Realizing Persistent Lithium Protection and Revival with Dissolution‐Equilibrium‐Driven Sustainable Additives Reservoir

X Xiao‐Xi Luo (CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China) S Shuang‐Jie Tan (CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China) J Juan Zhang J Jun‐Chen Guo (CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China) C Chao‐Hui Zhang (CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China) Y Yu‐Hao Wang (CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China) W Wan‐Li Wang (CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China) J Jian‐Song Wu (CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China) X Xing‐Long Wu (MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China) Y Yu‐Guo Guo (CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory For Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences (CAS) Beijing P. R. China)

Abstract

Abstract Additive chemistry plays a pivotal role in enhancing the cycling stability of lithium metal batteries. Conventional additives with high solubility facilitate the formation of a stable interface in the early stages of cycling, yet typically act as “sacrificial agents”, failing to maintain a durable interface over long time. Herein, we demonstrate a sustainable lithium protection and retrieval strategy based on additive reservoirs driven by chemical dissolution equilibrium. A sparingly soluble AgI coating on the separator provides a continuous supply of constant concentration of Ag + and I − , where Ag + contributes to the formation of a Li–Ag alloy interphase, promoting uniform Li deposition, while I − assisting in the recovery of inactive Li. With this strategy, symmetric Li||Li batteries deliver an extended cycle life over of 1000 h at 5 mA cm −2 with a capacity of 5 mAh cm −2 . Additionally, practical pouch cells demonstrate a prolonged cycle life of over 200 cycles with 82% capacity retention. This work offers new insights into additive chemistry and paves the way for the development of durable lithium metal batteries.

Article Details

Volume / Issue Vol. 64, Issue 33
Published August 11, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (10)

X

Xiao‐Xi Luo

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China

S

Shuang‐Jie Tan

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China

J

Juan Zhang

J

Jun‐Chen Guo

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China

C

Chao‐Hui Zhang

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China

Y

Yu‐Hao Wang

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China

W

Wan‐Li Wang

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China

J

Jian‐Song Wu

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry, Chinese Academy of Sciences (CAS) Beijing 100190 P.R. China

X

Xing‐Long Wu

MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China

Y

Yu‐Guo Guo

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory For Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences (CAS) Beijing P. R. China