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. 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.

Authors:

Zhao, Yanyan ^[1]; Yang, Ke R. ^[2]; Wang, Zechao ^[3]; Yan, Xingxu ^[4]; Cao, Sufeng ^[5]; Ye, Yifan ^[6]; Dong, Qi ^[1]; Zhang, Xizi ^[1]; Thorne, James E. ^[1]; Jin, Lei ^[7]; Materna, Kelly L. ^[2]; Trimpalis, Antonios ^[5]; Bai, Hongye ^[1]; Fakra, Sirine C. ^[6]; Zhong, Xiaoyan ^[8]; Wang, Peng  ^[9];

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Pan, Xiaoqing ^[10]; Guo, Jinghua ^[6]; Flytzani-Stephanopoulos, Maria ^[5]; Brudvig, Gary W. ^[2] more »; Batista, Victor S. ^[2]; Wang, Dunwei  ^[1]

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+ Show Author Affiliations

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,, National Center for Electron Microscopy in Beijing, School of Materials Science and Engineering, Tsinghua University, 100084 Beijing, China,
4. National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, 210093 Nanjing, China,, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093 Nanjing, China,, Department of Chemical Engineering and Materials Science, University of California, Irvine, CA 92697,
5. Department of Chemical and Biological Engineering, Tufts University, Medford, MA 02155,
6. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,
7. Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany,
8. National Center for Electron Microscopy in Beijing, School of Materials Science and Engineering, Tsinghua University, 100084 Beijing, China,
9. National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, 210093 Nanjing, China,, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093 Nanjing, China,
10. Department of Chemical Engineering and Materials Science, University of California, Irvine, CA 92697,, Department of Physics and Astronomy, University of California, Irvine, CA 92697

Publication Date:

2018-03-05

Research Org.:

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Key Research and Development Program (China); National Basic Research Program of China; National Natural Science Foundation of China (NSFC); Natural Science Foundation of Jiangsu Province (China); Fundamental Research Funds for the Central Universities (China)

OSTI Identifier:

1423731

Alternate Identifier(s):

OSTI ID: 1506300

Grant/Contract Number:  

SC0001059; SC0024430; AC02-05CH11231; SC0014430; FG02-05ER15730; DMR 1055762; 2016YFB0700402; 2015CB654901; 11474147; BK20151383; 021314380077

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 115 Journal Issue: 12; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalyst; water splitting; solar energy; STEM; spectroscopy