Citation: Hongmei Ai, Hongyuan Yang, Qing Liu, Guoming Zhao, Jing Yang, Fangna Gu. ZrO₂-modified Ni/LaAl₁₁O₁₈ catalyst for CO methanation:Effects of catalyst structure on catalytic performance[J]. Chinese Journal of Catalysis, ;2018, 39(2): 297-308. doi: 10.1016/S1872-2067(17)62995-4 shu

ZrO₂-modified Ni/LaAl₁₁O₁₈ catalyst for CO methanation:Effects of catalyst structure on catalytic performance

Hongmei Ai ^a,b, ,
Hongyuan Yang ^a ,
Qing Liu ^a ,
Guoming Zhao ^a ,
Jing Yang ^a ,
Fangna Gu ^c

a Key Laboratory of Low Carbon Energy and Chemical Engineering, College of Chemical and Environmental Engineering, Shandong University of Science and Technology, Qingdao 266590, Shandong, China;
b Assets Management Division, Shandong University of Science and Technology, Qingdao 266590, Shandong, China;
c State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China

Received Date: 26 September 2017
Revised Date: 11 December 2017

Fund Project: This work was supported by the National Natural Science Foundation of China (21606146), Natural Science Foundation of Shandong Province (ZR2016BB17, 2016ZRB01037), Scientific Research Foundation of Shandong University of Science and Technology for Recruited Talents (2016RCJJ005, 2016RCJJ006), Government Sponsored Visiting Scholar Foundation of Shandong University of Science and Technology (2016), Qingdao Postdoctoral Applied Research Project (2015202), and China National Coal Association Science and Technology Research Program (MTKJ2016-266).

We report Ni/LaHA@ZrO₂ catalysts prepared by a facile modified successive adsorption and reaction method for CO methanation. N₂ adsorption, X-ray diffraction, transmission electron microscopy, scanning electron microscopy, thermogravimetric analysis, H₂ temperature-programmed reduction, H₂ temperature-programmed desorption, X-ray photoelectron spectroscopy, thermogravimetric analysis, and inductively coupled plasma atomic emission spectrometry were used to characterize the samples. The results indicated that the ZrO₂ nanoparticles were distributed over the surface of the Ni/LaHA@ZrO₂ catalyst and even partially covered some Ni particles, resulting in the coating exerting a confinement effect. The excess ZrO₂ had an adverse effect on the enhancement of CO conversion because of the coverage of the surface Ni particles; however, the Ni/LaHA@ZrO₂ catalyst displayed much higher CH₄ selectivity than Ni/LaHA because of the activation of the byproduct CO₂ molecules by ZrO₂ species. Therefore, even though 20Ni/LaHA@ZrO₂-5 exhibited similar CO conversion as 20Ni/LaHA, the use of the former resulted in a higher CH₄ yield than the use of the latter. A 107-h-lifetime test revealed that the Ni/LaHA@ZrO₂ catalyst was highly stable with superior anti-sintering and anti-coking properties because of its coating structure and the promoter effect of ZrO₂.
- Lanthanum hexaaluminate,
- ZrO₂,
- Nickel catalyst,
- Coating structure,
- CO methanation
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ZrO₂-modified Ni/LaAl₁₁O₁₈ catalyst for CO methanation:Effects of catalyst structure on catalytic performance