A high-energy-density lithium-oxygen battery based on a reversible four-electron conversion to lithium oxide
An elevated lithium battery
Batteries based on lithium metal and oxygen could offer energy densities an order of magnitude larger than that of lithium ion cells. But, under normal operation conditions, the lithium oxidizes to form peroxide or superoxide. Xia et al. show that, at increased temperatures, the formation of lithium oxide is favored, through a process in which four electrons are transferred for each oxygen molecule (see the Perspective by Feng et al.). Reversible cycling is achieved through the use of a thermally stable inorganic electrolyte and a bifunctional catalyst for both oxygen reduction and evolution reactions.
Abstract
Lithium-oxygen (Li-O2) batteries have attracted much attention owing to the high theoretical energy density afforded by the two-electron reduction of O2 to lithium peroxide (Li2O2). We report an inorganic-electrolyte Li-O2 cell that cycles at an elevated temperature via highly reversible four-electron redox to form crystalline lithium oxide (Li2O). It relies on a bifunctional metal oxide host that catalyzes O–O bond cleavage on discharge, yielding a high capacity of 11 milliampere-hours per square centimeter, and O2 evolution on charge with very low overpotential. Online mass spectrometry and chemical quantification confirm that oxidation of Li2O involves transfer of exactly 4 e–/O2. This work shows that Li-O2 electrochemistry is not intrinsically limited once problems of electrolyte, superoxide, and cathode host are overcome and that coulombic efficiency close to 100% can be achieved.
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Supplementary Material
Summary
Materials and Methods
Figs. S1 to S11
Table S1
Resources
File (aas9343-xia-sm.pdf)
References and Notes
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Science
Volume 361 | Issue 6404
24 August 2018
24 August 2018
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Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.
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Submission history
Received: 8 January 2018
Accepted: 10 July 2018
Published in print: 24 August 2018
Acknowledgments
The authors thank V. Goodfellow and R. Smith at the University of Waterloo Mass Spectrometry Facility for their scientific input in the gas chromatography–mass spectrometry measurements. We also thank S. H. Vajargah for performing the TEM measurements. Funding: Research was supported by the Natural Sciences and Engineering Council of Canada through their Discovery and Canada Research Chair programs (L.F.N.), and a doctoral scholarship to C.Y.K. Partial funding for this work (C.Y.K.) was also provided by the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. Author contributions: C.X. led the design of the study, and all the authors contributed to the implementation and writing of the manuscript; data collection and analysis were conducted by C.X. and C.Y.K. Competing interests: The authors have no competing interests. Data and materials availability: All data are available in the manuscript or in the supplementary materials.
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U.S. Department of Energy: Office of Basic Sciences (JCESR)
Government of Canada: Natural Sciences and Engineering Research Council
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