Hydrocarbon Surface Reactions Over Transition Metals

这项工作旨在对影响碳氢化合物在负载金属上反应的活性和选择性的变量进行定量理解。这项工作既与碳氢化合物（包括合成燃料）的催化生产有关，也与碳氢化合物的活化及其转化为更复杂的产品以用作工业原料、燃料或其他最终用途有关。在存在和不存在共吸附物质的情况下，简单碳氢化合物在具有不同物理形态的负载金属上进行了研究。利用透射红外光谱对吸附的烃类进行了表征，并利用原位红外技术监测了向更稳定的表面烃类转化的速率。人们试图测量碳氢和碳-碳键断裂的速率，并量化颗粒大小和形态对吸附碳氢碎片的浓度和固有反应性的影响。该研究强调了二碳碳氢化合物（乙烷、乙烯和乙炔）在氧化铝或二氧化硅支撑的镍或铂晶体上的行为。

This work seeks to develop a quantitative understanding of the variables that influence the activity and selectivity of the reactions of hydrocarbons over supported metals. The work is relevant both to the catalytic production of hydrocarbons (including synfuels) and to the activation of hydrocarbons and their conversion into more complex products for use as industrial feedstocks, fuels, or other end uses. Simple hydrocarbons are studied over supported metals having different physical morphologies in the presence and absence of coadsorbed species. The adsorbed hydrocarbon species are characterized using transmission infrared spectroscopy and the rates of transformation into more stable surface species are monitored using in situ infrared techniques. Attempts are made to measure the rates of carbon-hydrogen and of carbon-carbon bond scission and to quantify the effects of particle size and morphology on the concentration and inherent reactivity of adsorbed hydrocarbon fragments. The study emphasizes the behavior of two-carbon hydrocarbons (ethane, ethylene, and acetylene) on crystallites of nickel or platinum supported on alumina or silica.