In:
EcoMat, Wiley, Vol. 5, No. 5 ( 2023-05)
Abstract:
An advanced electrocatalyst to accelerate the sluggish kinetics of multistep redox reactions and suppress the severe shuttle effects is desirable in Li‐S batteries (LSBs). Phase engineering can provide a fascinating way to modulate electronic structures and boost catalytic activity of electrocatalysts. In this study, few‐layered 1T‐MoSe 2 nanosheets grown on carbon cloth (1T‐MoSe 2 /CC) are synthesized and employed as a multifunctional interlayer as well as a catalytic 3D current collector in LSBs to promote both physiochemical confinement and catalytic conversion toward lithium polysulfides (LiPSs). Density functional theory (DFT) calculations reveal that 1T‐MoSe 2 has metallic properties beneficial for rapid electronic transport and exhibits a superior catalytic activity to reduce the Gibbs free energy barriers toward LiPS conversion. Significant improvements in chemisorption toward LiPSs, diffusion coefficients of Li ions, and Li 2 S deposition/decomposition reaction kinetics are realized by the 1T‐MoSe 2 /CC film. Consequently, the Al@S/AB@1T‐MoSe 2 /CC LSB, where 1T‐MoSe 2 /CC is used an interlayer, presents high rate capability of 1253 (1C), 1052 (2C) and 882 (4C) mAh g −1 and excellent long‐term cycling stability at a high rate (2000 cycles at 4C) with a low capacity fading rate (0.017% per cycle). Moreover, with a sandwiched cathode of 1T‐MoSe 2 /CC@S/AB@1T‐MoSe 2 /CC, where 1T‐MoSe 2 /CC works as both a catalytic 3D current collector and a multifunctional interlayer, the LSB at high S loading of 5.7 mg cm −2 and low electrolyte/sulfur ratio of 7.8 μL mg −1 exhibits a high initial areal capacity of 5.43 mAh cm −2 and remarkable rate‐cycling performance (200 cycles). image
Type of Medium:
Online Resource
ISSN:
2567-3173
,
2567-3173
Language:
English
Publisher:
Wiley
Publication Date:
2023
detail.hit.zdb_id:
2902933-8
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