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化学进展 2022, Vol. 34 Issue (11): 2517-2539 DOI: 10.7536/PC220340 前一篇   后一篇

• 综述 •

锂硒电池研究进展

黄祺1, 邢震宇1,2,*()   

  1. 1 华南师范大学化学学院 广州 510006
    2 环境理论化学教育部重点实验室 广州 510006
  • 收稿日期:2022-03-30 修回日期:2022-05-23 出版日期:2022-11-24 发布日期:2022-07-20
  • 通讯作者: 邢震宇
  • 作者简介:

    邢震宇 2012年吉林大学取得化学学士学位, 2016年美国Oregon State University取得化学博士学位, 之后在加拿大University of Waterloo从事博士后研究, 自2018年被引进华南师范大学工作. 主要研究方向集中于基于金属热反应的材料制备以及其在能源存储领域的应用, 尤其在碳材料和硫化锂材料的制备方面取得了系统性的研究进展。

  • 基金资助:
    国家自然科学基金青年基金项目(22002045); 广东省基础与应用基础研究基金自然科学基金项目(2020A1515011549); 广州市基础与应用基础研究项目(202102020396)
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Advances in Lithium Selenium Batteries

Qi Huang1, Zhenyu Xing1,2()   

  1. 1 School of Chemistry, South China Normal University,Guangzhou 510006, China
    2 Key Laboratory of Theoretical Chemistry of Environment, Ministry of Education,Guangzhou 510006, China
  • Received:2022-03-30 Revised:2022-05-23 Online:2022-11-24 Published:2022-07-20
  • Contact: Zhenyu Xing
  • Supported by:
    National Natural Science Foundation of China(22002045); Guangdong Basic and Applied Basic Research Foundation(2020A1515011549); Basic Research and Applicable Basic Research in Guangzhou City(202102020396)

锂硒电池因其高能量密度、高体积比容量和适中的输出电压等优点而成为备受关注的二次电池。然而,由于穿梭效应、较差的导电性、低活性物质利用率以及较快的容量衰减等问题,锂硒电池的实际应用受到了极大的阻碍。近些年,研究人员深入研究了锂硒电池的充放电机理,同时也探索了各种碳材料、金属化合物等新材料作为正极载体、中间层和电解液添加剂对于电化学性能的影响。本文系统地总结了锂硒电池的电极材料、中间层和添加剂等的研究进展,并且重点介绍了在充放电机理和系统优化方面的进步,以期为锂硒电池的进一步发展提供新的思路。

关键词： 锂硒电池, 穿梭效应, 电极材料, 电解液, 中间层

Lithium-selenium batteries have attracted much attention as secondary batteries due to their high energy density, high specific volumetric capacity, and moderate output voltage. However, the practical application of Li-Se batteries is hindered by the shuttle effect, poor conductivity, low active material utilization and fast capacity fading. In recent years, researchers investigated the charge-discharge mechanism of Li-Se batteries thoroughly, and studied effects on electrochemical performance from various new materials, including carbon materials and metal compounds, as cathode host, interlayer and electrolyte additives at the same time. This review systematically summarized the research progress of electrode materials, interlayer and electrolyte additives, with focus on charge-discharge mechanism and system optimization. We hope this review could provide perspective for the further development of Li-Se batteries.

Key words: lithium selenium battery, shuttle effect, electrode materials, electrolyte, interlayer
()
图1 (a)硒、硫、钴酸锂、磷酸铁锂和三元材料正极理论容量; (b)锂硒电池近几年发表论文数量; (c)高性能锂硒电池结构组成
Fig. 1 (a) Theoretical capacity of Se, S, LiCoO2, LiFePO4, Ternary material cathodes; (b) the number of publications on lithium-selenium batteries in recent years; (c) schematic of the structure composition for advanced Li-Se batteries
图2 (a) 锂硒电池首圈充放电过程; (b) c/a-Se的初始充放电曲线[43]; (c) Li/SeS2-C电池的循环性能[44]; (d) Li-SeS2电池在醚类电解液中的循环曲线[45]; (e) 采用PVDF黏结剂的Li/SeS2电池在醚类电解质中的循环伏安曲线[45]; (f) Li+在Sex狭缝孔隙中运输的剖面图和主视图[51]; (g) 硒分子直接生成Li2Se过程中每个电子释放的能量[51]; (h) 界面锂化机理示意图[53]; (i) EC-EMC电解液、不溶性Se、Li2Se、Se与Li2Se两者混合的图片[22]
Fig. 2 (a) Initial charge-discharge process of lithium-selenium battery. (b) Initial charge-discharge curves of the c/a-Se[43]. (c) Cycling performance of Li/SeS2-C systems[44]. (d) Cycle performance of Li cells with SeS2-carbon composite as cathodes in ether-based electrolyte[45]. (e) Cyclic voltammetry curves of Li/SeS2 batteries in ether-based electrolyte with PVDF binder[45]; (f) Sectional view and front view showing the Li+ migration in a Sex preoccupied slit pore[51]. (g) Energy released by each electron in the direct formation of Li2Se from selenium molecules[51]. (h) Schematic illustration of the interfacial lithiation mechanism[53]. (i) Photograph of electrolyte solvent EC-EMC alone, with insoluble Se, with Li2Se, and with a combination of the two[22]
图3 锂硒电池现存问题
Fig. 3 Existing problems in lithium-selenium batteries
图4 (a)新型盐烘法制备Se/MnMC-B示意图[115]; (b) Se粉、CMK-3、Se/CMK-3的XRD图谱[122]; (c) Se粉、CMK-3、Se/CMK-3的拉曼光谱[122]; (d) Se@PCNFs的电压曲线[123]; (e) TEM HAADF图像及Se@HHCS中C、Se、O元素的EDXS图像[124]; (f~h) Se纳米线、Se/PANI、G@Se/PANI的TEM图像[41]
Fig. 4 (a) Illustration of the strategy behind the baked-in-salt approach for confining selenium[115]; (b) XRD patterns and (c) Raman spectra of the CMK-3, Se/CMK-3 composite and Se powder[122]; (d) Voltage profiles of Se@PCNFs[123]; (e) TEM HAADF image and associated EDXS maps of C, Se and O, respectively for Se@HHCS[124]; (f-h) TEM images of Se nanowires, Se/PANI and G@Se/PANI[41]
图5 (a) Se@KF65复合材料的制备示意图[138]; (b)双层空心Se@CNx纳米带的TGA曲线[139]; (c, d) Se、Se-treated、HDHPC和Se50/HDHPC复合材料的XRD图谱和拉曼光谱[140]; (e, f) Se50/SO-HPC3复合材料的SEM和TEM图像[141]; (g) HPCNBs电极在电流密度为500mA/g下的循环性能[142]
Fig. 5 (a) Schematic illustration for the preparation of Se@KF65 composite[138]. (b) TGA curve of hollow double-shell Se@CNx nanobelts[139]. (c) XRD patterns and (d) Raman spectra of pristine Se, Se-treated, HDHPC, and Se50/HDHPC composites[140]; (e) SEM and (f) TEM images of the synthesized Se50/SO-HPC3 composite[141]. (g) Cycling performance at a current density of 500mAh/g of the HPCNBs electrode[142]
图6 两种新型一维纳米结构的形成机理[151]
Fig. 6 Formation mechanism of two novel one-dimensional nanostructures[151]
图7 (a) Se和Se-TiO2/NFF电极在1.0~3.0 V电压范围内0.5 C下的首圈充/放电曲线[164]; (b) Se-TiO2/NFF和Se在不同电流密度下的倍率特性[164]
Fig. 7 (a) First discharge/charge curves of Se and Se-TiO2/NFF electrodes at 0.5 C in a voltage range of 1.0-3.0 V[164]. (b) Rate properties of Se-TiO2/NFF and Se at various current rates
图8 (a) CoS2@LRC/SeS2相对于LRC/SeS2的优势[180]; (b) NiCo2S4@NC-SeS2正极的嵌锂过程[181]
Fig. 8 (a) Proposed advantages of CoS2@LRC/SeS2 over LRC/SeS2[180]; (b) lithiation of NiCo2S4@NC-SeS2 cathode[181]
图9 (a) 带正电的屏蔽层将排斥进入的Li+,迫使Li+进一步沉积到负极的邻近区域,直到形成光滑的沉积层[190];在电流密度为0.1 mA/cm2时,在CsPF6浓度为 (b) 0 和 (c) 0.01 mol·L-1的1 mol·L-1 LiPF6/PC电解液中沉积的锂膜SEM图像[190]; 锂金属在(d)平面集流体和(e)三维集流体上的电化学沉积过程[192]; (f) 层状Li/还原氧化石墨烯复合电极合成过程[193]
Fig. 9 (a) The positively charged shield will repel Li+ incoming from the protrusion forcing further Li+ deposition to adjacent regions of the anode until a smooth deposition layer is formed[190]; SEM images of the morphologies of Li films deposited in electrolyte of 1 mol·L-1 LiPF6/PC with CsPF6 concentrations of (b) 0 mol·L-1 and (c) 0.01 mol·L-1, at a current density of 0.1 mA/cm2[190]; the electrochemical deposition processes of Li metal on (d) planar current collector and (e) 3D current collector[192]; (f) the synthesis process of Li/RGO composite electrode[193]
图10 (a,b) TPB-DMTP-COF双功能分离涂层材料分子结构及捕获多硫化物/多硒化物的机理示意图[200]; (c~e) 在0.5 C下,(正极80%硒)电池前三圈循环的CV曲线、恒流充放电曲线和循环性能[201]; (f) Co-N-C@C中间层的结构设计及其捕获LiPSs/LiPSes的机理示意图[209]; (g) Se/PCC正极和PAN中间层的制备工艺及组装锂硒电池的简要模型[208]; (h) 无中间层[211],(i)有GS中间层[211],(j) 有GST中间层[211]的电池内部结构示意图
Fig. 10 (a,b) Molecular structure of TPB-DMTP-COF bifunctional separation coating material and mechanism for capturing polysulfide/polyselenide[200]; (c) the first three CV curves, (d) galvanostatic discharge and charge profiles and (e) cycling performance of Se-80% cathode based battery at 0.5 C[201]; (f) the structural design of Co-N-C@C interlayer and the LiPSs/LiPSes trapping mechanism[209]; (g) Preparation process for the Se/PCC cathode and PAN interlayer, and the brief model of the assembled Li-Se battery[208]; Schematic illustration of the structure composition of the cells (h) without interlayer, (i) with GS interlayer, and (j) with GST interlayer[211]
图11 (a) 正极表面的成膜机理和循环500圈后的SEM图像[219]; (b) 横截面SEM图像显示了从分隔层到正极的多层结构[222]; (c) PF 5 -信号的三维空间构型[222]; (d) 不同LiPF6浓度电解液聚合程度的光学图像[222]; (e,f) Li-Se电池在醚基LE和GPE电解质中的电化学示意图[223]; (g) 在0.2 C下充放电的不同阶段收集的Se-KB正极与混合电解液的SEM/EDX图像[225]; (h) 基于原位拉曼光谱轮廓的容量示意图[226]; (i) 不同充放电状态下的原位拉曼光谱[226]
Fig. 11 (a) The film formation mechanism of the cathode surface and the SEM image after 500 cycles[219]. (b) Cross-sectional SEM image illustrating multilayered structure from the separator to the cathode[222]. (c) Three-dimensional configuration of PF 5 - signal[222]. (d) Optical images showing the various polymerization degrees of liquid electrolyte with different LiPF6 concentrations[222]. The electrochemistry of Li-Se batteries with ether-based LE (e) and GPE (f)[223]. (g) SEM/EDX images of the Se-KB cathode with hybrid electrolytes collected at various stages of discharge and charge at 0.2 C[225]. (h) Capacity dependent in situ Raman spectral contour plots[226]. (i) in situ Raman spectra at different discharge/charge states[226]
表1 近些年锂硒电池正极材料及其电化学性能
Table 1 Electrochemical performances of reported lithium-selenium batteries cathode materials in recent years
Material Mass fraction of Se (%) Initial capacity/(mAh/g) Cycle Number Rate Capacity retention/(mAh/g) ref
Se/MnMC-B 72 904 1000 1 C 580 115
Se@PCNFs 52.3 643 (0.05A/g) 900 0.5 A/g 516 123
Se@HHCS 48 1026 (0.2C) 500 2 C 558 124
Se@KF65 70 1460.8 50 0.1 A/g 1288.7 138
Se@CNx 62.5 597.4 (6th) 400 0.8 A/g 453.2 139
Se/HDHPC 48 613 1500 0.5 C 545 140
Se/HPCNBs 60 574 100 0.2 C 560 142
Se/Fe2O3 5 1458 400 1 A/g 1456 151
Se/MCN-RGO 62 655 100 0.1 C 568 158
Se/GPNF 75 847.5 200 0.1 C 489 159
Se@CoSA-HC 73 613 100 0.1 C 564 128
Se-TiO2 52 816.8 200 0.5 C 600.4 164
图12 近些年锂硒电池正极材料及其电化学性能
Fig. 12 Electrochemical performances of reported lithium-selenium batteries cathode materials in recent years
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锂硒电池研究进展