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Synthesis of hierarchical Sn-Beta zeolite and its catalytic performance in glucose conversion

机译:层次β沸石的合成及其在葡萄糖转化中的催化性能

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Hierarchical Beta zeolites are successfully synthesized with hydrothermal method in the presence of polydiallyldimethylammonium chloride (PDADMA). Followed a dealumination process, hierarchical Sn-Beta are post-synthesized by the solid-gas reaction of dealuminated Beta zeolite with SnCl4 vapor. All samples are charcterized with XRD, N2 sorption, SEM and TEM. SEM images show that both Beta zeolite and Sn-Beta zeolite exhibit rough spherical-like morphology of about 500-900 nm in diameters, N2 sorptions show the pore size distributions in micropore and mesopore ranges, indicating the formation of mesoporous Beta zeolites. It is proofed that Sn species are doped into the framework in a tetrahedral environment during solid-gas reaction and the introduction of Sn species has negligible impact on the structure of Beta zeolites. Furthermore, the dehydration of glucose into HMF which needs both Bro?nsted and Lewis acid is selected to evaluate the catalytic performance of hierarchical Sn-Beta. It displays good catalytic activity, the conversion of glucose (99 %) and selectivity to HMF (42 %) are higher than those of the conventional Beta (96 % and 32 %, respectively). This is attributed to the intra-crystalline mesoporous structure and efficient diffusion of reactant/product molecules. Moreover, the catalyst exhibits steady catalytic performance after the fifth repeated run.
机译:在聚二烯丙基二甲基氯化铵(PDADMA)存在下,采用水热法成功合成了分级β沸石。在脱铝过程之后,通过脱铝β沸石与SnCl4蒸汽的固气反应后合成了分级的Snβ。用XRD、N2吸附、SEM和TEM对样品进行了表征。SEM图像显示,β沸石和Snβ沸石均呈现出直径约500-900 nm的粗糙球形形貌,N2吸附显示了微孔和介孔范围内的孔径分布,表明形成了介孔β沸石。证明了在固-气反应过程中,锡物种在四面体环境中被掺杂到骨架中,锡物种的引入对β沸石的结构影响很小。此外,葡萄糖脱水成HMF需要两种Bro?选择nsted和Lewis酸来评价分级Sn-Beta的催化性能。它表现出良好的催化活性,葡萄糖的转化率(99%)和HMF的选择性(42%)均高于常规β(分别为96%和32%)。这归因于晶内介孔结构和反应物/产物分子的有效扩散。此外,催化剂在第五次重复运行后表现出稳定的催化性能。

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