Citation: NIE Wang-Xin, ZOU Xiu-Jing, WANG Xue-Guang, DING Wei-Zhong, LU Xiong-Gang. Preparation of Highly Dispersed Ni-Ce-Zr Oxides over Mesoporous γ-Alumina and Their Catalytic Properties for CO₂ Methanation[J]. Acta Physico-Chimica Sinica, ;2016, 32(11): 2803-2810. doi: 10.3866/PKU.WHXB201607291 shu

Preparation of Highly Dispersed Ni-Ce-Zr Oxides over Mesoporous γ-Alumina and Their Catalytic Properties for CO₂ Methanation

Shanghai Key Laboratory of Advanced Ferrometallurgy, State Key Laboratory of Advanced Special Steel, School of Materials Science and Engineering, Shanghai University, Shanghai 200072, P. R. China

Received Date: 2 June 2016
Revised Date: 28 July 2016

Fund Project: The project was supported by the Innovation Program of Shanghai Municipal Education Commission, National Key Basic Research Program of China (973) (2014CB643403), National Science Fund for Distinguished Young Scholars, China (51225401), and Basic Major Research Program of Science and Technology Commission Foundation of Shanghai, China (14JC1491400).

Highly dispersed Ni-Ce-Zr mixed oxides supported on mesoporous γ-alumina (Ni-Ce-Zr/γ-MA) were prepared by a citric acid (CA)-assisted impregnation method and evaluated as catalysts for the methanation of CO₂ with H₂. The effects of the CA content of the reaction solution on the physicochemical properties and the catalytic performance of the Ni-Ce-Zr/γ-MA catalysts were investigated in detail. The addition of CA promoted the dispersion of the Ni-Ce-Zr oxide species on the γ-alumina surface and improved the interactions between the Ni oxide species and the support, resulting in the formation of homogeneously dispersed Ni nanoparticles in the γ-MA frameworks upon reduction with H₂. The resulting Ni-Ce-Zr/γ-MA catalysts were highly active and showed almost 100% selectivity for CH4 during the methanation of CO₂ at temperatures in the range of 150-400℃. Notably, the catalytic activity increased as the molar ratio of CA/(Ni+Ce+Zr) increased in the range of 0-2. This effect was most likely caused by the associated decrease in the Ni particle size and the improved electronic and structural properties of the Ni-Ce-ZrO_x species. The results of a stability test for the Ni-Ce-Zr/γ-MA catalyst prepared with a CA/(Ni+Ce+Zr) molar ratio of 1.0 showed that there was only a 7% decrease in the CO₂ conversion following a reaction time of 300 h at 300℃ with negligible coke deposition, indicating excellent catalytic stability and good anti-coking ability of these systems for the methanation of CO₂.
- Nickel catalyst,
- Citric acid-assistance,
- Mixed metal oxide,
- Carbon dioxide,
- Methanation
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Preparation of Highly Dispersed Ni-Ce-Zr Oxides over Mesoporous γ-Alumina and Their Catalytic Properties for CO₂ Methanation