Mechanistic study of acetic acid synthesis over Cu-ZSM-5 framework : A QM/MM study

초록

CO2 is well-known as a greenhouse gas. Most researchers have been working to reduce its concentration in the atmosphere. At the same time, however, the carbon dioxide is a potentially valuable chemical as a source of one carbon supplier. It can produce carboxylic acids and alcohol that can convert to various useful materials. The simultaneous activation of CH4 and CO2 is possible in the presence of some alkali metals on the zeolite framework. In this work, the simultaneous co-activation of methane and carbon dioxide over Cu-ZSM-5 were investigated by theoretical approach. We utilised the 34T cluster model of ZSM-5 zeolite in the calculations. We adopted QM/MM approach which is an advantageous approach for the large sized system because it reduces the computational cost. In our QM treatment of the ZSM-5, an active site includes aluminium and copper atoms. The other atoms assigned as the MM region. In this QM/MM study, we employed the M06-L functional and ReaxFF 6.0 forcefield. All the calculations were performed by using the Materials Studio DMol3 and QMERA codes.