Ni/Al2O3 catalysts for CO methanation：Effect of Al2O3 supports calcined at different temperatures

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (6): 919-927.

Ni/Al₂O₃ catalysts for CO methanation：Effect of Al₂O₃ supports calcined at different temperatures

Jiajian Gao^a,b, Chunmiao Jia^a, Jing Li^a, Meiju Zhang^a, Fangna Gu^a, Guangwen Xu^a, Ziyi Zhong^c, Fabing Su^a

a. State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
b. University of Chinese Academy of Sciences, Beijing 100049, China;
c. Institute of Chemical Engineering and Sciences, A^*star, 1 Pesek Road, Jurong Island 627833, Singapore

收稿日期:2013-01-04 修回日期:2013-03-21 出版日期:2013-11-20 发布日期:2013-11-28
通讯作者: Fangna Gu, Fabing Su
基金资助:
This work was supported by the Hundred Talents Program of the Chinese Academy of Sciences (CAS), State Key Laboratory of Multiphase Complex Systems of China (No. MPCS-2009-C-01), the National Key Technology R&D Program of China (No. 2010BAC66B01), and the Knowledge Innovation Program of the CAS (No. KGCX2-YW-396).F. Gu is grateful to the support of K. C. Wang Post-doctoral Fellowships of the CAS and China Postdoctoral Science Foundation (No. 20100480026 and 201104151).

Ni/Al₂O₃ catalysts for CO methanation：Effect of Al₂O₃ supports calcined at different temperatures

Jiajian Gao^a,b, Chunmiao Jia^a, Jing Li^a, Meiju Zhang^a, Fangna Gu^a, Guangwen Xu^a, Ziyi Zhong^c, Fabing Su^a

a. State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
b. University of Chinese Academy of Sciences, Beijing 100049, China;
c. Institute of Chemical Engineering and Sciences, A^*star, 1 Pesek Road, Jurong Island 627833, Singapore

Received:2013-01-04 Revised:2013-03-21 Online:2013-11-20 Published:2013-11-28
Supported by:
This work was supported by the Hundred Talents Program of the Chinese Academy of Sciences (CAS), State Key Laboratory of Multiphase Complex Systems of China (No. MPCS-2009-C-01), the National Key Technology R&D Program of China (No. 2010BAC66B01), and the Knowledge Innovation Program of the CAS (No. KGCX2-YW-396).F. Gu is grateful to the support of K. C. Wang Post-doctoral Fellowships of the CAS and China Postdoctoral Science Foundation (No. 20100480026 and 201104151).

摘要/Abstract

摘要： The correlation between phase structures and surface acidity of Al₂O₃ supports calcined at different temperatures and the catalytic performance of Ni/Al₂O₃ catalysts in the production of synthetic natural gas (SNG) via CO methanation was systematically investigated. A series of 10 wt% NiO/Al₂O₃ catalysts were prepared by the conventional impregnation method, and the phase structures and surface acidity of Al₂O₃ supports were adjusted by calcining the commercial γ-Al₂O₃ at different temperatures (600-1200 ℃). CO methanation reaction was carried out in the temperature range of 300-600 ℃ at different weight hourly space velocities (WHSV = 30000 and 120000 mL·g^-1·h^-1) and pressures (0.1 and 3.0 MPa). It was found that high calcination temperature not only led to the growth in Ni particle size, but also weakened the interaction between Ni nanoparticles and Al₂O₃ supports due to the rapid decrease of the specific surface area and acidity of Al₂O₃ supports. Interestingly, Ni catalysts supported on Al₂O₃ calcined at 1200 ℃ (Ni/Al₂O₃-1200) exhibited the best catalytic activity for CO methanation under different reaction conditions. Lifetime reaction tests also indicated that Ni/Al₂O₃-1200 was the most active and stable catalyst compared with the other three catalysts, whose supports were calcined at lower temperatures (600, 800 and 1000 ℃). These findings would therefore be helpful to develop Ni/Al₂O₃ methanation catalyst for SNG production.

关键词: Ni catalyst, alumina, CO methanation, synthetic natural gas, carbon deposition

Abstract: The correlation between phase structures and surface acidity of Al₂O₃ supports calcined at different temperatures and the catalytic performance of Ni/Al₂O₃ catalysts in the production of synthetic natural gas (SNG) via CO methanation was systematically investigated. A series of 10 wt% NiO/Al₂O₃ catalysts were prepared by the conventional impregnation method, and the phase structures and surface acidity of Al₂O₃ supports were adjusted by calcining the commercial γ-Al₂O₃ at different temperatures (600-1200 ℃). CO methanation reaction was carried out in the temperature range of 300-600 ℃ at different weight hourly space velocities (WHSV = 30000 and 120000 mL·g^-1·h^-1) and pressures (0.1 and 3.0 MPa). It was found that high calcination temperature not only led to the growth in Ni particle size, but also weakened the interaction between Ni nanoparticles and Al₂O₃ supports due to the rapid decrease of the specific surface area and acidity of Al₂O₃ supports. Interestingly, Ni catalysts supported on Al₂O₃ calcined at 1200 ℃ (Ni/Al₂O₃-1200) exhibited the best catalytic activity for CO methanation under different reaction conditions. Lifetime reaction tests also indicated that Ni/Al₂O₃-1200 was the most active and stable catalyst compared with the other three catalysts, whose supports were calcined at lower temperatures (600, 800 and 1000 ℃). These findings would therefore be helpful to develop Ni/Al₂O₃ methanation catalyst for SNG production.

Key words: Ni catalyst, alumina, CO methanation, synthetic natural gas, carbon deposition

Jiajian Gao, Chunmiao Jia, Jing Li, Meiju Zhang, Fangna Gu, Guangwen Xu, Ziyi Zhong, Fabing Su. Ni/Al₂O₃ catalysts for CO methanation：Effect of Al₂O₃ supports calcined at different temperatures[J]. 能源化学(英文), 2013, 22(6): 919-927.

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Ni/Al₂O₃ catalysts for CO methanation：Effect of Al₂O₃ supports calcined at different temperatures

Ni/Al₂O₃ catalysts for CO methanation：Effect of Al₂O₃ supports calcined at different temperatures

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