XPS 和高分辨率透射电子显微镜揭示担载单原子铱催化剂在旋选择性丙烯加氢反应中多样性的本质。
XPS and HR TEM Elucidation of the Diversity of Titania-Supported Single-Site Ir Catalyst Performance in Spin-Selective Propene Hydrogenation.
机构信息
Department of Physical-Chemical Methods of Investigation, Boreskov Institute of Catalysis SB RAS, Lavrentiev Ave. 5, 630090 Novosibirsk, Russia.
Laboratory of Magnetic Resonance Microimaging, International Tomography Center SB RAS, Institutskaya St. 3A, 630090 Novosibirsk, Russia.
出版信息
Int J Mol Sci. 2023 Oct 27;24(21):15643. doi: 10.3390/ijms242115643.
Immobilized [Ir(COD)Cl]-Linker/TiO catalysts with linkers containing Py, P(Ph) and N(CH) functional groups were prepared. The catalysts were tested via propene hydrogenation with parahydrogen in a temperature range from 40 °C to 120 °C which was monitored via NMR. The catalytic behavior of [Ir(COD)Cl]-Linker/TiO is explained on the basis of quantitative and qualitative XPS data analysis performed for the catalysts before and after the reaction at 120 °C. It is shown that the temperature dependence of propene conversion and the enhancement of the NMR signal are explained via a combination of the stabilities of both the linker and immobilized [Ir(COD)Cl] complex. It is demonstrated that the N(CH)-linker is the most stable at the surface of TiO under used reaction conditions. As a result, only this sample shows a rise in the enhancement of the NMR signal in the 100-120 °C temperature range.
固定化 [Ir(COD)Cl]-配体/TiO 催化剂，配体中含有 Py、P(Ph)和 N(CH)官能团。通过在 40°C 至 120°C 的温度范围内用氘代氢对催化剂进行丙烯加氢反应进行测试，通过 NMR 进行监测。在 120°C 下进行反应前后，对催化剂进行定量和定性 XPS 数据分析，解释了 [Ir(COD)Cl]-Linker/TiO 的催化行为。结果表明，丙烯转化率的温度依赖性和 NMR 信号的增强可以通过配体和固定化 [Ir(COD)Cl] 配合物的稳定性的结合来解释。结果表明，在使用的反应条件下，N(CH)配体在 TiO 表面最稳定。因此，只有该样品在 100-120°C 温度范围内显示出 NMR 信号增强的上升。
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