Lattice site–dependent metal leaching in perovskites toward a honeycomb-like water oxidation catalyst

Yubo Chen; Yuanmiao Sun; Maoyu Wang; Jingxian Wang; Haiyan Li; Shibo Xi; Chao Wei; Pinxian Xi; George E. Sterbinsky; John W. Freeland; Adrian C. Fisher; Joel W. Ager; Zhenxing Feng; Zhichuan J. Xu

doi:10.1126/sciadv.abk1788

Lattice site–dependent metal leaching in perovskites toward a honeycomb-like water oxidation catalyst

Yubo Chen, Yuanmiao Sun, Maoyu Wang, Jingxian Wang, Haiyan Li, Shibo Xi, Chao Wei, Pinxian Xi, George E. Sterbinsky, John W. Freeland, Adrian C. Fisher, Joel W. Ager, Zhenxing Feng^*, Zhichuan J. Xu^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

81 Citations (Scopus)

Abstract

Metal leaching during water oxidation has been typically observed in conjunction with surface reconstruction on perovskite oxide catalysts, but the role of metal leaching at each geometric site has not been distinguished. Here, we manipulate the occurrence and process of surface reconstruction in two model ABO₃ perovskites, i.e., SrSc_0.5Ir_0.5O₃ and SrCo_0.5Ir_0.5O₃, which allow us to evaluate the structure and activity evolution step by step. The occurrence and order of leaching of Sr (A-site) and Sc/Co (B-site) were controlled by tailoring the thermodynamic stability of B-site. Sr leaching from A-site mainly generates more electrochemical surface area for the reaction, and additional leaching of Sc/Co from B-site triggers the formation of a honeycomb-like IrO_xH_y phase with a notable increase in intrinsic activity. A thorough surface reconstruction with dual-site metal leaching induces an activity improvement by approximately two orders of magnitude, which makes the reconstructed SrCo_0.5Ir_0.5O₃ among the best for water oxidation in acid.

Original language	English
Article number	eabk1788
Journal	Science advances
Volume	7
Issue number	50
DOIs	https://doi.org/10.1126/sciadv.abk1788
Publication status	Published - Dec 2021
Externally published	Yes

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Copyright © 2021 The Authors, some rights reserved;

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@article{4ac7351f778f4c089c4a37571b63e7a7,

title = "Lattice site–dependent metal leaching in perovskites toward a honeycomb-like water oxidation catalyst",

abstract = "Metal leaching during water oxidation has been typically observed in conjunction with surface reconstruction on perovskite oxide catalysts, but the role of metal leaching at each geometric site has not been distinguished. Here, we manipulate the occurrence and process of surface reconstruction in two model ABO3 perovskites, i.e., SrSc0.5Ir0.5O3 and SrCo0.5Ir0.5O3, which allow us to evaluate the structure and activity evolution step by step. The occurrence and order of leaching of Sr (A-site) and Sc/Co (B-site) were controlled by tailoring the thermodynamic stability of B-site. Sr leaching from A-site mainly generates more electrochemical surface area for the reaction, and additional leaching of Sc/Co from B-site triggers the formation of a honeycomb-like IrOxHy phase with a notable increase in intrinsic activity. A thorough surface reconstruction with dual-site metal leaching induces an activity improvement by approximately two orders of magnitude, which makes the reconstructed SrCo0.5Ir0.5O3 among the best for water oxidation in acid.",

author = "Yubo Chen and Yuanmiao Sun and Maoyu Wang and Jingxian Wang and Haiyan Li and Shibo Xi and Chao Wei and Pinxian Xi and Sterbinsky, {George E.} and Freeland, {John W.} and Fisher, {Adrian C.} and Ager, {Joel W.} and Zhenxing Feng and Xu, {Zhichuan J.}",

note = "Publisher Copyright: Copyright {\textcopyright} 2021 The Authors, some rights reserved;",

year = "2021",

month = dec,

doi = "10.1126/sciadv.abk1788",

language = "English",

volume = "7",

journal = "Science advances",

issn = "2375-2548",

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T1 - Lattice site–dependent metal leaching in perovskites toward a honeycomb-like water oxidation catalyst

AU - Chen, Yubo

AU - Sun, Yuanmiao

AU - Wang, Maoyu

AU - Wang, Jingxian

AU - Li, Haiyan

AU - Xi, Shibo

AU - Wei, Chao

AU - Xi, Pinxian

AU - Sterbinsky, George E.

AU - Freeland, John W.

AU - Fisher, Adrian C.

AU - Ager, Joel W.

AU - Feng, Zhenxing

AU - Xu, Zhichuan J.

PY - 2021/12

Y1 - 2021/12

N2 - Metal leaching during water oxidation has been typically observed in conjunction with surface reconstruction on perovskite oxide catalysts, but the role of metal leaching at each geometric site has not been distinguished. Here, we manipulate the occurrence and process of surface reconstruction in two model ABO3 perovskites, i.e., SrSc0.5Ir0.5O3 and SrCo0.5Ir0.5O3, which allow us to evaluate the structure and activity evolution step by step. The occurrence and order of leaching of Sr (A-site) and Sc/Co (B-site) were controlled by tailoring the thermodynamic stability of B-site. Sr leaching from A-site mainly generates more electrochemical surface area for the reaction, and additional leaching of Sc/Co from B-site triggers the formation of a honeycomb-like IrOxHy phase with a notable increase in intrinsic activity. A thorough surface reconstruction with dual-site metal leaching induces an activity improvement by approximately two orders of magnitude, which makes the reconstructed SrCo0.5Ir0.5O3 among the best for water oxidation in acid.

AB - Metal leaching during water oxidation has been typically observed in conjunction with surface reconstruction on perovskite oxide catalysts, but the role of metal leaching at each geometric site has not been distinguished. Here, we manipulate the occurrence and process of surface reconstruction in two model ABO3 perovskites, i.e., SrSc0.5Ir0.5O3 and SrCo0.5Ir0.5O3, which allow us to evaluate the structure and activity evolution step by step. The occurrence and order of leaching of Sr (A-site) and Sc/Co (B-site) were controlled by tailoring the thermodynamic stability of B-site. Sr leaching from A-site mainly generates more electrochemical surface area for the reaction, and additional leaching of Sc/Co from B-site triggers the formation of a honeycomb-like IrOxHy phase with a notable increase in intrinsic activity. A thorough surface reconstruction with dual-site metal leaching induces an activity improvement by approximately two orders of magnitude, which makes the reconstructed SrCo0.5Ir0.5O3 among the best for water oxidation in acid.

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Lattice site–dependent metal leaching in perovskites toward a honeycomb-like water oxidation catalyst

Abstract

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