Understanding LiOH Chemistry in a Ruthenium-Catalyzed Li-O<sub>2</sub> Battery.
Angewandte Chemie (International ed. in English)
John Wiley & Sons Ltd.
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Liu, T., Liu, Z., Kim, G., Frith, J. T., Garcia-Araez, N., & Grey, C. (2017). Understanding LiOH Chemistry in a Ruthenium-Catalyzed Li-O<sub>2</sub> Battery.. Angewandte Chemie (International ed. in English), 56 (50), 16057-16062. https://doi.org/10.1002/anie.201709886
Non-aqueous Li-O2 batteries are promising for next generation energy storage. New battery chemistries based on LiOH, rather than Li2O2, have recently been reported in systems with added water, one using a soluble additive LiI and the other using solid Ru catalysts. Here, we focus on the mechanism of Ru-catalyzed LiOH chemistry. Using nuclear magnetic resonance, operando electrochemical pressure measurements and mass spectrometry, we show that on discharging LiOH forms via a 4 e- oxygen reduction reaction, the H in LiOH coming solely from added H2O and the O from both O2 and H2O. On charging, quantitative LiOH oxidation occurs at 3.1 V, with O being trapped in a form of dimethyl sulfone in the electrolyte. Compared to Li2O2, LiOH formation over Ru incurs hardly any side reactions, a critical advantage for developing a long-lived battery. An optimized metal catalyst-electrolyte couple needs to be sought that aids LiOH oxidation and is able stable towards attack by hydroxyl radicals.
European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (696656)
EC FP7 FET FLAGSHIP (604391)
European Research Council (247411)
United States Department of Energy (DOE) (via University of California) (7057154)
UNIVERSITY OF OXFORD (FB EPSRC) (EP/L019469/1)
Technology Strategy Board (132220)
EPSRC (via University of Oxford) (EP/M009521/1)
External DOI: https://doi.org/10.1002/anie.201709886
This record's URL: https://www.repository.cam.ac.uk/handle/1810/277546
Attribution 4.0 International
Licence URL: http://creativecommons.org/licenses/by/4.0/
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