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Title: 1000 Wh L−1 lithium-ion batteries enabled by crosslink-shrunk tough carbon encapsulated silicon microparticle anodes

Journal Article · · National Science Review
DOI:https://doi.org/10.1093/nsr/nwab012· OSTI ID:1819775
 [1];  [2];  [3];  [4];  [1];  [1];  [5];  [2];  [2];  [4];  [2];  [6]
  1. Nanoyang Group, State Key Laboratory of Chemical Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
  2. Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
  3. CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China
  4. Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, IL 60439, USA
  5. International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), Tsukuba 305-0044, Japan
  6. Nanoyang Group, State Key Laboratory of Chemical Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China, Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, China
+ Show Author Affiliations

Microparticulate silicon (Si), normally shelled with carbons, features higher tap density and less interfacial side reactions compared to its nanosized counterpart, showing great potential to be applied as high-energy lithium-ion battery anodes. However, localized high stress generated during fabrication and particularly, under operating, could induce cracking of carbon shells and release pulverized nanoparticles, significantly deteriorating its electrochemical performance. Here we design a strong yet ductile carbon cage from an easily processing capillary shrinkage of graphene hydrogel followed by precise tailoring of inner voids. Such a structure, analog to the stable structure of plant cells, presents ‘imperfection-tolerance’ to volume variation of irregular Si microparticles, maintaining the electrode integrity over 1000 cycles with Coulombic efficiency over 99.5%. This design enables the use of a dense and thick (3 mAh cm–2) microparticulate Si anode with an ultra-high volumetric energy density of 1048 Wh L–1 achieved at pouch full-cell level coupled with a LiNi0.8Co0.1Mn0.1O2 cathode.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; National Natural Science Foundation of China (NSFC); National Science Fund for Distinguished Young Scholars of China; Japan Society for the Promotion of Science (JSPS); Beijing Natural Science Foundation
Grant/Contract Number:
AC02-06CH11357; 51872195; 51525204; 20K05281; 2192061
OSTI ID:
1819775
Alternate ID(s):
OSTI ID: 1846425
Journal Information:
National Science Review, Journal Name: National Science Review Vol. 8 Journal Issue: 9; ISSN 2095-5138
Publisher:
Oxford University PressCopyright Statement
Country of Publication:
China
Language:
English

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25 ENERGY STORAGE
anode
lithium-ion batteries
mechanical stability
silicon microparticles
volumetric capacity