Selective Single-Site Pd-In Hydrogenation Catalyst for Production of Enhanced Magnetic Resonance Signals Using Parahydrogen | Sciact - CRIS-system of Boreskov Institute of Catalysis

Selective Single-Site Pd-In Hydrogenation Catalyst for Production of Enhanced Magnetic Resonance Signals Using Parahydrogen Full article

Journal

Chemistry - A European Journal
ISSN: 0947-6539 , E-ISSN: 1521-3765

Output data

Year: 2018, Volume: 24, Number: 11, Pages: 2547-2553 Pages count : 7 DOI: 10.1002/chem.201705644, 10.1002/chem.201881163

Tags

bimetallic catalysts, heterogeneous hydrogenation, MRI, parahydrogen, parahydrogen-induced polarization

Authors

Burueva Dudari B. ^1,2 , Kovtunov Kirill V. ^1,2 , Bukhtiyarov Andrey V. ³ , Barskiy Danila A. ⁴ , Prosvirin Igor P. ^2,3 , Mashkovsky Igor S. ⁵ , Baeva Galina N. ⁵ , Bukhtiyarov Valerii I. ³ , Stakheev Aleksandr Yu. ⁵ , Koptyug Igor V. ^1,2

Affiliations

1	Laboratory of Magnetic Resonance Microimaging International Tomography Center, SB RAS, 3A Institutskaya St., 630090 Novosibirsk (Russia)
2	Novosibirsk State University 2 Pirogova St., 630090 Novosibirsk (Russia)
3	Boreskov Institute of Catalysis, SB RAS, 5 Acad. Lavrentiev Pr., 630090 Novosibirsk (Russia)
4	Department of Chemistry, University of California at Berkeley, Berkeley, CA 94720-3220 (USA)
5	N.D. Zelinsky Institute of Organic Chemistry, RAS, 47 Leninsky Pr., 119991 Moscow (Russia)

Funding (4)

1	Russian Science Foundation	16-13-10530
2	Russian Science Foundation	17-73-20030
3	Federal Agency for Scientific Organizations	0333-2017-0002
4	Haldor Topsoe A/S

Pd-In/Al2O3 single-site catalyst was able to show high selectivity (up to 98%) in the gas phase semihydrogenation of propyne. Formation of intermetallic Pd-In compound was studied by XPS during reduction of the catalyst. FTIR-CO spectroscopy confirmed single-site nature of the intermetallic Pd-In phase reduced at high temperature. Utilization of Pd-In/Al2O3 in semihydrogenation of propyne with parahydrogen allowed to produce ≈3400-fold NMR signal enhancement for reaction product propene (polarization=9.3%), demonstrating the large contribution of pairwise hydrogen addition route. Significant signal enhancement as well as the high catalytic activity of the Pd-In catalyst allowed to acquire 1HMR images of flowing hyperpolarized propene gas selectively for protons in CH, CH2 and CH3 groups. This observation is unique and can be easily transferred to the development of a useful MRI technique for an in situ investigation of selective semihydrogenation in catalytic reactors.

Burueva D.B. , Kovtunov K.V. , Bukhtiyarov A.V. , Barskiy D.A. , Prosvirin I.P. , Mashkovsky I.S. , Baeva G.N. , Bukhtiyarov V.I. , Stakheev A.Y. , Koptyug I.V.
Selective Single-Site Pd-In Hydrogenation Catalyst for Production of Enhanced Magnetic Resonance Signals Using Parahydrogen
Chemistry - A European Journal. 2018. V.24. N11. P.2547-2553. DOI: 10.1002/chem.201705644, 10.1002/chem.201881163 WOS Scopus РИНЦ AN PMID OpenAlex

Submitted:	Nov 28, 2017
Published online:	Jan 11, 2018
Published print:	Feb 21, 2018

Web of science:	WOS:000425626800003
Scopus:	2-s2.0-85041099380
Elibrary:	35499110
Chemical Abstracts:	2018:179575
PMID:	29322571
OpenAlex:	W2783883563

DB	Citing
Web of science	53
Scopus	54
Elibrary	59
OpenAlex	65