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author:

Li, H. (Li, H..) [1] | Cui, L. (Cui, L..) [2] | Wu, F. (Wu, F..) [3] | Wang, J. (Wang, J..) [4] | Cheng, Y. (Cheng, Y..) [5] | Li, C. (Li, C..) [6] | Song, J. (Song, J..) [7] | Li, Y. (Li, Y..) [8] | Liu, D. (Liu, D..) [9] | Cabot, A. (Cabot, A..) [10] | Zhang, C. (Zhang, C..) [11] | Tang, H. (Tang, H..) [12]

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Scopus

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 ≈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 °C to as low as −30 °C, it exhibits excellent adaptivity attributed to the fast kinetics, shedding light on future practical applications. © 2025 The Author(s). Advanced Energy Materials published by Wiley-VCH GmbH.

Keyword:

all-solid-state lithium-sulfur battery electrode/electrolyte interface solid electrolyte ultralong life wide-temperature range

Community:

  • [ 1 ] [Li H.]State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 2 ] [Li H.]Hubei Key Laboratory of Fuel Cells, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 3 ] [Cui L.]State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 4 ] [Wu F.]State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 5 ] [Wu F.]Hubei Key Laboratory of Fuel Cells, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 6 ] [Wang J.]Karlsruhe Institute of Technology (KIT), P.O. Box 3640, Karlsruhe, D-7621, Germany
  • [ 7 ] [Wang J.]Helmholtz Institute Ulm (HIU), Helmholtzstrasse 11, Ulm, D-89081, Germany
  • [ 8 ] [Cheng Y.]Catalonia Institute for Energy Research – IREC Sant Adrià de Besòs, Barcelona, 08930, Spain
  • [ 9 ] [Li C.]Catalonia Institute for Energy Research – IREC Sant Adrià de Besòs, Barcelona, 08930, Spain
  • [ 10 ] [Song J.]Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory, Foshan, 528200, China
  • [ 11 ] [Li Y.]State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 12 ] [Li Y.]Hubei Key Laboratory of Fuel Cells, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 13 ] [Liu D.]Hubei Key Laboratory of Fuel Cells, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 14 ] [Cabot A.]Catalonia Institute for Energy Research – IREC Sant Adrià de Besòs, Barcelona, 08930, Spain
  • [ 15 ] [Cabot A.]ICREA Pg. Lluis Companys, Catalonia, Barcelona, 08010, Spain
  • [ 16 ] [Zhang C.]College of Materials Science and Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
  • [ 17 ] [Tang H.]State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 18 ] [Tang H.]Hubei Key Laboratory of Fuel Cells, Wuhan University of Technology, Hubei, Wuhan, 430070, China
  • [ 19 ] [Tang H.]Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory, Foshan, 528200, China

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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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30 Days PV: 0

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