制备方法对Pd-MnOx/γ-Al2O3催化剂分解地表O3性能的影响

doi:10.1016/S1872-2067(14)60176-5

催化学报 ›› 2014, Vol. 35 ›› Issue (11): 1883-1891.DOI: 10.1016/S1872-2067(14)60176-5

制备方法对Pd-MnO_x/γ-Al₂O₃催化剂分解地表O₃性能的影响

任成军, 周丽娜, 尚鸿燕, 陈耀强

四川大学化学学院, 教育部绿色化学重点实验室, 四川成都610064

收稿日期:2014-04-24 修回日期:2014-06-16 出版日期:2014-11-06 发布日期:2014-11-06
通讯作者: 陈耀强
基金资助:
国家自然科学基金(J1103315,J1310008).

Effect of preparation method on the performance of Pd-MnO_x/γ-Al₂O₃ monolithic catalysts for ground-level O₃ decomposition

Chengjun Ren, Lina Zhou, Hongyan Shang, Yaoqiang Chen

Key Laboratory of Green Chemistry & Technology of the Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichuan China

Received:2014-04-24 Revised:2014-06-16 Online:2014-11-06 Published:2014-11-06
Supported by:
This work was supported by the National Natural Science Foundation of China (J1103315, J1310008).

摘要/Abstract

摘要：

分别用溶胶凝胶法和分步沉淀法制备了MnO_x + γ-Al₂O₃和MnO_x/γ-Al₂O₃, 用等体积浸渍法将等量的Pd(NO₃)₂分别浸渍于其上, 再将它们分别涂覆于堇青石上, 得到不同物理化学性质的整体式催化剂, 并采用X射线衍射、X射线光电子能谱、程序升温还原和低温N₂吸附-脱附等技术对催化剂进行表征. 结果表明, 制备方法和MnO_x焙烧温度明显影响催化剂中MnO_x的物相、表面Mn物种和表面活性氧物种的分布及织构性质. 活性测试结果表明, 两种制备方法得到的催化剂于16-90 ℃, 380000-580000 h^-1条件下均可将0.6 μL·L^-1 O₃完全分解; 尤其是溶胶凝胶法制备的Pd/γ-Al₂O₃+MnO_x/γ-Al₂O₃催化剂分解O₃活性较好, 催化剂表面Mn²⁺:Mn³⁺:Mn⁴⁺ = 1.7:1:3 (mol).

关键词: 锰氧化物, 钯, 臭氧, 催化分解, 制备方法

Abstract:

MnO_x+γ-Al₂O₃and MnO_x/γ-Al₂O₃ catalysts were prepared by the sol-gel and sequential precipitation methods, respectively. The same amount of Pd was loaded on these catalysts by incipient wetness impregnation. The two Pd-MnO_x/γ-Al₂O₃catalysts with different physicochemical properties were coated on cordierite. The catalysts were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, H₂ temperature-programmed reduction, and N₂ adsorption-desorption measurement. The preparation method and calcination temperature of MnO_x have significant impact on the crystalline phase of MnO_x, MnO_x species and active oxygen species, and textural properties of the catalysts. The experimental results showed that 0.60 μL·L^-1 of ozone was completely decomposed on these catalysts in the temperature range of 16 to 90 ℃ at space velocities from 380000 to 580000 h^-1. In particular, the activity for O₃ decomposition was excellent on the Pd/MnO_x+Pd/γ-Al₂O₃catalyst that used MnO_x prepared by the sol-gel method. Mnⁿ⁺ is beneficial for O₃ decomposition, and Mn²⁺, Mn³⁺, and Mn⁴⁺were presented in a mole ratio of 1.7:1:3 on the surface of the catalyst.

Key words: Manganese oxide, Palladium, Ozone, Catalytic decomposition, Preparation method

任成军, 周丽娜, 尚鸿燕, 陈耀强. 制备方法对Pd-MnO_x/γ-Al₂O₃催化剂分解地表O₃性能的影响[J]. 催化学报, 2014, 35(11): 1883-1891.

Chengjun Ren, Lina Zhou, Hongyan Shang, Yaoqiang Chen. Effect of preparation method on the performance of Pd-MnO_x/γ-Al₂O₃ monolithic catalysts for ground-level O₃ decomposition[J]. Chinese Journal of Catalysis, 2014, 35(11): 1883-1891.

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制备方法对Pd-MnO_x/γ-Al₂O₃催化剂分解地表O₃性能的影响

Effect of preparation method on the performance of Pd-MnO_x/γ-Al₂O₃ monolithic catalysts for ground-level O₃ decomposition

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