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

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

Журнал

Catalysis Science & Technology
ISSN: 2044-4761

Вых. Данные

Год: 2020, Том: 10, Номер: 1, Страницы: 99-104 Страниц : 6 DOI: 10.1039/c9cy02100k

Авторы

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

Организации

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

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 & Technology. 2020. V.10. N1. P.99-104. DOI: 10.1039/c9cy02100k WOS Scopus РИНЦ CAPlusCA OpenAlex Sciact

Полный текст от издателя

Поступила в редакцию:	18 окт. 2019 г.
Принята к публикации:	17 нояб. 2019 г.
Опубликована online:	21 нояб. 2019 г.
Опубликована в печати:	7 янв. 2020 г.

Web of science:	WOS:000505550900005
Scopus:	2-s2.0-85077515136
РИНЦ:	43228286
Chemical Abstracts:	2019:2208318
Chemical Abstracts (print):	172:74339
OpenAlex:	W2991556543
Sciact:	34382

БД	Цитирований
Scopus	18
OpenAlex	18