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Origin and regulation of oxygen redox instability in high-voltage battery cathodes

Journal Article · · Nature Energy
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  1. Argonne National Laboratory (ANL), Lemont, IL (United States)
  2. Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials; University of Florida, Gainesville, FL (United States)
  3. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  4. Argonne National Laboratory (ANL), Lemont, IL (United States). Center for Nanoscale Materials
  5. Xiamen University (China)
  6. Tsinghua University, Beijing (China)
  7. Argonne National Laboratory (ANL), Lemont, IL (United States); Stanford University, CA (United States); Mohammed VI Polytechnic University (UM6P), Ben Guerir (Morocco)
+ Show Author Affiliations
Oxygen redox at high-voltage has emerged as a transformative paradigm for high-energy battery cathodes such as layered transition-metal oxides by offering extra capacity beyond conventional transition-metal redox. However, these cathodes suffer from voltage hysteresis, voltage fade, and capacity drop upon cycling; single-crystalline cathodes have recently shown some improvements but these challenges still remain. We reveal the fundamental origin of oxygen redox instability to be originated from the domain boundaries that are present in single-crystalline cathode particles. By synthesizing single-crystalline cathodes free of domain boundaries, we show that the elimination of domain boundaries enhances the reversible lattice oxygen redox while inhibiting the irreversible oxygen release. Further, this leads to significantly suppressed structural degradation and improved mechanical integrity during battery cycling and abuse heating. The robust oxygen redox enabled through domain boundary control provides practical opportunities towards high-energy, long-cycling, and safe batteries.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; US–China Clean Energy Research Centre
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357
OSTI ID:
1962346
Alternate ID(s):
OSTI ID: 1963049
Journal Information:
Nature Energy, Journal Name: Nature Energy Journal Issue: 9 Vol. 7; ISSN 2058-7546
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
Batteries
Electrochemistry