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Catalytic hydrogenation with parahydrogen: a bridge from homogeneous to heterogeneous catalysis

Authors
  • Kovtunov, Kirill V.1, 2
  • Salnikov, Oleg G.1, 2, 3
  • Skovpin, Ivan V.1, 2, 3
  • Chukanov, Nikita V.1, 2
  • Burueva, Dudari B.1, 2
  • Koptyug, Igor V.1, 2, 3
  • 1 SB RAS, Institutskaya St. 3A , (Russia)
  • 2 Novosibirsk State University, Pirogova St. 1 , (Russia)
  • 3 SB RAS, 5 Acad. Lavrentiev Ave. , (Russia)
Type
Published Article
Journal
Pure and Applied Chemistry
Publisher
Walter de Gruyter GmbH
Publication Date
Jun 22, 2020
Volume
92
Issue
7
Pages
1029–1046
Identifiers
DOI: 10.1515/pac-2020-0203
Source
De Gruyter
Keywords
License
Yellow

Abstract

One of the essential themes in modern catalysis is that of bridging the gap between its homogeneous and heterogeneous counterparts to combine their individual advantages and overcome shortcomings. One more incentive can now be added to the list, namely the ability of transition metal complexes to provide strong nuclear magnetic resonance (NMR) signal enhancement upon their use in homogeneous hydrogenations of unsaturated compounds with parahydrogen in solution. The addition of both H atoms of a parahydrogen molecule to the same substrate, a prerequisite for such effects, is implemented naturally with metal complexes that operate via the formation of a dihydride intermediate, but not with most heterogeneous catalysts. Despite that, it has been demonstrated in recent years that various types of heterogeneous catalysts are able to perform the required pairwise H2 addition at least to some extent. This has opened a major gateway for developing highly sensitive and informative tools for mechanistic studies of heterogeneous hydrogenations and other processes involving H2. Besides, production of catalyst-free fluids with NMR signals enhanced by 3-4 orders of magnitude is essential for modern applications of magnetic resonance imaging (MRI), including biomedical research and practice. The ongoing efforts to design heterogeneous catalysts which can implement the homogeneous (pairwise) hydrogenation mechanism are reported.

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