功能化固态电解质膜改性锂金属负极的研究进展

doi:10.3866/PKU.WHXB202008092

摘要/Abstract

摘要：

对高比能量锂离子电池需求的不断增加激发了锂金属负极的应用研究。锂金属具有高放电比容量(3860 mAh·g^-1)，低电极电位(-3.04 V)，是锂离子电池的理想负极材料。然而，锂金属在循环过程中会形成不稳定的固态电解质(SEI)膜，而且会生成枝晶，枝晶的生长会引发电池短路等安全问题，极大地阻碍了其应用。理想的SEI膜应具有良好的锂离子传导性、表面电子绝缘性和机械强度，可调控锂离子在表面均匀沉积，促进离子传输，抑制枝晶生长，因此构筑功能化SEI膜是解决锂金属负极所面临挑战的一项有效策略。本综述以锂金属枝晶形成和生长的机理为出发点，分析总结SEI膜的构建策略、不同组成SEI膜的结构和功能特性及其对锂金属负极性能的影响，并对锂金属实用化面临的挑战及未来发展方向进行了展望。

关键词: 锂金属负极, 锂枝晶生长, 功能化SEI膜, 锂均匀沉积, 高比能电池

Abstract:

The ever-increasing demand for high-energy Li-ion batteries has acted as a powerful stimulus for the development of Li metal as an anode material. Li metal has long been regarded as a "Holy Grail" in Li-ion batteries due to its high discharge capacity (3860 mAh·g^-1) and low electric potential (-3.04 V). However, the formation of unstable solid electrolyte interphases (SEIs) and Li dendrites, as well as the resultant safety issues initiated by catastrophic dendrite growth, have greatly impeded further application. High ion conductivity, surface electron insulation, and favorable mechanical strength are essential properties for an ideal SEI film, which can allow for uniform Li deposition, providing a fast transfer path for Li ions and suppressing Li dendrite growth. Therefore, designing a functional SEI layer is an effective strategy to solve the problems encountered with Li metal anodes. So far, a variety of inorganic, organic, and inorganic/organic hybird SEI layers have been designed and fabricated. Inorganic SEIs are characterized by mechanical strength and ion conductivity; organic SEIs are flexible and have electron insulation properties. Inorganic/organic composite SEIs show favorable ion conductivity derived from the inorganic components, electron insulation properties originating from the organic components, and mechanical strength benefiting from the reinforcing effect between the inorganic and organic components. Oxides, metal sulfides, lithium nitride (Li₃N) and its derivates, lithium halide (LiX, X = F, Cl), two-dimensional (2D) layered structure materials, lithium phosphate and "Janus" composite are the representative examples of inorganic SEIs. The design principle of various SEI layers is based on the inhibition of Li dendrite formation and growth. Therefore, it is a prerequisite to better understand the relevant intrinsic mechanisms. Despite past investigations, further studies are still required to fully elucidate the related mechanisms by providing more broadly accepted evidence combined with theoretical calculations and offer reliable guidance for the design of multifunctional SEI layers, boosting the performance of Li metal anodes. In this review, on the basis of the mechanisms underlying Li dendrite formation and growth, strategies for constructing various functional SEI films, highlights in structure and property of the films, and their effects on the performance of Li metal anodes are summarized. Moreover, some challenges encountered with the practical applications of Li metal anodes and the future direction for the development of Li metal anodes are addressed. This review can reveal possible strategies for the commercialization of high-energy, safe and stable Li-ion batteries.

Key words: Li metal anode, Li dendrite growth, Functional SEI film, Uniform Li deposition, High-energy battery

钱华明, 李喜飞. 功能化固态电解质膜改性锂金属负极的研究进展[J]. 物理化学学报, 2021, 37(2), 2008092. doi: 10.3866/PKU.WHXB202008092

Huaming Qian, Xifei Li. Progress in Functional Solid Electrolyte Interphases for Boosting Li Metal Anode[J]. Acta Phys. -Chim. Sin. 2021, 37(2), 2008092. doi: 10.3866/PKU.WHXB202008092

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202008092

https://www.whxb.pku.edu.cn/CN/Y2021/V37/I2/2008092

图/表 10

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表1

不同类型、结构及组分的SEI膜在调控锂离子沉积中的作用"

Type of SEI film			Ion conductivity	Mechanical strength	Electron insulation	Highlights	Ref.
Inorganic SEI	Oxides	MgO nanosheet	√	√		Uniform Li ion transfer towards interface	61
		ALD Al₂O₃	√	√		Uniform and dense SEI	4
		ALD ZrO₂	√	√		Uniform and dense SEI	62
						Anti oxidation and hightemperature
		SiO₂	√	√		Chemical stability	63
	Metal sulfide	Li₂S/LiI	√	√		Self-healing ability	64
		Li₂S/Li₂Se	√	√		Superior ion conductivity	65
		MoS₂ sheet	√	√		Uniform Li plating within the sheet structure	66
	Nitrides	Li₃N particles	√	√		3D network Li deposits	67
		g-C₃N₄ nanosheet	√	√		Abundant nucleation sites High modulus	68
		[LiNBH]_n	√	√	√	Li deposition under the SEI layer	69
		Li₃N/Zn/ZnLi_x/Li₂O	√	√		Well interface contact with solid electrolyte	70
Inorganic SEI	Halides	LiF/Cu	√	√		Preferential Li deposition at the grain boundary	73
		CeF₃	√	√		Li deposition along specific crystal facet	74
		LiCl/Ge/GeO_xLi₂CO₃/	√	√		Favorable waterproofness	75
		LiOH/Li₂O
		LiF/F-doped	√	√		Uniform Li plating between	76
		carbon layer				LiF and Li metal
		LiF/graphene	√	√		Stable in air at room temperature	77
		Cu/LiF@Li/	√	√		Uniform Li plating	78
		carbon fiber				Large Li storage space
		Metal chloride perovskite	√	√		Fast lithium ion shuttle under a low energy barrier	79
		2D layered Layered graphene	√	√		In situ covalent binding	80
		structure Ti₃C₂T_x multilayered	√	√		Fast Li ion transfer	81, 82
		structure				Li growth along horizontal direction
		Phosphates Li₃PO₄, Li₂HPO₄	√	√		High modulus	84
						Interfacial compatibility	86
		“Janus” Li_0.33La_0.56TiO₃/Al₂O₃	√	√		Gradient lithiophilicity Uniform	87,
		composites ZnO/Carbon nanotubes				Li plating near the substrate	88
Organic SEI	Covalent Organic Frameworks		√	√		Shortened transport path for Li ion	90
	Cross-linked	Sill Putty		√	√	Dynamic response characteristic	6
	polymer	PDMS/DFB		√	√	3D network Self-healing ability	91
		MSP/Oligomer	√	√	√	Li plating near the matrix	92
						High-density Li deposits
Inorganic/organic	Graphene oxide/LiF/P(SF-DOL)		√	√		In situ dense and uniform film Buffer layer	97
composite SEI	Li₃N/Styrene-butadiene copolymer		√	√		Promising flexibility	98
	Li₃N/LiN_xO_y/PECA		√	√		In situ formed composite film	99
	LiCl/Organic framework composed of Si—O —Si bond		√	√		Even and fast Li plating	100
	Li₆(Si₂O₇)/Polymer containing Si—O—Si bond		√	√		Reduced side reactions with H₂O and O₂	101
	Mesoporous SiO₂/PVDF		√	√		Facilitated Li diffusion Uniform Li deposition	102

表1

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