Impacts of La addition on formation of the reaction intermediates over alumina and silica supported nickel catalysts in methanation of CO2 |
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| Affiliation: | 1. School of Material Science and Engineering, University of Jinan, Jinan, 250022, PR China;2. College of Materials Science and Engineering, Nanjing Forestry University, Nanjing, 210037, PR China;3. Key Laboratory of Low Carbon Energy and Chemical Engineering, College of Chemical and Environmental Engineering, Shandong University of Science and Technology, Qingdao, 266590, PR China;4. School of Chemical Science and Technology, Key Laboratory of Medicinal Chemistry for Nature Resource, Ministry of Education, Yunnan University, Kunming, 650091, PR China;1. Collaborative Innovation Center of the Atmospheric Environment and Equipment Technology, School of Environmental Science and Engineering, Nanjing University of Information Science & Technology, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, 210044 Nanjing, China;2. College of Light Industry and Food Engineering, Nanjing Forestry University, Nanjing 210037, China;3. School of Chemistry and Chemical Engineering, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, China;4. School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, China;5. School of Material Science and Engineering, University of Jinan, Jinan 250022, China;6. CAS Key Laboratory of Bio-Based Materials, Qingdao Institute of Bioenergy and Bioprocess Technology (QIBEBT), Chinese Academy of Sciences(CAS), Qingdao 266101, China;1. School of Resources and Environmental Sciences, Wuhan University, Wuhan 430079, PR China;2. International Cooperation Base for Sustainable Utilization of Resources and Energy in Hubei Province, Wuhan 430072, PR China;1. Department of Catalysis Science and Technology, School of Chemical Engineering, Tianjin University, Tianjin 300350, China;2. Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, PR China;3. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, China;1. Department of Physics, South China University of Technology, Guangzhou 510640, China;2. School of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China;3. Key Laboratory of Advanced Energy Storage Materials of Guangdong Province, South China University of Technology, Guangzhou 510640, China;1. Institute of Hydrogen Economy, Universiti Teknologi Malaysia, 81310 UTM Johor Bahru, Johor, Malaysia;2. Department of Chemical Engineering, Faculty of Chemical Engineering, Universiti Teknologi Malaysia, 81310 UTM Johor Bahru, Johor, Malaysia;3. Department of Chemistry, Faculty of Science, Universiti Teknologi Malaysia, 81310 UTM Johor Bahru, Johor, Malaysia;1. Key Laboratory of Low Carbon Energy and Chemical Engineering, Shandong University of Science and Technology, Qingdao, 266590, China;2. Schneider Electric (China) Co., Ltd., Beijing, 100102, China;3. College of Marxism, Shandong University of Science and Technology, Qingdao, 266590, China |
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| Abstract: | This study aimed to investigate impacts of Al2O3 and SiO2, the supports of Ni catalysts with distinct properties, and the additive of La on catalytic behaviors and reaction intermediates formed during methanation of CO2. The results showed that the addition of La to either Ni/Al2O3 or Ni/SiO2 led to the reduced size of metallic nickel, the reduced reduction degree of nickel oxide, the increased alkalinity number and the increased activity for methanation of CO2. Furthermore, the addition of La to the Ni/SiO2 catalyst could suppress the formation of CO via the reverse water gas shift (RWGS) reaction. Ni/SiO2 was much more active than the Ni/Al2O3, even though nickel size was much bigger. The in situ Diffuse Reflection Infrared Fourier Transform Spectroscopy (DRIFTS) studies showed that the addition of La to Ni/Al2O3 interfered with integration of hydroxyl group with *CO2 species and formation of the bicarbonate and carbonate, while favored formation of the formate specie, enhancing the catalytic activity. For Ni/SiO2, instead of formate, CO* became the main reaction intermediate. The strong absorption of CO* favored its further conversion and explained the low selectivity of the silica-based catalysts toward CO. The addition of La to Ni/SiO2 catalyst facilitated further hydrogenation of CO* species to CH4 and promoted the catalytic activity. |
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| Keywords: | La promoter Reaction intermediates In situ DRIFTS Different supports |
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