Single-Atom Gold Catalysis in the Context of Developments in Parahydrogen-Induced Polarization
Single-Atom Gold Catalysis in the Context of Developments in Parahydrogen-Induced Polarization
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DOI：
10.1002/chem.201406664
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发表时间：
2015-05-04
影响因子：
4.3
通讯作者：
Koptyug, Igor V.
中科院分区：
文献类型：
--
作者：
Corma, Avelino;Salnikov, Oleg G.;Koptyug, Igor V.
一种高度分离的单原子金催化剂，其单金原子分散在多壁碳纳米管 (MWCNT) 上，已合成、表征并在 1,3-丁二烯和 1-丁炔与仲氢的非均相氢化中进行测试，以最大限度地提高极化水平和成对氢加成路线的贡献。人们发现Au/MWCNTs催化剂在成对氢加成中具有活性和效率，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的贡献至少高一个数量级。因此，使用高度分离的单原子催化剂非常有希望生产可用于显着增强核磁共振信号的超极化流体。还提出了在高度分离的单原子 Au/MWCNT 催化剂上用仲氢进行 1,3-丁二烯加氢的机理。
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.