期刊
FUEL
卷 262, 期 -, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2019.116521
关键词
Methanation of CO2; Basic sites; Acidic sites; Synergistic effects; Reaction intermediates
资金
- Strategic International Scientific and Technological Innovation Cooperation Special Funds of National Key R & D Program of China [2016YFE0204000]
- Program for Taishan Scholars of Shandong Province Government
- Recruitment Program of Global Young Experts (Thousand Youth Talents Plan)
- Natural Science Fund of Shandong Province [ZR2017BB002]
- Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong
Methanation of carbon oxides is an important route to produce synthetic gas for civil use. Understanding acidic/basic properties of catalyst on the reaction intermediates in methanation provides important information for developing highly active catalysts. In this study, the Ni/Al2O3, Ni/SiO2 and Ni/H beta 40 catalysts with varied distribution of acidic/basic sites were prepared and evaluated. The results indicated the importance of basic/acidic sites in determining the catalytic activities and the reaction intermediates formed. Ni/SiO2 and Ni/H beta 40 with medium to strong basic sites were far more active and selective than the Ni/Al2O3 in CO2 methanation. The in situ Diffuse Reflection Infrared Fourier Transform Spectroscopy (DRIFTS) study indicated that formate species, the important reaction intermediate for CH4 formation, was absent over Ni/H beta 40 and Ni/SiO2 while was accumulated over Ni/Al2O3, relating to presence of the positively charged Lewis acidic sites that had a strong affinity to the negatively charged formate species, deterring subsequent conversion of formate to CH4. In addition, the absorption of *CO over Ni/H beta 40 and Ni/SiO2 facilitated its activation and further conversion to methane, resulting in low CO selectivity and low tendency towards coking.
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