On effective locations of catalytic active sites in phase boundary catalysts

Hadi Nur, Nur Hidayah Mohd Ran, Nursyafreena Attan, S. Ikeda, B. Ohtani
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引用次数: 5

Abstract

Zeolite loaded with alkylsilane-covered titanium oxide was found to be more effective than its nonporous silica counterpart as phase-boundary catalyst (PBC) to promote epoxidation of alkenes with aqueous hydrogen peroxide. It was demonstrated that the phase-boundary catalyst system required neither stirring to make an emulsion, nor addition of a cosolvent to make a homogeneous solution to drive the reaction. However, some basic facts about them remain unclear, such as the question as to where an effective location of the active sites of PBC resides: is it on the external surface of the catalysts, or in their pores? In order to elucidate this problem, TS-1, HZSM-5 and zeolite loaded with alkylsilane–covered sulfonic acid in which the location of the active sites is mainly inside the pore system, were chosen as model catalysts. Catalytic activities of the catalysts TS-1 and HZSM-5 were examined after modification with n-octadecyltrichlorosilane (ODS). Their activities were compared with zeolite loaded with alkysilane-covered titanium oxide particles, in which the active sites are on the external surface in reactions of 1-octene with aqueous H2O2 and cyclohexene with water as model reactions. The study suggests that the location of the active sites on the external surface plays an important role in the phenomenon of phase-boundary catalysis.
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相界催化剂中催化活性位点的有效位置
负载烷基硅烷包覆氧化钛的沸石作为相界催化剂(PBC)在促进烯烃与过氧化氢的环氧化反应中比负载无孔二氧化硅的沸石更有效。结果表明,相界催化剂体系既不需要搅拌形成乳液,也不需要添加助溶剂形成均相溶液来驱动反应。然而,关于它们的一些基本事实仍然不清楚,比如PBC活性位点的有效位置在哪里:是在催化剂的外表面,还是在它们的孔隙中?为了阐明这一问题,选择活性位点主要位于孔系统内的TS-1、HZSM-5和负载烷基硅烷包覆磺酸的沸石作为模型催化剂。采用正十八烷基三氯硅烷(ODS)对催化剂TS-1和HZSM-5进行改性,考察其催化活性。并与负载烷基硅烷包覆氧化钛颗粒的沸石进行了活性比较,以1-辛烯与H2O2水溶液反应和环己烯与水反应为模型反应,活性位点位于沸石的外表面。研究表明,外表面活性位点的位置对相界催化现象起着重要的作用。
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On effective locations of catalytic active sites in phase boundary catalysts
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