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

Yanyan Zhao, Ke R. Yang, Zechao Wang, Xingxu Yan, Sufeng Cao, Yifan Ye, Qi Dong, Xizi Zhang, James E. Thorne, Lei Jin, Kelly L. Materna, Antonios Trimpalis, Hongye Bai, Sirine C. Fakra, Xiaoyan Zhong, Peng Wang, Xiaoqing Pan, Jinghua Guo, Maria Flytzani-Stephanopoulos, Gary W. Brudvig, Victor S. Batista and Dunwei Wang
PNAS March 5, 2018. 201722137; published ahead of print March 5, 2018. https://doi.org/10.1073/pnas.1722137115
Yanyan Zhao
aDepartment of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA 02467;
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Ke R. Yang
bDepartment of Chemistry, Yale Energy Sciences Institute, Yale University, New Haven, CT 06520;
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Zechao Wang
cErnst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany;dNational Center for Electron Microscopy in Beijing, School of Materials Science and Engineering, Tsinghua University, 100084 Beijing, China;
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Xingxu Yan
eNational Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, 210093 Nanjing, China;fCollaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093 Nanjing, China;gDepartment of Chemical Engineering and Materials Science, University of California, Irvine, CA 92697;
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Sufeng Cao
hDepartment of Chemical and Biological Engineering, Tufts University, Medford, MA 02155;
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Yifan Ye
iAdvanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Qi Dong
aDepartment of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA 02467;
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Xizi Zhang
aDepartment of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA 02467;
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James E. Thorne
aDepartment of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA 02467;
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Lei Jin
cErnst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany;
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Kelly L. Materna
bDepartment of Chemistry, Yale Energy Sciences Institute, Yale University, New Haven, CT 06520;
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Antonios Trimpalis
hDepartment of Chemical and Biological Engineering, Tufts University, Medford, MA 02155;
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Hongye Bai
aDepartment of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA 02467;
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Sirine C. Fakra
iAdvanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Xiaoyan Zhong
dNational Center for Electron Microscopy in Beijing, School of Materials Science and Engineering, Tsinghua University, 100084 Beijing, China;
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Peng Wang
eNational Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, 210093 Nanjing, China;fCollaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093 Nanjing, China;
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  • ORCID record for Peng Wang
Xiaoqing Pan
gDepartment of Chemical Engineering and Materials Science, University of California, Irvine, CA 92697;jDepartment of Physics and Astronomy, University of California, Irvine, CA 92697
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Jinghua Guo
iAdvanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Maria Flytzani-Stephanopoulos
hDepartment of Chemical and Biological Engineering, Tufts University, Medford, MA 02155;
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Gary W. Brudvig
bDepartment of Chemistry, Yale Energy Sciences Institute, Yale University, New Haven, CT 06520;
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  • For correspondence: gary.brudvig@yale.eduvictor.batista@yale.edudwang@bc.edu
Victor S. Batista
bDepartment of Chemistry, Yale Energy Sciences Institute, Yale University, New Haven, CT 06520;
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  • For correspondence: gary.brudvig@yale.eduvictor.batista@yale.edudwang@bc.edu
Dunwei Wang
aDepartment of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA 02467;
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  • ORCID record for Dunwei Wang
  • For correspondence: gary.brudvig@yale.eduvictor.batista@yale.edudwang@bc.edu
  1. Edited by Alexis T. Bell, University of California, Berkeley, CA, and approved February 13, 2018 (received for review December 20, 2017)

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Significance

While research on single-atom catalysts (SACs) is arguably mature, rare work has been done on atomically dispersed catalyst featuring two atoms. We synthesized Ir dinuclear heterogeneous catalyst in a facile photochemical way. It exhibits outstanding stability and high activity toward water oxidation. The significance of this work can also be appreciated from the catalysis perspective. A grand challenge in heterogeneous catalysis is how to understand the detailed mechanisms at the molecular level, because the most active heterogeneous catalysts are often poorly defined in their atomic structures. Our finding is built upon recent advances aimed at studying SACs but takes a crucial step forward. It provides a material platform to study reactions that would require more than one active site.

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.

  • catalyst
  • water splitting
  • solar energy
  • STEM
  • spectroscopy

Footnotes

  • ↵1Y.Z. and K.R.Y. contributed equally to this work.

  • ↵2Z.W., X.Y., S.C., and Y.Y. contributed equally to this work.

  • ↵3To whom correspondence may be addressed. Email: gary.brudvig{at}yale.edu, victor.batista{at}yale.edu, or dwang{at}bc.edu.
  • Author contributions: Y.Z. and D.W. designed research; Y.Z., K.R.Y., Z.W., X.Y., S.C., Y.Y., Q.D., X. Zhang, J.E.T., L.J., K.L.M., A.T., H.B., S.C.F., X. Zhong, P.W., X.P., J.G., M.F.-S., G.W.B., and V.S.B. performed research; X.Z., P.W., and X.P. supervised the HAADF-STEM efforts; M.F.-S. supervised DRIFTS experiments; Y.Z., K.R.Y., Z.W., X.Y., L.J., X.P., J.G., M.F.-S., G.W.B., V.S.B., and D.W. analyzed data; and Y.Z. and D.W. wrote the paper with comments from all authors.

  • The authors declare no conflict of interest.

  • This article is a PNAS Direct Submission.

  • This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1722137115/-/DCSupplemental.

Published under the PNAS license.

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Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation
Yanyan Zhao, Ke R. Yang, Zechao Wang, Xingxu Yan, Sufeng Cao, Yifan Ye, Qi Dong, Xizi Zhang, James E. Thorne, Lei Jin, Kelly L. Materna, Antonios Trimpalis, Hongye Bai, Sirine C. Fakra, Xiaoyan Zhong, Peng Wang, Xiaoqing Pan, Jinghua Guo, Maria Flytzani-Stephanopoulos, Gary W. Brudvig, Victor S. Batista, Dunwei Wang
Proceedings of the National Academy of Sciences Mar 2018, 201722137; DOI: 10.1073/pnas.1722137115

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Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation
Yanyan Zhao, Ke R. Yang, Zechao Wang, Xingxu Yan, Sufeng Cao, Yifan Ye, Qi Dong, Xizi Zhang, James E. Thorne, Lei Jin, Kelly L. Materna, Antonios Trimpalis, Hongye Bai, Sirine C. Fakra, Xiaoyan Zhong, Peng Wang, Xiaoqing Pan, Jinghua Guo, Maria Flytzani-Stephanopoulos, Gary W. Brudvig, Victor S. Batista, Dunwei Wang
Proceedings of the National Academy of Sciences Mar 2018, 201722137; DOI: 10.1073/pnas.1722137115
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