Non-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries

Hua, Xiao and Allan, Phoebe K. and Gong, Chen and Chater, Philip A. and Schmidt, Ella M. and Geddes, Harry S. and Robertson, Alex W. and Bruce, Peter G. and Goodwin, Andrew L. (2021) Non-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries. Nature Communications, 12. ISSN 2041-1723

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Abstract

Binary metal oxides are attractive anode materials for lithium-ion batteries. Despite sustained effort into nanomaterials synthesis and understanding the initial discharge mechanism, the fundamental chemistry underpinning the charge and subsequent cycles—thus the reversible capacity—remains poorly understood. Here, we use in operando X-ray pair distribution function analysis combining with our recently developed analytical approach employing Metropolis Monte Carlo simulations and non-negative matrix factorisation to study the charge reaction thermodynamics of a series of Fe- and Mn-oxides. As opposed to the commonly believed conversion chemistry forming rocksalt FeO and MnO, we reveal the two oxide series topotactically transform into non-native body-centred cubic FeO and zincblende MnO via displacement-like reactions whose kinetics are governed by the mobility differences between displaced species. These renewed mechanistic insights suggest avenues for the future design of metal oxide materials as well as new material synthesis routes using electrochemically-assisted methods.

Item Type:
Journal Article
Journal or Publication Title:
Nature Communications
Uncontrolled Keywords:
/dk/atira/pure/subjectarea/asjc/3100
Subjects:
?? ELECTRODE MATERIALSMETAL OXIDESPAIR DISTRIBUTION FUNCTIONBIOCHEMISTRY, GENETICS AND MOLECULAR BIOLOGY(ALL)CHEMISTRY(ALL)PHYSICS AND ASTRONOMY(ALL) ??
ID Code:
171407
Deposited By:
Deposited On:
07 Jun 2022 15:40
Refereed?:
Yes
Published?:
Published
Last Modified:
02 Nov 2023 11:25