Selective Single-Site Pd-In Hydrogenation Catalyst for Production of Enhanced Magnetic Resonance Signals Using Parahydrogen
Научная публикация
| Общее |
Язык:
Английский,
Жанр:
Статья (Full article),
Статус опубликования:
Опубликована,
Оригинальность:
Оригинальная
|
| Журнал |
Chemistry - A European Journal
ISSN: 0947-6539
, E-ISSN: 1521-3765
|
| Вых. Данные |
Год: 2018,
Том: 24,
Номер: 11,
Страницы: 2547-2553
Страниц
: 7
DOI:
10.1002/chem.201705644
|
| Ключевые слова |
bimetallic catalysts, heterogeneous hydrogenation, MRI, parahydrogen, parahydrogen-induced polarization |
| Авторы |
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
|
| Организации |
| 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)
|
|
Информация о финансировании (4)
|
1
|
Российский научный фонд
|
16-13-10530
|
|
2
|
Российский научный фонд
|
17-73-20030
|
|
3
|
Федеральное агентство научных организаций России
|
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.