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CO Poisoning of Ru Catalysts in CO2 Hydrogenation under Thermal and Plasma Conditions: A Combined Kinetic and Diffuse Reflectance Infrared Fourier Transform Spectroscopy-Mass Spectrometry Study
Xu, Shanshan1; Chansai, Sarayute1; Xu, Shaojun2,3; Stere, Cristina E.1; Jiao, Yilai4; Yang, Sihai5; Hardacre, Christopher1; Fan, Xiaolei1
Corresponding AuthorHardacre, Christopher(c.hardacre@manchester.ac.uk) ; Fan, Xiaolei(xiaolei.fan@manchester.ac.uk)
2020-11-06
Source PublicationACS CATALYSIS
ISSN2155-5435
Volume10Issue:21Pages:12828-12840
AbstractPlasma-catalysis systems are complex and require further understanding to advance the technology. Herein, CO poisoning in CO2 hydrogenation over supported ruthenium (Ru) catalysts in a nonthermal plasma (NTP)-catalysis system was investigated by a combined kinetic and diffuse reflectance infrared Fourier transform spectroscopy-mass spectrometry (DRIFTS-MS) study and compared with the thermal catalytic system. The relevant findings suggest the coexistence of the Langmuir-Hinshelwood and Eley-Rideal mechanisms in the NTP-catalysis. Importantly, comparative study of CO poisoning of the Ru catalyst was performed under the thermal and NTP conditions, showing the advantage of the hybrid NTP-catalysis system over the thermal counterpart to mitigate CO poisoning of the catalyst. Specifically, compared with the CO poisoning in thermal catalysis due to strong CO adsorption and associated metal sintering, in situ DRIFTS-MS analysis revealed that the collisions of reactive plasma-derived species in NTP-catalysis could remove the strongly adsorbed carbon species to recover the active sites for CO2 activation. Thus, the NTP-catalysis was capable of preventing CO poisoning of the Ru catalyst in CO2 hydrogenation. Additionally, under the NTP conditions, the NTP-enabled water-gas shift reaction of CO with H2O (which was produced by CO/CO2 hydrogenation) shifted the equilibrium of CO2 hydrogenation toward CH4 production.
Keywordnonthermal plasma (NTP) catalysis CO poisoning Ru catalyst CO2 hydrogenation kinetics DRIFTS-MS
Funding OrganizationDean's Doctoral Scholar Awards from the University of Manchester ; EPSRC
DOI10.1021/acscatal.0c03620
Indexed BySCI
Language英语
Funding ProjectDean's Doctoral Scholar Awards from the University of Manchester ; EPSRC[EP/R026939/1] ; EPSRC[EP/R026815/1] ; EPSRC[EP/R026645/1] ; EPSRC[EP/R027129/1] ; EPSRC[EP/M013219/1]
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:000589939900042
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:36[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/158922
Collection中国科学院金属研究所
Corresponding AuthorHardacre, Christopher; Fan, Xiaolei
Affiliation1.Univ Manchester, Dept Chem Engn & Analyt Sci, Sch Engn, Manchester M13 9PL, Lancs, England
2.UK Catalysis Hub, Res Complex & Harwell, Didcot OX11 0FA, Oxon, England
3.Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, Wales
4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
5.Univ Manchester, Sch Nat Sci, Dept Chem, Manchester M13 9PL, Lancs, England
Recommended Citation
GB/T 7714
Xu, Shanshan,Chansai, Sarayute,Xu, Shaojun,et al. CO Poisoning of Ru Catalysts in CO2 Hydrogenation under Thermal and Plasma Conditions: A Combined Kinetic and Diffuse Reflectance Infrared Fourier Transform Spectroscopy-Mass Spectrometry Study[J]. ACS CATALYSIS,2020,10(21):12828-12840.
APA Xu, Shanshan.,Chansai, Sarayute.,Xu, Shaojun.,Stere, Cristina E..,Jiao, Yilai.,...&Fan, Xiaolei.(2020).CO Poisoning of Ru Catalysts in CO2 Hydrogenation under Thermal and Plasma Conditions: A Combined Kinetic and Diffuse Reflectance Infrared Fourier Transform Spectroscopy-Mass Spectrometry Study.ACS CATALYSIS,10(21),12828-12840.
MLA Xu, Shanshan,et al."CO Poisoning of Ru Catalysts in CO2 Hydrogenation under Thermal and Plasma Conditions: A Combined Kinetic and Diffuse Reflectance Infrared Fourier Transform Spectroscopy-Mass Spectrometry Study".ACS CATALYSIS 10.21(2020):12828-12840.
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