Corma Avelino, Salnikov Oleg G, Barskiy Danila A, Kovtunov Kirill V, Koptyug Igor V
Instituto de Tecnologia Quimica UPV-CSIC, Avda. de los Naranjos, s/n, 46022 Valencia (Spain).
Chemistry. 2015 May 4;21(19):7012-5. doi: 10.1002/chem.201406664. Epub 2015 Mar 6.
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.
一种高度孤立的单原子金催化剂已被合成、表征并用于1,3 - 丁二烯和1 - 丁炔与仲氢的多相氢化反应中进行测试，该催化剂的单个金原子分散在多壁碳纳米管（MWCNTs）上，以最大化极化水平和成对氢加成途径的贡献。发现Au/MWCNTs催化剂在成对氢加成中具有活性和高效性，并且成对氢加成途径的估计贡献比负载型金属纳米颗粒催化剂至少高一个数量级。因此，使用高度孤立的单原子催化剂对于生产可用于显著增强NMR信号的超极化流体非常有前景。还提出了在高度孤立的单原子Au/MWCNTs催化剂上仲氢对1,3 - 丁二烯氢化的反应机理。
