Coking-resistant Ni-ZrO2/Al2O3 catalyst for CO methanation

被引:64
作者
Liu, Qing [1 ]
Gu, Fangna [1 ]
Gao, Jiajian [1 ]
Li, Huifang [1 ]
Xu, Guangwen [1 ]
Su, Fabing [1 ]
机构
[1] Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China
基金
中国国家自然科学基金;
关键词
Ni/gamma-Al2O3; ZrO2; coke resistance; syngas methanation; NI/AL2O3; CATALYSTS; SYNGAS PRODUCTION; NI/ZRO2; CATALYST; NATURAL-GAS; OVEN GAS; NI-AL2O3; SUPPORTS;
D O I
10.1016/S2095-4956(14)60210-2
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Highly coke-resisting ZrO2-decorated Ni/Al2O3 catalysts for CO methanation were prepared by a two-step process. The support was first loaded with NiO by impregnating method and then modified with ZrO2 by deposition-precipitation method (IM-DP). Nitrogen adsorption-desorption, X-ray diffraction, scanning electron microscopy, transmission electron microscopy, thermogravimetric analysis, H-2 temperature-programmed reduction and desorption, NH3 temperature-programmed desorption, and zeta potential analysis were employed to characterize the samples. The results revealed that, compared with the catalysts with the same composition prepared by co-impregnation (CI) and sequential impregnation (SI) methods, the Ni/Al2O3 catalyst prepared by IM-DP showed much enhanced catalytic performance for syngas methanation under the condition of atmospheric pressure and a high weight hourly space velocity of 120000 mL.g(-1).h(-1). In a 80 h life time test under the condition of 300-600 degrees C and 3.0 MPa, this catalyst showed high stability and resistance to coking, and the amount of deposited carbon was only 0.4 wt%. On the contrary, the deposited carbon over the catalyst without ZrO2 reached 1.5 wt% after a 60 h life time test. The improved catalytic performance was attributed to the selective deposition of ZrO2 nanoparticles on the surface of NiO rather than Al2O3, which could be well controlled via changing the electrostatic interaction in the DP procedure. This unique structure could enhance the dissociation of CO2 and generate surface oxygen intermediates, thus preventing carbon deposition on the Ni particles in syngas methanation.
引用
收藏
页码:761 / 770
页数:10
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