Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction

Zhe Weng, Yueshen Wu, Maoyu Wang, Jianbing Jiang, Ke Yang, Shengjuan Huo, Xiao-Feng Wang, Qing Ma, Gary W. Brudvig, Victor S. Batista, Yongye Liang (), Zhenxing Feng () and Hailiang Wang ()
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Zhe Weng: South University of Science and Technology of China
Yueshen Wu: Yale University
Maoyu Wang: Oregon State University
Jianbing Jiang: Yale University
Ke Yang: Yale University
Shengjuan Huo: Yale University
Xiao-Feng Wang: University of South China
Qing Ma: Northwestern University
Gary W. Brudvig: Yale University
Victor S. Batista: Yale University
Yongye Liang: South University of Science and Technology of China
Zhenxing Feng: Oregon State University
Hailiang Wang: Yale University

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract 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 ~ 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.

Date: 2018
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DOI: 10.1038/s41467-018-02819-7

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