Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts

Author:

Zhao Yanyan1,Dai Sheng2ORCID,Yang Ke R.3ORCID,Cao Sufeng14,Materna Kelly L.3,Lant Hannah M. C.3,Kao Li Cheng5,Feng Xuefei5,Guo Jinghua5ORCID,Brudvig Gary W.3ORCID,Flytzani-Stephanopoulos Maria4,Batista Victor S.3ORCID,Pan Xiaoqing2,Wang Dunwei1ORCID

Affiliation:

1. Department of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA 02467

2. Department of Physics and Astronomy, University of California–Irvine, Irvine, CA 92697

3. Yale Energy Sciences Institute and Department of Chemistry, Yale University, New Haven, CT 06520

4. Department of Chemical and Biological Engineering, Tufts University, Medford, MA 02155

5. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720

Abstract

Atomically dispersed catalysts have been shown highly active for preferential oxidation of carbon monoxide in the presence of excess hydrogen (PROX). However, their stability has been less than ideal. We show here that the introduction of a structural component to minimize diffusion of the active metal center can greatly improve the stability without compromising the activity. Using an Ir dinuclear heterogeneous catalyst (DHC) as a study platform, we identify two types of oxygen species, interfacial and bridge, that work in concert to enable both activity and stability. The work sheds important light on the synergistic effect between the active metal center and the supporting substrate and may find broad applications for the use of atomically dispersed catalysts.

Funder

NSF | MPS | Division of Chemistry

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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