Operando Raman spectroscopy and kinetic study of low-temperature CO oxidation on an α-Mn2O3 nanocatalyst

被引：112
作者：
Xu, Jing [1 ]
Deng, Ya-Qing [1 ]
Luo, Yan [1 ]
Mao, Wei [1 ]
Yang, Xue-Jing [1 ]
Han, Yi-Fan [1 ]
机构：
[1] E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
来源：
JOURNAL OF CATALYSIS | 2013年 / 300卷
基金：
美国国家科学基金会;
关键词：
Raman spectroscopy; Operando; Kinetics; CO oxidation; Manganese oxides; alpha-Mn2O3; nanocrystals; Temperature-programmed surface reaction; MANGANESE OXIDE CATALYSTS; CARBON-MONOXIDE OXIDATION; SUPPORTED MANGANESE; PHASE-TRANSFORMATION; COMBUSTION; MECHANISM; COPPER; NANOPARTICLES; METHANE; MN2O3;
D O I：
10.1016/j.jcat.2013.01.010
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
alpha-Mn2O3 nanocrystals with uniform morphology prepared by calcining a self-assembled Mn3O4 precursor have proved active (ca. 0.14 molecule nm(-2) s(-1) at 153 degrees C) toward CO oxidation at low temperatures. The reaction orders with respect to CO and O-2 were measured in the temperature range 100-190 degrees C. Operando and in situ Raman spectroscopy are used to determine the near-surface structure of alpha-Mn2O3 nanocrystals during the adsorption and oxidation of CO for the first time. A surface phase transformation from alpha-Mn2O3 to MnjOk (1 < j < 2, 1 < k < 3, and 1 < k/j < 1.5) intermediate species was observed in gaseous CO with the change in temperature. In addition, with the combination of the temperature-programmed desorption of O-2, temperature-programmed surface reaction of CO oxidation, operando Raman spectra, and kinetics parameters, we conclude that the oxidation of CO may proceed through the Langmuir-Hinshelwood mechanism (<200 degrees C) to the Mars van Krevelen mechanism (>350 degrees C) with increasing reaction temperature. In particular, the adsorbed oxygen is deduced to be responsible for CO oxidation at lower temperatures. (C) 2013 Elsevier Inc. All rights reserved.
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页码：225 / 234
页数：10
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