载体材料对单Pd三效催化剂性能及催化活性的影响

引用本文: 崔亚娟, 方瑞梅, 尚鸿燕, 史忠华, 龚茂初, 陈耀强. 载体材料对单Pd三效催化剂性能及催化活性的影响[J]. 无机化学学报, 2015, (5): 989-1002. doi: 10.11862/CJIC.2015.120 shu

Citation: CUI Ya-Juan, FANG Rui-Mei, SHANG Hong-Yan, SHI Zhong-Hua, GONG Mao-Chu, CHEN Yao-Qiang. Effect of Support Materials on Property and Catalytic Performance of Pd-Only Three-Way Catalyst[J]. Chinese Journal of Inorganic Chemistry, 2015, (5): 989-1002. doi: 10.11862/CJIC.2015.120 shu

载体材料对单Pd三效催化剂性能及催化活性的影响

1.
1 四川大学建筑与环境学院, 成都 610065;
2.
2 四川大学化学工程学院, 成都 610065;
3.
3 四川大学绿色化学与技术教育部重点实验室, 成都 610064;
4.
4 四川省机动车尾气净化工程技术研究中心, 成都 610064;
5.
5 四川省环境保护环境催化材料工程技术中心, 成都 610064

通讯作者: 陈耀强 nic7501@scu.edu.cn

基金项目:
国家自然科学基金(No.21173153) (No.21173153)

四川省科技厅科技支撑项目(2011GZ0035)资助。 (2011GZ0035)

摘要: 采用共沉淀法制备了耐高温高比表面的La₂O₃-Al₂O₃(LA)以及铈含量分别为15%、33%和47%的储氧材料CeO₂-ZrO₂-La₂O₃-Al₂O₃(CZLA)、CeO₂-ZrO₂-La₂O₃+La₂O₃-Al₂O₃(CZL+LA)和CeO₂-ZrO₂-La₂O₃(CZL)₄类载体材料,并用浸渍法制备了整体式Pd/LA、Pd/CZLA、Pd/CZL+LA和Pd/CZL汽油车尾气净化三效催化剂,考察了载体材料对单Pd三效催化剂的影响。采用低温N₂吸附-脱附、H₂-程序升温还原(H₂-TPR)以及X射线光电子能谱(XPS)对载体材料及催化剂进行了表征,并考察了催化剂的空燃比性能和三效催化性能。结果表明,CZLA有效地结合了铈基和铝基载体材料的优点,表现出了优异的织构性能、热稳定性及还原性能。老化前后,其负载的单Pd三效催化剂在低温还原率、表面元素含量及Pd的电子结合能等性能方面表现出了最小的差异。催化剂活性测试结果表明,Pd/CZLA的三效窗口明显较宽,且拥有最低的起燃温度,尤其经1000℃老化处理后,其催化活性最高,C₃H₈、NO_x和CO的起燃温度分别为370、257和223℃。可见,相较于其他3种载体材料,CZLA更适合于负载单Pd三效催化剂,从而满足更高标准的三效催化剂的性能要求。

关键词:

钯;催化剂;多相催化;载体材料;织构性能;热稳定性;单Pd三效催化剂;催化性能。

English

Effect of Support Materials on Property and Catalytic Performance of Pd-Only Three-Way Catalyst

1.
1 College of Architecture and Environment, Sichuan University, Sichuan, Chengdu 610065, China;
2.
2 College of Chemical Engineering, Sichuan University, Sichuan, Chengdu 610065, China;
3.
3 Key Laboratory of Green Chemistry & Technology, Ministry of Education, College of Chemistry, Sichuan University, Sichuan, Chengdu 610064, China;
4.
4 Center of Engineering of Vehicular Exhaust Gases Abatement, Sichuan Province, Sichuan, Chengdu 610064, China;
5.
5 Center of Engineering of Environmental Catalytic Material, Sichuan Province, Sichuan, Chengdu 610064, China

Corresponding author: 陈耀强 nic7501@scu.edu.cn

Received Date: 08 November 2014
Fund Project:
国家自然科学基金(No.21173153)

四川省科技厅科技支撑项目(2011GZ0035)资助。

Abstract: Four kinds of support materials, i.e. a thermally stable material La₂O₃-Al₂O₃(LA), three oxygen storage materials CeO₂-ZrO₂-La₂O₃-Al₂O₃(CZLA), CeO₂-ZrO₂-La₂O₃+La₂O₃-Al₂O₃(CZL+LA) and CeO₂-ZrO₂-La₂O₃(CZL) with ceria content of 15%, 33% and 47%, respectively, were prepared by co-precipitation. The corresponding Pd-only catalysts Pd/LA, Pd/CZLA, Pd/CZL+LA and Pd/CZL were obtained by wet-impregnation and further fabricated as three-way catalysts in a monolith form. The support materials were characterized by low temperature nitrogen adsorption-desorption and H₂-temperature programmed reduction (H₂-TPR). The catalysts were characterized by H₂-TPR and XPS, and were evaluated with a simulated automobile exhaust in terms of the relationships of three way performance with the air/fuel operation window and with temperatures. The results indicate that the support material CZLA integrates the advantages of ceria-based and alumina-based materials effectively thus having superior textural property, thermal stability and reduction property. Additionally, Pd/CZLA catalyst shows little difference in low temperature reducibility, surface elemental distribution and elemental oxidation states before and after aging treatment. As a result, Pd/CZLA exhibits the widest air/fuel operation window and the lowest light-off temperature among the four catalysts, especially after aging treatment, the light-off temperature of C₃H₈, NO_x and CO is 370 ℃, 257 ℃, 223 ℃, respectively. Then material CZLA is the most suitable support for Pd-only three-way catalyst compared with the other three supports.

Key words:

palladium;catalysts;Heterogeneous catalysis;support materials;textural properties;thermal stability;Pd-only three-way catalysts;catalytic performance

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

载体材料对单Pd三效催化剂性能及催化活性的影响

通讯作者: 陈耀强 nic7501@scu.edu.cn

English

Effect of Support Materials on Property and Catalytic Performance of Pd-Only Three-Way Catalyst

Corresponding author: 陈耀强 nic7501@scu.edu.cn

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CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

载体材料对单Pd三效催化剂性能及催化活性的影响

通讯作者: 陈耀强 nic7501@scu.edu.cn

English

Effect of Support Materials on Property and Catalytic Performance of Pd-Only Three-Way Catalyst

Corresponding author: 陈耀强 nic7501@scu.edu.cn

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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