其性质有重要影响，可通过适当引入chaotropic阴离子、构建多元阳离子体系、引入电解质添加剂等策略提升电池电化学性能。目前锰酸镁、锰酸铁镁等的复合正极材料展现了他们的优越性。此外对于负极材料，可通过表面包覆改性、微合金化等方法。也可以选用其他负极材料，如聚合物材料，帮助发挥水系镁离子电池的潜力。第一性原理密度泛函理论(DFT)等计算手段对水系镁离子电池体系的研究也卓有成效，结合机器学习、原位光学观察、EIR改进的拉曼光谱技术、EC-AFM原位观察技术等高精度实验测试方法和技术，相信在未来水系镁离子电池体系将得到更深入的理解以及更广泛的贴合实际场景的应用。
- 水系镁离子电池 /
- 水系电解液 /
- 电极材料 /
- 储能 /
- 研究进展
Abstract: As a newly developed energy storage system, aqueous magnesium ion battery takes its edge by lower cost, more abundant source of raw materials, higher theoretical energy storage capacity. However, the problems brought by aqueous electrolytes and magnesium themselves greatly limit the further development of aqueous magnesium ion batteries. Here, the influence of the type and concentration of anions in aqueous electrolyte and electrolyte additives on the battery performance is described, and the research of some electrode materials, including new materials and new theories, is introduced. Finally, some efficient characterization and analysis methods are summarized.
- aqueous magnesium ion batteries /
- aqueous electrolytes /
- electrode materials /
- energy storage /
- research progress

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图 1 水系镁离子电池发展中遇到的问题

Figure 1. Problems encountered in the development of the aqueous magnesium ion battery

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图 2 PNTAQ在MgCl₂电解液中的循环性能(a)和离子迁移示意图(b)^[29]

Figure 2. Schematic diagram of cycling performance (a) and ion migration (b) of PNTAQ in MgCl₂ electrolyte ^[29]

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图 3 阴离子类型与电解液凝固点(a)、氢键强度(b)的关系^[31]

Figure 3. Relationship between the anion type and the freezing point (a), the hydrogen bond strength (b) of electrolyte^[31]

T—Temperature; t—Time

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图 4 水包盐和盐包水溶剂化分子的区别(a)和盐包水电解液对电化学稳定窗口的扩大(b)^[33]

Figure 4. Solvation molecule difference between salt-in-water and water-in-salt (a) and the expansion of electrochemical stability window by water-in-salt electrolyte (b)^[33]

TFSI—Bis(trifluoromethane sulfonimide); i—Current difference

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图 5 电化学转化法制备的MgMn₂O₄及其电化学性能^[55]：(a) MgMn₂O₄材料的恒流充放电测试(GCD)；(b) MgMn₂O₄材料的循环性能；(c) 循环伏安(CV)曲线；(d) MgMn₂O₄材料的SEM图像；(e) MgMn₂O₄材料的TEM图像

Figure 5. MgMn₂O₄ prepared by electrochemical conversion method and its electrochemical performance^[55]: (a) Galvanostatic charge-discharge (GCD) test of MgMn₂O₄ material; (b) Cyclic performance of MgMn₂O₄ material; (c) Cyclic voltammetry (CV) curves; (d) SEM image of MgMn₂O₄ material; (e) TEM image of MgMn₂O₄ material

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图 6 腐蚀与自腐蚀过程^[16]

Figure 6. Corrosion and self-corrosion process^[16]

I—Electric current

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图 7 不同镁合金块效应对比^[16]

Figure 7. Comparison of chunk effect of different magnesium alloys^[16]

3.4-DHB—3, 4-dihydroxybenzoic acid; ZE41, WE43, AM50—Different types of magnesium alloys

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图 8 聚酰亚胺基材料负极的电化学性能(a)和电化学反应过程(b)^[65]

Figure 8. Electrochemical performance (a) and electrochemical reaction process (b) of polyimide based material cathode^[65]

i_p—Measured current; a, b—Variable parameters; v—Voltage sweep rate; P—Polyimide

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图 9 原位表征下有无保护层的对比^[77]：(a) 无保护层；(b) 有保护层

Figure 9. Comparison between the presence and absence of protective layer under in-situ characterization^[77]: (a) No protective layer; (b) With protective layer

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图 10 利用电化学原子力显微镜技术 (EC-AFM) 原位观测双三氟甲基磺酰亚胺锂(LiTFSI)水电解质存在下的固体电解质界面(SEI)层^[81]

Figure 10. In-situ observation of solid electrolyte interphase (SEI) layer in the presence of lithium bis(trifluoromethane sulfonyl) imide (LiTFSI)-water electrolyte by electrochemical-controlled atomic force microscopy (EC-AFM)^[81]

OCP—Open circuit potential

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表 1 水系电解液主要研究方向

Table 1. Main research directions of aqueous electrolyte

Research direction	Specific research	Reference
Anion type	Cl⁻ as the main anion	[26-29]
	Kosmotropic anion as the main anion, e.g., SO₄²⁻	[30-32]
	Chaotropic anion as the main anion, e.g., NO₃⁻	[19]
Electrolyte concentration	“Water-in-salt” electrolyte	[33-35]
	Hydrated eutectic electrolyte system	[19]
	Hydrate melts, water in water ionomers, molecular crowding, etc.	[36-40]
Mixed cation	Mg/Na, Mg/Zn, etc.	[29, 41-42]
Electrolyte additive	Improve battery performance or alleviate various problems caused by electrolyte	[43-44]

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