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Methanation of CO2 over Ni/Al2O3 modified with alkaline earth metals: Impacts of oxygen vacancies on catalytic activity
Liang, CF (Liang, Chuanfei)[ 1 ]; Hu, X (Hu, Xun)[ 1 ]; Wei, T (Wei, Tao)[ 1 ]; Jia, P (Jia, Peng)[ 1 ]; Zhang, ZM (Zhang, Zhanming)[ 1 ]; Dong, DH (Dong, Dehua)[ 1 ]; Zhang, S (Zhang, Shu)[ 2 ]; Liu, Q (Liu, Qing)[ 3 ]; Hu, GZ (Hu, Guangzhi)[ 4 ]
2019
Source PublicationINTERNATIONAL JOURNAL OF HYDROGEN ENERGY
ISSN0360-3199
Volume44Issue:16Pages:8197-8213
Abstract

This study investigates the impacts of the alkaline earth metal (Mg, Ca, Sr, Ba) additives on properties and performances of nickel catalysts for CO2 methanation. The results show that addition of Mg, Sr, and Ba creates more pores while Ca addition leads to merge of small pores. The alkalinity of the catalyst increases with the addition of Mg, Ca, Sr or Ba, however, it does not necessarily enhance the catalytic activity. The degree of reduction of nickel species is another important factor affecting catalyst activity. Mg or Ca addition promotes the reverse water gas shift reaction to form more CO but not the methanation. In converse, with the addition of Sr or Ba, the activities for methanation increased drastically, especially in the low temperature region. In situ Diffuse Reflection Infrared Fourier Transform Spectroscopy (DRIFTS) studies show that *OH, *CO3, *CO2, -CHx, HCOO*, *CO and H2CO* species are main reaction intermediates. Mg or Ca promotes the carbonate formation. Sr or Ba promotes *CO and H2CO* formation, which are the important reaction intermediates in the conversion of CO2 to CH4. In addition, the Electron Paramagnetic Resonance (EPR) characterization shows that the catalyst modified with Sr species generates the oxygen vacancies that prevent electrons from being paired, forming a Lewis basic position. The oxygen vacancies generated are crucial for enhancing the catalytic activities for methanation at the low reaction temperatures.

KeywordMethanation of CO2 Alkaline earth metals Reaction intermediates Oxygen vacancies DRIFTS and EPR study
DOI10.1016/j.ijhydene.2019.02.014
Indexed BySCI
WOS IDWOS:000463688600028
Citation statistics
Document Type期刊论文
Identifierhttp://ir.xjipc.cas.cn/handle/365002/5728
Collection省部共建新疆特有药用资源利用重点实验室
Affiliation1.Univ Jinan, Sch Mat Sci & Engn, Jinan 250022, Shandong, Peoples R China
2.Nanjing Forestry Univ, Coll Mat Sci & Engn, Nanjing 210037, Jiangsu, Peoples R China
3.Shandong Univ Sci & Technol, Coll Chem & Environm Engn, Key Lab Low Carbon Energy & Chem Engn, Qingdao 266590, Shandong, Peoples R China
4.Chinese Acad Sci, Xinjiang Tech Inst Phys & Chem, Key Lab Chem Plant Resources Arid Reg, State Key Lab Basis Xinjiang Indigenous Med Plant, Urumqi 830011, Peoples R China
Recommended Citation
GB/T 7714
Liang, CF ,Hu, X ,Wei, T ,et al. Methanation of CO2 over Ni/Al2O3 modified with alkaline earth metals: Impacts of oxygen vacancies on catalytic activity[J]. INTERNATIONAL JOURNAL OF HYDROGEN ENERGY,2019,44(16):8197-8213.
APA Liang, CF .,Hu, X .,Wei, T .,Jia, P .,Zhang, ZM .,...&Hu, GZ .(2019).Methanation of CO2 over Ni/Al2O3 modified with alkaline earth metals: Impacts of oxygen vacancies on catalytic activity.INTERNATIONAL JOURNAL OF HYDROGEN ENERGY,44(16),8197-8213.
MLA Liang, CF ,et al."Methanation of CO2 over Ni/Al2O3 modified with alkaline earth metals: Impacts of oxygen vacancies on catalytic activity".INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 44.16(2019):8197-8213.
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