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Metal-Catalyzed Chemical Activation of Calcium Carbide: New Way to Hierarchical Metal/Alloy-on-Carbon Catalysts Full article

Journal Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694
Output data Year: 2022, Volume: 407, Pages: 281-289 Pages count : 9 DOI: 10.1016/j.jcat.2022.01.034
Tags supported catalyst, metal-on-carbon, Pd/C, Pd alloy catalyst, calcium carbide
Authors Lebedev Andrey N. 1 , Rodygin Konstantin S. 1 , Mironenko Roman M. 2 , Saybulina Elina R. 2 , Ananikov Valentine P. 1,2,3
Affiliations
1 Saint Petersburg State University, Universitetsky pr. 26, Saint Petersburg 198504, Russia
2 Center of New Chemical Technologies BIC, Neftezavodskaya st. 54, Omsk 644040, Russia
3 N.D. Zelinsky Institute of Organic Chemistry, Leninsky pr. 47, Moscow 119991, Russia

Funding (2)

1 Ministry of Science and Higher Education of the Russian Federation 0239-2021-0004
2 Russian Science Foundation 21-73-20003 (121040100067-8)

Abstract: A simple and efficient strategy for the synthesis of “metal/alloy-on-carbon” catalysts was developed. A highly ordered extra pure graphite-like carbon material as a catalyst support was obtained after calcium carbide decomposition at 700 °C in a stream of gaseous chlorine. When Pd, Pt, Ag, Au, Co, Ni, Fe, Cu salts were added to calcium carbide prior to decomposition, a metal was reduced from a salt by elemental carbon, despite an oxidizing atmosphere. Metal particles were formed on the surface of the layered carbon material, covered with a thin layer of high-purity carbon and partially immersed in it. A catalytically active remaining metal was available for organic molecules due to the porous structure of carbon. At the same time, a metal was firmly held inside the carbon shells and was not washed out during a reaction and after washing procedures, keeping its catalytic activity unchanged for several cycles. Mixing various salts together before the reaction led to the alloys, and the ratio of the salts simply determined the ratio of the metals in the desired alloy. This approach allowed the synthesis of highly active metals/alloys on carbon catalysts with intrinsic hierarchical organization, which ensures a long-life cycle in the reaction. The obtained catalysts were successfully tested in the Suzuki-Miyaura cross-coupling reaction and showed excellent stability with a yield change <1% over several cycles (compared with a 64% yield decrease of commercial catalyst). The obtained catalysts have also shown very good performance in the semihydrogenation of C≡C bonds in phenylacetylene and other alkynes with selectivity up to 96% at 99% conversion.
Cite: Lebedev A.N. , Rodygin K.S. , Mironenko R.M. , Saybulina E.R. , Ananikov V.P.
Metal-Catalyzed Chemical Activation of Calcium Carbide: New Way to Hierarchical Metal/Alloy-on-Carbon Catalysts
Journal of Catalysis. 2022. V.407. P.281-289. DOI: 10.1016/j.jcat.2022.01.034 WOS Scopus РИНЦ AN OpenAlex publication_identifier_short.sciact_ihcp_identifier_type
Dates:
Submitted: Aug 17, 2021
Accepted: Jan 31, 2022
Published online: Feb 4, 2022
Published print: Mar 1, 2022
Identifiers:
Web of science: WOS:000780380500014
Scopus: 2-s2.0-85124869578
Elibrary: 48150035
Chemical Abstracts: 2022:490357
OpenAlex: W4210288627
publication_identifier.sciact_ihcp_identifier_type: 3656
Citing:
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Scopus 25
Web of science 22
Elibrary 23
OpenAlex 25
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