Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 115, Issue 12, Pages 2902-2907Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1722137115
Keywords
catalyst; water splitting; solar energy; STEM; spectroscopy
Categories
Funding
- Argonne-Northwestern Solar Energy Research Center, an Energy Frontier Research Center - US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) [DE-SC0001059]
- National Key Research and Development Program [2016YFB0700402]
- DOE, BES, Division of Materials Science and Engineering [DE-SC0014430]
- National Basic Research Program of China [2015CB654901]
- National Natural Science Foundation of China [11474147]
- Natural Science Foundation of Jiangsu Province [BK20151383]
- Fundamental Research Funds for the Central Universities [021314380077]
- DOE [DE-FG02-05ER15730]
- Office of Science, DOE, BES [DE-AC02-05CH11231]
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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 alpha-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 alpha-Fe2O3 anchor the catalysts to provide outstanding stability against detachment or aggregation. The resulting catalysts exhibit high activities toward H2O photooxidation.
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