Catalytic hydrolysis of COS over CeO 2 (110) surface: A density functional theory study

Abstract Density functional theory (DFT) calculations were performed to investigate the reaction pathways for catalytic hydrolysis of COS over CeO 2 (110) surface using Dmol 3 model. The thermodynamic stability analysis for the suggested routes of COS hydrolysis to CO 2 and H 2 S was evaluated. The absolute values of adsorption energy of H 2 O-CeO 2 are higher than that of COS-CeO 2 . Meanwhile, the adsorption energy and geometries show that H 2 O is easier adsorbed on the surface of CeO 2 (110) than COS. H 2 O plays a role as a bridge in the process of joint adsorption. H 2 O forms more Ce O H groups on the CeO 2 (110) surface. CeO 2 decreases the maximum energy barrier by 76.15 kcal/mol. The migration of H from H 2 O to COS is the key for the hydrolysis reaction. C O channel is easier to occur than C S channel. Experimental result shows that adding of CeO 2 can increase COS removal rate and prolong the 100% COS removal rate from 180 min to 210 min. The difference between Fe 2 O 3 and CeO 2 for the hydrolysis of COS is characterized in the atomic charge transfer and the formation of H O bond and H S bond. The transfer effect of H in H 2 O to S in COS over CeO 2 decreases the energy barriers of hydrolysis reaction, and enhances the reaction activity of COS hydrolysis.