학술논문
Mechanistic in situ investigation of heterogeneous hydrogenation over Rh/TiO 2 catalysts: selectivity, pairwise route and catalyst nature.
Document Type
Academic Journal
Author
Pokochueva EV; Laboratory of Magnetic Resonance Microimaging, International Tomography Center SB RAS, 3A Institutskaya St., 630090 Novosibirsk, Russia. kovtunov@tomo.nsc.ru and Novosibirsk State University, 2 Pirogova St., 630090 Novosibirsk, Russia.; Burueva DB; Laboratory of Magnetic Resonance Microimaging, International Tomography Center SB RAS, 3A Institutskaya St., 630090 Novosibirsk, Russia. kovtunov@tomo.nsc.ru and Novosibirsk State University, 2 Pirogova St., 630090 Novosibirsk, Russia.; Kovtunova LM; Boreskov Institute of Catalysis SB RAS, 5 Acad. Lavrentiev Pr., 630090 Novosibirsk, Russia. vib@catalysis.ru and Novosibirsk State University, 2 Pirogova St., 630090 Novosibirsk, Russia.; Bukhtiyarov AV; Boreskov Institute of Catalysis SB RAS, 5 Acad. Lavrentiev Pr., 630090 Novosibirsk, Russia. vib@catalysis.ru and Novosibirsk State University, 2 Pirogova St., 630090 Novosibirsk, Russia.; Gladky AY; Boreskov Institute of Catalysis SB RAS, 5 Acad. Lavrentiev Pr., 630090 Novosibirsk, Russia. vib@catalysis.ru.; Kovtunov KV; Laboratory of Magnetic Resonance Microimaging, International Tomography Center SB RAS, 3A Institutskaya St., 630090 Novosibirsk, Russia. kovtunov@tomo.nsc.ru and Novosibirsk State University, 2 Pirogova St., 630090 Novosibirsk, Russia.; Koptyug IV; Laboratory of Magnetic Resonance Microimaging, International Tomography Center SB RAS, 3A Institutskaya St., 630090 Novosibirsk, Russia. kovtunov@tomo.nsc.ru and Boreskov Institute of Catalysis SB RAS, 5 Acad. Lavrentiev Pr., 630090 Novosibirsk, Russia. vib@catalysis.ru and Novosibirsk State University, 2 Pirogova St., 630090 Novosibirsk, Russia.; Bukhtiyarov VI; Boreskov Institute of Catalysis SB RAS, 5 Acad. Lavrentiev Pr., 630090 Novosibirsk, Russia. vib@catalysis.ru and Novosibirsk State University, 2 Pirogova St., 630090 Novosibirsk, Russia.
Source
Publisher: Faraday Division, Royal Society of Chemistry Country of Publication: England NLM ID: 9212301 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1364-5498 (Electronic) Linking ISSN: 13596640 NLM ISO Abbreviation: Faraday Discuss Subsets: PubMed not MEDLINE; MEDLINE
Subject
Language
English
Abstract
The selectivity of product formation is strongly correlated with the nature of the catalyst active centers. Therefore, the selective synthesis of active sites with certain structure is a big challenge in modern catalysis. Here synthetic procedures are adopted for the formation of 1% Rh/TiO 2 catalysts with different properties. It is shown that the nature of the precursor used for catalyst preparation is important, and that the use of a solution of rhodium acetate instead of rhodium nitrate leads to the selective formation of butenes during 1,3-butadiene hydrogenation. The use of parahydrogen in the reaction results in the enhancement of NMR signals via parahydrogen-induced polarization (PHIP) for all synthesized catalysts, and this signal enhancement increases with increasing catalyst calcination temperature. This effect is explained by the decoration of rhodium nanoparticles with titania which restricts hydrogen mobility on the surface, leading to the highest reported to date selectivity toward the pairwise hydrogen addition route of 7% for supported metal catalysts.