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
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
收藏
页码:7012 / 7015
页数:4
相关论文
共 39 条
[21]   Parahydrogen-Induced Polarization in Heterogeneous Catalytic Processes [J].
Kovtunov, Kirill V. ;
Zhivonitko, Vladimir V. ;
Skovpin, Ivan V. ;
Barskiy, Danila A. ;
Koptyug, Igor V. .
HYPERPOLARIZATION METHODS IN NMR SPECTROSCOPY, 2013, 338 :123-180
[22]   Heterogeneous addition of H2 to double and triple bonds over supported Pd catalysts: a parahydrogen-induced polarization technique study [J].
Kovtunov, Kirill V. ;
Beck, Irene E. ;
Zhivonitko, Vladimir V. ;
Barskiy, Danila A. ;
Bukhtiyarov, Valery I. ;
Koptyug, Igor V. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2012, 14 (31) :11008-11014
[23]   Parahydrogen-induced polarization in alkyne hydrogenation catalyzed by Pd nanoparticles embedded in a supported ionic liquid phase [J].
Kovtunov, Kirill V. ;
Zhivonitko, Vladimir V. ;
Kiwi-Minsker, Lioubov ;
Koptyug, Igor V. .
CHEMICAL COMMUNICATIONS, 2010, 46 (31) :5764-5766
[24]   Parahydrogen-Induced Polarization in Heterogeneous Hydrogenations Catalyzed by an Immobilized Au(III) Complex [J].
Kovtunov, Kirill V. ;
Zhivonitko, Vladimir V. ;
Corma, Avelino ;
Koptyug, Igor V. .
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2010, 1 (11) :1705-1708
[25]  
Kovtunov KirillV., 2008, Angewandte Chemie, V120, P1514, DOI [10.1002/ange.200704881, DOI 10.1002/ANGE.200704881]
[26]   Isolated Metal Atom Geometries as a Strategy for Selective Heterogeneous Hydrogenations [J].
Kyriakou, Georgios ;
Boucher, Matthew B. ;
Jewell, April D. ;
Lewis, Emily A. ;
Lawton, Timothy J. ;
Baber, Ashleigh E. ;
Tierney, Heather L. ;
Flytzani-Stephanopoulos, Maria ;
Sykes, E. Charles H. .
SCIENCE, 2012, 335 (6073) :1209-1212
[27]   Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects [J].
Lei, Y. ;
Mehmood, F. ;
Lee, S. ;
Greeley, J. ;
Lee, B. ;
Seifert, S. ;
Winans, R. E. ;
Elam, J. W. ;
Meyer, R. J. ;
Redfern, P. C. ;
Teschner, D. ;
Schlogl, R. ;
Pellin, M. J. ;
Curtiss, L. A. ;
Vajda, S. .
SCIENCE, 2010, 328 (5975) :224-228
[28]   Parahydrogen induced polarization [J].
Natterer, J ;
Bargon, J .
PROGRESS IN NUCLEAR MAGNETIC RESONANCE SPECTROSCOPY, 1997, 31 :293-315
[29]   Observation of new intermediates in the reaction of dihydrogen with iridium, rhodium, and mixed metal A-frame complexes with parahydrogen-induced polarization [J].
Oldham, SM ;
Houlis, JF ;
Sleigh, CJ ;
Duckett, SB ;
Eisenberg, R .
ORGANOMETALLICS, 2000, 19 (16) :2985-2993
[30]   NET NMR ALIGNMENT BY ADIABATIC TRANSPORT OF PARA-HYDROGEN ADDITION-PRODUCTS TO HIGH MAGNETIC-FIELD [J].
PRAVICA, MG ;
WEITEKAMP, DP .
CHEMICAL PHYSICS LETTERS, 1988, 145 (04) :255-258