Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework
Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal–organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theor...
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| Published in | Journal of the American Chemical Society Vol. 139; no. 30; pp. 10294 - 10301 |
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| Main Authors | , , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
02.08.2017
American Chemical Society (ACS) |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal–organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theory calculations are used to determine structure/activity relations in the Cu-NU-1000 catalytic system. The Cu-loaded MOF contained Cu-oxo clusters of a few Cu atoms. The Cu was present under ambient conditions as a mixture of ∼15% Cu+ and ∼85% Cu2+. The oxidation of methane on Cu-NU-1000 was accompanied by the reduction of 9% of the Cu in the catalyst from Cu2+ to Cu+. The products, methanol, dimethyl ether, and CO2, were desorbed with the passage of 10% water/He at 135 °C, giving a carbon selectivity for methane to methanol of 45–60%. Cu oxo clusters stabilized in NU-1000 provide an active, first generation MOF-based, selective methane oxidation catalyst. |
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| AbstractList | Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal-organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theory calculations are used to determine structure/activity relations in the Cu-NU-1000 catalytic system. The Cu-loaded MOF contained Cu-oxo clusters of a few Cu atoms. The Cu was present under ambient conditions as a mixture of ∼15% Cu+ and ∼85% Cu2+. The oxidation of methane on Cu-NU-1000 was accompanied by the reduction of 9% of the Cu in the catalyst from Cu2+ to Cu+. The products, methanol, dimethyl ether, and CO2, were desorbed with the passage of 10% water/He at 135 °C, giving a carbon selectivity for methane to methanol of 45-60%. Cu oxo clusters stabilized in NU-1000 provide an active, first generation MOF-based, selective methane oxidation catalyst.Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal-organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theory calculations are used to determine structure/activity relations in the Cu-NU-1000 catalytic system. The Cu-loaded MOF contained Cu-oxo clusters of a few Cu atoms. The Cu was present under ambient conditions as a mixture of ∼15% Cu+ and ∼85% Cu2+. The oxidation of methane on Cu-NU-1000 was accompanied by the reduction of 9% of the Cu in the catalyst from Cu2+ to Cu+. The products, methanol, dimethyl ether, and CO2, were desorbed with the passage of 10% water/He at 135 °C, giving a carbon selectivity for methane to methanol of 45-60%. Cu oxo clusters stabilized in NU-1000 provide an active, first generation MOF-based, selective methane oxidation catalyst. Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal–organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theory calculations are used to determine structure/activity relations in the Cu-NU-1000 catalytic system. The Cu-loaded MOF contained Cu-oxo clusters of a few Cu atoms. The Cu was present under ambient conditions as a mixture of ∼15% Cu+ and ∼85% Cu2+. The oxidation of methane on Cu-NU-1000 was accompanied by the reduction of 9% of the Cu in the catalyst from Cu2+ to Cu+. The products, methanol, dimethyl ether, and CO2, were desorbed with the passage of 10% water/He at 135 °C, giving a carbon selectivity for methane to methanol of 45–60%. Cu oxo clusters stabilized in NU-1000 provide an active, first generation MOF-based, selective methane oxidation catalyst. Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal–organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theory calculations are used to determine structure/activity relations in the Cu-NU-1000 catalytic system. The Cu-loaded MOF contained Cu-oxo clusters of a few Cu atoms. The Cu was present under ambient conditions as a mixture of ∼15% Cu⁺ and ∼85% Cu²⁺. The oxidation of methane on Cu-NU-1000 was accompanied by the reduction of 9% of the Cu in the catalyst from Cu²⁺ to Cu⁺. The products, methanol, dimethyl ether, and CO₂, were desorbed with the passage of 10% water/He at 135 °C, giving a carbon selectivity for methane to methanol of 45–60%. Cu oxo clusters stabilized in NU-1000 provide an active, first generation MOF-based, selective methane oxidation catalyst. Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal-organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theory calculations are used to determine structure/activity relations in the Cu-NU-1000 catalytic system. The Cu-loaded MOF contained Cu-oxo clusters of a few Cu atoms. The Cu was present under ambient conditions as a mixture of ∼15% Cu and ∼85% Cu . The oxidation of methane on Cu-NU-1000 was accompanied by the reduction of 9% of the Cu in the catalyst from Cu to Cu . The products, methanol, dimethyl ether, and CO , were desorbed with the passage of 10% water/He at 135 °C, giving a carbon selectivity for methane to methanol of 45-60%. Cu oxo clusters stabilized in NU-1000 provide an active, first generation MOF-based, selective methane oxidation catalyst. |
| Author | Ray, Debmalya Hupp, Joseph T Pahls, Dale R Farha, Omar K Fulton, John L Camaioni, Donald M Zheng, Jian Sanchez-Sanchez, Maricruz Li, Zhanyong Vjunov, Aleksei Ikuno, Takaaki Gagliardi, Laura Lercher, Johannes A Ortuño, Manuel A Mehdi, B. Layla Cramer, Christopher J Browning, Nigel D |
| AuthorAffiliation | Department of Chemistry Department of Chemistry, Faculty of Science Technische Universität München Materials Science and Engineering Department of Chemistry and Catalysis Research Institute University of Washington Department of Chemistry, Supercomputing Institute, and Chemical Theory Center University of Minnesota Northwestern University Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate Pacific Northwest National Laboratory King Abdulaziz University |
| AuthorAffiliation_xml | – name: Department of Chemistry, Supercomputing Institute, and Chemical Theory Center – name: Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate – name: Department of Chemistry – name: Technische Universität München – name: Pacific Northwest National Laboratory – name: Department of Chemistry, Faculty of Science – name: Materials Science and Engineering – name: Northwestern University – name: University of Minnesota – name: King Abdulaziz University – name: Department of Chemistry and Catalysis Research Institute – name: University of Washington |
| Author_xml | – sequence: 1 givenname: Takaaki surname: Ikuno fullname: Ikuno, Takaaki organization: Technische Universität München – sequence: 2 givenname: Jian orcidid: 0000-0003-2054-9482 surname: Zheng fullname: Zheng, Jian organization: Pacific Northwest National Laboratory – sequence: 3 givenname: Aleksei surname: Vjunov fullname: Vjunov, Aleksei organization: Pacific Northwest National Laboratory – sequence: 4 givenname: Maricruz surname: Sanchez-Sanchez fullname: Sanchez-Sanchez, Maricruz organization: Technische Universität München – sequence: 5 givenname: Manuel A orcidid: 0000-0002-6175-3941 surname: Ortuño fullname: Ortuño, Manuel A organization: University of Minnesota – sequence: 6 givenname: Dale R surname: Pahls fullname: Pahls, Dale R organization: University of Minnesota – sequence: 7 givenname: John L surname: Fulton fullname: Fulton, John L organization: Pacific Northwest National Laboratory – sequence: 8 givenname: Donald M orcidid: 0000-0002-2213-0960 surname: Camaioni fullname: Camaioni, Donald M organization: Pacific Northwest National Laboratory – sequence: 9 givenname: Zhanyong orcidid: 0000-0002-3230-5955 surname: Li fullname: Li, Zhanyong organization: Northwestern University – sequence: 10 givenname: Debmalya surname: Ray fullname: Ray, Debmalya organization: University of Minnesota – sequence: 11 givenname: B. Layla surname: Mehdi fullname: Mehdi, B. Layla organization: Pacific Northwest National Laboratory – sequence: 12 givenname: Nigel D surname: Browning fullname: Browning, Nigel D organization: University of Washington – sequence: 13 givenname: Omar K orcidid: 0000-0002-9904-9845 surname: Farha fullname: Farha, Omar K organization: King Abdulaziz University – sequence: 14 givenname: Joseph T orcidid: 0000-0003-3982-9812 surname: Hupp fullname: Hupp, Joseph T organization: Northwestern University – sequence: 15 givenname: Christopher J orcidid: 0000-0001-5048-1859 surname: Cramer fullname: Cramer, Christopher J organization: University of Minnesota – sequence: 16 givenname: Laura orcidid: 0000-0001-5227-1396 surname: Gagliardi fullname: Gagliardi, Laura organization: University of Minnesota – sequence: 17 givenname: Johannes A orcidid: 0000-0002-2495-1404 surname: Lercher fullname: Lercher, Johannes A email: johannes.lercher@pnnl.gov, johannes.lercher@ch.tum.de organization: Pacific Northwest National Laboratory |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/28613861$$D View this record in MEDLINE/PubMed https://www.osti.gov/biblio/1375358$$D View this record in Osti.gov |
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| Snippet | Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal–organic framework (MOF) NU-1000 are active for oxidation of methane to... Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal-organic framework (MOF) NU-1000 are active for oxidation of methane to... |
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| SubjectTerms | carbon carbon dioxide catalysts coordination polymers cupric oxide density functional theory methane methanol oxidation X-ray absorption spectroscopy |
| Title | Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework |
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