Designer interphases for the lithium-oxygen electrochemical cell

Snehashis Choudhury, Charles Tai-Chieh Wan, Wajdi I. Al Sadat, Zhengyuan Tu, Sampson Lau, Michael J. Zachman, Lena F. Kourkoutis, Lynden A. Archer

Research output: Contribution to journalArticlepeer-review

69 Scopus citations

Abstract

An 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.
Original languageEnglish (US)
Pages (from-to)e1602809
JournalScience Advances
Volume3
Issue number4
DOIs
StatePublished - Apr 19 2017
Externally publishedYes

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): KUS-C1-018-02
Acknowledgements: We 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.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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