Burueva Dudari B, Kovtunov Kirill V, Bukhtiyarov Andrey V, Barskiy Danila A, Prosvirin Igor P, Mashkovsky Igor S, Baeva Galina N, Bukhtiyarov Valerii I, Stakheev Aleksandr Yu, Koptyug Igor V
Laboratory of Magnetic Resonance Microimaging, International Tomography Center, SB RAS, 3A Institutskaya St., 630090, Novosibirsk, Russia.
Novosibirsk State University, 2 Pirogova St., 630090, Novosibirsk, Russia.
Chemistry. 2018 Feb 21;24(11):2547-2553. doi: 10.1002/chem.201705644. Epub 2018 Jan 29.
Pd-In/Al O single-site catalyst was able to show high selectivity (up to 98 %) in the gas phase semihydrogenation of propyne. Formation of intermetallic Pd-In compound was studied by XPS during reduction of the catalyst. FTIR-CO spectroscopy confirmed single-site nature of the intermetallic Pd-In phase reduced at high temperature. Utilization of Pd-In/Al O in semihydrogenation of propyne with parahydrogen allowed to produce ≈3400-fold NMR signal enhancement for reaction product propene (polarization=9.3 %), demonstrating the large contribution of pairwise hydrogen addition route. Significant signal enhancement as well as the high catalytic activity of the Pd-In catalyst allowed to acquire H MR images of flowing hyperpolarized propene gas selectively for protons in CH, CH and CH groups. This observation is unique and can be easily transferred to the development of a useful MRI technique for an in situ investigation of selective semihydrogenation in catalytic reactors.
钯-铟/氧化铝单中心催化剂在丙炔气相加氢反应中表现出高选择性（高达98%）。在催化剂还原过程中，通过X射线光电子能谱（XPS）研究了金属间钯-铟化合物的形成。傅里叶变换红外光谱-一氧化碳（FTIR-CO）光谱证实了高温还原的金属间钯-铟相的单中心性质。在使用仲氢对丙炔进行加氢反应中，钯-铟/氧化铝的应用使得反应产物丙烯的核磁共振（NMR）信号增强了约3400倍（极化率=9.3%），这表明双氢加成途径的贡献很大。显著的信号增强以及钯-铟催化剂的高催化活性使得能够选择性地获取流动的超极化丙烯气体中CH、CH和CH基团质子的氢核磁共振图像。这一观察结果是独一无二的，并且可以很容易地应用于开发一种有用的磁共振成像（MRI）技术，用于原位研究催化反应器中的选择性加氢反应。
