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Carbon Mediated In Situ Cathode Interface Stabilization for High Rate and Highly Stable Operation of All‐Solid‐State Lithium Batteries

Bhadra, Abhirup LU orcid ; Brunisholz, Maxime ; Bonsu, Jacob Otabil and Kundu, Dipan (2025) In Advanced Energy Materials 15(14).
Abstract
Interfacial stability issues at the cathode remain a bottleneck to
developing durable and high-power all-solid-state lithium batteries
(ASSLBs). In fact, the presence of conductive carbon in the cathode,
necessary for high capacity and power capability, is believed to
aggravate the stability woes. Thus, it is typically excluded from the
cathode mix. Herein, employing a model functionalized carbon, it is
shown that a small carbon surface oxygen functionality can in situ
engineer a robust carbon–solid electrolyte interphase, which arrests
conductive carbon-mediated degradation of Li6PS5Cl into reactive polysulfides that degrades the active... (More)
Interfacial stability issues at the cathode remain a bottleneck to
developing durable and high-power all-solid-state lithium batteries
(ASSLBs). In fact, the presence of conductive carbon in the cathode,
necessary for high capacity and power capability, is believed to
aggravate the stability woes. Thus, it is typically excluded from the
cathode mix. Herein, employing a model functionalized carbon, it is
shown that a small carbon surface oxygen functionality can in situ
engineer a robust carbon–solid electrolyte interphase, which arrests
conductive carbon-mediated degradation of Li6PS5Cl into reactive polysulfides that degrades the active LiNi1/3Mn1/3Co1/3O2
(NMC) cathode. Such interfacial stabilization, as confirmed by ex situ
spectroscopic and in situ impedance analysis, combined with fast charge
transport facilitated by functionalized yet conductive carbon and lowly
resistive cathode interphases, elevates the performance. This is
evidenced by stable cycling at room temperature (22 °C) and elevated
temperatures (60 °C), high rate capability, a Coulombic efficiency of
99.8%, and ≈100% capacity retention after 1000 cycles and >90%
retention over 2000 cycles at 60 °C. Functionalized carbon-mediated in
situ cathode interfacial engineering offers a simple and scalable
approach to designing durable ASSLB cathodes, with the potential for
broader application across various NMC cathodes and compatible solid
electrolytes. (Less)
Please use this url to cite or link to this publication:
author
; ; and
publishing date
type
Contribution to journal
publication status
published
in
Advanced Energy Materials
volume
15
issue
14
article number
2403608
publisher
Wiley-Blackwell
external identifiers
  • scopus:105002142773
ISSN
1614-6840
DOI
10.1002/aenm.202403608
language
English
LU publication?
no
id
9b464ad9-c4fc-42bb-aa3d-58c91fb590d2
date added to LUP
2026-03-04 09:48:59
date last changed
2026-03-10 11:18:51
@article{9b464ad9-c4fc-42bb-aa3d-58c91fb590d2,
  abstract     = {{Interfacial stability issues at the cathode remain a bottleneck to <br>
developing durable and high-power all-solid-state lithium batteries <br>
(ASSLBs). In fact, the presence of conductive carbon in the cathode, <br>
necessary for high capacity and power capability, is believed to <br>
aggravate the stability woes. Thus, it is typically excluded from the <br>
cathode mix. Herein, employing a model functionalized carbon, it is <br>
shown that a small carbon surface oxygen functionality can in situ <br>
engineer a robust carbon–solid electrolyte interphase, which arrests <br>
conductive carbon-mediated degradation of Li<sub>6</sub>PS<sub>5</sub>Cl into reactive polysulfides that degrades the active LiNi<sub>1/3</sub>Mn<sub>1/3</sub>Co<sub>1/3</sub>O<sub>2</sub><br>
 (NMC) cathode. Such interfacial stabilization, as confirmed by ex situ <br>
spectroscopic and in situ impedance analysis, combined with fast charge <br>
transport facilitated by functionalized yet conductive carbon and lowly <br>
resistive cathode interphases, elevates the performance. This is <br>
evidenced by stable cycling at room temperature (22 °C) and elevated <br>
temperatures (60 °C), high rate capability, a Coulombic efficiency of <br>
99.8%, and ≈100% capacity retention after 1000 cycles and &gt;90% <br>
retention over 2000 cycles at 60 °C. Functionalized carbon-mediated in <br>
situ cathode interfacial engineering offers a simple and scalable <br>
approach to designing durable ASSLB cathodes, with the potential for <br>
broader application across various NMC cathodes and compatible solid <br>
electrolytes.}},
  author       = {{Bhadra, Abhirup and Brunisholz, Maxime and Bonsu, Jacob Otabil and Kundu, Dipan}},
  issn         = {{1614-6840}},
  language     = {{eng}},
  month        = {{04}},
  number       = {{14}},
  publisher    = {{Wiley-Blackwell}},
  series       = {{Advanced Energy Materials}},
  title        = {{Carbon Mediated In Situ Cathode Interface Stabilization for High Rate and Highly Stable Operation of All‐Solid‐State Lithium Batteries}},
  url          = {{http://dx.doi.org/10.1002/aenm.202403608}},
  doi          = {{10.1002/aenm.202403608}},
  volume       = {{15}},
  year         = {{2025}},
}