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The Effect of Oxidative and Reductive Treatments of Titania-Supported Metal Catalysts on the Pairwise Hydrogen Addition to Unsaturated Hydrocarbons Full article

Journal Catalysis Today
ISSN: 0920-5861 , E-ISSN: 1873-4308
Output data Year: 2017, Volume: 283, Pages: 82-88 Pages count : 7 DOI: 10.1016/j.cattod.2016.02.030
Tags Heterogeneous catalysis, Hydrogenation, Parahydrogen-induced polarization (PHIP), Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS)
Authors Salnikov Oleg G. 1,2 , Burueva Dudari B. 1,2 , Gerasimov Evgeniy Yu. 2,3 , Bukhtiyarov Andrey V. 2,3 , Khudorozhkov Alexander K. 2,3 , Prosvirin Igor P. 2,3 , Kovtunova Larisa M. 2,3 , Barskiy Danila A. 1,4 , Bukhtiyarov Valerii I. 2,3 , Kovtunov Kirill V. 1,2 , 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 Laboratory of Surface Science, Boreskov Institute of Catalysis, SB RAS, 5 Acad. Lavrentiev Pr., 630090 Novosibirsk, Russia
4 Department of Radiology and Radiological Sciences, Institute of Imaging Science, Vanderbilt University, 1161 21st Avenue South, Medical Center North, AA-1105, Nashville, TN 37232-2310, USA

Funding (5)

1 Russian Science Foundation 14-23-00146
2 Russian Foundation for Basic Research 14-03-93183
3 Russian Foundation for Basic Research 14-03-00374
4 Russian Science Foundation 14-13-00445
5 Federal Agency for Scientific Organizations

Abstract: Heterogeneous hydrogenation of unsaturated compounds with parahydrogen is a highly promising technique for boosting the sensitivity of magnetic resonance spectroscopy and imaging by hyperpolarizing reaction products in gaseous and liquid phases, and potentially reaction intermediates as well. This demands an efficient heterogeneous catalyst providing both the high selectivity toward pairwise hydrogen addition (i.e., ability to incorporate both H atoms of H2 molecule in the same product molecule) as well as sufficient overall hydrogenation activity. In this work, we studied the influence of oxidative and reductive treatments of the supported metal catalysts on the NMR signal enhancements provided by parahydrogen-induced polarization (PHIP) effects in hydrogenation of propene, propyne, 1,3-butadiene and 1-butyne. The 5 wt% titania-supported Pt, Pd, Rh and Ir catalysts used here were characterized by X-ray photoelectron spectroscopy (XPS) and high-resolution transmission electron microscopy (HRTEM). Generally, the preliminarily reduced catalysts were found to be more efficient than the oxidized ones. For instance, while the reduced Ir/TiO2 catalyst provided the intense PHIP NMR signals, its oxidized counterpart showed almost no activity in hydrogenation. For the oxidized Pd/TiO2 catalyst, HRTEM revealed the formation of titania pedestals under large (ca. 5–7 nm) PdO nanoparticles. At the same time, the small (ca. 1 nm) partially reduced Pdδ+ particles were observed on the facets of TiO2 support. These changes in catalyst structure led to a significant decrease in pairwise hydrogen addition selectivity.
Cite: Salnikov O.G. , Burueva D.B. , Gerasimov E.Y. , Bukhtiyarov A.V. , Khudorozhkov A.K. , Prosvirin I.P. , Kovtunova L.M. , Barskiy D.A. , Bukhtiyarov V.I. , Kovtunov K.V. , Koptyug I.V.
The Effect of Oxidative and Reductive Treatments of Titania-Supported Metal Catalysts on the Pairwise Hydrogen Addition to Unsaturated Hydrocarbons
Catalysis Today. 2017. V.283. P.82-88. DOI: 10.1016/j.cattod.2016.02.030 WOS Scopus РИНЦ ANCAN OpenAlex
Dates:
Submitted: Oct 5, 2015
Accepted: Feb 5, 2016
Published online: Mar 17, 2016
Published print: Apr 1, 2017
Identifiers:
Web of science: WOS:000393244700008
Scopus: 2-s2.0-84961219162
Elibrary: 29464379
Chemical Abstracts: 2016:413304
Chemical Abstracts (print): 166:65132
OpenAlex: W2302515789
Citing:
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Web of science 20
Scopus 20
OpenAlex 20
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