LAUSR

Abstract Two-dimensional tungstenite (WS2) has great potential to efficiently control gaseous Hg0 release, because of its wide surface area and the high affinity between mercury and sulfur in WS2. The mercury species adsorption and conversion mechanism over raw and defective WS2(0 0 1) surface was investigated on the basis of density functional theory (DFT). The results show that Sdefect site on the WS2 surface exhibits more outstanding ability than Stop site to strongly adsorb Hg0. The oxidizing mercury species (HgO, HgS, HgCl and HgBr) are much easier to be adsorbed by WS2 than elemental mercury, with higher adsorption energy (from −76.09 to −182.59 kJ/mol). The reaction path in the formation of HgS includes a two-step process on S-WS2: Hg0 → HgS(ads) → HgS. In the first reaction step, the energy barrier of surface reaction between elemental mercury and defective S-WS2 is just 4.02 kJ/mol. The second desorption step is an endothermic process and the rate-determining step. The verifying experiment show that WS2 has excellent mercury removal ability at low reaction temperatures under different kinds of flue gas environment. In the whole, WS2 is one of most promising sorbent materials, which can be used for the efficient control of gaseous mercury.