Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction
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 t...
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| Published in | Nature communications Vol. 9; no. 1; pp. 415 - 9 |
|---|---|
| Main Authors | , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
29.01.2018
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
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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 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.
The catalytic conversion of carbon dioxide into value-added products requires an understanding of the active species present under working conditions. Here, the authors discover copper-containing complexes to reversibly transform during electrocatalysis into methane-producing copper nanoclusters. |
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| AbstractList | 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.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. 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. The catalytic conversion of carbon dioxide into value-added products requires an understanding of the active species present under working conditions. Here, the authors discover copper-containing complexes to reversibly transform during electrocatalysis into methane-producing copper nanoclusters. 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. 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.The catalytic conversion of carbon dioxide into value-added products requires an understanding of the active species present under working conditions. Here, the authors discover copper-containing complexes to reversibly transform during electrocatalysis into methane-producing copper nanoclusters. 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. 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 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. The catalytic conversion of carbon dioxide into value-added products requires an understanding of the active species present under working conditions. Here, the authors discover copper-containing complexes to reversibly transform during electrocatalysis into methane-producing copper nanoclusters. 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. |
| ArticleNumber | 415 |
| Author | Feng, Zhenxing Wang, Maoyu Liang, Yongye Wang, Hailiang Jiang, Jianbing Ma, Qing Wang, Xiao-Feng Brudvig, Gary W. Huo, Shengjuan Yang, Ke Batista, Victor S. Weng, Zhe Wu, Yueshen |
| Author_xml | – sequence: 1 givenname: Zhe orcidid: 0000-0002-6005-9552 surname: Weng fullname: Weng, Zhe organization: Department of Materials Science and Engineering, South University of Science and Technology of China, Department of Chemistry, Yale University, Energy Sciences Institute, Yale University – sequence: 2 givenname: Yueshen surname: Wu fullname: Wu, Yueshen organization: Department of Chemistry, Yale University, Energy Sciences Institute, Yale University – sequence: 3 givenname: Maoyu surname: Wang fullname: Wang, Maoyu organization: School of Chemical, Biological, and Environmental Engineering, Oregon State University – sequence: 4 givenname: Jianbing surname: Jiang fullname: Jiang, Jianbing organization: Department of Chemistry, Yale University, Energy Sciences Institute, Yale University – sequence: 5 givenname: Ke surname: Yang fullname: Yang, Ke organization: Department of Chemistry, Yale University, Energy Sciences Institute, Yale University – sequence: 6 givenname: Shengjuan surname: Huo fullname: Huo, Shengjuan organization: Department of Chemistry, Yale University, Energy Sciences Institute, Yale University, Department of Chemistry, Science Colleges, Shanghai University – sequence: 7 givenname: Xiao-Feng surname: Wang fullname: Wang, Xiao-Feng organization: School of Chemistry and Chemical Engineering, University of South China – sequence: 8 givenname: Qing surname: Ma fullname: Ma, Qing organization: DND-CAT, Synchrotron Research Center, Northwestern University – sequence: 9 givenname: Gary W. surname: Brudvig fullname: Brudvig, Gary W. organization: Department of Chemistry, Yale University, Energy Sciences Institute, Yale University – sequence: 10 givenname: Victor S. surname: Batista fullname: Batista, Victor S. organization: Department of Chemistry, Yale University, Energy Sciences Institute, Yale University – sequence: 11 givenname: Yongye surname: Liang fullname: Liang, Yongye email: liangyy@sustc.edu.cn organization: Department of Materials Science and Engineering, South University of Science and Technology of China – sequence: 12 givenname: Zhenxing surname: Feng fullname: Feng, Zhenxing email: zhenxing.feng@oregonstate.edu organization: School of Chemical, Biological, and Environmental Engineering, Oregon State University – sequence: 13 givenname: Hailiang orcidid: 0000-0003-4409-2034 surname: Wang fullname: Wang, Hailiang email: hailiang.wang@yale.edu organization: Department of Chemistry, Yale University, Energy Sciences Institute, Yale University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/29379087$$D View this record in MEDLINE/PubMed https://www.osti.gov/servlets/purl/1419868$$D View this record in Osti.gov |
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| ContentType | Journal Article |
| Copyright | The Author(s) 2018 2018. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License. The Author(s) 2018. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License. |
| Copyright_xml | – notice: The Author(s) 2018 – notice: 2018. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License. – notice: The Author(s) 2018. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License. |
| CorporateAuthor | Yale Univ., New Haven, CT (United States) Argonne National Laboratory (ANL), Argonne, IL (United States) |
| CorporateAuthor_xml | – name: Argonne National Laboratory (ANL), Argonne, IL (United States) – name: Yale Univ., New Haven, CT (United States) |
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| Snippet | Restructuring-induced catalytic activity is an intriguing phenomenon of fundamental importance to rational design of high-performance catalyst materials. We... The catalytic conversion of carbon dioxide into value-added products requires an understanding of the active species present under working conditions. Here,... |
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| SubjectTerms | 119/118 147/135 639/301/299/886 639/638/298 639/638/77/886 Absorption spectroscopy Carbon dioxide Catalysis Catalysts Catalytic activity Catalytic converters Clusters Conversion Coordination compounds Copper Copper compounds Copper converters Electrochemistry Humanities and Social Sciences Hydrogen storage INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY MATERIALS SCIENCE Metal ions Metal phthalocyanines Methane Molecular structure multidisciplinary Nanoclusters Oxidation Science Science (multidisciplinary) Valence Working conditions X ray absorption X-ray absorption spectroscopy |
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| Title | Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction |
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