Density Functional Theory Study on Mechanism of Mercury Removal by CeO2 Modified Activated Carbon

Doping of CeO2 on activated carbon (AC) can promote its performance for mercury abatement in flue gas, while the Hg-0 removal mechanism on the AC surface has been rarely reported. In this research, density functional theory (DFT) calculations were implemented to unveil the mechanism of mercury removal on plain AC and CeO2 modified AC (CeO2-AC) sorbents. Calculation results indicate that Hg-0, HCl, HgCl and HgCl2 are all chemisorbed on the adsorbent. Strong interaction and charge transfer are shown by partial density of states (PDOS) analysis of the Hg-0 adsorption configuration. HCl, HgCl and HgCl2 can be dissociatively adsorbed on the AC model and subsequently generate HgCl or HgCl2 released to the gas phase. The adsorption energies of HgCl and HgCl2 on the CeO2-AC model are relatively high, indicating a great capacity for removing HgCl and HgCl2 in flue gas. DFT calculations suggest that AC sorbents exhibit a certain catalytic effect on mercury oxidation, the doping of CeO2 enhances the catalytic ability of Hg-0 oxidation on the AC surface and the reactions follow the Langmuir-Hinshelwood mechanism.