TY - JOUR
T1 - Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal-Organic Framework
AU - Ikuno, Takaaki
AU - Zheng, Jian
AU - Vjunov, Aleksei
AU - Sanchez-Sanchez, Maricruz
AU - Ortuño, Manuel A.
AU - Pahls, Dale R.
AU - Fulton, John L.
AU - Camaioni, Donald M.
AU - Li, Zhanyong
AU - Ray, Debmalya
AU - Mehdi, B. Layla
AU - Browning, Nigel D.
AU - Farha, Omar K.
AU - Hupp, Joseph T.
AU - Cramer, Christopher J.
AU - Gagliardi, Laura
AU - Lercher, Johannes A.
N1 - Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/8/2
Y1 - 2017/8/2
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85026744879&partnerID=8YFLogxK
U2 - 10.1021/jacs.7b02936
DO - 10.1021/jacs.7b02936
M3 - Article
C2 - 28613861
AN - SCOPUS:85026744879
SN - 0002-7863
VL - 139
SP - 10294
EP - 10301
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 30
ER -