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钙改性的Pd/CeO2-ZrO2-Al2O3催化剂催化甲醇裂解反应
引用本文:李雪,王晓文,赵明,刘建英,龚茂初,陈耀强.钙改性的Pd/CeO2-ZrO2-Al2O3催化剂催化甲醇裂解反应[J].催化学报,2011,32(11):1739-1746.
作者姓名:李雪  王晓文  赵明  刘建英  龚茂初  陈耀强
作者单位:1. 四川大学化学学院绿色化学与技术教育部重点实验室,四川成都,610064
2. 四川大学化学工程学院,四川成都,610065
摘    要:采用共沉淀法制备了未改性的和Ca掺杂的CeO2-ZrO2-Al2O3样品,进一步用浸渍法制备了Pd/CeO2-ZrO2-Al2O3(Pd/CZA)和Pd/CeO2-ZrO2-Al2O3-CaO (Pd/CZACa)催化剂.运用X射线衍射、N2吸附-脱附、储氧量测定、CO化学吸附、NH3程序升温脱附、CO2程序升温脱附、...

关 键 词:    甲醇裂解  氧化铈  氧化锆  氧化铝

Ca-Modified Pd/CeO2-ZrO2-Al2O3 Catalysts for Methanol Decomposition
LI Xue,WANG Xiaowen,ZHAO Ming,LIU Jianying,GONG Maochu,CHEN Yaoqiang.Ca-Modified Pd/CeO2-ZrO2-Al2O3 Catalysts for Methanol Decomposition[J].Chinese Journal of Catalysis,2011,32(11):1739-1746.
Authors:LI Xue  WANG Xiaowen  ZHAO Ming  LIU Jianying  GONG Maochu  CHEN Yaoqiang
Institution:1Key Laboratory of Green Chemistry and Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichuan, China 2College of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan, China
Abstract:CeO2-ZrO2-Al2O3 and CeO2-ZrO2-Al2O3-CaO supports were prepared by the coprecipitation method and were loaded with Pd by impregnation to form Pd/CeO2-ZrO2-Al2O3 (Pd/CZA) and Pd/CeO2-ZrO2-Al2O3-CaO (Pd/CZACa) catalysts. The catalysts were characterized by X-ray diffraction, low temperature N2 adsorption-desorption, oxygen storage capacity, CO chemisorption, NH3 temperature-programmed desorption (NH3-TPD), CO2 temperature-programmed desorption (CO2-TPD), H2 temperature-programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS). The catalyst activity for methanol decomposition showed that the Ca modification improved the low-temperature activity of the catalyst, which lowered the complete conversion temperature on 34 oC. NH3-TPD and CO2-TPD showed that the addition of Ca poisoned the acid sites of the support or increased the number of weak basic sites and therefore changed the adsorption-desorption equilibria of the adsorbed species. It also enhanced the metal-support interaction and increased the electronic surroundings of Pd sites, which maintained Pd in a partly oxidized (Pdδ+) state and consequently increased the activity for methanol decomposition according to H2-TPR and XPS measurements.
Keywords:palladium  calcium  methanol decomposition  ceria  zirconia  alumina
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