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 language | English |
|---|---|
| Article number | 415 |
| Journal | Nature Communications |
| Volume | 9 |
| Issue number | 1 |
| DOIs | |
| Publication status | Published - 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
Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction. / 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.
In: Nature Communications, Vol. 9, No. 1, 415, 01.12.2018.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction
AU - Weng, Zhe
AU - Wu, Yueshen
AU - Wang, Maoyu
AU - Jiang, Jianbing
AU - Yang, Ke
AU - Huo, Shengjuan
AU - Wang, Xiao Feng
AU - Ma, Qing
AU - Brudvig, Gary W
AU - Batista, Victor S.
AU - Liang, Yongye
AU - Feng, Zhenxing
AU - Wang, Hailiang
PY - 2018/12/1
Y1 - 2018/12/1
N2 - 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.
AB - 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.
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U2 - 10.1038/s41467-018-02819-7
DO - 10.1038/s41467-018-02819-7
M3 - Article
VL - 9
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
IS - 1
M1 - 415
ER -