物理化学学报 >> 2016, Vol. 32 >> Issue (7): 1734-1746.doi: 10.3866/PKU.WHXB201603235

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复合沉淀剂制备的CeO2-ZrO2-Al2O3材料及其负载的单Pd三效催化剂

李红梅1,2,3,兰丽1,2,*(),陈山虎4,刘达玉1,王卫1,龚茂初2,陈耀强2,*()   

  1. 1 成都大学药学与生物工程学院,成都610106
    2 四川大学化学学院,教育部绿色化学重点实验室,成都610064
    3 四川理工学院,绿色化学重点实验室,四川自贡643000
    4 中自环保科技股份有限公司,成都611731
  • 收稿日期:2016-01-18 发布日期:2016-07-08
  • 通讯作者: 兰丽,陈耀强 E-mail:wskadlb@163.com;chenyaoqiang@scu.edu.cn
  • 基金资助:
    国家自然科学基金(21173153);国家高技术研究发展计划项目(863)(2015AA034603);绿色催化四川省高校重点实验室开放基金项目(LYJ1407)

Preparation of CeO2-ZrO2-Al2O3 with a Composite Precipitant and Its Supported Pd-Only Three-Way Catalyst

Hong-Mei LI1,2,3,Li LAN1,2,*(),Shan-Hu CHEN4,Da-Yu LIU1,Wei WANG1,Mao-Chu GONG2,Yao-Qiang CHEN2,*()   

  1. 1 Faculty of Pharmacy and Bioengineering, Chengdu University, Chengdu 610106, P. R. China
    2 Key Laboratory of Green Chemistry & Technology, Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, P. R. China
    3 Key Laboratory of Green Chemistry, Sichuan University of Science and Engineering, Zigong 643000, Sichuan Province, P. R. China
    4 4Sinocat Environmental Protection Co., Ltd., Chengdu 611731, P. R. China
  • Received:2016-01-18 Published:2016-07-08
  • Contact: Li LAN,Yao-Qiang CHEN E-mail:wskadlb@163.com;chenyaoqiang@scu.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(21173153);National Hi-tech Research and Development Program of China (863)(2015AA034603);Opening Project of Key Laboratory of Green Chemistry of Sichuan Institutes of Higher Education, China(LYJ1407)

摘要:

采用了一种由氨水和碳酸铵组成的复合沉淀剂来制备CeO2-ZrO2-Al2O3 (CZA)复合氧化物。作为对比,分别采用氨水和碳酸铵为沉淀剂制备了另外两个CZA复合氧化物。系统地研究了各CZA材料在织构、结构、氧化还原性能、热老化行为之间的区别,以及其负载的单Pd三效催化剂的催化性能。结果表明,不同的沉淀剂制得的材料中其CeO2-ZrO2 (CZ)和Al2O3之间的相互作用不同。用氨水做沉淀剂时,得到的材料中CZ和Al2O3之间的相互作用很小,导致其热稳定性较差。在碳酸铵做沉淀剂的情况下,CZ和Al2O3之间具有很强的相互作用,可以提高材料的热稳定性,但同时,CZ固溶体的均一性被严重破坏,使得材料的氧化还原性能不理想。而复合沉淀剂的使用可以有效地平衡CZ和Al2O3之间的相互作用,导致得到的CZA材料具有优异的织构、结构性能及良好的热稳定性。因此,其负载的单Pd催化剂表现出最为优异的氧化还原性能和三效催化活性。

关键词: CeO2-ZrO2-Al2O3复合氧化物, 复合沉淀剂, 单Pd三效催化剂, 相互作用, 热稳定性

Abstract:

Acomposite precipitant composed of ammonia and ammoniumcarbonate was used to prepare CeO2-ZrO2-Al2O3 (CZA). For comparison, two other CZA samples were prepared using ammonia and ammonium carbonate as the precipitants, respectively. Differences in the textural, structural and redox properties, together with the evolution upon thermal aging treatment and the catalytic performance of the corresponding Pd-only three-way catalysts, were investigated systematically. The choice of precipitant was found to affect the interactions between CeO2-ZrO2 (CZ) and Al2O3. When ammonia was used as the precipitant, the resulting CZ and Al2O3 seemed insusceptible to each other, thus the obtained CZA composite displayed inferior thermal stability due to the weakest interaction between CZ and Al2O3. In the case of ammonium carbonate, stronger interaction between CZ and Al2O3 enhanced the thermal stability of CZA, but in the meantime, the homogeneity of the CZ solid solution was severely impaired by Al2O3, leading to undesirable redox performance. Fortunately, the use of the composite precipitant brought about favorable interaction between CZ and Al2O3, leading to excellent textural and structural properties along with the highest thermal stability of the CZA compound. Consequently, the corresponding Pd-based catalyst displayed prominent reducibility and oxygen storage capacity (OSC) performance, as well as superior three-way catalytic performance.

Key words: CeO2-ZrO2-Al2O3 compound, Composite precipitant, Pd-only three-way catalyst, Interaction, Thermal stability

MSC2000: 

  • O643