非亲核镁硫电池电解液的研究进展

doi:10.6023/A21010038

化学学报 ›› 2021, Vol. 79 ›› Issue (5): 628-640.DOI: 10.6023/A21010038 上一篇下一篇

综述

非亲核镁硫电池电解液的研究进展

李宛飞^a^,^b^,^*(), 李鑫^a^,^b, 范海燕^c, 肖建华^c, 刘倩倩^a^,^b, 程淼^a^,^b, 胡敬^a^,^b, 魏涛^a^,^b, 吴正颖^b, 凌云^a, 刘波^a^,^b, 张跃钢^c^,^*()

a 苏州科技大学纳米光电材料与微结构研究中心苏州 215009
b 苏州科技大学材料科学与工程学院苏州 215009
c 清华大学物理系北京 100084

投稿日期:2021-01-31 发布日期:2021-05-18
通讯作者: 李宛飞, 张跃钢

作者简介:

李宛飞, 苏州科技大学副教授, 硕士生导师. 承担国家自然科学基金2项, 曾参与国家自然科学基金重点项目、中国科学院国际合作局对外合作重点项目、国家重点研发计划新能源汽车重点专项项目、省市级科研项目以及企业横向合作项目10余项. 已在Angew. Chem. Int. Ed., Nano Lett., J. Mater. Chem. A等学术期刊发表文章60余篇, 获授权发明专利18项. 主要研究方向为功能纳米材料合成及结构表征、新型电化学能源存储器件研究等.

李鑫, 硕士研究生. 本科毕业于河南师范大学化学化工学院, 2019年起于苏州科技大学材料科学与工程学院攻读材料学硕士学位. 主要研究方向为镁离子电池材料和电解液.

范海燕, 理学博士, 2020年毕业于中国科学技术大学, 现为清华大学博士后. 主要研究方向为可充镁二次电池电解液的设计合成和性能调控.

肖建华, 博士研究生. 本科毕业于湖南大学物理与微电子科学学院, 2018年起于清华大学物理系攻读物理学博士学位. 主要研究方向为新型镁电池电解液的设计合成和性能优化.

刘波, 博士生导师, 研究员. 主持国家纳米重大科学研究计划(973)项目、国家863计划重点项目子课题、国家863计划目标导向类项目、上海市和江苏省等科研项目19项; 发表SCI论文220篇、授权发明专利123项. 主要研究方向为纳米光电材料与器件(信息存储材料与器件、新能源材料与器件、传感器材料与器件).

张跃钢, 清华大学物理系长聘教授, 博士生导师. 先后在Science、JACS、Angew. Chem. Int. Ed.、Nano Lett.等国际期刊发表论文160余篇, 获得授权专利30余项. 主要研究方向为纳米材料合成与表征、纳米器件制造与测试、能源存储器件研究及原位测试技术等.

基金资助:
项目受国家自然科学基金(21773291); 项目受国家自然科学基金(U1832218); 内蒙古自治区纳米碳材料重点实验室(MDK2019008)

Progress of Non-Nucleophilic Electrolytes for Magnesium/Sulfur Battery

Wanfei Li^a^,^b^,^*(), Xin Li^a^,^b, Haiyan Fan^c, Jianhua Xiao^c, Qianqian Liu^a^,^b, Miao Cheng^a^,^b, Jing Hu^a^,^b, Tao Wei^a^,^b, Zhengying Wu^b, Yun Ling^a, Bo Liu^a^,^b, Yuegang Zhang^c^,^*()

a Research Center for Nanophotonic and Nanoelectronic Materials, Suzhou University of Science and Technology, Suzhou 215009, China
b School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, China
c Department of Physics, Tsinghua University, Beijing 100084, China

Received:2021-01-31 Published:2021-05-18
Contact: Wanfei Li, Yuegang Zhang
About author:
*E-mail: wfli2018@mail.usts.edu.cn
E-mail:yuegang.zhang@tsinghua.edu.cn
Supported by:
National Natural Science Foundation of China(21773291); National Natural Science Foundation of China(U1832218); Inner Mongolia Autonomous Region Key Laboratory of Nanocarbon Materials(MDK2019008)

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摘要/Abstract

自从Muldoon课题组在2011年首次报道以[Mg₂(μ-Cl)₃(THF)₆]⁺为阳离子电化学活性中心的非亲核有机铝镁盐用于镁硫电池以来, 非亲核镁电解液便引起了人们的广泛关注. 本文综述了非亲核镁电解质的合成、阳离子结构及其镁硫电池电解液电化学性能的研究进展. 最后对非亲核镁硫电池电解液未来的发展方向进行了前瞻性的探讨, 指出要推动镁硫电池的产业化, 除了要开发高性能、低成本、结构简单的非亲核电解质材料以外, 深入研究电解质盐及电解液组分与正/负电极材料最优匹配机制也至关重要.

关键词: 镁硫电池, 非亲核电解液, 阳离子结构, 硫正极, 二次电池

Non-nucleophilic magnesium electrolyte has attracted significant attention since the first non-nucleophilic organic aluminum magnesium salt with [Mg₂(μ-Cl)₃(THF)₆]⁺ as the cation of electrochemical active center for magnesium/sulfur (Mg/S) cells was reported by Muldoon group in 2011. In this work, we reviewed the synthesis, cation structure and electrochemical performance of non-nucleophilic magnesium electrolyte for Mg/S battery. The future research directions of non-nucleophilic Mg/S battery electrolyte are discussed. It is pointed out that in order to promote the industrialization of Mg/S battery, in addition to the development of non-nucleophilic electrolyte materials with high performance, low cost and simple structure, further mechanistic understanding for optimization of electrolyte composition and for better matching between the electrolyte with positive or negative electrode materials is also very important.

Key words: magnesium/sulfur battery, non-nucleophilic electrolyte, cation structure, sulfur cathode, rechargeable battery

引用此文

李宛飞, 李鑫, 范海燕, 肖建华, 刘倩倩, 程淼, 胡敬, 魏涛, 吴正颖, 凌云, 刘波, 张跃钢. 非亲核镁硫电池电解液的研究进展[J]. 化学学报, 2021, 79(5): 628-640.

Wanfei Li, Xin Li, Haiyan Fan, Jianhua Xiao, Qianqian Liu, Miao Cheng, Jing Hu, Tao Wei, Zhengying Wu, Yun Ling, Bo Liu, Yuegang Zhang. Progress of Non-Nucleophilic Electrolytes for Magnesium/Sulfur Battery[J]. Acta Chimica Sinica, 2021, 79(5): 628-640.

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图/表 15

图1. 锂镁金属及其硫基电池的理论容量对比图

Figure 1. Comparison of theoretical capacities of lithium and magnesium anode and their S-based cells

图2. 镁电解液的研究发展历程

Figure 2. Research and development of magnesium electrolyte

图3. (a) Mg/S电池结构; (b) Mg/S电池电化学放电反应机制示意图[49]

Figure 3. (a) Schematic illustration of Mg/S battery; (b) discharge reaction mechanism of Mg/S battery[49]

图4. (a) [Mg(THF)6][AlCl4]2的合成路线和晶体结构; (b) [Mg(THF)6][AlCl4]2的镁硫电池电化学性能[53]; (c) LiCl添加的[Mg(THF)6][AlCl4]2电解液的镁硫电池循环性能[54]

Figure 4. (a) Proposed formation mechanism and X-ray crystal structure of [Mg(THF)6][AlCl4]2; (b) electrochemical performance of the Mg/S battery with the electrolyte of [Mg(THF)6][AlCl4]2[53]; (c) cycling performance of Mg/S batteries with pristine and LiCl-added [Mg(THF)6][AlCl4]2 electrolytes[54]

图5. MgCl-FTGB镁硫电池凝胶电解液[56]

Figure 5. MgCl-FTGB gel electrolyte for Mg/S battery[56]

图6. (a) Mg[B(hfip)4]2?3DME的合成路线和X射线晶体结构; (b) Mg[B(hfip)4]2?3DME电解液的Mg/S-CMK-3电池的循环性能[60]; (c) Mg[B(hfip)4]2?3DME电解液的ACCS-Mg电池的循环性能[61]

Figure 6. (a) Proposed formation mechanism and X-ray crystal structure of Mg[B(hfip)4]2?3DME; (b) cycling performance of the Mg/S-CMK-3 cell with the electrolyte of Mg[B(hfip)4]2?3DME[60]; (c) cycling performance of the ACCS-Mg cell with the electrolyte of Mg[B(hfip)4]2?3DME[61]

图7. (a) Mg-FPB?(DGM)2的合成路线和X射线晶体结构; (b) 以DGM为溶剂的Mg-FPB电解液的循环伏安曲线; (c) 以DGM为溶剂的Mg-FPB电解液的线性扫描伏安曲线(LSV) [63]

Figure 7. (a) Proposed formation mechanism and X-ray crystal structure of Mg-FPB?(DGM)2; (b) CV curve of Mg-FPB electrolyte in DGM; (c) linear sweep voltammetry (LSV) curves of the Mg-FPB electrolyte in DGM[63]

图8. (a) BCM, BMOC和Mg(BH4)2/THFPB-DGM电解液的合成路线以及BCM电解液中的阴阳离子种类; (b) 0.05 A?g-1电流条件下, BCM电解液的S/C正极的循环稳定性[64]; (c) BMOC电解液的镁硫电池恒流充放电曲线[65]; (d) 50 mA?g-1电流条件下, Mg(BH4)2/THFPB-DGM电解液的循环性能[66]

Figure 8. (a) Proposed formation mechanism of BCM, BMOC and Mg(BH4)2/THFPB-DGM electrolyte and species in BCM electrolyte; (b) cycling stability of the S/C electrode with the BCM electrolyte at 0.05 A?g-1 [64]; (c) galvanostatic charge/discharge profiles of Mg-S cell with BMOC electrolyte[65]; (d) cycling performance of Mg-S cell with Mg(BH4)2/THFPB-DGM electrolyte at 50 mA?g-1[66]

图9. (a) [Mg2(μ-Cl)3?6THF][HMDSAlCl3]的路易斯酸碱反应合成路线; (b) [Mg2(μ-Cl)3?6THF][HMDSAlCl3]的晶体结构; (c) HMDSMgCl(绿色), HMDSMgCl/AlCl3(蓝色)和[Mg2(μ-Cl)3?6THF][HMDSAlCl3](红色)电解液的循环伏安曲线; (d) [Mg2(μ-Cl)3?6THF][HMDSAlCl3]电解液镁硫电池充放电曲线[45]

Figure 9. (a) Synthetic route to [Mg2(μ-Cl)3?6THF][HMDSAlCl3] via Lewis acid-base reaction; (b) X-ray crystal structure of [Mg2(μ-Cl)3?6THF]- [HMDSAlCl3]; (c) CV of HMDSMgCl (green), HMDSMgCl/AlCl3(blue) and [Mg2(μ-Cl)3?6THF][HMDSAlCl3] electrolyte (red); (d) discharge and charge of Mg/S cell for [Mg2(μ-Cl)3?6THF][HMDSAlCl3] electrolyte[45]

图10. (a) [Mg2Cl3][HMDSAlCl3]的合成路线; (b) [Mg2Cl3][HMDSAlCl3]电解液的循环伏安曲线; (c) [Mg2Cl3][HMDSAlCl3]电解液的S/CMK400PEG为正极的镁硫电池循环性能[49]

Figure 10. (a) Synthetic route to [Mg2Cl3][HMDSAlCl3]; (b) CV of [Mg2Cl3][HMDSAlCl3] electrolyte; (c) cycling performance of S/CMK400PEG cathode for [Mg2Cl3][HMDSAlCl3] electrolytes[49]

图11. (a) [Mg2(μ-Cl)2?6THF][AlCl4]2的合成路线; (b) [Mg2(μ-Cl)2?6THF][AlCl4]2的晶体结构; (c) [Mg2(μ-Cl)2?6THF][AlCl4]2电解液的循环伏安曲线; (d) 氯化锂添加的[Mg2(μ-Cl)2?6THF][AlCl4]2电解液的镁硫电池性能[74]

Figure 11. (a) Synthetic route to [Mg2(μ-Cl)2?6THF][AlCl4]2; (b) X-ray crystal structure of [Mg2(μ-Cl)2?6THF][AlCl4]2; (c) CV of [Mg2(μ-Cl)2?6THF]- [AlCl4]2 electrolyte; (d) electrochemical performance of the Mg/S battery with LiCl additive in the electrolyte of [Mg2(μ-Cl)2?6THF][AlCl4]2[74]

图12. (a) DME/Pyr14TFSI溶剂条件下[Mg2(μ-Cl)2?4DME][AlCl4]2的合成路线; (b) [Mg2(μ-Cl)2?4DME][AlCl4]2电解液的恒流充放电曲线; (c) [Mg2(μ-Cl)2?4DME][AlCl4]2电解液的循环伏安曲线; (d) [Mg2(μ-Cl)2?4DME][AlCl4]2电解液的镁硫电池电化学性能[75]

Figure 12. (a) Synthetic route to [Mg2(μ-Cl)2?4DME][AlCl4]2 in DME/Pyr14TFSI; (b) galvanostatic cycling voltage profiles of [Mg2(μ-Cl)2?4DME]- [AlCl4]2 in DME/Pyr14TFSI; (c) CV of [Mg2(μ-Cl)2?4DME][AlCl4]2 in DME/Pyr14TFSI; (d) electrochemical performance of the Mg/S battery with the electrolyte of [Mg2(μ-Cl)2?4DME][AlCl4]2 in DME/Pyr14TFSI[75]

图13. (a) [Mg2(μ-Cl)3?6THF][TFSI]的合成路线; (b) [Mg2(μ-Cl)3?6THF][TFSI]的X射线晶体结构[76]; (c) MgTFSI2/MgCl2/DME电解液的镁硫电池电化学性能; (d) MgTFSI2/MgCl2/DME电解液中硫和多硫化物的溶解性[77]

Figure 13. (a) Synthetic route to [Mg2(μ-Cl)3?6THF][TFSI]; (b) X-ray crystal structure of [Mg2(μ-Cl)3?6THF] [TFSI][76]; (c) electrochemical performance of the Mg/S battery with MgTFSI2/MgCl2/DME electrolyte; (d) solubility of sulfur and polysulfide in the MgTFSI2/MgCl2/DME electrolyte[77]

图14. (a) OMBB电解质的合成路线和X射线晶体结构; (b) OMBB电解液的镁硫电池循环稳定性[78]

Figure 14. (a) Proposed formation mechanism and X-ray crystal structure of OMBB electrolyte; (b) cycling stability of different S/C electrode with the OMBB electrolyte[78]

Non-nucleophilic magnesium sulfur battery electrolytes		Oxidative stability/V	Coulombic efficiency	Sulfur cathode	Mg-S battery capacity/(mAh/g)@current rate/(mA/g) (cycle)	Ref.
Mononuclear electrolytes	[Mg(THF)₆][AlCl₄]₂	2.5	100%	S/N-doped graphene (mechanic mixing)	40@17 (20th)	^[53]
	[Mg(THF)₆][AlCl₄]₂+LiCl	3.6	98%	NG-NCNT@NCS@S (melt-diffusion)	300@670 (500th)	^[54]
	[Mg(DG)₂][HMDSAlCl₃]₂	3.5	100%	S/C/Graphene/CNT (mechanic mixing)	400@83 (100th)	^[55]
	MgCl-FTGB	4.8	100%	NG-NCNT@NCS@S (melt-diffusion)	1100@167 (50th)	^[56]
	[Mg(DME)₃][B(hfip)₄]₂)	4.5	100%	ACCS (melt-diffusion)	200@167 (100th)	^[61]
	BCM	3.5	99%	S/C (melt-diffusion)	934@50 (30th)	^[64]
	BMOC	4.2	—	S/C (melt-diffusion)	1133@10 (10th)	^[65]
	Mg(BH₄)₂/THFPB-DGM	2.8	99%	S/C (melt-diffusion)	526@50 (30th)	^[66]
	Mg(TFSI)₂	3.4	96%	CMK-3/S (melt-diffusion)	200@34 (4th)	^[67]
	Mg[BH₄]₂+Li[BH₄]	—	—	SPAN (high-temperature reaction)	800@833 (300th)	^[68]
Binuclear electrolytes	[Mg₂(μ-Cl)₃][HMDSAlCl₃] (HMDSMgCl+AlCl₃)	3.3	100%	S/C (mechanic mixing)	394@83 (2nd)	^[45]
	[Mg₂(μ-Cl)₃][HMDSAlCl₃] (Mg(HMDS)₂+AlCl₃+MgCl₂)	3.2	98%	S/CMK (melt-diffusion)	260@20 (20th)	^[49]
Non-nucleophilic magnesium sulfur battery electrolytes		Oxidative stability/V	Coulombic efficiency	Sulfur cathode	Mg-S battery capacity/(mAh/g)@current rate/(mA/g) (cycle)	Ref.
	[Mg₂(μ-Cl)₂?6THF][AlCl₄]₂	2.6	97%	S@MC (melt-diffusion)	400@67 (100th)	^[74]
	[Mg₂(μ-Cl)₂?4DME][AlCl₄]₂	3.7	100%	CMK/S (melt-diffusion)	360@100 (50th)	^[75]
	[Mg₂(μ-Cl)₃?6THF][TFSI]	3.0	93%	ACC/S (melt-diffusion)	600@100 (100th)	^[77]
Multinuclear electrolyte	[Mg₄Cl₆(DME)₆]?[B(OCH(CF₃)₂)₄]₂	3.3	98%	S/C (melt-diffusion)	1000@160 (100th)	^[78]
Other electrolytes	(PhMgCl)₂+AlCl₃+LiCl	—	—	S@MC (melt-diffusion)	400@167 (200th)	^[79]
Other electrolytes	MgCl₂+YCl₃	3.0	98%	MgS₈@G-CNT	1000@80 (50th)	^[80]

Non-nucleophilic magnesium sulfur battery electrolytes		Oxidative stability/V	Coulombic efficiency	Sulfur cathode	Mg-S battery capacity/(mAh/g)@current rate/(mA/g) (cycle)	Ref.
Mononuclear electrolytes	[Mg(THF)₆][AlCl₄]₂	2.5	100%	S/N-doped graphene (mechanic mixing)	40@17 (20th)	^[53]
	[Mg(THF)₆][AlCl₄]₂+LiCl	3.6	98%	NG-NCNT@NCS@S (melt-diffusion)	300@670 (500th)	^[54]
	[Mg(DG)₂][HMDSAlCl₃]₂	3.5	100%	S/C/Graphene/CNT (mechanic mixing)	400@83 (100th)	^[55]
	MgCl-FTGB	4.8	100%	NG-NCNT@NCS@S (melt-diffusion)	1100@167 (50th)	^[56]
	[Mg(DME)₃][B(hfip)₄]₂)	4.5	100%	ACCS (melt-diffusion)	200@167 (100th)	^[61]
	BCM	3.5	99%	S/C (melt-diffusion)	934@50 (30th)	^[64]
	BMOC	4.2	—	S/C (melt-diffusion)	1133@10 (10th)	^[65]
	Mg(BH₄)₂/THFPB-DGM	2.8	99%	S/C (melt-diffusion)	526@50 (30th)	^[66]
	Mg(TFSI)₂	3.4	96%	CMK-3/S (melt-diffusion)	200@34 (4th)	^[67]
	Mg[BH₄]₂+Li[BH₄]	—	—	SPAN (high-temperature reaction)	800@833 (300th)	^[68]
Binuclear electrolytes	[Mg₂(μ-Cl)₃][HMDSAlCl₃] (HMDSMgCl+AlCl₃)	3.3	100%	S/C (mechanic mixing)	394@83 (2nd)	^[45]
	[Mg₂(μ-Cl)₃][HMDSAlCl₃] (Mg(HMDS)₂+AlCl₃+MgCl₂)	3.2	98%	S/CMK (melt-diffusion)	260@20 (20th)	^[49]
Non-nucleophilic magnesium sulfur battery electrolytes		Oxidative stability/V	Coulombic efficiency	Sulfur cathode	Mg-S battery capacity/(mAh/g)@current rate/(mA/g) (cycle)	Ref.
	[Mg₂(μ-Cl)₂?6THF][AlCl₄]₂	2.6	97%	S@MC (melt-diffusion)	400@67 (100th)	^[74]
	[Mg₂(μ-Cl)₂?4DME][AlCl₄]₂	3.7	100%	CMK/S (melt-diffusion)	360@100 (50th)	^[75]
	[Mg₂(μ-Cl)₃?6THF][TFSI]	3.0	93%	ACC/S (melt-diffusion)	600@100 (100th)	^[77]
Multinuclear electrolyte	[Mg₄Cl₆(DME)₆]?[B(OCH(CF₃)₂)₄]₂	3.3	98%	S/C (melt-diffusion)	1000@160 (100th)	^[78]
Other electrolytes	(PhMgCl)₂+AlCl₃+LiCl	—	—	S@MC (melt-diffusion)	400@167 (200th)	^[79]
Other electrolytes	MgCl₂+YCl₃	3.0	98%	MgS₈@G-CNT	1000@80 (50th)	^[80]

表1. 非亲核镁硫电池电解液性能比较

Table 1. Comparison of non-nucleophilic magnesium sulfur battery electrolytes

表1. 非亲核镁硫电池电解液性能比较

Table 1. Comparison of non-nucleophilic magnesium sulfur battery electrolytes

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非亲核镁硫电池电解液的研究进展

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