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Coupling non-thermal plasma with Ni catalysts supported on BETA zeolite for catalytic CO2 methanation
Chen, Huanhao1; Mu, Yibing1; Shao, Yan1,2; Chansai, Sarayute1; Xu, Shaojun1; Stere, Cristina E.1; Xiang, Huan1; Zhang, Rongxin1; Jiao, Yilai3; Hardacre, Christopher1; Fan, Xiaolei1
Corresponding AuthorChen, Huanhao(huanhao.chen@manchester.ac.uk) ; Hardacre, Christopher(c.hardacre@manchester.ac.uk) ; Fan, Xiaolei(xiaolei.fan@manchester.ac.uk)
2019-08-07
Source PublicationCATALYSIS SCIENCE & TECHNOLOGY
ISSN2044-4753
Volume9Issue:15Pages:4135-4145
AbstractCatalytic carbon dioxide (CO2) methanation is a promising and effective process for CO2 utilisation and the production of CH4 as an alternative to using natural gas. Non-thermal plasma (NTP) activation has been proven to be highly effective in overcoming the thermodynamic limitation of reactions under mild conditions and intensifying the CO2 hydrogenation process greatly. Herein, we present an example of NTP-assisted catalytic CO2 methanation over Ni catalysts (15 wt%) supported on BETA zeolite employing lanthana (La) as the promoter. It was found that a NTP-assisted system presents remarkable catalytic performance in catalytic CO2 methanation without an external heat source. Significantly, the use of Na-form BETA zeolite and the addition of La (i.e. 15Ni-20La/Na-BETA catalyst) resulted in an improvement in CO2 conversions, surpassing the 15Ni/H-BETA catalyst, i.e. a seven-fold increase in the turnover frequency, TOF (1.45 s(-1)vs. 0.21 s(-1)), and selectivity towards CH4 (up to ca. 97%). In addition, the developed catalyst also exhibited excellent stability under NTP conditions, i.e. a stable performance over a 15 h longevity test (with a TOF of 1.44 +/- 0.01 s(-1)). Comparative in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) characterisation of the developed catalysts revealed that the introduction of La2O3 to the Ni catalyst provides more surface hydroxyl groups, and hence enhances CO2 methanation. Additionally, by analysing the surface species over 15Ni-20La/Na-BETA comparatively under thermal and NTP conditions (by in situ DRIFTS analysis), it is proposed that both the Langmuir-Hinshelwood and Eley-Rideal mechanisms co-exist in the NTP system due to the presence of dissociated H species in the gas phase. Conversely, for the thermal system, the reaction has to go through reactions between the surface-dissociated H and carbonate-like adsorbed CO(2)via the Langmuir-Hinshelwood mechanism. The current mechanistic understanding of the NTP-activated system paves the way for the exploration of the reaction mechanisms/pathways of NTP-assisted catalytic CO2 methanation.
Funding OrganizationEuropean Commission Marie Skodowska-Curie Individual Fellowship ; University of Manchester President's Doctoral Scholar (PDS) Award ; China Scholarship Council (CSC) ; CSC ; Foundation of Department of Education of Guangdong Province
DOI10.1039/c9cy00590k
Indexed BySCI
Language英语
Funding ProjectEuropean Commission Marie Skodowska-Curie Individual Fellowship[H2020-MSCA-IF-NTPleasure-748196] ; University of Manchester President's Doctoral Scholar (PDS) Award ; China Scholarship Council (CSC)[201606150068] ; CSC[201708440477] ; Foundation of Department of Education of Guangdong Province[2017KZDXM085]
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:000484168400027
PublisherROYAL SOC CHEMISTRY
Citation statistics
Cited Times:20[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/135304
Collection中国科学院金属研究所
Corresponding AuthorChen, Huanhao; Hardacre, Christopher; Fan, Xiaolei
Affiliation1.Univ Manchester, Sch Chem Engn & Analyt Sci, Manchester M13 9PL, Lancs, England
2.Wuyi Univ, Sch Biotechnol & Hlth Sci, Hangmen 52920, Peoples R China
3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China
Recommended Citation
GB/T 7714
Chen, Huanhao,Mu, Yibing,Shao, Yan,et al. Coupling non-thermal plasma with Ni catalysts supported on BETA zeolite for catalytic CO2 methanation[J]. CATALYSIS SCIENCE & TECHNOLOGY,2019,9(15):4135-4145.
APA Chen, Huanhao.,Mu, Yibing.,Shao, Yan.,Chansai, Sarayute.,Xu, Shaojun.,...&Fan, Xiaolei.(2019).Coupling non-thermal plasma with Ni catalysts supported on BETA zeolite for catalytic CO2 methanation.CATALYSIS SCIENCE & TECHNOLOGY,9(15),4135-4145.
MLA Chen, Huanhao,et al."Coupling non-thermal plasma with Ni catalysts supported on BETA zeolite for catalytic CO2 methanation".CATALYSIS SCIENCE & TECHNOLOGY 9.15(2019):4135-4145.
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