Mechanistic analysis of transformative Pd/NHC catalyst evolution in the 1,2-diphenylacetylene semihydrogenation using molecular hydrogen

Mechanistic analysis of transformative Pd/NHC catalyst evolution in the 1,2-diphenylacetylene semihydrogenation using molecular hydrogen Full article

Journal

Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694

Output data

Year: 2024, Volume: 430, Article number : 115293, Pages count : DOI: 10.1016/j.jcat.2024.115293

Authors

Saybulina Elina R. ¹ , Mironenko Roman M. ¹ , Galushko Alexey S. ² , Ilyushenkova Valentina V. ² , Izmailov Rinat R. ¹ , Ananikov Valentine P. ²

Affiliations

1	Center of New Chemical Technologies BIC, Boreskov Institute of Catalysis, Neftezavodskaya st. 54, Omsk 644040, Russia
2	N.D. Zelinsky Institute of Organic Chemistry, Russian Academy of Sciences, Leninsky pr. 47, Moscow 119991, Russia

This study explored the dynamic transformations of the Pd/NHC catalytic system during the semihydrogenation of alkynes using molecular hydrogen under mild reaction conditions. Focusing on the appearance of a “cocktail”-type system, we harnessed advanced characterization methods, such as NMR, ESI-HRMS, and SEM/TEM. In the hydrogenation process of 1,2–diphenylacetylene, the Pd/NHC complex evolves to produce novel palladium-based compounds and a heterogeneous phase, which partially precipitates into catalytically active nanoparticles. A pivotal finding revealed that the modification of the Pd nanoparticle surface by organic ligands under reaction conditions significantly influenced the catalytic activity of the Pd particles. The split test results suggest an enhanced selectivity toward (Z)-stilbene when the precipitate is maintained in the reaction mixture, highlighting that the palladium nanoparticles act as active catalysts (or reservoirs of active species) synergistically with dissolved molecular complexes. This research reports important findings for understanding the dynamics of the Pd/NHC system, contributing to the development of more efficient catalytic systems.

Saybulina E.R. , Mironenko R.M. , Galushko A.S. , Ilyushenkova V.V. , Izmailov R.R. , Ananikov V.P.
Mechanistic analysis of transformative Pd/NHC catalyst evolution in the 1,2-diphenylacetylene semihydrogenation using molecular hydrogen
Journal of Catalysis. 2024. V.430. 115293 . DOI: 10.1016/j.jcat.2024.115293 WOS Scopus OpenAlex

Web of science:	WOS:001175470300001
Scopus:	2-s2.0-85184266120
OpenAlex:	W4390725649

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