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A highly efficient single site Rh-POL-PPh3 catalyst for heterogeneous methanol carbonylation
Molecular Catalysis ( IF 4.6 ) Pub Date : 2017-09-15 , DOI: 10.1016/j.mcat.2017.09.007
Zhou Ren , Yuan Lyu , Siquan Feng , Xiangen Song , Yunjie Ding

In Contrast to the Monsanto homogeneous system, the Rh heterogeneous methanol carbonylation universally displays lower activity and stability. Here, a single site catalyst Rh-POL-PPh3 was successfully prepared by impregnation of the Rh2(CO)4Cl2 dichloromethane solution, and applied to heterogeneous methanol carbonylation in a continuous fixed-bed reactor for the first time. Due to single site Rh species and the electron-donating effect of P ligands and the strong multicoordination bonds between Rh and P, the Rh-POL-PPh3 catalyst exhibited a little higher TOF of 1550 h−1 than that of optimized Monsanto process and maintained relatively stable activity for near 180 h under 2.5 MPa, 195 °C. Thus, POL-PPh3 not only acts as a stable support but also a promotion of methanol carbonylation process.



中文翻译:

用于异质甲醇羰基化的高效单中心Rh-POL-PPh 3催化剂

与孟山都均相系统相反,Rh异质甲醇羰基化普遍显示出较低的活性和稳定性。在此,通过浸渍Rh 2(CO)4 Cl 2二氯甲烷溶液成功制备了单中心催化剂Rh-POL-PPh 3,并首次将其用于连续固定床反应器中的非均相甲醇羰基化。由于具有单一位点的Rh物种和P配体的电子给体作用以及Rh与P之间的强多配位键,Rh-POL-PPh 3催化剂的TOF略高,为1550 h -1与优化的孟山都(Monsanto)工艺相比,在2.5 MPa,195°C的温度下保持了近180小时的相对稳定的活性。因此,POL-PPh 3不仅充当稳定的载体,而且促进甲醇羰基化过程。

更新日期:2017-09-15
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