The mechanism for CO(2)reduction over Fe-modified Cu(100) surfaces with thermodynamics and kinetics: a DFT study

摘要

The adsorption, activation and reduction of CO(2)over Fe-x/Cu(100) (x= 1-9) surfaces were examined by density functional theory. The most stable structure of CO(2)adsorption on the Fe-x/Cu(100) surface was realized. The electronic structure analysis showed that the doped Fe improved the adsorption, activation and reduction of CO(2)on the pure Cu(100) surface. From the perspective of thermodynamics and kinetics, the Fe-4/Cu(100) surface acted as a potential catalyst to decompose CO(2)into CO with a barrier of 32.8 kJ mol(-1). Meanwhile, the first principle molecular dynamics (FPMD) analysis indicated that the decomposition of the C-O1 bond of CO(2)on the Fe-4/Cu(100) surface was only observed from 350 K to 450 K under a CO(2)partial pressure from 0 atm to 10 atm. Furthermore, the results of FPMD analysis revealed that CO(2)would rather decompose than hydrogenate when CO(2)and H co-adsorbed on the Fe-4/Cu(100) surface.