Single-Atom Gold Catalysis in the Context of Developments in Parahydrogen-Induced Polarization

被引：70

作者：

Corma, Avelino ^{[3
]}

Salnikov, Oleg G. ^{[1
,2
]}

Barskiy, Danila A. ^{[1
,2
]}

Kovtunov, Kirill V. ^{[1
,2
]}

Koptyug, Igor V. ^{[1
,2
]}

机构：

[1] Int Tomog Ctr SB RAS, Lab Magnet Resonance Microimaging, Novosibirsk 630090, Russia

[2] Novosibirsk State Univ, Novosibirsk 630090, Russia

[3] Inst Tecnol Quim UPV CSIC, Valencia 46022, Spain

来源：

CHEMISTRY-A EUROPEAN JOURNAL | 2015年 / 21卷 / 19期

基金：

俄罗斯科学基金会;

关键词：

gold; heterogeneous catalysis; hydrogenation; NMR spectroscopy; signal enhancement; HETEROGENEOUS HYDROGENATION; HYPERPOLARIZED GAS; ACTIVE-SITES; CLUSTERS;

D O I：

10.1002/chem.201406664

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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.

引用

页码：7012 / 7015

页数：4

共 39 条

[1] Synthesis, Solid-State NMR Characterization, and Application for Hydrogenation Reactions of a Novel Wilkinson's-Type Immobilized Catalyst [J].

Abdulhussain, Safaa ;

Breitzke, Hergen ;

Ratajczyk, Tomasz ;

Gruenberg, Anna ;

Srour, Mohamad ;

Arnaut, Danjela ;

Weidler, Heiko ;

Kunz, Ulrike ;

Kleebe, Hans Joachim ;

Bommerich, Ute ;

Bernarding, Johannes ;

Gutmann, Torsten ;

Buntkowsky, Gerd .

CHEMISTRY-A EUROPEAN JOURNAL, 2014, 20 (04) :1159-1166

[2]

[Anonymous], 2005, ANGEW CHEM

[3] Para-hydrogen induced polarisation effects in liquid phase hydrogenations catalysed by supported metal nanoparticles [J].

Balu, Alina M. ;

Duckett, Simon B. ;

Luque, Rafael .

DALTON TRANSACTIONS, 2009, (26) :5074-5076

[4] NMR Signal Enhancement for Hyperpolarized Fluids Continuously Generated in Hydrogenation Reactions with Parahydrogen [J].

Barskiy, Danila A. ;

Salnikov, Oleg G. ;

Kovtunov, Kirill V. ;

Koptyug, Igor V. .

JOURNAL OF PHYSICAL CHEMISTRY A, 2015, 119 (06) :996-1006

[5] Selective Hydrogenation of 1,3-Butadiene and 1-Butyne over a Rh/Chitosan Catalyst Investigated by using Parahydrogen-Induced Polarization [J].

Barskiy, Danila A. ;

Kovtunov, Kirill V. ;

Primo, Ana ;

Corma, Avelino ;

Kaptein, Robert ;

Koptyug, Igor V. .

CHEMCATCHEM, 2012, 4 (12) :2031-2035

[6] Applications of the parahydrogen phenomenon in inorganic chemistry [J].

Blazina, D ;

Duckett, SB ;

Dunne, JP ;

Godard, C .

DALTON TRANSACTIONS, 2004, (17) :2601-2609

[7] PARA-HYDROGEN AND SYNTHESIS ALLOW DRAMATICALLY ENHANCED NUCLEAR ALIGNMENT [J].

BOWERS, CR ;

WEITEKAMP, DP .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1987, 109 (18) :5541-5542

[8]

Corma A, 2013, NAT CHEM, V5, P775, DOI [10.1038/nchem.1721, 10.1038/NCHEM.1721]

[9] Application of Parahydrogen Induced Polarization Techniques in NMR Spectroscopy and Imaging [J].

Duckett, Simon B. ;

Mewis, Ryan E. .

ACCOUNTS OF CHEMICAL RESEARCH, 2012, 45 (08) :1247-1257

[10] PARA HYDROGEN INDUCED POLARIZATION IN HYDROGENATION REACTIONS [J].

EISENSCHMID, TC ;

KIRSS, RU ;

DEUTSCH, PP ;

HOMMELTOFT, SI ;

EISENBERG, R ;

BARGON, J ;

LAWLER, RG ;

BALCH, AL .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1987, 109 (26) :8089-8091

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