@article{103f841fde644adbb99bc05b5b63d8e7,
title = "Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation",
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 = "Catalyst, STEM, Solar energy, Spectroscopy, Water splitting",
author = "Yanyan Zhao and Yang, {Ke R.} and Zechao Wang and Xingxu Yan and Sufeng Cao and Yifan Ye and Qi Dong and Xizi Zhang and Thorne, {James E.} and Lei Jin and Materna, {Kelly L.} and Antonios Trimpalis and Hongye Bai and Fakra, {Sirine C.} and Xiaoyan Zhong and Peng Wang and Xiaoqing Pan and Jinghua Guo and Maria Flytzani-Stephanopoulos and Brudvig, {Gary W.} and Batista, {Victor S.} and Dunwei Wang",
note = "Funding Information: ACKNOWLEDGMENTS. We thank Dr. Xiahui Yao for support during the acquisition of XPS data and helping draw the schematic figure, and Wei Li and Da He for assistance with PEC data analysis. We thank Dr. Stafford W. Sheehan and Dr. Song Li for discussions. We also thank Dongsheng Song and Shucheng Yu for STEM data analysis discussions. X.Y. and X.P. thank the support of the University of California, Irvine Materials Research Institute for the use of TEM facilities. Work done at Boston College was in part supported by the National Science Foundation (DMR 1055762) for materials synthesis and photoelectrochemical studies; precursor synthesis and theoretical computations at Yale University were supported by the Argonne-Northwestern Solar Energy Research Center, an Energy Frontier Research Center funded by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), under Award DE-SC0001059. HAADF-STEM work was supported by the National Key Research and Development Program (2016YFB0700402), DOE, BES, Division of Materials Science and Engineering, under Grant DE-SC0014430, the National Basic Research Program of China (Grant 2015CB654901), the National Natural Science Foundation of China (11474147), the Natural Science Foundation of Jiangsu Province (Grant BK20151383), and the Fundamental Research Funds for the Central Universities (021314380077). In situ DRIFTS studies are supported by the DOE under Award DE-FG02-05ER15730. The Advanced Light Source is supported by the Director, Office of Science, DOE, BES, under Contract DE-AC02-05CH11231.",
year = "2018",
month = mar,
day = "20",
doi = "10.1073/pnas.1722137115",
language = "English",
volume = "115",
pages = "2902--2907",
journal = "Proceedings of the National Academy of Sciences of the United States of America",
issn = "0027-8424",
publisher = "National Academy of Sciences",
number = "12",
}