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The conversion of Li2S4 to Li2S is the most important and slowest rate-limiting step in the complex sulfur reduction reaction (SRR) for Li-S batteries, the adjustment of which can effectively inhibit the notorious "shuttle effect". Herein, a CoSe2-FeSe2 heterostructure embedded in 3D N-doped nanocage as a modified layer on commercial separator is designed (CoSe2-FeSe2@NC//PP). The CoSe2-FeSe2 heterostructure forms a built-in electric field at the two-phase interface, which leads to the optimized adsorption force on polysulfides and the accelerated reaction kinetics for Li2S4-Li2S evolution. Density functional theory (DFT) calculations and experimental results combine to show that the liquid-solid reaction (Li2S4-Li2S2/Li2S) is significantly enhanced in terms of thermodynamics and electrodynamics. Consequently, the batteries assembled with CoSe2-FeSe2@NC//PP delivered an excellent rate capability (606 mAh g(-1) under 8.0 C) and a long cycling lifespan (only 0.056% at 1.0 C after 1000 cycles). In addition, the cells can provide high initial capacity of 887 mAh g(-1) at sulfur loading of 5.8 mg cm(-2) and 0.1 C. This work would provide valuable insights into binary metal selenide heterostructures for liquid-solid conversion in Li-S batteries.
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SMALL
ISSN: 1613-6810
Year: 2024
Issue: 49
Volume: 20
1 3 . 0 0 0
JCR@2023
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SCOPUS Cited Count:
ESI Highly Cited Papers on the List: 0 Unfold All
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Chinese Cited Count:
30 Days PV: 4
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