沸石配位阳离子对Pd/H-ZSM-5催化剂加氢性能的影响
Effects of Coordination Cations over Zeolite on Hydrogenation Performance of Pd/H-ZSM-5 Catalyst
作者单位E-mail
张传浩 太原理工大学化学化工学院, 太原 030024  
路宁悦 太原理工大学化学化工学院, 太原 030024  
范彬彬 太原理工大学化学化工学院, 太原 030024 fanbinbin@tyut.edu.cn 
李瑞丰 太原理工大学化学化工学院, 太原 030024  
摘要: 选用商业多级孔NH4-ZSM-5和H-ZSM-5(NH4-ZSM-5在550℃空气气氛中焙烧6 h)沸石为载体,H2PdCl4为金属前驱物,采用常规浸渍法制备了Pd/H-ZSM-5负载催化剂。利用X射线衍射、扫描电子显微镜、N2吸附-脱附、紫外可见光谱、X射线光电子能谱、氨气-程序升温脱附和透射电子显微镜等手段对所制备催化剂的物化性质进行详细表征,并对Pd/H-ZSM-5的萘加氢催化性能进行了考察。结果表明,ZSM-5载体上配位的NH4+的存在不仅有利于负载金属Pd物种的分散,使Pd在NH4-ZSM-5载体上具有较高的分散度,而且所制备的Pd/H-ZSM-5(NH4)较Pd/H-ZSM-5(H)具有更多的酸位。Pd/H-ZSM-5(NH4)在萘加氢反应中表现出比Pd/H-ZSM-5(H)更优异的催化性能。
关键词: ZSM-5沸石  配位阳离子    加氢反应
基金项目: 国家重点研发项目(No.2020YFB0606405)和国家自然科学基金(No.21576177)资助。
Abstract: Pd/H-ZSM-5 catalysts were prepared by conventional impregnation method with commercial hierarchical NH4-ZSM-5 and H-ZSM-5 (NH4-ZSM-5 calcined at 550℃ for 6 h in air atmosphere) zeolite as the supports, and H2PdCl4 as the metal precursor. The physicochemical properties and catalytic performance of the prepared samples were characterized by X-ray diffraction, scanning electron microscopy, N2 adsorption-desorption, UV-Vis spectroscopy, X-ray photoelectron spectroscopy, NH3-temperature programmed desorption, transmission electron microscopy and naphthalene hydrogenation reaction. The results showed that the coordination cations over zeolites greatly influence the dispersion of the supported metal species and catalyst acidity. The NH4+ over ZSM-5 supports was conducive to the dispersion of the supported Pd species, and the prepared Pd/H-ZSM-5(NH4) had more acid sites than Pd/H-ZSM-5(H), which resulted in that Pd/H-ZSM-5(NH4) exhibited higher catalytic activity in naphthalene hydrogenation than Pd/H-ZSM-5(H).
Keywords: ZSM-5 zeolite  coordination cations  naphthalene  hydrogenation reaction
投稿时间:2021-03-18 修订日期:2021-06-24
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张传浩,路宁悦,范彬彬,李瑞丰.沸石配位阳离子对Pd/H-ZSM-5催化剂加氢性能的影响[J].无机化学学报,2021,37(9):1625-1632.
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