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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.
Original language | English (US) |
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Pages (from-to) | 10294-10301 |
Number of pages | 8 |
Journal | Journal of the American Chemical Society |
Volume | 139 |
Issue number | 30 |
DOIs | |
State | Published - Aug 2 2017 |
Bibliographical note
Publisher Copyright:© 2017 American Chemical Society.
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Dive into the research topics of 'Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal-Organic Framework'. Together they form a unique fingerprint.Projects
- 1 Finished
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Energy Frontier Research Center For Inorganometallic Catalyst Design (DE-SC0012702)
Gagliardi, L., Cramer, C., Lu, C. C., Penn, L., Stein, A. & Truhlar, D. G.
U.S. DEPARTMENT OF ENERGY (USDOE)
8/1/14 → 7/31/18
Project: Research project