Journal
LANGMUIR
Volume 30, Issue 28, Pages 8558-8569Publisher
AMER CHEMICAL SOC
DOI: 10.1021/la501184b
Keywords
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Funding
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy [DE-FG02-12ER16353]
- U.S. Department of Energy [DE-FG02-03ER15476]
- Synchrotron Catalysis Consortium, U.S. Department of Energy [DE-FG02-05ER15688]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1126374] Funding Source: National Science Foundation
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The oxidation of methane to methanol is a pathway to utilizing this relatively abundant, inexpensive energy resource. Here we report a new catalyst, bent mono(mu-oxo)dinickel anchored on an internal surface of micropores,which is active for direct oxidation. It is synthesized from the direct loading of a nickel precursor to the internal surface of micropores of ZSM5 following activation in O-2. Ni 2p(3/2) of this bent mono(mu-oxo)dinickel species formed on the internal surface of ZSMS exhibits a unique photoemission feature, which distinguishes the mono(mu-oxo)dinickel from NiO nanoparticles. The formation of the mono(mu-oxo)dinickel species was confirmed with X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS). This mono(mu-oxo)dinickel species is active for the direct oxidation of methane to methanol under the mild condition of a temperature as low as 150 degrees C in CH4 at 1 bar. In-situ studies using UV-vis, XANES, and EXAFS suggest that this bent mono(mu-oxo)dinickel species is the active site for the direct oxidation of methane to methanol. The energy barrier of this direct oxidation of methane is 83.2 kJ/mol.
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