Spatially Resolved NMR Spectroscopy of Heterogeneous Gas Phase Hydrogenation of 1,3-Butadiene with Parahydrogen | Sciact - CRIS-system of Boreskov Institute of Catalysis

Spatially Resolved NMR Spectroscopy of Heterogeneous Gas Phase Hydrogenation of 1,3-Butadiene with Parahydrogen Full article

Journal

Catalysis Science and Technology
ISSN: 2044-4753 , E-ISSN: 2044-4761

Output data

Year: 2020, Volume: 10, Number: 1, Pages: 99-104 Pages count : 6 DOI: 10.1039/c9cy02100k

Tags

INDUCED POLARIZATION; MASS-TRANSPORT; SPIN-EXCHANGE; MRI; CATALYSTS; REACTORS; HYPERPOLARIZATION; FLOW

Authors

Svyatova Alexandra ^1,2 , Kononenko Elizaveta S. ^1,2 , Kovtunov Kirill V. ^1,2 , Lebedev Dmitry ³ , Gerasimov Evgeniy Yu. ^2,4 , Bukhtiyarov Andrey V. ^2,4 , Prosvirin Igor P. ^2,4 , Bukhtiyarov Valerii I. ⁴ , Müller Christoph R. ⁵ , Fedorov Alexey ⁵ , Koptyug Igor V. ^1,2,4

Affiliations

1	International Tomography Center, SB RAS, 3 A Institutskaya St., Novosibirsk 630090, Russia
2	Novosibirsk State University, 2 Pirogova St., Novosibirsk 630090, Russia
3	Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1–5, Zürich, CH 8093, Switzerland
4	Boreskov Institute of Catalysis SB RAS, 5 Lavrenteva Pr, Novosibirsk 630090, Russia
5	Department of Mechanical and Process Engineering, ETH Zürich, Leonhardstrasse 21, Zürich, CH 8092, Switzerland

Funding (4)

1	Federal Agency for Scientific Organizations	0333-2016-0002 (АААА-А16-116121510087-5)
2	Swiss National Science Foundation	200020_182692
3	Federal Agency for Scientific Organizations	0333-2018-0006 (II.1.13.1.)
4	Russian Science Foundation	19-13-00047 (АААА-А19-119042990019-3)

Magnetic resonance-based methods such as nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are widely used to provide in situ/operando information of chemical reactions. However, the low spin density and magnetic field inhomogeneities associated with heterogeneous catalytic systems containing gaseous reactants complicate such studies. Hyperpolarization techniques, in particular parahydrogen-induced polarization (PHIP), increase significantly the NMR signal intensity. In this study, we test 16 glass tube reactors containing Pd, Pt, Rh or Ir nanoparticles dispersed on a thin layer of TiO2, CeO2, SiO2 or Al2O3 for the hydrogenation of 1,3-butadiene using parahydrogen. The catalytic coatings of Ir and Rh gave hydrogenation products with the highest nuclear spin polarization while the coatings of Pd are the most selective ones for the semihydrogenation of 1,3-butadiene to 1- and 2-butenes. Spatially resolved NMR spectroscopy of the reagent and the product distribution along the reactor axis provided further mechanistic insight into the catalytic function of these reactive coatings under operando conditions.

Svyatova A. , Kononenko E.S. , Kovtunov K.V. , Lebedev D. , Gerasimov E.Y. , Bukhtiyarov A.V. , Prosvirin I.P. , Bukhtiyarov V.I. , Müller C.R. , Fedorov A. , Koptyug I.V.
Spatially Resolved NMR Spectroscopy of Heterogeneous Gas Phase Hydrogenation of 1,3-Butadiene with Parahydrogen

Catalysis Science and Technology. 2020. V.10. N1. P.99-104. DOI: 10.1039/c9cy02100k WOS Scopus РИНЦ ANCAN OpenAlex

Full text from publisher

Submitted:	Oct 18, 2019
Accepted:	Nov 17, 2019
Published online:	Nov 21, 2019
Published print:	Jan 7, 2020

Web of science:	WOS:000505550900005
Scopus:	2-s2.0-85077515136
Elibrary:	43228286
Chemical Abstracts:	2019:2208318
Chemical Abstracts (print):	172:74339
OpenAlex:	W2991556543

DB	Citing
Web of science	16
Scopus	17
Elibrary	13
OpenAlex	17