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dc.contributor.authorChoudhury, Snehashis
dc.contributor.authorWan, Charles Tai-Chieh
dc.contributor.authorAl Sadat, Wajdi I.
dc.contributor.authorTu, Zhengyuan
dc.contributor.authorLau, Sampson
dc.contributor.authorZachman, Michael J.
dc.contributor.authorKourkoutis, Lena F.
dc.contributor.authorArcher, Lynden A.
dc.date.accessioned2017-05-15T10:35:07Z
dc.date.available2017-05-15T10:35:07Z
dc.date.issued2017-04-19
dc.identifier.citationChoudhury S, Wan CT-C, Al Sadat WI, Tu Z, Lau S, et al. (2017) Designer interphases for the lithium-oxygen electrochemical cell. Science Advances 3: e1602809. Available: http://dx.doi.org/10.1126/sciadv.1602809.
dc.identifier.issn2375-2548
dc.identifier.doi10.1126/sciadv.1602809
dc.identifier.urihttp://hdl.handle.net/10754/623533
dc.description.abstractAn electrochemical cell based on the reversible oxygen reduction reaction: 2Li+ + 2e− + O2 ↔ Li2O2, provides among the most energy dense platforms for portable electrical energy storage. Such Lithium-Oxygen (Li-O2) cells offer specific energies competitive with fossil fuels and are considered promising for electrified transportation. Multiple, fundamental challenges with the cathode, anode, and electrolyte have limited practical interest in Li-O2 cells because these problems lead to as many practical shortcomings, including poor rechargeability, high overpotentials, and specific energies well below theoretical expectations. We create and study in-situ formation of solid-electrolyte interphases (SEIs) based on bromide ionomers tethered to a Li anode that take advantage of three powerful processes for overcoming the most stubborn of these challenges. The ionomer SEIs are shown to protect the Li anode against parasitic reactions and also stabilize Li electrodeposition during cell recharge. Bromine species liberated during the anchoring reaction also function as redox mediators at the cathode, reducing the charge overpotential. Finally, the ionomer SEI forms a stable interphase with Li, which protects the metal in high Gutmann donor number liquid electrolytes. Such electrolytes have been reported to exhibit rare stability against nucleophilic attack by Li2O2 and other cathode reaction intermediates, but also react spontaneously with Li metal anodes. We conclude that rationally designed SEIs able to regulate transport of matter and ions at the electrolyte/anode interface provide a promising platform for addressing three major technical barriers to practical Li-O2 cells.
dc.description.sponsorshipWe are grateful to the Advanced Research Projects Agency-Energy (award DE-AR-0000750) for supporting this study. The study made use of the characterization facilities of the King Abdullah University of Science and Technology (KAUST)–Cornell University Center for Energy and Sustainability, which was supported by the KAUST through award number KUS-C1-018-02. Electron microscopy facilities at the Cornell Center for Materials Research, an NSF-supported Materials Research Science and Engineering Center through grant DMR-1120296, were also used for the study. Additional support for the FIB/SEM cryo-stage and transfer system was provided by the Kavli Institute at Cornell and the Energy Materials Center at Cornell and the U.S. Department of Energy, Energy Frontier Research Center, Basic Energy Sciences (DE-SC0001086). M.J.Z. and L.F.K. acknowledge support by the David and Lucile Packard Foundation.
dc.publisherAmerican Association for the Advancement of Science (AAAS)
dc.relation.urlhttp://advances.sciencemag.org/content/3/4/e1602809
dc.rightsThis is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.
dc.rights.urihttp://creativecommons.org/licenses/by-nc/4.0/
dc.subjectlithium-oxygen cells
dc.subjectsolid-electrolyte interphases
dc.subjectEnergy storage
dc.subjectredox mediators
dc.subjecthigh donor number electroly
dc.subjectteslithium dendrites
dc.titleDesigner interphases for the lithium-oxygen electrochemical cell
dc.typeArticle
dc.identifier.journalScience Advances
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionSchool of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY 14853, USA
dc.contributor.institutionDepartment of Materials Science and Engineering, Cornell University, Ithaca, NY 14853, USA
dc.contributor.institutionSchool of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, USA
dc.contributor.institutionKavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY 14853, USA
kaust.grant.numberKUS-C1-018-02
dc.date.published-online2017-04-19
dc.date.published-print2017-04


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This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.
Except where otherwise noted, this item's license is described as This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.