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Progress in Chemistry 2022, Vol. 34 Issue (11): 2517-2539 DOI: 10.7536/PC220340 Previous Articles   Next Articles

• Review •

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: Revised: Online: Published:
  • 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)
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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
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
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]
Fig. 3 Existing problems in lithium-selenium batteries
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]
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]
Fig. 6 Formation mechanism of two novel one-dimensional nanostructures[151]
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
Fig. 8 (a) Proposed advantages of CoS2@LRC/SeS2 over LRC/SeS2[180]; (b) lithiation of NiCo2S4@NC-SeS2 cathode[181]
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]
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]
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]
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
Fig. 12 Electrochemical performances of reported lithium-selenium batteries cathode materials in recent years
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Abstract

Advances in Lithium Selenium Batteries