锂硫电池电解液功能性添加剂研究进展

doi:10.13208/j.electrochem.2217005

摘要/Abstract

摘要：

由于具有能量密度高、成本低等优点，锂硫电池成为最有前景的下一代电池体系之一。然而，锂硫电池的实际应用仍面临着严峻挑战，如硫和硫化锂的低电导率、多硫化物的穿梭效应和锂枝晶的生长等。通过电解液的优化，可以改善电极|电解质界面，减弱副反应，提高电池性能。其中，电解液中的功能添加剂能有效调节电极界面和电池的氧化还原机制。本文系统性总结了锂硫电池添加剂的最新研究进展，并根据添加剂对锂金属负极的保护作用和对硫正极的稳定作用进行了分类。另外，本文详细讨论了添加剂在硫正极的作用，如抑制多硫化物的溶解和穿梭、充当氧化还原介质、激活硫化锂的沉积与溶解等。最后，本文展望了锂硫电池添加剂的发展前景，希望能对高性能锂硫电池电解液的设计提供借鉴。

关键词: 锂硫电池, 添加剂, 穿梭效应, 多硫化物, 电解液

Abstract:

Lithium-sulfur (Li-S) batteries have become one of the most promising next-generation battery systems due to their high energy density and low cost. However, the application of Li-S batteries still faces critical challenges, such as the low conductivities of S and Li₂S, shuttle effect of polysulfides and dendrite growth of Li, etc. The optimization of the electrolyte can ameliorate the electrolyte|electrode interphase, conveniently regulating the parasitic reaction and improving the performance of the resultant batteries. The functional additives in electrolytes provide chances to tune the interphase and even the redox mechanism to improve the performance of the batteries. In this review, we systematically summarize the latest progresses of additives for Li-S batteries. The additives are classified according to the category that lies on the protection of Li metal anode or the stabilization of S cathode. The functions of additives on the S cathode such as the inhibitions of dissolution and shuttle of the polysulfides, the redox mediators, and the activation of Li₂S deposits are discussed in detail. Finally, the prospects of additives for Li-S batteries are supplied in brief. We hope that the review can provide a guidance in the design of electrolyte for high-performance Li-S batteries.

Key words: Lithium-sulfur batteries, Additives, Shuttle effect, Polysulfides, Electrolyte

张修庆, 唐帅, 付永柱. 锂硫电池电解液功能性添加剂研究进展[J]. 电化学（中英文）, 2023, 29(4): 2217005.

Xiu-Qing Zhang, Shuai Tang, Yong-Zhu Fu. Recent Advances of Functional Electrolyte Additives for Lithium-Sulfur Batteries[J]. Journal of Electrochemistry, 2023, 29(4): 2217005.

图/表 10

Additive	Electrolyte	Initial capacity (mAh·g^-1)/C rate	Sulfur loading (mg·cm^-2)	Final capacity (mAh·g^-1)/cycle number	Ref.
2 wt% ZrO(NO₃)₂	Li-S electrolyte^a	1226/0.5	1.5	398/280	[27]
2 wt% LaNO₃	Li-S electrolyte	1280/0.2	0.9	807/300	[31]
2 wt% LiN₃ (70 ℃)	LiTFSI PEO (EO:Li 20:1)	0.1	1.0	800/30	[33]
7 mg·mL^-1 boron nitride nanosheet (BNNS)	Li-S electrolyte	1223/0.1	1.5	881/200	[34]
0.2 mol·L^-1 triazole (Ta) and tetrazole (Tta)	Li-S electrolyte	(1425)1322/0.2	1	704(780)/200	[36]
40 wt% CS₂	Li-S electrolyte	962/0.5	1	747/300	[40]
4 wt% Alpha-lipoic acid (ALA)	Li-S electrolyte	1005/0.2	1.2	787/200	[41]
8 wt% Poly(sulfur-random-triallylamine) (PST)	Li-S electrolyte	1431/1	1.5	735/1000	[42]
50 mmol·L^-1 biphenyl-4,4′-dithiol (BPD)	1 mol·L^-1 LiTFSI G4/DOL	900/0.1	0.7-1.2	650/100	[44]
80 mmol·L^-1 3,5-bis(trifluoromethyl) thiophenol (BTB)	Li-S electrolyte	950/0.1	4.5	700/82	[45]
0.15 mol·L^-1 1,4-benzenedithiols (1,4-BDT)	Li-S electrolyte	1347/0.5	1	909/500	[46]
0.15 mol·L^-1 1,3,5-benzenetrithiol (BTT)	Li-S electrolyte	1036/1	1	907/300	[47]
0.7 mol·L^-1 benzoselenol (PhSeH)	Li-S electrolyte	1436/0.5	1.1	1300/200	[48]
0.1 mol·L^-1 SiCl₄	1 mol·L^-1 LiPF₆/PC	ca. 1350/1	1	751/200	[55]
5 mmol·L^-1 nitrofullerene (Nitro-C₆₀)	1 mol·L^-1 LiPF₆ in EC:DEC	ca. 2000/0.05	1.5	ca. 630/500	[58]
2 mg 4 mL^-1 graphene quantum dots (GQDs)	Li-S electrolyte	830/0.5	4	498/200	[61]
N, S-codoped carbon dots (N,S-CDs)	Li-S electrolyte	915/0.5	1	600/300	[62]
5 wt% pyrrole	Li-S electrolyte	1649/0.2	1	908/100	[64]
2 wt% triphenylphosphine (TPP)	Li-S electrolyte	994/1	2.1	698/1000	[65]
0.11 mol·L^-1 Bis(4-nitrophenyl) Carbonate (BNC)	Li-S electrolyte	841/1	1.49	778/300	[66]
20 mmol·L^-1 Quinhydrone (QH)	0.5 mol·L^-1 LiOTf and 0.5 mol·L^-1 LiNO₃ in DME/DOL	963/1	1.5	933/300	[67]
0.5 wt% nitrogen-doped carbon dots (N-CD)	Li-S electrolyte	891/0.5	2	589/500	[68]
10 g·L⁻¹ dithiothreitol (DTT)	Li-S electrolyte	808/0.5	1.8-2	471/500	[72]
4% glutamate	Li-S electrolyte	605/2	1.5	363/1000	[74]
Diphenyl diselenide (DPDSe)	Li-S electrolyte	1056/0.5	1.2	720/350	[80]
80 mmol·L^-1 1,5-bis(2-(2-(2- methoxyethoxy)ethoxy)ethoxy) anthra-9,10-quinone	Li-S electrolyte	1300/0.1	0.7 (Li₂S)	850/500	[81]
20 mmol·L^-1 cobaltocene (CoCp₂)	Li-S electrolyte	757/2	1.3	552/100	[91]
100 mmol·L^-1 di-t-butyl disulfide (DtbDS)	Li-S electrolyte	ca. 1000/0.5	1.2	600/300	[87]

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