催化作用
材料科学
原位
甲烷
氧化物
过渡金属
离解(化学)
甲醇
化学
碳氢化合物
化学工程
甲烷厌氧氧化
金属
无机化学
物理化学
有机化学
工程类
作者
J. A. Rodriguez,F. Zhang,Z. Liu,S. D. Senanayake
出处
期刊:Catalysis
日期:2019-02-12
被引量:1
标识
DOI:10.1039/9781788016971-00198
摘要
Research focussed on in situ studies for the activation and conversion of methane on well-defined metal-oxide surfaces is reviewed. In recent years, experiments with single-crystal surfaces and well-ordered films have increased our understanding of the interaction of methane with solid surfaces. Late transition metals interact weakly with methane and elevated temperatures (>400 K) are necessary to enable a significant dissociation on the hydrocarbon. In contrast, an IrO2(110) surface dissociates methane at temperatures below 200 K. Cooperative interactions between O and Ir are responsible for the binding of methane and the breaking of a C–H bond. This type of cooperative interactions involving O and a metal cation have also been seen on Ni/CeO2(111) and Co/CeO2(111) surfaces which dissociate methane at room temperature. Experiments of AP-XPS and in situ TR-XRD have shown that the active phase of metal/oxide catalysts used for the dry-reforming of methane frequently is a dynamic entity which evolves when the reaction conditions change. The addition of water to a mixture of CH4/O2 shifts the selectivity towards methanol production on CeO2/CuOx/Cu(111) and Ni/CeO2(111) surfaces. Metal-support interactions and water site-blocking play a crucial role in the conversion of methane to methanol on these catalysts.
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