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

被引：79

作者：

Chen, Yubo ^{[1
,2
]}

Sun, Yuanmiao ^{[1
]}

Wang, Maoyu ^{[3
]}

Wang, Jingxian ^{[1
]}

Li, Haiyan ^{[1
]}

Xi, Shibo ^{[4
]}

Wei, Chao ^{[1
]}

Xi, Pinxian ^{[5
]}

Sterbinsky, George E. ^{[6
]}

Freeland, John W. ^{[6
]}

Fisher, Adrian C. ^{[2
,7
]}

Ager, Joel W. I. I. I. I. I. I. ^{[8
,9
]}

Feng, Zhenxing ^{[3
]}

Xu, Zhichuan J. ^{[1
,2
,10
]}

机构：

[1] Nanyang Technol Univ, Sch Mat Sci & Engn, 50 Nanyang Ave, Singapore 639798, Singapore

[2] Cambridge Ctr Adv Res & Educ Singapore, 1 CREATE Way, Singapore 138602, Singapore

[3] Oregon State Univ, Sch Chem Biol & Environm Engn, Corvallis, OR 97331 USA

[4] ASTAR, Inst Chem & Engn Sci, 1 Pesek Rd, Singapore 627833, Singapore

[5] Lanzhou Univ, Coll Chem & Chem Engn, State Key Lab Appl Organ Chem, Key Lab Nonferrous Met Chem & Resources Utilizat, Lanzhou 730000, Peoples R China

[6] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA

[7] Univ Cambridge, Dept Chem Engn, Cambridge CB2 3RA, England

[8] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA

[9] Berkeley Educ Alliance Res Singapore Ltd, 1 CREATE Way, Singapore 138602, Singapore

[10] Nanyang Technol Univ, Energy Res Inst, 50 Nanyang Ave, Singapore 639798, Singapore

来源：

SCIENCE ADVANCES | 2021年 / 7卷 / 50期

基金：

美国国家科学基金会; 新加坡国家研究基金会;

关键词：

OXYGEN EVOLUTION ELECTROCATALYSIS; HIGHLY-EFFICIENT; SURFACE; OXIDE; STABILITY; REDUCTION; IRIDIUM; KEY; DISSOLUTION; PREDICTION;

D O I：

10.1126/sciadv.abk1788

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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 ABO(3) 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.

引用

页数：13

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