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首页> 外文期刊>Catalysis science & technology >3D charged grid induces a high performance catalyst: ruthenium clusters enclosed in X-zeolite for hydrogenation of phenol to cyclohexanone
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3D charged grid induces a high performance catalyst: ruthenium clusters enclosed in X-zeolite for hydrogenation of phenol to cyclohexanone

机译：3 d网格产生一个高绩效催化剂:钌集群封闭X-zeolite为苯酚加氢环己酮

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摘要

The hydrogenation of phenol to cyclohexanone is an important industrial reaction and supported palladium catalysts are the most popular catalysts applied nowadays. Hitherto, there has been no success in using ruthenium catalysts for this reaction because of their poor catalytic performance, in spite of the fact that ruthenium is a frequently used metallic component in hydrogenation catalysts. Herein, we report our effort in creating a meso-structured catalyst composed of ruthenium clusters enclosed in the super cages of Xzeolite, which is prepared by mixing precursors of ruthenium and X-zeolite at the beginning stage of preparation, i.e., before the crystallization of the zeolite. This well-defined Ru catalyst exhibits excellent catalytic performance for the selective hydrogenation of phenol, similar to palladium catalysts. The results demonstrate that the joint effects of the 3D negatively charged grid of X-zeolite and the enclosed electrondeficient ruthenium clusters enhance the activity of metallic ruthenium and suppress the further hydrogenation of the valuable product cyclohexanone, which is not possible with traditional Ru catalysts. This investigation reveals the fact that although catalytic reactions are always initiated on the active centers of the catalyst at dimensions on the atomic scale, the effect of the neighboring environment surrounding the active species might extend it to the meso-scale, which should not be ignored as it might induce electronic and structural changes in the active species as well as possibly dramatic changes in the performance of the catalyst. The meso-structured catalyst integrated active species and the neighboring environment as a whole should be considered in discussing the performance of catalysts.
机译：苯酚加氢的环己酮是一种重要的工业反应和支持钯催化剂是最受欢迎的催化剂的应用。在使用钌催化剂没有成功因为他们的可怜的催化这个反应性能,尽管钌的事实是一个常用的金属组件加氢催化剂。努力创建一个meso-structured催化剂钌集群组成的封闭的超级Xzeolite的笼子里,准备的混合钌和X-zeolite的前兆之前准备的开始阶段,即沸石的结晶。定义良好的俄文展览优秀的催化剂选择性的催化性能苯酚加氢,类似于钯催化剂。3 d网格带负电荷的影响X-zeolite和封闭electrondeficient钌集群提高的活动金属钌和进一步抑制加氢有价值的产品环己酮,这是不可能的传统的俄文催化剂。揭示了一个事实:尽管催化反应总是发起的活动在维中心的催化剂原子尺度,邻国的影响周围环境中活跃的物种扩展它的数值,不应该可能诱发电子和忽视结构变化的活性物种戏剧性的变化,很可能是性能的催化剂。活跃的物种和邻近的集成环境作为一个整体应该考虑讨论了催化剂的性能。

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