Journal
NATURE COMMUNICATIONS
Volume 9, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-018-02819-7
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Funding
- National Science Foundation [CHE-1651717]
- ACS Petroleum Research Fund
- Global Innovation Initiative from Institute of International Education
- Callahan Faculty Scholar Endowment Fund from Oregon State University
- U.S. Department of Energy, Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science [DEFG02-07ER15909]
- TomKat Foundation
- Air Force Office of Scientific Research grant [FA9550-13-1-0020]
- Shenzhen Fundamental Research Funding [JCYJ20160608140827794]
- Peacock Plan [KQTD20140630160825828]
- E. I. duPont de Nemours Co.
- Northwestern University
- Dow Chemical Company
- DOE [DE-AC02-06CH11357]
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Restructuring-induced catalytic activity is an intriguing phenomenon of fundamental importance to rational design of high-performance catalyst materials. We study three copper-complex materials for electrocatalytic carbon dioxide reduction. Among them, the copper(II) phthalocyanine exhibits by far the highest activity for yielding methane with a Faradaic efficiency of 66% and a partial current density of 13 mA cm(-2) at the potential of -1.06 V versus the reversible hydrogen electrode. Utilizing in-situ and operando X-ray absorption spectroscopy, we find that under the working conditions copper(II) phthalocyanine undergoes reversible structural and oxidation state changes to form similar to 2 nm metallic copper clusters, which catalyzes the carbon dioxide-to-methane conversion. Density functional calculations rationalize the restructuring behavior and attribute the reversibility to the strong divalent metal ion-ligand coordination in the copper(II) phthalocyanine molecular structure and the small size of the generated copper clusters under the reaction conditions.
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