Sciact
  • EN
  • RU

Anchored Complexes of Rhodium and Iridium for the Hydrogenation of Alkynes and Olefins with Parahydrogen Full article

Journal Catalysis Science and Technology
ISSN: 2044-4753 , E-ISSN: 2044-4761
Output data Year: 2022, Volume: 12, Number: 10, Pages: 3247-3253 Pages count : 7 DOI: 10.1039/d1cy02258j
Tags Catalyst activity; Gases; Hydrogenation; Iridium compounds; Metal complexes; Nuclear magnetic resonance; Phosphorus compounds; Propylene; Rhodium compounds; Silica gel; Synthesis (chemical)
Authors Skovpin Ivan V. 1 , Kovtunova Larisa M. 1,2 , Nartova Anna V. 2 , Kvon Ren I. 2 , Bukhtiyarov Valerii I. 2 , Koptyug Igor V. 1
Affiliations
1 International Tomography Center, SB RAS, 3A Institutskaya St., Novosibirsk, 630090, Russian Federation
2 Boreskov Institute of Catalysis, SB RAS, 5 Acad. Lavrentiev Pr., Novosibirsk, 630090, Russian Federation

Funding (3)

1 Russian Foundation for Basic Research 19-29-10003 (АААА-А19-119100890052-8)
2 Ministry of Science and Higher Education of the Russian Federation 0239-2021-0002
3 Ministry of Science and Higher Education of the Russian Federation

Abstract: Several catalysts synthesized by covalently binding Rh and Ir complexes to NH2- and PPh2- functional groups of the linker chains on the functionalized silica gel surface were compared in gas-phase hydrogenation of propyne and propene. Their stability, activity and product selectivity were evaluated. Furthermore, the use of parahydrogen in the reaction provided useful mechanistic information by delivering nuclear spin hyperpolarization of the reaction products with the associated enhancement of their NMR signals. In contrast to Rh-based catalysts which showed a pronounced tendency to reduction, for Ir-based catalysts an XPS analysis did not reveal any indication of the formation of a metal phase under reducing conditions upon hydrogenation of propyne or propene at 120 °C. Catalysts with a π-acceptor ligand PPh2- demonstrated greater activity in the gas-phase hydrogenation of propyne/propene in comparison with σ-donor ligand NH2-. Furthermore, NMR signal enhancements of up to ca. 700- (Rh) and 800-fold (Ir) were achieved. Remarkably, the Ir metal complex bound via the phosphine moiety demonstrated high stability in gas-phase hydrogenation of propyne along with high catalytic activity and pairwise H2 addition selectivity, yielding substantial quantities of strongly hyperpolarized propene.
Cite: Skovpin I.V. , Kovtunova L.M. , Nartova A.V. , Kvon R.I. , Bukhtiyarov V.I. , Koptyug I.V.
Anchored Complexes of Rhodium and Iridium for the Hydrogenation of Alkynes and Olefins with Parahydrogen
Catalysis Science and Technology. 2022. V.12. N10. P.3247-3253. DOI: 10.1039/d1cy02258j WOS Scopus РИНЦ ANCAN OpenAlex
Dates:
Submitted: Dec 14, 2021
Accepted: Mar 10, 2022
Published online: Mar 30, 2022
Published print: May 21, 2022
Identifiers:
Web of science: WOS:000779872400001
Scopus: 2-s2.0-85129315196
Elibrary: 48582553
Chemical Abstracts: 2022:924980
Chemical Abstracts (print): 179:213913
OpenAlex: W4225856904
Citing:
DB Citing
Elibrary 14
Scopus 17
Web of science 17
OpenAlex 22
Altmetrics: