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Abstract:
Inadequate ionic transport across the electrode/electrolyte interface hampers the lithium-sulfur reaction kinetics, thereby limiting the electrochemical performance of all-solid-state lithium-sulfur batteries (ASSLSBs). Herein, a kinetically-enhanced gradient modulator layer (KEGML) is proposed and fabricated via potential modulation. In situ/ex situ analyses reveal the optimal modulated potential difference driving the chemical reaction between Li ions and the P2S5 pre-interphase product for stabilized KEGML and maintained full-sulfur conversion. Cryo-focused ion beam-scanning electron microscopy characterization and ab-initio molecular dynamics confirm the interfacial reinforcement by gradient uniformization of ion transport and enhanced interface stability by efficiently avoiding the side effects between sulfur/sulfides solid electrolyte/carbon, respectively. As a result, an eightfold increase in ionic transport capability is achieved with KEGML at the end of the 200 cycles. Impressively, KEGML-based ASSLSBs not only accelerate the redox conversions but also display an exceptional cycling stability of a specific capacity of 1578.9 mAh g(-1) for approximate to 1.5 years with a 99.9% capacity retention and a high areal capacity of 13 mAh cm(-2) over 200 cycles, which is among the record-level. Even in the ambient environment from 60 degrees C to as low as -30 degrees C, it exhibits excellent adaptivity attributed to the fast kinetics, shedding light on future practical applications.
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ADVANCED ENERGY MATERIALS
ISSN: 1614-6832
Year: 2025
2 4 . 4 0 0
JCR@2023
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ESI Highly Cited Papers on the List: 0 Unfold All
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