期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 1, 页码 730-739出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b17062
关键词
molecular oxygen activation; MnxZr1-xO2 solid solution; toluene oxidation; oxygen vacancy contribution; DFT calculations
资金
- National Natural Science Foundation of China [91544227, 21777166]
- National Key Research and Development Program of China [2016YFC0202202]
- Beijing Synchrotron Radiation Laboratory
Oxygen vacancy is conducive to molecular oxygen adsorption and activation, and it is necessary to estimate its contribution on catalysts, especially the doped system for volatile organic compound (VOC) oxidation. Herein, a series of doped MnxZr1-xO2 catalysts with oxygen vacancy were prepared by partially substituting Zr4+ in a zirconia with low-valent manganese (Mn2+). Compared with the corresponding mechanically mixed samples (MB-x) without oxygen vacancy, MnxZr1-xO2 catalysts exhibited better toluene conversion and specific reaction rate, where the differential values were calculated to estimate the contribution of oxygen vacancy on catalytic performance. The increase in oxygen vacancy concentrations in MnxZr1-xO2 catalysts can boost the differential values, implying the enhancement of oxygen vacancy contribution. Density functional theory (DFT) calculations further confirmed the contribution of oxygen vacancy, and molecular oxygen is strongly absorbed and activated on a defective Mn-doped c-ZrO2 (111) surface with oxygen vacancy rather than a perfect m-ZrO2 (-111) surface or a perfect Mn-doped c-ZrO2 (111) surface, thus resulting in the significant improvement in catalytic activity for toluene oxidation. In situ DRIFTS spectra revealed that the oxygen vacancy can alter the toluene degradation pathway and accelerate the intermediates to convert into CO2 and H2O, thus leading to a low activation energy and high specific reaction rate.
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