高电压钴酸锂电池电解液研究进展

doi:10.11949/0438-1157.20240283

摘要/Abstract

摘要：

钴酸锂(LiCoO₂)具有高压实密度、高体积能量密度、优异的导电性能以及使用寿命长等优点，占据消费类电子产品的主要市场。LiCoO₂材料的理论比容量高达274 mAh/g，而其在4.2 V的电压下比容量仅为140 mAh/g。随着消费类电子产品对高能量密度的迫切需求，提高LiCoO₂材料工作电压成为当前研究的热点。材料改性和功能电解液设计是实现高电压LiCoO₂电池的主要途径。相比较而言，功能电解液设计是一种高效且经济的途径，对高能量密度LiCoO₂电池的研发具有重要意义。从高压有机溶剂、高压添加剂以及局部高浓度电解液三个方面入手，综述了近年来国内外高电压LiCoO₂电池电解液的研究进展，重点阐述了电解液溶剂的氧化窗口、电极与电解液界面反应以及锂离子溶剂化结构对高电压LiCoO₂电池性能的影响。最后，对高电压LiCoO₂电池电解液的发展前景作出了总结和展望。

关键词: 电化学, 锂离子电池, 界面, 电解液, 高电压, 钴酸锂

Abstract:

Lithium cobalt oxide (LiCoO₂) has the advantages of high compaction density, high volume energy density, excellent conductivity and long service life, which makes it still occupy the main market of consumer electronic products. The theoretical specific capacity of LiCoO₂material is as high as 274 mAh/g, while its capacity at a voltage of 4.2 V is only 140 mAh/g. As the increasing demand for high ^{energy density of lithium-ion batteries, elevating the operating voltage becomes the direct route to enhancing the energy density of LiCoO₂ batteries. Correspondingly, great attention has been paid to develop high voltage electrolyte with the advantages of high efficient and economical for practical application. Herein, the recent progress of functional electrolyte for high voltage LiCoO₂ batteries has been reviewed elaborately, which could be divided to high voltage organic solvent, high voltage additive and localized high concentration electrolyte. The effect of electrochemical stability window, the film forming ability and the solvation structure of electrolyte on the performance of high voltage LiCoO₂ batteries are discussed systematically. Finally, the further development of high voltage electrolytes for LiCoO₂ cathode is prospected accordingly.}

Key words: electrochemistry, lithium-ion battery, interface, electrolyte, high-voltage, LiCoO₂

中图分类号:

O 646.1

彭丹, 卢俊杰, 倪文静, 杨媛, 汪靖伦. 高电压钴酸锂电池电解液研究进展[J]. 化工学报, 2024, 75(9): 3028-3040.

Dan PENG, Junjie LU, Wenjing NI, Yuan YANG, Jinglun WANG. Research progress of functional electrolyte for high-voltage LiCoO₂ battery[J]. CIESC Journal, 2024, 75(9): 3028-3040.

图/表 14

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电池体系	电解液	电压/V	容量保持率/%	文献
Li/LiCoO₂	1.2 mol/L LiPF₆+0.15 mol/L LiDFOB-FEC∶DMC∶HFE (1∶1∶1，体积比)	2.75~4.50	83.4（200 mA/g，300 cycles）	[24]
Li/Li-Al-F@LiCoO₂	1.0 mol/L LiPF₆-FEC∶DFEC∶DMC (1∶1∶8，体积比)	3.0~4.60	>78.0（0.5 C，500 cycles）	[25]
MCMB/LiCoO₂	1.0 mol/L LiPF₆-FEC∶FEMC∶TTE (3∶6∶1，质量比)	3.0~4.45	76.0（0.5 C，100 cycles）	[26]
Li/LiCoO₂	1 mol/L LiPF₆-MTFP	2.8~4.50	97.0（25 mA/g，50 cycles）	[27]
graphite/LiCoO₂	1.0 mol/L LiPF₆-FEC∶F5EON (1∶3，体积比)	2.8~4.50	77.4（0.3 C，200 cycles）	[28]
Li/LiCoO₂	3.0 mol/L LiFSI-FMS	3.0~4.60	92.5（0.2 C，100 cycles）	[29]
	2.2 mol/L LiFSI-FMS	3.0~4.50	95.0（0.2/0.5 C，400 cycles）	[30]
	1.5 mol/L LiFSI-TFTMS	2.8~4.60	90.0（0.2/0.5 C，320 cycles）	[31]

电池体系	电解液	电压/V	容量保持率/%	文献
Li/LiCoO₂	1.2 mol/L LiPF₆+0.15 mol/L LiDFOB-FEC∶DMC∶HFE (1∶1∶1，体积比)	2.75~4.50	83.4（200 mA/g，300 cycles）	[24]
Li/Li-Al-F@LiCoO₂	1.0 mol/L LiPF₆-FEC∶DFEC∶DMC (1∶1∶8，体积比)	3.0~4.60	>78.0（0.5 C，500 cycles）	[25]
MCMB/LiCoO₂	1.0 mol/L LiPF₆-FEC∶FEMC∶TTE (3∶6∶1，质量比)	3.0~4.45	76.0（0.5 C，100 cycles）	[26]
Li/LiCoO₂	1 mol/L LiPF₆-MTFP	2.8~4.50	97.0（25 mA/g，50 cycles）	[27]
graphite/LiCoO₂	1.0 mol/L LiPF₆-FEC∶F5EON (1∶3，体积比)	2.8~4.50	77.4（0.3 C，200 cycles）	[28]
Li/LiCoO₂	3.0 mol/L LiFSI-FMS	3.0~4.60	92.5（0.2 C，100 cycles）	[29]
	2.2 mol/L LiFSI-FMS	3.0~4.50	95.0（0.2/0.5 C，400 cycles）	[30]
	1.5 mol/L LiFSI-TFTMS	2.8~4.60	90.0（0.2/0.5 C，320 cycles）	[31]

电池体系	电解液	电压/V	容量保持率/%	文献
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶PC∶DEC∶PP (1∶1∶1，质量比)+5.0%(质量分数) FEC+ 2.0%(质量分数) HTCN	3.0~4.50	90.0（1.0 C，800 cycles）	[38]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)10%FEC+ 1.0%(质量分数) SUN/HTCN	3.0~4.60	72.0 （1.0 C，300 cycles） 75.0（1.0 C，300 cycles）	[39]
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶DEC (1∶1，体积比)+0.1%(质量分数) TTEP	3.0~4.40	90.72（1.0 C，130 cycles）	[40]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶DEC (3∶7，质量比)+0.2%(质量分数) TPPSe	3.0~4.65	74.1（1.0 C，500 cycles）	[41]
graphite/LiCoO₂	1.15 mol/L LiPF₆-EC∶PC∶DEC∶PP (1∶1∶1，质量比)+5.0%(质量分数) FEC+3.0%(质量分数) ADN+0.5%(质量分数) DMTMSP	3.0~4.45	90.5（1.0 C，400 cycles）	[42]
Li/LiCoO₂	1.0 mol/L LiPF₆-PC∶EC∶EMC (5∶25∶70，体积比)+2.0%(质量分数) TTFPB	3.0~4.70	74.0（0.5 C，150 cycles）	[43]
	1.0 mol/L LiPF₆-EC∶DEC (3∶7，质量比)+0.5%(质量分数) TPCB	3.0~4.60	82.2（1.0 C，200 cycles）	[44]
	1.0 mol/L LiPF₆-EC∶DEC (3∶7，质量比)+0.1%(质量分数) TFPB	3.0~4.60	84.6（1.0 C，200 cycles）	[45]
	1.0 mol/L LiPF₆-EC∶EMC∶DEC (1∶1∶1，体积比)+2.0%(质量分数) TCEB	2.75~4.50	78.2（1.0 C，200 cycles）	[46]
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC∶DEC (3∶5∶2，质量比)+1.0%(质量分数) LiDFOB	3.0~4.50	80.2（1.0 C，300 cycles）	[47]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶DMC∶DEC (1∶1∶1，体积比)+1.0%(质量分数) BBSI	3.0~4.60	81.3（0.5 C，300 cycles）	[48]
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) HBAG	3.0~4.40	94.88（1.0 C，160 cycles）	[49]
	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) MDFA	3.0~4.45	93.1（1.0 C，100 cycles）	[50]
	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) PTSI	3.0~4.40	95.3（0.5 C，200 cycles）	[51]
	1.0 mol/L LiPF₆-EC∶DMC∶EMC (1∶1∶1，质量比)+0.5%(质量分数) DMSE	3.0~4.50	66.5（0.2 C，100 cycles）	[52]
	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) TFBS	3.0~4.50	96.8（0.5 C，100 cycles）	[53]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶DEC (3∶7，质量比)+0.03%(质量分数) MMD	3.0~4.60	83.5（1.0 C，200 cycles）	[54]
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC (3∶7，体积比)+2.0%(质量分数) NPA	3.0~4.60	77.1（0.3 C，200 cycles）	[55]
graphite/LiCoO₂	1.3 mol/L LiPF₆-EC/PC/EB (10∶15∶75，体积比)+7% FEC+ 1% LiFMDFB+3% HTCN+0.2% TMSP	3.0~4.55	51.8（1.5 C charge/ 0.5 C discharge，500 cycles）	[56]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) DMMA	3.0~4.65	70.7（1.0 C，500 cycles）	[57]

电池体系	电解液	电压/V	容量保持率/%	文献
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶PC∶DEC∶PP (1∶1∶1，质量比)+5.0%(质量分数) FEC+ 2.0%(质量分数) HTCN	3.0~4.50	90.0（1.0 C，800 cycles）	[38]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)10%FEC+ 1.0%(质量分数) SUN/HTCN	3.0~4.60	72.0 （1.0 C，300 cycles） 75.0（1.0 C，300 cycles）	[39]
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶DEC (1∶1，体积比)+0.1%(质量分数) TTEP	3.0~4.40	90.72（1.0 C，130 cycles）	[40]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶DEC (3∶7，质量比)+0.2%(质量分数) TPPSe	3.0~4.65	74.1（1.0 C，500 cycles）	[41]
graphite/LiCoO₂	1.15 mol/L LiPF₆-EC∶PC∶DEC∶PP (1∶1∶1，质量比)+5.0%(质量分数) FEC+3.0%(质量分数) ADN+0.5%(质量分数) DMTMSP	3.0~4.45	90.5（1.0 C，400 cycles）	[42]
Li/LiCoO₂	1.0 mol/L LiPF₆-PC∶EC∶EMC (5∶25∶70，体积比)+2.0%(质量分数) TTFPB	3.0~4.70	74.0（0.5 C，150 cycles）	[43]
	1.0 mol/L LiPF₆-EC∶DEC (3∶7，质量比)+0.5%(质量分数) TPCB	3.0~4.60	82.2（1.0 C，200 cycles）	[44]
	1.0 mol/L LiPF₆-EC∶DEC (3∶7，质量比)+0.1%(质量分数) TFPB	3.0~4.60	84.6（1.0 C，200 cycles）	[45]
	1.0 mol/L LiPF₆-EC∶EMC∶DEC (1∶1∶1，体积比)+2.0%(质量分数) TCEB	2.75~4.50	78.2（1.0 C，200 cycles）	[46]
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC∶DEC (3∶5∶2，质量比)+1.0%(质量分数) LiDFOB	3.0~4.50	80.2（1.0 C，300 cycles）	[47]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶DMC∶DEC (1∶1∶1，体积比)+1.0%(质量分数) BBSI	3.0~4.60	81.3（0.5 C，300 cycles）	[48]
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) HBAG	3.0~4.40	94.88（1.0 C，160 cycles）	[49]
	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) MDFA	3.0~4.45	93.1（1.0 C，100 cycles）	[50]
	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) PTSI	3.0~4.40	95.3（0.5 C，200 cycles）	[51]
	1.0 mol/L LiPF₆-EC∶DMC∶EMC (1∶1∶1，质量比)+0.5%(质量分数) DMSE	3.0~4.50	66.5（0.2 C，100 cycles）	[52]
	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) TFBS	3.0~4.50	96.8（0.5 C，100 cycles）	[53]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶DEC (3∶7，质量比)+0.03%(质量分数) MMD	3.0~4.60	83.5（1.0 C，200 cycles）	[54]
graphite/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC (3∶7，体积比)+2.0%(质量分数) NPA	3.0~4.60	77.1（0.3 C，200 cycles）	[55]
graphite/LiCoO₂	1.3 mol/L LiPF₆-EC/PC/EB (10∶15∶75，体积比)+7% FEC+ 1% LiFMDFB+3% HTCN+0.2% TMSP	3.0~4.55	51.8（1.5 C charge/ 0.5 C discharge，500 cycles）	[56]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC (3∶7，质量比)+1.0%(质量分数) DMMA	3.0~4.65	70.7（1.0 C，500 cycles）	[57]

电池体系	电解液	容量保持率/%	文献
3.0～4.50 V Li/LiCoO₂	[5 mol/L LiTFSI-MP-FEC (9∶1，体积比)]∶TTE(2∶1，质量比)	87.7（1.0 C，300 cycles）	[67]
	1.4 mol/L LiFSI-DME-TTME (1∶4，体积比)	90.0（0.2 C charge/0.5 C discharge，170 cycles）	[68]
	1.9 mol/L LiFSI-DME-HM (2∶1，体积比)	80.0（0.2 C charge/0.5 C discharge，505 cycles）	[69]
	LiFSI∶DME∶FB∶3FB (1∶1.2∶2.8∶0.2，摩尔比)	80.0（2.0 C，600 cycles）	[70]
	2.0 mol/L LiDFOB-DME∶DFEC (1∶1，体积比)	82.32（0.3 C，1000 cycles）	[71]
	1.4 mol/L LiFSI-DME∶HFC (1∶3，摩尔比)	88.0（0.2 C charge/0.5 C discharge，200 cycles）	[72]