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Weng, Zhe; Wu, Yueshen; Wang, Maoyu; Jiang, Jianbing; Yang, Ke; Huo, Shengjuan; Wang, Xiao-Feng; Ma, Qing; Brudvig, Gary W; Batista, Victor S; Liang, Yongye; Feng, Zhenxing; Wang, Hailiang
Nature communications, 01/2018, Volume: 9, Issue: 1Journal Article
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 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.
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