Abstract: NMR spectroscopy studies using parahydrogen-induced polarization have previously established the existence of the pairwise hydrogen addition route in the hydrogenation of unsaturated hydrocarbons over heterogeneous catalysts, including those based on rhodium (Rh0). This pathway requires the incorporation of both hydrogen atoms from one hydrogen molecule to the same product molecule. However, the underlying mechanism for such pairwise hydrogen addition must be better understood. The involvement of carbon, either in the form of carbonaceous deposits on the surface of a catalyst or as a metal carbide phase, is known to modify catalytic properties significantly and thus could also affect the pairwise hydrogen addition route. Here, we explored carbon’s role by studying the hydrogenation of propene and propyne with parahydrogen on a Rh2C catalyst and comparing the results with those for a Rh0/C catalyst obtained from Rh2C via H2 pretreatment. While the catalysts Rh2C and Rh0/C differ notably in the rate of conversion of parahydrogen to normal hydrogen as well as in terms of hydrogenation activity, our findings suggest that the carbide phase does not play a significant role in the pairwise H2 addition route on rhodium catalysts.

Cite: Pokochueva E.V. , Kountoupi E. , Janák M. , Kuznetsov D.A. , Prosvirin I.P. , Müller C. , Fedorov A. , Koptyug I.V.
Implications for the Hydrogenation of Propyne and Propene with Parahydrogen due to the in situ Transformation of Rh2C to Rh0/C
ChemPhysChem. 2024. V.25. N17. e202400270 :1-8. DOI: 10.1002/cphc.202400270 WOS Scopus РИНЦ AN PMID OpenAlex

Dates:

Submitted:	Mar 30, 2024
Accepted:	May 27, 2024
Published online:	Jun 4, 2024
Published print:	Sep 1, 2024

Identifiers:

Web of science:	WOS:001265916600001
Scopus:	2-s2.0-85198048797
Elibrary:	68805571
Chemical Abstracts:	2024:1530296
PMID:	38837531
OpenAlex:	W4399333284

Citing:

DB	Citing
OpenAlex	1
Web of science	1
Scopus	1

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