Single-Atom Gold Catalysis in the Context of Developments in Parahydrogen-Induced Polarization
A highly isolated monoatomic gold catalyst, with single gold atoms dispersed on multiwalled carbon nanotubes (MWCNTs), has been synthesized, characterized, and tested in heterogeneous hydrogenation of 1,3‐butadiene and 1‐butyne with parahydrogen to maximize the polarization level and the contributio...
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| Published in | Chemistry : a European journal Vol. 21; no. 19; pp. 7012 - 7015 |
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| Main Authors | , , , , |
| Format | Journal Article |
| Language | English |
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Weinheim
WILEY-VCH Verlag
04.05.2015
WILEY‐VCH Verlag Wiley Subscription Services, Inc |
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| Abstract | A highly isolated monoatomic gold catalyst, with single gold atoms dispersed on multiwalled carbon nanotubes (MWCNTs), has been synthesized, characterized, and tested in heterogeneous hydrogenation of 1,3‐butadiene and 1‐butyne with parahydrogen to maximize the polarization level and the contribution of the pairwise hydrogen addition route. The Au/MWCNTs catalyst was found to be active and efficient in pairwise hydrogen addition and the estimated contributions from the pairwise hydrogen addition route are at least an order of magnitude higher than those for supported metal nanoparticle catalysts. Therefore, the use of the highly isolated monoatomic catalysts is very promising for production of hyperpolarized fluids that can be used for the significant enhancement of NMR signals. A mechanism of 1,3‐butadiene hydrogenation with parahydrogen over the highly isolated monoatomic Au/MWCNTs catalyst is also proposed.
The hydrogens went in 2 by 2: Hydrogenation of 1,3‐butadiene and 1‐butyne with parahydrogen is carried out by using a highly isolated heterogeneous monoatomic gold catalyst supported on multiwalled carbon nanotubes. The percentage of pairwise hydrogen addition is found to be approximately 10 % for this catalyst in which the catalytically active center is a single atom. |
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| AbstractList | A highly isolated monoatomic gold catalyst, with single gold atoms dispersed on multiwalled carbon nanotubes (MWCNTs), has been synthesized, characterized, and tested in heterogeneous hydrogenation of 1,3-butadiene and 1-butyne with parahydrogen to maximize the polarization level and the contribution of the pairwise hydrogen addition route. The Au/MWCNTs catalyst was found to be active and efficient in pairwise hydrogen addition and the estimated contributions from the pairwise hydrogen addition route are at least an order of magnitude higher than those for supported metal nanoparticle catalysts. Therefore, the use of the highly isolated monoatomic catalysts is very promising for production of hyperpolarized fluids that can be used for the significant enhancement of NMR signals. A mechanism of 1,3-butadiene hydrogenation with parahydrogen over the highly isolated monoatomic Au/MWCNTs catalyst is also proposed. The hydrogens went in 2 by 2: Hydrogenation of 1,3-butadiene and 1-butyne with parahydrogen is carried out by using a highly isolated heterogeneous monoatomic gold catalyst supported on multiwalled carbon nanotubes. The percentage of pairwise hydrogen addition is found to be approximately 10% for this catalyst in which the catalytically active center is a single atom. A highly isolated monoatomic gold catalyst, with single gold atoms dispersed on multiwalled carbon nanotubes (MWCNTs), has been synthesized, characterized, and tested in heterogeneous hydrogenation of 1,3‐butadiene and 1‐butyne with parahydrogen to maximize the polarization level and the contribution of the pairwise hydrogen addition route. The Au/MWCNTs catalyst was found to be active and efficient in pairwise hydrogen addition and the estimated contributions from the pairwise hydrogen addition route are at least an order of magnitude higher than those for supported metal nanoparticle catalysts. Therefore, the use of the highly isolated monoatomic catalysts is very promising for production of hyperpolarized fluids that can be used for the significant enhancement of NMR signals. A mechanism of 1,3‐butadiene hydrogenation with parahydrogen over the highly isolated monoatomic Au/MWCNTs catalyst is also proposed. The hydrogens went in 2 by 2: Hydrogenation of 1,3‐butadiene and 1‐butyne with parahydrogen is carried out by using a highly isolated heterogeneous monoatomic gold catalyst supported on multiwalled carbon nanotubes. The percentage of pairwise hydrogen addition is found to be approximately 10 % for this catalyst in which the catalytically active center is a single atom. A highly isolated monoatomic gold catalyst, with single gold atoms dispersed on multiwalled carbon nanotubes (MWCNTs), has been synthesized, characterized, and tested in heterogeneous hydrogenation of 1,3-butadiene and 1-butyne with parahydrogen to maximize the polarization level and the contribution of the pairwise hydrogen addition route. The Au/MWCNTs catalyst was found to be active and efficient in pairwise hydrogen addition and the estimated contributions from the pairwise hydrogen addition route are at least an order of magnitude higher than those for supported metal nanoparticle catalysts. Therefore, the use of the highly isolated monoatomic catalysts is very promising for production of hyperpolarized fluids that can be used for the significant enhancement of NMR signals. A mechanism of 1,3-butadiene hydrogenation with parahydrogen over the highly isolated monoatomic Au/MWCNTs catalyst is also proposed. Abstract A highly isolated monoatomic gold catalyst, with single gold atoms dispersed on multiwalled carbon nanotubes (MWCNTs), has been synthesized, characterized, and tested in heterogeneous hydrogenation of 1,3‐butadiene and 1‐butyne with parahydrogen to maximize the polarization level and the contribution of the pairwise hydrogen addition route. The Au/MWCNTs catalyst was found to be active and efficient in pairwise hydrogen addition and the estimated contributions from the pairwise hydrogen addition route are at least an order of magnitude higher than those for supported metal nanoparticle catalysts. Therefore, the use of the highly isolated monoatomic catalysts is very promising for production of hyperpolarized fluids that can be used for the significant enhancement of NMR signals. A mechanism of 1,3‐butadiene hydrogenation with parahydrogen over the highly isolated monoatomic Au/MWCNTs catalyst is also proposed. |
| Author | Koptyug, Igor V. Barskiy, Danila A. Corma, Avelino Salnikov, Oleg G. Kovtunov, Kirill V. |
| Author_xml | – sequence: 1 givenname: Avelino surname: Corma fullname: Corma, Avelino organization: Instituto de Tecnologia Quimica UPV-CSIC, Avda. de los Naranjos, s/n, 46022 Valencia (Spain) – sequence: 2 givenname: Oleg G. surname: Salnikov fullname: Salnikov, Oleg G. organization: Laboratory of Magnetic Resonance Microimaging, International Tomography Center SB RAS, Insitutskaya Street, 3 A, 630090, Novosibirsk (Russia) and Novosibirsk State University, 2 Pirogova St., Novosibirsk 630090 (Russia), Fax: (+7) 383-3331399 – sequence: 3 givenname: Danila A. surname: Barskiy fullname: Barskiy, Danila A. organization: Laboratory of Magnetic Resonance Microimaging, International Tomography Center SB RAS, Insitutskaya Street, 3 A, 630090, Novosibirsk (Russia) and Novosibirsk State University, 2 Pirogova St., Novosibirsk 630090 (Russia), Fax: (+7) 383-3331399 – sequence: 4 givenname: Kirill V. surname: Kovtunov fullname: Kovtunov, Kirill V. email: kovtunov@tomo.nsc.ru organization: Laboratory of Magnetic Resonance Microimaging, International Tomography Center SB RAS, Insitutskaya Street, 3 A, 630090, Novosibirsk (Russia) and Novosibirsk State University, 2 Pirogova St., Novosibirsk 630090 (Russia), Fax: (+7) 383-3331399 – sequence: 5 givenname: Igor V. surname: Koptyug fullname: Koptyug, Igor V. organization: Laboratory of Magnetic Resonance Microimaging, International Tomography Center SB RAS, Insitutskaya Street, 3 A, 630090, Novosibirsk (Russia) and Novosibirsk State University, 2 Pirogova St., Novosibirsk 630090 (Russia), Fax: (+7) 383-3331399 |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/25754067$$D View this record in MEDLINE/PubMed |
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| Copyright | 2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim |
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| Keywords | gold heterogeneous catalysis NMR spectroscopy hydrogenation signal enhancement |
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| Snippet | A highly isolated monoatomic gold catalyst, with single gold atoms dispersed on multiwalled carbon nanotubes (MWCNTs), has been synthesized, characterized, and... Abstract A highly isolated monoatomic gold catalyst, with single gold atoms dispersed on multiwalled carbon nanotubes (MWCNTs), has been synthesized,... |
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| SubjectTerms | Catalysis Catalysts Chemistry Fluid dynamics Gold heterogeneous catalysis Hydrogen storage Hydrogenation Multi wall carbon nanotubes Nanotechnology Nanotubes NMR spectroscopy Polarization signal enhancement |
| Title | Single-Atom Gold Catalysis in the Context of Developments in Parahydrogen-Induced Polarization |
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