The Zn-Cu(I)/HMCM-41 catalysts were successfully prepared in laboratory scale by solid-state ion exchange with CuCl salt, together with introduction of Zn to improve the dispersion degree of the active component Cu(I)...The Zn-Cu(I)/HMCM-41 catalysts were successfully prepared in laboratory scale by solid-state ion exchange with CuCl salt, together with introduction of Zn to improve the dispersion degree of the active component Cu(I) on the surface. With increase of the amounts of Zn and CuCl from 0% to 9.0% and 25.0% respectively, CO adsorption the amounts of increased from 10.6 mmol/g to 183.0 mmol/g correspondingly. The in situ FT-IR spectra for CO adsorption demonstrated that there existed two dynamic equilibriums between surface carbonyl complexes: Cu(CO)3+ Cu(CO)2++ CO and Cu(CO)2+ Cu(CO)+ + CO. The equilibriums can be shifted reversibly by changing the temperature and pressure. Due to the modified MCM-41 mesoporous materials possess both of the acidic and metallic carbonyl centers, this kind of material can be developed into mesoporous bifunctional catalysts for carbonylation reactions, in which larger molecules are involved.展开更多
文摘The Zn-Cu(I)/HMCM-41 catalysts were successfully prepared in laboratory scale by solid-state ion exchange with CuCl salt, together with introduction of Zn to improve the dispersion degree of the active component Cu(I) on the surface. With increase of the amounts of Zn and CuCl from 0% to 9.0% and 25.0% respectively, CO adsorption the amounts of increased from 10.6 mmol/g to 183.0 mmol/g correspondingly. The in situ FT-IR spectra for CO adsorption demonstrated that there existed two dynamic equilibriums between surface carbonyl complexes: Cu(CO)3+ Cu(CO)2++ CO and Cu(CO)2+ Cu(CO)+ + CO. The equilibriums can be shifted reversibly by changing the temperature and pressure. Due to the modified MCM-41 mesoporous materials possess both of the acidic and metallic carbonyl centers, this kind of material can be developed into mesoporous bifunctional catalysts for carbonylation reactions, in which larger molecules are involved.
