高电压/宽温域水系碱金属离子电池的研究进展

doi:10.3866/PKU.WHXB202211005

物理化学学报 >> 2023, Vol. 39 >> Issue (5): 2211005.doi: 10.3866/PKU.WHXB202211005

高电压/宽温域水系碱金属离子电池的研究进展

陈晨阳¹, 赵永智¹, 李园园²^,*(), 刘金平¹^,*()

¹ 武汉理工大学化学化工与生命科学学院, 材料复合新技术国家重点实验室, 武汉 430070
² 华中科技大学光学与电子信息学院, 武汉 430074

收稿日期:2022-11-03 录用日期:2022-12-12 发布日期:2022-12-19
通讯作者: 李园园,刘金平 E-mail:liyynano@hust.edu.cn;liujp@whut.edu.cn
基金资助:
国家自然科学基金(51972257);国家自然科学基金(52172229);国家自然科学基金(52072136);中央高校基本科研业务费专项资金(2022IVA197);材料复合新技术国家重点实验室(武汉理工大学)开放基金(2022-KF-20)

Research Progress of High-Voltage/Wide-Temperature-Range Aqueous Alkali Metal-Ion Batteries

Chenyang Chen¹, Yongzhi Zhao¹, Yuanyuan Li²^,*(), Jinping Liu¹^,*()

¹ School of Chemistry, Chemical Engineering and Life Science, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
² School of Optical and Electronic Information, Huazhong University of Science and Technology, Wuhan 430074, China

Received:2022-11-03 Accepted:2022-12-12 Published:2022-12-19
Contact: Yuanyuan Li, Jinping Liu E-mail:liyynano@hust.edu.cn;liujp@whut.edu.cn
Supported by:
the National Natural Science Foundation of China(51972257);the National Natural Science Foundation of China(52172229);the National Natural Science Foundation of China(52072136);the Fundamental Research Funds for the Central Universities(2022IVA197);the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology)(2022-KF-20)

摘要/Abstract

摘要：

水系储能器件具有固有的高安全性、环境友好性和成本低的优势，在未来智能电网、便携式/可穿戴电子产品等领域显示出巨大的应用潜力。然而水的热力学分解电压低、冰点高，导致水系电解液电化学稳定电压窗口窄以及凝固点高，极大地限制了水系储能器件的能量密度与宽温域应用。因此，设计耐高电压、抗冻的水系电解液，成为水系储能器件大规模、多场景应用的关键。本文系统综述了高电压/宽温域水系碱金属离子电池电解液设计的研究进展，从热力学和动力学角度出发，分别重点介绍提高电解液电压窗口和工作温度范围的各类策略以及相关作用机制。进一步提出宽温域、高压水系电解液的潜在设计思路，并对高性能水系碱金属离子电池的发展方向进行展望。

关键词: 碱金属离子电池, 水系电解液, 电解液调控, 高电压, 宽温域

Abstract:

Aqueous electrochemical energy storage (EES) devices have inherent advantages, such as high safety, environmental-friendliness, and low cost, exhibiting significant potential for application in future smart grids, portable/wearable electronics, and other fields. However, the low thermodynamic decomposition voltage of water (1.23 V) results in a narrow electrochemical stability window (ESW) of the aqueous electrolyte, limiting the selection of electrode materials. Therefore, aqueous alkali metal-ion batteries (AABs) have a low operating voltage and energy density. Considering the diverse application of AABs, the operation of AABs under extreme temperature conditions faces critical challenges. At a low temperature, the electrolyte freezes easily owing to the high freezing point of water (0 ℃); the ionic conductivity of the electrolyte decreases significantly, and the charge/discharge polarization increases. Therefore, AABs generally have a low capacity, poor rate performance, and low energy/power densities, and are unable to operate normally. At a high temperature, the water activity improves, and the side reaction of water decomposition intensifies. Hence, the cycle performance of AABs deteriorates, and the battery exhibits safety issues, such as expansion and thermal runaway. In recent years, significant research has been conducted to overcome the shortcomings of the aqueous EES, inspiring further research and development of future high-performance aqueous EESs. Reducing the water activity and increasing the hydrogen evolution reaction (HER) or oxygen evolution reaction (OER) overpotential are effective strategies to widen the ESW of aqueous electrolytes, which are mostly realized by utilizing high concentration salts, additives, and co-solvents. Using salt additives or organic co-solvents to break the intermolecular hydrogen bonds of water and reduce the interfacial charge transfer resistance are effective strategies to improve the low-temperature performance of AABs. Additionally, salt additives/co-solvents with high thermal stability can form strong hydrogen bonds with water, effectively improving the water retention and reducing the water activity, which ensure the enhanced electrochemical performance of the AABs at high temperatures. This review systematically summarizes the research progress of electrolyte design for AABs with a high voltage/wide operating temperature range. From the perspective of thermodynamics and kinetics, various strategies to widen the ESW and operating temperature range of the electrolyte as well as the relevant mechanisms are introduced. Potential concepts for designing high-voltage aqueous electrolytes with operation ability at a wide temperature range are proposed, and the development direction of high-performance AABs is presented.

Key words: Alkali metal-ion battery, Aqueous electrolyte, Electrolyte regulation, High-voltage, Wide-temperature-range

陈晨阳, 赵永智, 李园园, 刘金平. 高电压/宽温域水系碱金属离子电池的研究进展[J]. 物理化学学报, 2023, 39(5), 2211005. doi: 10.3866/PKU.WHXB202211005

Chenyang Chen, Yongzhi Zhao, Yuanyuan Li, Jinping Liu. Research Progress of High-Voltage/Wide-Temperature-Range Aqueous Alkali Metal-Ion Batteries[J]. Acta Phys. -Chim. Sin. 2023, 39(5), 2211005. doi: 10.3866/PKU.WHXB202211005

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202211005

https://www.whxb.pku.edu.cn/CN/Y2023/V39/I5/2211005

图/表 14

图1

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图7

表1

电解液设计实现的高电压AABs"

Strategy		Electrolyte	ESW (V vs. Li/Na/K)	Ionic conductivity (mS∙cm⁻¹)@.(℃)	Cathode//Anode	Output voltage (V)	Energy density* (Wh∙kg⁻¹)	Ref.
Highly Concentrated Salt	Li⁺	21 m LiTFSI	3.0 (1.9–4.9)	8.21@25	LiMn₂O₄//Mo₆S₈	2.0	84	18
		21 m LiTFSI + 7 m LiOTf	3.1 (1.8–4.9)	6.5@25	LiMn₂O₄//TiO₂	2.1	100	28
		19.4 m LiTFSI + 8.3 m LiBETI	3.8 (1.2–5.0)	3.0@30	LiCoO₂//Li₄Ti₅O₁₂	2.35	–	29
		22.2 m LiTFSI + 33.3 m LiPTFSI	2.7 (2.3–5.0)	0.1@25	LiCoO₂//Li₄Ti₅O₁₂	2.4	–	30
		40.4 m KOAc + 9.8 m LiOAc	2.85 (1.55–4.4)	25.2@25	LiMn₂O₄//AC	2.0	77.9	31
		42 m LiTFSI + 21 m Me3EtN·TFSI	3.25 (1.75–5.0）	0.91@25	LiMn₂O₄//Li₄Ti₅O₁₂	2.55	145	32
		50 m LiTFSI + 25 m TMBTFSI	3.25	–	LiMn₂O₄//TiO₂(B)	2.35	150	33
	Na⁺	17 m NaClO₄	2.8 (1.7–4.4)	108@25	Na₄Fe₃(PO₄)₂(P₂O₇)// NaTi₂(PO₄)₃	–	36	34
		17 m NaClO₄ + 2 m NaOTF	2.8 (1.6–4.4)	95.25@25	Na₃V₂(PO₄)₃// Na₃V₂(PO₄)₃	1.75	70	35
		32 m KOAc + 8 m NaOAc	2.4 (0.7–3.1)	12@25	Na₂VTi(PO₄)₃// Na₂VTi(PO₄)₃	1.13	–	60
		9 m NaOTF + 22 m TEAOTF	3.3 (0.8–4.1)	11.2@25	Na_1.88Mn[Fe(CN)₆]_0.97∙1.35H₂O//NaTiOPO₄	–	–	61
		Na(PTFSI)_0.65(TFSI)_0.14 (OTf)_0.21∙3H₂O	2.7 (1.9–4.6)	14@25	Na₃V₂(PO₄)₂F₃// NaTi₂(PO₄)₃	1.75	77.9	62
		35 m NaFSI	2.6 (1.8–4.4)	8@25	Na₃(VOPO₄)₂F// NaTi₂(PO₄)₃	–	–	63
	K⁺	30 m KFSI	3.97 (1.14–5.11)	–	K_1.85Fe_0.33Mn_0.67 [Fe(CN)₆]_0.98∙ 0.77H₂O//β-PTCDA			36
		K(PTFSI)_0.12(TFSI)_0.08 (OTf)_0.8∙2H₂O	2.5 (2.1–4.6)	34.6@25	–	–	–	62
		61.7 m K(FSI)_0.55(OTf)_0.45∙ 0.9H₂O	2.7 (2.1–4.8)	12@25	KVPO₄F// NaTi₂(PO₄)₃	3.0	–	64
		37 m KFSI	2.8 (1.6–4.4)	23.12@25	AC//AC	2.3	20.5	65
Additive	Li⁺	Urea-LiClO₄	3.6 (1.2–4.8)	–	LiMn₂O₄//Li₄Ti₅O₁₂	2.3	140	27
		0.1wt% TMSB- 21 m LiTFSI	3.0	–	LiCoO₂/Mo₆S₈	2.5	120	38
		HFE gel-21 m LiTFSI + 7 m LiOTf	4.9 (0–4.9)	–	LiVPO₄F//Graphite	4.0	~400	40
		5% PAM-21 m LiTFSI	3.1 (1.8–4.9)	6.5@30	LiMn₂O₄//L-TiO₂	–	–	41
		5% AM-21 m LiTFSI	3.1 (1.8–4.9)	9.6@25	LiMn₂O₄//L-TiO₂	–	–	42
		Urea-LiTFSI	3.3 (1.5–4.8)	1@25	LiMn₂O₄//Li₄Ti₅O₁₂	2.5	-	44
		CO₂-5 m LiTFSI	3.08 (1.67–4.75)	54.6@25	LiMn₂O₄/Mo₆S₈	–	–	46
		Urea-LiClO₄	3.2	26@25	LiMn₂O₄//Li₄Ti₅O₁₂	2.2	135	66
Co-solvent	Li⁺	DMC-LiTFSI	4.1 (1.0–5.1)	5.0@25	LiNi_0.5Mn_1.5O₄// Li₄Ti₅O₁₂	3.2	165	47
		AN-LiTFSI	4.5 (0.7–5.2)	3.27@30	LiMn₂O₄//Li₄Ti₅O₁₂	2.55	109	48
		TEGDME-LiTFSI	4.2 (0.6–4.8)	0.625@25	LiMn₂O₄//Li₄Ti₅O₁₂	2.5	120	49
		PEG(400)-LiTFSI	3.2 (1.3–4.5)	0.8@25	LiMn₂O₄//Li₄Ti₅O₁₂	2.5	75–100	51
		PEGDME(450)-LiTFSI	3.2 (1.3–4.5)	2.4@25	LiMn₂O₄//Li₄Ti₅O₁₂	2.5	–	52
		PD-LiNO₃	2.9 (2.2–5.2)	22.8@25	LiMn₂O₄//Mo₆S₈	–	–	54
		MSM-LiClO₄	3.5 (1.6–5.1)	3.71@25	LiMn₂O₄//Li₄Ti₅O₁₂	2.6	–	56
		Sulfolane-LiTFSI	3.4 (1.3–4.7)	2.5@25	LiMn₂O₄//Li₄Ti₅O₁₂	2.5	141	57
		TMS-LiTFSI	5.4 (0.3–5.7)	0.41@25	LiNi_0.5Mn_1.5O₄// Li₄Ti₅O₁₂	3.15	136	58
		MU-LiTFSI	4.5 (0.5 – 5.0)	3.2@25	LiMn₂O₄//Li₄Ti₅O₁₂	–	–	59
		DOL-LiTFSI	4.7 (0.3 – 5.0)	7.09@60	LiMn₂O₄//Li₄Ti₅O₁₂	–	–	67
		SL-LiClO₄	3.8 (1.1–4.9)	3.74@25	LiMn₂O₄//Li₄Ti₅O₁₂	2.45	71	68
	Na⁺	Urea-DMF-NaClO₄	2.8 (1.1–3.9)	8.1@20	NiHCF//NaTi₂(PO₄)₃	–	–	43
		Sugar-NaNO₃	2.812	8.536@25	–	–	–	53
		TMP-NaClO₄	3.0 (1.2–4.2)	23@25	–	–	–	55
		DMSO-NaClO₄	3.1 (1.0–4.1)	–	Na₃V₂(PO₄)₃// Na₃V₂(PO₄)₃	1.7	–	69

表1

图8

图9

图10

图11

表2

图12

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Strategy		Electrolyte	Freezing point (℃)	Ionic conductivity (mS∙cm⁻¹)@.(℃)	Cathode//Anode	Capacity retention (%)@.(℃)	Ref.
Highly Concentrated Salt	Li⁺	40.4 m KOAc + 9.8 m LiOAc	~ −30	1.2@−30	LiMn₂O₄//AC	60@−20	31
		5.2 m LiTFSI	< −40	1.8@−40	LiCoO₂//Li₄Ti₅O₁₂	66.49@−40	67
		Saturated LiCl	~ −50	-	LiCoO₂ (Three-electrode system)	72@−40	77
		21 m LiTFSI		-	LiMn₂O₄//TiO₂	79@0	78
		LiCl-P(SBMA-co-HEA) Gel	-	12.6@−40	AC//AC	78@−30	93
		Li₂SO₄-EMIMBF₄- PVA/Agar Gel	-	-	AC//AC	90@−30	96
		LiCl/KCl-CG/PAM Gel	-	19@−40	AC//AC	78.9@−40	97
		LiTFSI-ARS-PAM Gel	-	4@−15	MnO₂//MnO₂	72.5@−15	98
		NaCl-Li₂SO₄- CS-P(AM-co-AA) Gel	< −41	36@−20	Ti₃C₂T_x MXene//CNTs	50.5@−20	99
	Na⁺	2 m NaClO₄	< −20	3.49	Ni(OH)₂//NaTi₂(PO₄)₃	85@−20	68
	Na⁺	CaCl₂-NaClO₄	< −100	7.13@−50	Na₂CoFe(CN)₆//AC	64.8@−30	69
	K⁺	22 mol∙L⁻¹ KCF₃SO₃	-	10@−20	K_1.85Fe_0.33Mn_0.67[Fe(CN)₆]_0.98 ·0.77H₂O//PTCDI	76.3@−20	70
Co-solvent	Li⁺	AN-LiTFSI	< −60	0.63@−60	LiMn₂O₄//Li₄Ti₅O₁₂	95@0	48
		TMS-LiTFSI	< −85	1.03 × 10⁻⁴ @−80	LiNi_0.5Mn_1.5O₄//Li₄Ti₅O₁₂	86.1@−20	58
		DOL-LiTFSI	< −95	–	LiMn₂O₄//Li₄Ti₅O₁₂	52@−50	67
		SL-LiClO₄	~ −110	0.05@−50	LiMn₂O₄//Li₄Ti₅O₁₂	98@−20	68
		EG-LiCl- P(AMPS-co-AM) Gel	-	1.9@−20	AC//AC	71@−20	84
		EG-Li₂SO₄	~ −24.6	4.25@−20	LiFePO₄ (Three-electrode system)	82@−20	86
		Gly-LiClO₄-HPC/PVA Gel	-	5.7@−40	AC//AC	73.75@−40	95
		EG-LiCl-PVA Gel	< −62.8	0.83@−40	AC//AC	68.3@−30	100
		EG-LiTFSI-PAM Gel	< −100	1.5@−40	PANI//PANI	70.4@−40	101
	Na⁺	TMP-NaClO₄	–	-	aMEGO//aMEGO	67.9@−20	55
		DMSO-NaClO₄	< −130	0.11@−50	AC//NaTi₂(PO₄)₃	60@−50	69
		AN-NaClO₄	-	4.95@−50	AC//AC	86.5@−50	89
		MeOH-Na₂SO₄-SiO₂ Gel	-	0.07@−30	AC//NaTi₂(PO₄)₃	65.05@−30	102

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高电压/宽温域水系碱金属离子电池的研究进展

Research Progress of High-Voltage/Wide-Temperature-Range Aqueous Alkali Metal-Ion Batteries

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