α-MnO2负载纳米Au催化剂低温催化氧化CO和苯的性能

doi:10.3866/PKU.WHXB20112872

物理化学学报 >> 2011, Vol. 27 >> Issue (12): 2872-2880.doi: 10.3866/PKU.WHXB20112872

α-MnO₂负载纳米Au催化剂低温催化氧化CO和苯的性能

叶青, 霍飞飞, 闫立娜, 王娟, 程水源, 康天放

北京工业大学环境与能源工程学院, 北京 100124

收稿日期:2011-06-13 修回日期:2011-09-13 发布日期:2011-11-25
通讯作者: 叶青 E-mail:yeqing@bjut.edu.cn
基金资助:
国家自然科学基金(20777005), 北京市自然科学基金(8082008)和北京市组织部优秀人才基金(20071D0501500210)资助项目

Highly Active Au/α-MnO₂ Catalysts for the Low-Temperature Oxidation of Carbon Monoxide and Benzene

YE Qing, HUO Fei-Fei, YAN Li-Na, WANG Juan, CHENG Shui-Yuan, KANG Tian-Fang

College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124, P. P. China

Received:2011-06-13 Revised:2011-09-13 Published:2011-11-25
Contact: YE Qing E-mail:yeqing@bjut.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (20777005), Natural Science Foundation of Beijing, China (8082008) and Beijing Municipal Foundation for Excellent Person of Ability, China (20071D0501500210).

摘要/Abstract

摘要： 以尿素为沉淀剂用沉积-沉淀法制备了α-MnO₂负载Au 催化剂xAu/α-MnO₂ (x=0-7(对应的Au 负载量(质量分数)分别为0-7%)), 使用X 射线粉末衍射(XRD)、N₂-吸附/脱附、透射电镜(TEM)、X 射线光电子能谱(XPS)和H₂-程序升温还原(H₂-TPR)等技术对所制样品进行了表征, 并测定其对CO和苯的催化氧化性能. XRD结果表明, 负载Au对α-MnO₂载体结构影响不大, 随Au含量的增加, Au颗粒明显增大. N₂-吸附/脱附和TEM结果表明, Au的加入对xAu/α-MnO₂的比表面积、孔容和孔径等结构性能影响较小, 表明Au分布在α-MnO₂载体表面, 未阻塞其孔道. XPS结果表明, 随着Au负载量的增加, xAu/α-MnO₂中的O^2-/(O₂^2- 或O^-)、Mn⁴⁺/Mn³⁺和Au³⁺/Au⁰的摩尔比在增加, 表明其晶格氧、Mn⁴⁺和Au³⁺的浓度在增加. 由于贵金属的溢氢作用, Au 明显促进xAu/α-MnO₂氧化还原能力, 其中3Au/α-MnO₂具有最高的氧化还原性. 负载Au明显影响xAu/α-MnO₂样品的催化活性, xAu/α-MnO₂的催化性能与Au 的分散性、氧化还原性能及表面氧物种的种类密切相关, 其中3Au/α-MnO₂显示出最佳活性, 其催化氧化CO的T₉₀=80 °C, 苯的T₉₀=200 °C.

关键词: &, alpha, -MnO₂负载Au催化剂, 低温还原性, 相互作用, CO氧化, 苯催化燃烧

Abstract: α-MnO₂-supported gold catalysts (xAu/α-MnO₂, x=0-7 (corresponding to the Au loading (mass fraction) of 0-7%) were prepared by a deposition- precipitation method using urea as a precipitation agent and characterized by different techniques such as X-ray diffraction (XRD), N₂ adsorption-desorption measurements, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and H₂ temperature-programmed reduction (TPR). The catalytic activities of the materials were evaluated for the oxidation of CO and benzene. The Au particle size was found to be related to the Au loading of the xAu/ α-MnO₂ samples and increased with Au loading. XPS results showed that the mole ratios of O^2-/(O₂^2- or O^-), Mn⁴⁺/Mn³⁺ and Au³⁺/Au⁰ increased upon the addition of Au. The loading of gold over α-MnO₂ significantly modified the catalytic activities. The catalytic performance of xAu/α-MnO₂ strongly depended on the Au loading, and 3Au/α-MnO₂ gained the best activity at T₉₀=80 °C and T₉₀=20 °C for the catalytic oxidation of CO and benzene, respectively. The excellent performance of 3Au/α-MnO₂ is associated with highly dispersed Au, good low-temperature reducibility, and a synergism at the interface between theAu and MnO₂ nanodomains.

Key words: &, alpha, -MnO₂ supported gold catalyst, Low-temperature reducibility, Synergistic action, Carbon monoxide oxidation, Benzene combustion

叶青, 霍飞飞, 闫立娜, 王娟, 程水源, 康天放. α-MnO₂负载纳米Au催化剂低温催化氧化CO和苯的性能[J]. 物理化学学报, 2011, 27(12), 2872-2880. doi: 10.3866/PKU.WHXB20112872

YE Qing, HUO Fei-Fei, YAN Li-Na, WANG Juan, CHENG Shui-Yuan, KANG Tian-Fang. Highly Active Au/α-MnO₂ Catalysts for the Low-Temperature Oxidation of Carbon Monoxide and Benzene[J]. Acta Phys. -Chim. Sin. 2011, 27(12), 2872-2880. doi: 10.3866/PKU.WHXB20112872

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB20112872

https://www.whxb.pku.edu.cn/CN/Y2011/V27/I12/2872

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α-MnO₂负载纳米Au催化剂低温催化氧化CO和苯的性能

Highly Active Au/α-MnO₂ Catalysts for the Low-Temperature Oxidation of Carbon Monoxide and Benzene

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