In Situ Ambient Pressure X-ray Photoelectron Spectroscopy Studies of Lithium-Oxygen Redox Reactions
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srep00715.pdf
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Author(s)
Lu, Yi-chun
Crumlin, Ethan J.
Veith, Gabriel M.
Harding, Jonathon R.
Mutoro, Eva
Baggetto, Loic
Dudney, Nancy J.
Liu, Zhi
Shao-Horn, Yang
Date Issued
October 2012
Journal
Scientific Reports
Publisher
Nature Publishing Group
Citation
Lu, Yi-Chun, Ethan J. Crumlin, Gabriel M. Veith, Jonathon R. Harding, Eva Mutoro, Loïc Baggetto, Nancy J. Dudney, Zhi Liu, and Yang Shao-Horn. In Situ Ambient Pressure X-ray Photoelectron Spectroscopy Studies of Lithium-Oxygen Redox Reactions. Scientific Reports 2 (October 8, 2012).
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Final published version
Abstract
The lack of fundamental understanding of the oxygen reduction and oxygen evolution in nonaqueous electrolytes significantly hinders the development of rechargeable lithium-air batteries. Here we employ a solid-state Li4+xTi5O12/LiPON/LixV2O5 cell and examine in situ the chemistry of Li-O2 reaction products on LixV2O5 as a function of applied voltage under ultra high vacuum (UHV) and at 500 mtorr of oxygen pressure using ambient pressure X-ray photoelectron spectroscopy (APXPS). Under UHV, lithium intercalated into LixV2O5 while molecular oxygen was reduced to form lithium peroxide on LixV2O5 in the presence of oxygen upon discharge. Interestingly, the oxidation of Li2O2 began at much lower overpotentials (~240 mV) than the charge overpotentials of conventional Li-O2 cells with aprotic electrolytes (~1000 mV). Our study provides the first evidence of reversible lithium peroxide formation and decomposition in situ on an oxide surface using a solid-state cell, and new insights into the reaction mechanism of Li-O2 chemistry.
MIT Department
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Massachusetts Institute of Technology. Department of Mechanical Engineering
Massachusetts Institute of Technology. Electrochemical Energy Laboratory
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DOI of Published Version
https://doi.org/10.1038/srep00715
