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

Research output: Contribution to journalArticlepeer-review

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Non-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries. / Hua, Xiao; Allan, Phoebe K.; Gong, Chen; Chater, Philip A.; Schmidt, Ella M.; Geddes, Harry S.; Robertson, Alex W.; Bruce, Peter G.; Goodwin, Andrew L.

In: Nature Communications, Vol. 12, No. 1, 561, 12.2021.

Research output: Contribution to journalArticlepeer-review

Harvard

Hua, X, Allan, PK, Gong, C, Chater, PA, Schmidt, EM, Geddes, HS, Robertson, AW, Bruce, PG & Goodwin, AL 2021, 'Non-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries', Nature Communications, vol. 12, no. 1, 561. https://doi.org/10.1038/s41467-020-20736-6

APA

Hua, X., Allan, P. K., Gong, C., Chater, P. A., Schmidt, E. M., Geddes, H. S., Robertson, A. W., Bruce, P. G., & Goodwin, A. L. (2021). Non-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries. Nature Communications, 12(1), [561]. https://doi.org/10.1038/s41467-020-20736-6

Vancouver

Author

Hua, Xiao ; Allan, Phoebe K. ; Gong, Chen ; Chater, Philip A. ; Schmidt, Ella M. ; Geddes, Harry S. ; Robertson, Alex W. ; Bruce, Peter G. ; Goodwin, Andrew L. / Non-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries. In: Nature Communications. 2021 ; Vol. 12, No. 1.

Bibtex

@article{38f8f36931a9471f87ef314d954dc89a,
title = "Non-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries",
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.",
author = "Xiao Hua and Allan, {Phoebe K.} and Chen Gong and Chater, {Philip A.} and Schmidt, {Ella M.} and Geddes, {Harry S.} and Robertson, {Alex W.} and Bruce, {Peter G.} and Goodwin, {Andrew L.}",
year = "2021",
month = jan,
day = "25",
doi = "10.1038/s41467-020-20736-6",
language = "English",
volume = "12",
journal = "Nature Communications",
issn = "2041-1723",
publisher = "Springer",
number = "1",

}

RIS

TY - JOUR

T1 - Non-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries

AU - Hua, Xiao

AU - Allan, Phoebe K.

AU - Gong, Chen

AU - Chater, Philip A.

AU - Schmidt, Ella M.

AU - Geddes, Harry S.

AU - Robertson, Alex W.

AU - Bruce, Peter G.

AU - Goodwin, Andrew L.

PY - 2021/1/25

Y1 - 2021/1/25

N2 - 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.

AB - 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.

U2 - 10.1038/s41467-020-20736-6

DO - 10.1038/s41467-020-20736-6

M3 - Article

VL - 12

JO - Nature Communications

JF - Nature Communications

SN - 2041-1723

IS - 1

M1 - 561

ER -