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-Fe 2 O 3 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-Fe 2 O 3 anchor the catalysts to provide outstanding stability against detachment or aggregation. The resulting catalysts exhibit high activities toward H 2 O photooxidation.
- Authors:
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- Publication Date:
- 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 (NNSFC); 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
Citation Formats
Zhao, Yanyan, Yang, Ke R., Wang, Zechao, Yan, Xingxu, Cao, Sufeng, Ye, Yifan, Dong, Qi, Zhang, Xizi, Thorne, James E., Jin, Lei, Materna, Kelly L., Trimpalis, Antonios, Bai, Hongye, Fakra, Sirine C., Zhong, Xiaoyan, Wang, Peng, Pan, Xiaoqing, Guo, Jinghua, Flytzani-Stephanopoulos, Maria, Brudvig, Gary W., Batista, Victor S., and Wang, Dunwei. Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation. United States: N. p., 2018.
Web. doi:10.1073/pnas.1722137115.
Zhao, Yanyan, Yang, Ke R., Wang, Zechao, Yan, Xingxu, Cao, Sufeng, Ye, Yifan, Dong, Qi, Zhang, Xizi, Thorne, James E., Jin, Lei, Materna, Kelly L., Trimpalis, Antonios, Bai, Hongye, Fakra, Sirine C., Zhong, Xiaoyan, Wang, Peng, Pan, Xiaoqing, Guo, Jinghua, Flytzani-Stephanopoulos, Maria, Brudvig, Gary W., Batista, Victor S., & Wang, Dunwei. Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation. United States. doi:10.1073/pnas.1722137115.
Zhao, Yanyan, Yang, Ke R., Wang, Zechao, Yan, Xingxu, Cao, Sufeng, Ye, Yifan, Dong, Qi, Zhang, Xizi, Thorne, James E., Jin, Lei, Materna, Kelly L., Trimpalis, Antonios, Bai, Hongye, Fakra, Sirine C., Zhong, Xiaoyan, Wang, Peng, Pan, Xiaoqing, Guo, Jinghua, Flytzani-Stephanopoulos, Maria, Brudvig, Gary W., Batista, Victor S., and Wang, Dunwei. Mon .
"Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation". United States. doi:10.1073/pnas.1722137115.
@article{osti_1423731,
title = {Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation},
author = {Zhao, Yanyan and Yang, Ke R. and Wang, Zechao and Yan, Xingxu and Cao, Sufeng and Ye, Yifan and Dong, Qi and Zhang, Xizi and Thorne, James E. and Jin, Lei and Materna, Kelly L. and Trimpalis, Antonios and Bai, Hongye and Fakra, Sirine C. and Zhong, Xiaoyan and Wang, Peng and Pan, Xiaoqing and Guo, Jinghua and Flytzani-Stephanopoulos, Maria and Brudvig, Gary W. and Batista, Victor S. and Wang, Dunwei},
abstractNote = {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-Fe 2 O 3 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-Fe 2 O 3 anchor the catalysts to provide outstanding stability against detachment or aggregation. The resulting catalysts exhibit high activities toward H 2 O photooxidation.},
doi = {10.1073/pnas.1722137115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 12,
volume = 115,
place = {United States},
year = {2018},
month = {3}
}
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DOI: 10.1073/pnas.1722137115
DOI: 10.1073/pnas.1722137115
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Cited by: 14 works
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Figures / Tables:
Fig. 1: Synthesis procedure of Ir DHC. It starts with the immobilization of molecular Ir catalysts, followed by photochemical removal of organic ligands. The binding details of H2O and OH groups are proposed.
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