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

doi:10.1021/acscatal.0c03620

IMR OpenIR

	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, Shanshan 1; Chansai, Sarayute 1; Xu, Shaojun 2,3; Stere, Cristina E.1; Jiao, Yilai 4; Yang, Sihai 5; Hardacre, Christopher 1; Fan, Xiaolei 1
通讯作者	Hardacre, Christopher(c.hardacre@manchester.ac.uk) ; Fan, Xiaolei(xiaolei.fan@manchester.ac.uk)
	2020-11-06
发表期刊	ACS CATALYSIS
ISSN	2155-5435
卷号	10 期号:21 页码:12828-12840
摘要	Plasma-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.
关键词	nonthermal plasma (NTP) catalysis CO poisoning Ru catalyst CO2 hydrogenation kinetics DRIFTS-MS
资助者	Dean's Doctoral Scholar Awards from the University of Manchester ; EPSRC
DOI	10.1021/acscatal.0c03620
收录类别	SCI
语种	英语
资助项目	Dean'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研究方向	Chemistry
WOS类目	Chemistry, Physical
WOS记录号	WOS:000589939900042
出版者	AMER CHEMICAL SOC
引用统计	被引频次：70[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/158922
专题	中国科学院金属研究所
通讯作者	Hardacre, Christopher; Fan, Xiaolei
作者单位	1.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
推荐引用方式 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.