期刊
ACS CATALYSIS
卷 4, 期 11, 页码 4106-4115出版社
AMER CHEMICAL SOC
DOI: 10.1021/cs5011376
关键词
Mn3O4@SiO2; nanostructure catalysts; Operand Raman spectroscopy; kinetics; CO oxidation
资金
- National Science Foundation [21176071, 21106041, 21273070]
- Program for New Century Excellent Talents in University [NCET-12-0852]
- Science and Technology Commission of Shanghai Municipality [11JC1402700]
- Chinese Education Ministry 111 Project [B08021]
Mn3O4@SiO2 prepared via a Stober route showed a steady reaction rate for CO oxidation at 250 degrees C after 12 h. The reaction orders, with respect to CO (0.490.12) and O2 (0.40.6), were obtained for a Mn3O4@SiO2 catalyst (dMn(3)O(4) = 7.6 nm) in the temperature range of 220-280 degrees C. Via Operando Raman spectroscopy, a COad-induced change in the symmetric stretch of MnOMn (from 636 cm1 to 642 cm1) was observed for Mn3O4@SiO2, indicating a tiny structure modification of core Mn3O4 by the adsorption of CO. With the combination of the catalyst structure and the kinetics of CO oxidation, we assume that this reaction proceeds mainly through the LangmuirHinshelwood mechanism at or below 280 degrees C. In comparison with the reference alpha-Mn2O3 catalyst, the presence of shell SiO2 does not change the reaction behavior but improves the catalyst stability.
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