4.8 Article

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

Journal

SCIENCE ADVANCES
Volume 7, Issue 50, Pages -

Publisher

AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.abk1788

Keywords

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Funding

  1. Singapore MOE [MOE2018-T2-2-027, 2019-T1-002-125]
  2. Singapore National Research Foundation under its Campus for Research Excellence And Technological Enterprise (CREATE) program, through the Singapore Berkeley Research Initiative for Sustainable Energy (SinBeRISE)
  3. Cambridge Center for Carbon Reduction in Chemical Technology (C4T)
  4. Oregon State University
  5. National Science Foundation [NNCI-2025489]
  6. DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357]
  7. eCO2EP program

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By manipulating the leaching of Sr and Sc/Co from different geometric sites, this study demonstrates that dual-site metal leaching induced surface reconstruction can significantly enhance the water oxidation activity of perovskite oxide catalysts.
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.

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