Metal–oxygen decoordination stabilizes anion redox in Li-rich oxides
Abstract
Reversible high-voltage redox chemistry is an essential component of many electrochemical technologies, from (electro)catalysts to lithium-ion batteries. Oxygen-anion redox has garnered intense interest for such applications, particularly lithium-ion batteries, as it offers substantial redox capacity at more than 4 V versus Li/Li+ in a variety of oxide materials. However, oxidation of oxygen is almost universally correlated with irreversible local structural transformations, voltage hysteresis and voltage fade, which currently preclude its widespread use. By comprehensively studying the Li2-xIr1-ySnyO3 model system, which exhibits tunable oxidation state and structural evolution with y upon cycling, we reveal that this structure-redox coupling arises from the local stabilization of short approximately 1.8 Å metal-oxygen π bonds and approximately 1.4 Å O-O dimers during oxygen redox, which occurs in Li2-xIr1-ySnyO3 through ligand-to-metal charge transfer. Crucially, formation of these oxidized oxygen species necessitates the decoordination of oxygen to a single covalent bonding partner through formation of vacancies at neighbouring cation sites, driving cation disorder. These insights establish a point-defect explanation for why anion redox often occurs alongside local structural disordering and voltage hysteresis during cycling. Our findings offer an explanation for the unique electrochemical properties of lithium-rich layered oxides, with implications generally for the design of materials employingmore »
- Authors:
-
- Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource. Stanford Inst. for Materials & Energy Sciences. Applied Energy Division
- Stanford Univ., CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Advanced Light Source
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
- Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Inst. for Materials & Energy Sciences; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Advanced Light Source
- Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource
- Argonne National Lab. (ANL), Argonne, IL (United States). The Advanced Photon Source
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Advanced Light Source
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource. Applied Energy Division
- Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Inst. for Materials & Energy Sciences. Applied Energy Division
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States); Stanford Univ., CA (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1494840
- Alternate Identifier(s):
- OSTI ID: 1503542; OSTI ID: 1594911
- Grant/Contract Number:
- AC02-76SF00515; AC02-05CH11231; AC02-06CH11357; SC0012583; ECCS-1542152
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 18; Journal ID: ISSN 1476-1122
- Publisher:
- Springer Nature - Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; batteries; materials chemistry; solid-state chemistry
Citation Formats
Hong, Jihyun, Gent, William E., Xiao, Penghao, Lim, Kipil, Seo, Dong-Hwa, Wu, Jinpeng, Csernica, Peter M., Takacs, Christopher J., Nordlund, Dennis, Sun, Cheng-Jun, Stone, Kevin H., Passarello, Donata, Yang, Wanli, Prendergast, David, Ceder, Gerbrand, Toney, Michael F., and Chueh, William C. Metal–oxygen decoordination stabilizes anion redox in Li-rich oxides. United States: N. p., 2019.
Web. doi:10.1038/s41563-018-0276-1.
Hong, Jihyun, Gent, William E., Xiao, Penghao, Lim, Kipil, Seo, Dong-Hwa, Wu, Jinpeng, Csernica, Peter M., Takacs, Christopher J., Nordlund, Dennis, Sun, Cheng-Jun, Stone, Kevin H., Passarello, Donata, Yang, Wanli, Prendergast, David, Ceder, Gerbrand, Toney, Michael F., & Chueh, William C. Metal–oxygen decoordination stabilizes anion redox in Li-rich oxides. United States. https://doi.org/10.1038/s41563-018-0276-1
Hong, Jihyun, Gent, William E., Xiao, Penghao, Lim, Kipil, Seo, Dong-Hwa, Wu, Jinpeng, Csernica, Peter M., Takacs, Christopher J., Nordlund, Dennis, Sun, Cheng-Jun, Stone, Kevin H., Passarello, Donata, Yang, Wanli, Prendergast, David, Ceder, Gerbrand, Toney, Michael F., and Chueh, William C. Mon .
"Metal–oxygen decoordination stabilizes anion redox in Li-rich oxides". United States. https://doi.org/10.1038/s41563-018-0276-1. https://www.osti.gov/servlets/purl/1494840.
@article{osti_1494840,
title = {Metal–oxygen decoordination stabilizes anion redox in Li-rich oxides},
author = {Hong, Jihyun and Gent, William E. and Xiao, Penghao and Lim, Kipil and Seo, Dong-Hwa and Wu, Jinpeng and Csernica, Peter M. and Takacs, Christopher J. and Nordlund, Dennis and Sun, Cheng-Jun and Stone, Kevin H. and Passarello, Donata and Yang, Wanli and Prendergast, David and Ceder, Gerbrand and Toney, Michael F. and Chueh, William C.},
abstractNote = {Reversible high-voltage redox chemistry is an essential component of many electrochemical technologies, from (electro)catalysts to lithium-ion batteries. Oxygen-anion redox has garnered intense interest for such applications, particularly lithium-ion batteries, as it offers substantial redox capacity at more than 4 V versus Li/Li+ in a variety of oxide materials. However, oxidation of oxygen is almost universally correlated with irreversible local structural transformations, voltage hysteresis and voltage fade, which currently preclude its widespread use. By comprehensively studying the Li2-xIr1-ySnyO3 model system, which exhibits tunable oxidation state and structural evolution with y upon cycling, we reveal that this structure-redox coupling arises from the local stabilization of short approximately 1.8 Å metal-oxygen π bonds and approximately 1.4 Å O-O dimers during oxygen redox, which occurs in Li2-xIr1-ySnyO3 through ligand-to-metal charge transfer. Crucially, formation of these oxidized oxygen species necessitates the decoordination of oxygen to a single covalent bonding partner through formation of vacancies at neighbouring cation sites, driving cation disorder. These insights establish a point-defect explanation for why anion redox often occurs alongside local structural disordering and voltage hysteresis during cycling. Our findings offer an explanation for the unique electrochemical properties of lithium-rich layered oxides, with implications generally for the design of materials employing oxygen redox chemistry.},
doi = {10.1038/s41563-018-0276-1},
journal = {Nature Materials},
number = ,
volume = 18,
place = {United States},
year = {Mon Feb 04 00:00:00 EST 2019},
month = {Mon Feb 04 00:00:00 EST 2019}
}
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