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Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction
Open accessAbstract
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.
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Cites
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Enhanced Electrochemical Methanation of Carbon Dioxide with a Dispersible Nanoscale Copper Catalyst
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Highly Dense Cu Nanowires for Low-Overpotential CO 2 Reduction
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Metal/Oxide Interface Nanostructures Generated by Surface Segregation for Electrocatalysis
Weng, Z., Liu, W., Yin, L.-C., Fang, R., Li, M., Altman, E. I., Fan, Q., Li, F., Cheng, H.-M., & Wang, H. (2015) · Nano Letters · doi:10.1021/acs.nanolett.5b03709 · Cited by 278
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Cited by
Bavykina, A., Kolobov, N., Khan, I. S., Bau, J. A., Ramirez, A., & Gascon, J. (2020) · Chemical Reviews · doi:10.1021/acs.chemrev.9b00685 · Cited by 1,754
Designing materials for electrochemical carbon dioxide recycling
Ross, M. B., De Luna, P., Li, Y., Dinh, C.-T., Kim, D., Yang, P., & Sargent, E. H. (2019) · Nature Catalysis · doi:10.1038/s41929-019-0306-7 · Cited by 1,302
Cao, L., Luo, Q., Liu, W., Lin, Y., Liu, X., Cao, Y., Zhang, W., Wu, Y., Yang, J., Yao, T., et al. (2018) · Nature Catalysis · doi:10.1038/s41929-018-0203-5 · Cited by 901
Self-citationLarge-Scale and Highly Selective CO2 Electrocatalytic Reduction on Nickel Single-Atom Catalyst
Zheng, T., Jiang, K., Ta, N., Hu, Y., Zeng, J., Liu, J., & Wang, H. (2019) · Joule · doi:10.1016/j.joule.2018.10.015 · Cited by 887
Self-citationLi, P., Wang, M., Duan, X., Zheng, L., Cheng, X., Zhang, Y., Kuang, Y., Li, Y., Ma, Q., Feng, Z., et al. (2019) · Nature Communications · doi:10.1038/s41467-019-09666-0 · Cited by 717
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Metadata
- Authors
- 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.
- Venue
- Nature Communications
- Published
- 2018-01-29
- Volume
- 9
- Issue
- 1
- Pages
- 415-415
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W2798038136
- Cited by
- 735
- References
- 6
- FWCI
- 17.42
- Type
- journal article
- Language
- en
- Open access
- gold
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