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The Insights into Chlorine Doping Effect on Performance of Ceria Supported Nickel Catalysts for Selective CO Methanation Full article

Journal Applied Catalysis B: Environmental
ISSN: 0926-3373 , E-ISSN: 1873-3883
Output data Year: 2018, Volume: 221, Pages: 413-421 Pages count : 9 DOI: 10.1016/j.apcatb.2017.09.038
Tags Cerium oxychloride, CO cleanup, Effect of chlorine doping, Hydrogen-rich gas, Nickel ceria catalysts, Reformate, Selective or preferential CO methanation
Authors Konishcheva M.V. 1,2 , Potemkin D.I. 1,2 , Snytnikov P.V. 1,2 , Stonkus O.A. 1 , Belyaev V.D. 1 , Sobyanin V.A. 1
Affiliations
1 Boreskov Institute of Catalysis, Pr. Lavrentieva, 5, Novosibirsk, 630090, Russia
2 Novosibirsk State University, Pirogova St., 2, Novosibirsk, 630090, Russia

Funding (2)

1 Federal Agency for Scientific Organizations 0303-2016-0011
2 Council for Grants of the President of the Russian Federation СП-922.2016.1

Abstract: Selective CO methanation (CO-SMET) in the reformate gas, containing (vol.%): 1.0 CO, 65H2, 10H2O, 20 CO2 with He as balance, was investigated over a number of nickel-ceria catalysts: treated with NH4Cl before (Ni/CeO2(Cl*)) and after (Ni(Cl*)/CeO2) Ni deposition, prepared by Cl-containing Ni precursor (Ni(Cl)/CeO2) and Cl-free one (Ni/CeO2). The effect of residual chlorine, originating from the catalyst preparation procedures, on the activity and CO selectivity of the samples was demonstrated. It was shown that all Cl-containing Ni/CeO2 catalysts provided efficient CO cleanup. They provided the removal of CO from reformate gas to the level below 10 ppm with a selectivity up to 90%. The catalyst characterization by BET, XRD, XPS, HAADF-STEM, EDX-mapping, FTIR in situ and CO chemisorption techniques revealed that the decrease in chlorine content in the order Ni(Cl)/CeO2 ≥ Ni(Cl*)/CeO2 > Ni/CeO2(Cl*) was accompanied by the increase of Ni dispersion that most likely provided high performance of Ni/CeO2(Cl*) in CO-SMET. The turnover frequencies of Ni surface atoms as well as activation energies in CO methanation were practically similar for all studied catalysts, indicating that Cl did not influence catalyst’s activity and CO methanation proceeded by similar ways over Ni surface in both Cl-free and Cl-containing samples. The advanced performance of Cl-containing catalysts was associated with the inhibition of undesirable side reaction of CO2 methanation. The chlorine doping effect was attributed to the blockage of surface Ce3+-coupled oxygen vacancy sites by CeOCl species that inhibited ceria-assisted CO2 activation and hydrogenation. The CeO2 treatment with NH4Cl before Ni deposition allows to prepare highly active and selective CO-SMET catalyst with high nickel dispersion and Cl-modified ceria surface.
Cite: Konishcheva M.V. , Potemkin D.I. , Snytnikov P.V. , Stonkus O.A. , Belyaev V.D. , Sobyanin V.A.
The Insights into Chlorine Doping Effect on Performance of Ceria Supported Nickel Catalysts for Selective CO Methanation
Applied Catalysis B: Environmental. 2018. V.221. P.413-421. DOI: 10.1016/j.apcatb.2017.09.038 WOS Scopus РИНЦ ANCAN OpenAlex
Dates:
Submitted: Jul 13, 2017
Accepted: Sep 16, 2017
Published online: Sep 20, 2017
Published print: Feb 1, 2018
Identifiers:
Web of science: WOS:000414109700042
Scopus: 2-s2.0-85029677202
Elibrary: 31055811
Chemical Abstracts: 2017:1554368
Chemical Abstracts (print): 167:531900
OpenAlex: W2755377127
Citing:
DB Citing
Web of science 44
Scopus 48
Elibrary 44
OpenAlex 48
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