Conversion of Methane to Methanol with a Bent Mono(渭-oxo)dinickel Anchored on the Internal Surfaces of Micropores

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• 作者：Junjun Shan ; Weixin Huang ; Luan Nguyen ; Ying Yu ; Shiran Zhang ; Yuanyuan Li ; Anatoly I. Frenkel ; Franklin (Feng) Tao
• 刊名：Langmuir
• 出版年：2014
• 出版时间：July 22, 2014
• 年：2014
• 卷：30
• 期：28
• 页码：8558-8569
• 全文大小：653K
• ISSN：1520-5827

文摘

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(渭-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 O₂. Ni 2p_3/2 of this bent mono(渭-oxo)dinickel species formed on the internal surface of ZSM5 exhibits a unique photoemission feature, which distinguishes the mono(渭-oxo)dinickel from NiO nanoparticles. The formation of the mono(渭-oxo)dinickel species was confirmed with X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS). This mono(渭-oxo)dinickel species is active for the direct oxidation of methane to methanol under the mild condition of a temperature as low as 150 掳C in CH₄ at 1 bar. In-situ studies using UV鈥搗is, XANES, and EXAFS suggest that this bent mono(渭-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.