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Proc Natl Acad Sci U S A. 2018 Mar 20;115(12):2902-2907. doi: 10.1073/pnas.1722137115. Epub 2018 Mar 5.

Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation.

Author information

1
Department of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA 02467.
2
Department of Chemistry, Yale Energy Sciences Institute, Yale University, New Haven, CT 06520.
3
Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany.
4
National Center for Electron Microscopy in Beijing, School of Materials Science and Engineering, Tsinghua University, 100084 Beijing, China.
5
National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, 210093 Nanjing, China.
6
Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093 Nanjing, China.
7
Department of Chemical Engineering and Materials Science, University of California, Irvine, CA 92697.
8
Department of Chemical and Biological Engineering, Tufts University, Medford, MA 02155.
9
Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720.
10
Department of Physics and Astronomy, University of California, Irvine, CA 92697.
11
Department of Chemistry, Yale Energy Sciences Institute, Yale University, New Haven, CT 06520; gary.brudvig@yale.edu victor.batista@yale.edu dwang@bc.edu.
12
Department of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA 02467; gary.brudvig@yale.edu victor.batista@yale.edu dwang@bc.edu.

Abstract

Atomically dispersed catalysts refer to substrate-supported heterogeneous catalysts featuring one or a few active metal atoms that are separated from one another. They represent an important class of materials ranging from single-atom catalysts (SACs) and nanoparticles (NPs). While SACs and NPs have been extensively reported, catalysts featuring a few atoms with well-defined structures are poorly studied. The difficulty in synthesizing such structures has been a critical challenge. Here we report a facile photochemical method that produces catalytic centers consisting of two Ir metal cations, bridged by O and stably bound to a support. Direct evidence unambiguously supporting the dinuclear nature of the catalysts anchored on α-Fe2O3 is obtained by aberration-corrected scanning transmission electron microscopy (AC-STEM). Experimental and computational results further reveal that the threefold hollow binding sites on the OH-terminated surface of α-Fe2O3 anchor the catalysts to provide outstanding stability against detachment or aggregation. The resulting catalysts exhibit high activities toward H2O photooxidation.

KEYWORDS:

STEM; catalyst; solar energy; spectroscopy; water splitting

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