THE ROLE OF NITROGEN AND OXYGEN-SURFACE GROUPS IN THE BEHAVIOR OF CARBON-SUPPORTED IRON AND RUTHENIUM CATALYSTS
THE ROLE OF NITROGEN AND OXYGEN-SURFACE GROUPS IN THE BEHAVIOR OF CARBON-SUPPORTED IRON AND RUTHENIUM CATALYSTS
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DOI：
10.1016/0008-6223(88)90140-6
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发表时间：
1988-01-01
期刊：
影响因子：
10.9
通讯作者：
LOPEZGONZALEZ, JD
中科院分区：
文献类型：
--
作者：
GUERRERORUIZ, A;RODRIGUEZRAMOS, I;LOPEZGONZALEZ, JD
以共聚物Saran为原料制备碳，并在不同的实验条件下与nh3和hno3反应生成氮和氧表面基团，作为Fe和Ru催化剂的载体。对催化剂进行了h2和CO的化学吸附表征，用x射线谱线展宽和透射电子显微镜对催化剂的金属粒度进行了估计。对于Fe催化剂，随着载体氮含量的增加，氢吸收量增加，CO吸收量减少；随着氧含量的增加，两种吸收量都减少。然而，在Ru的情况下，随着载体氮含量的增加，h2和CO的吸收量都增加。在523 K和101 KPa的条件下，CO加氢得到的结果并不都符合化学吸附实验中观察到的顺序；在这个反应中，在碳上引入的官能团似乎不足以对催化剂的活性或选择性产生明显的变化。仅在氨处理过的碳上负载的高度分散的铁催化剂上观察到一些效果。此外，在573 K （Fe催化剂）或413 K （Ru催化剂）下，正丁烷的氢解似乎明显受到载体氮含量的影响，特别是在由Fe(CO)5制备的催化剂中。
A carbon prepared from a copolymer Saran, and the products resulting from its reaction with NH3and HNO3under different experimental conditions to introduce nitrogen and oxygen surface groups, have been used as supports for Fe and Ru catalysts. The catalysts have been characterized by H2and CO chemisorption, X-ray line broadening and transmission electron microscopy were used to estimate metal particle sizes. There is, for Fe catalysts, an increase in hydrogen uptake and a decrease in CO uptake with increasing nitrogen content of the support and a decrease of both uptakes with increasing oxygen content. There is, however, in the case of Ru, an increase in both H2and CO uptake with increasing nitrogen content of the support.The results obtained in the hydrogenation of CO at 523 K and 101 KPa do not, in all cases, follow the sequence observed in the chemisorption experiments; it seems as if the functional groups introduced on the carbon are not sufficient to produce sensible changes in activity or selectivity of the catalysts in this reaction. Some effect is observed only in highly dispersed Fe catalysts supported on carbons treated with ammonia. Moreover, the hydrogenolysis ofn-butane at 573 K (Fe catalysts) or 413 K (Ru catalysts) seems to be clearly affected by the nitrogen content of the support, especially in catalysts prepared from Fe(CO)5.