Implications for the Hydrogenation of Propyne and Propene with Parahydrogen due to the in situ Transformation of Rh2C to Rh0/C | Sciact - CRIS-system of Boreskov Institute of Catalysis

Implications for the Hydrogenation of Propyne and Propene with Parahydrogen due to the in situ Transformation of Rh2C to Rh0/C Full article

Journal

ChemPhysChem
ISSN: 1439-4235 , E-ISSN: 1439-7641

Output data

Year: 2024, Volume: 25, Number: 17, Article number : e202400270, Pages count : 8 DOI: 10.1002/cphc.202400270

Tags

Atoms; Carbides; Carbon; Catalysts; Hydrogen; Hydrogenation; Molecules; Polarization; Propylene; Rhodium compounds

Authors

Pokochueva Ekaterina V. ¹ , Kountoupi Evgenia ² , Janák Marcel ² , Kuznetsov Denis A. ² , Prosvirin Igor P. ³ , Müller Christoph ² , Fedorov Alexey ² , Koptyug Igor V. ¹

Affiliations

1	Laboratory of Magnetic Resonance MicroimagingInternational Tomography Center, SB RASInstitutskaya st. 3А, Novosibirsk 630090 (Russia)
2	Department of Mechanical and Process Engineering, ETH ZürichLeonhardstrasse 21, Zürich 8092 (Switzerland)
3	Boreskov Institute of Catalysis, SB RAS,Acad. Lavrent'yeva Av. 5, Novosibirsk 630090 (Russia)

Funding (4)

1	Russian Science Foundation	22-43-04426
2	Swiss Federal Institute of Technology in Zurich	ETH-40 19-2
3	Ministry of Science and Higher Education of the Russian Federation
4	Swiss National Science Foundation	200021_196943

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.

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

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

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

DB	Citing
OpenAlex	1
Web of science	1
Scopus	1