Department of Chemistry, Joseph Black Building, University of Glasgow, Glasgow, G12 8QQ, Scotland, UK.
Phys Chem Chem Phys. 2010 Apr 7;12(13):3102-7. doi: 10.1039/b919977b. Epub 2010 Feb 24.
An alumina-supported nickel catalyst has been used to effect the 'dry' reforming of methane, using CO(2) as the oxidant. After 6 hours on-stream, reaction was stopped and the sample analysed by inelastic neutron scattering (INS). The INS spectrum reveals the presence of hydrocarbonaceous species as well as hydroxyl species present at the catalyst surface. Through the use of appropriate reference compounds, calibration procedures have been developed to determine the concentration of the retained hydrocarbon and hydroxyl moieties. Ancillary temperature programmed oxidation experiments establish the total carbon content. This approach not only enables the extent of overall carbon laydown to be determined but it also identifies the degree to which hydrogen is associated with carbon and oxygen atoms. The methodology described is generic and should be applicable to a wide number of heterogeneously catalysed systems.
一种氧化铝负载的镍催化剂已被用于在二氧化碳作为氧化剂的条件下实现甲烷的“干重整”。在连续运行 6 小时后,停止反应并通过非弹性中子散射(INS)对样品进行分析。INS 光谱揭示了在催化剂表面存在烃类物质以及羟基物质。通过使用适当的参考化合物,已经开发出校准程序来确定保留的烃和羟基部分的浓度。辅助的程序升温氧化实验确定了总碳含量。这种方法不仅能够确定总的碳沉积程度,还能够确定氢与碳原子和氧原子结合的程度。所描述的方法是通用的,应该适用于许多多相催化体系。