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, Hailiang Wang

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Abstract

Restructuring-induced catalytic activity is an intriguing phenomenon of fundamental importance to rational design of high-performance catalyst materials. We study three coppercomplex 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 cm2 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.

Original languageEnglish
Article number415
JournalNature Communications
Volume9
Issue number1
DOIs
Publication statusPublished - Dec 1 2018

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ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Cite this

Weng, Z., Wu, Y., Wang, M., Jiang, J., Yang, K., Huo, S., Wang, X. F., Ma, Q., Brudvig, G. W., Batista, V. S., Liang, Y., Feng, Z., & Wang, H. (2018). Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction. Nature Communications, 9(1), [415]. https://doi.org/10.1038/s41467-018-02819-7