期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 117, 期 19, 页码 9999-10006出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp400504m
关键词
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资金
- STCSM postdoctoral foundation [12R21413300]
- National Natural Science Foundation of China [51108258]
- Science and Technology Commission of Shanghai Municipality [10540500100, 11nm0502200]
- Research Fund for the Innovation Program of Shanghai University [A.10040711003]
- Shanghai Municipal Education Commission [B.37040711001]
- Doctoral Fund of the Ministry of Education of China [20123108120018]
- Key Subject of Shanghai Municipal Education Commission [J50102]
Manganese oxides (MnOx) supported on Ce0.9Zr0.1O2 (MnOx/Ce0.9Zr0.1O2) nanorods were synthesized and tested for low-temperature selective catalytic reduction of NO with ammonia. The catalysts were characterized by transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photo-electron spectroscopy, and hydrogen temperature-programmed reduction. The structure and morphology results show that the MnOx was highly dispersed on the surface of Ce0.9Zr0.1O2 nanorods. Various species, such as Mn2+, Mn3+, and Mn4+, were exposed due to a strong interaction between manganese and cerium oxides. Thus, the MnOx/Ce0.9Zr0.1O2 nanorods exhibited a better catalytic performance (90% NO conversion at 150 degrees C) compared with that of the as-prepared Ce0.9Zr0.1O2 nanorods. Density functional theory (DFT) calculations clearly demonstrated that the MnOx on the surface of supporting nanorods or Mn@ CeO2(110) could easily form an oxygen vacancy distortion. Furthermore, the Mn@CeO2(110) Model in the DFT analysis showed a prominent effect on the NO and NH3 adsorption which resulted in a stronger nitrite intermediate (NOO*) formations and more attractive interaction with the NH3 gas compared with those observed, with the CeO2(110) model. Therefore, a thorough understanding of the structure and catalytic performance of MnOx/Ce0.9Zr0.1O2 nanorods was successfully achieved by a combination of experimental and theoretical studies.
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