The design of high-entropy metal sulfides promising high-performance gaseous elemental mercury removal

Abstract

Regulating the surface coordination environment and improving the formation of active species represent the key factor in designing high-performance metal sulfide-based sorbents for gaseous Hg0 capture. This paper reported the Hg0 adsorption by high entropy metal sulfides for the first time, and clarified the mechanisms involved in the evolutions of active species as well as the Hg0 adsorption. The multiple metal components of the high entropy metal sulfides have great significance in improving the surface chemistry. The addition of Ce helps not only the formation of chemically homogeneous structure, but also the generation of high valence state metal cations and unsaturated sulfur species, thereby improving obviously the Hg0 removal ability. The synthesized CeNiCoMnCuSx has a high Hg0 adsorption capacity of 10.52 mg·g−1 at 80 %-breakthrough, and a Hg0 adsorption rate of 4.31 μg·g−1·min−1. The high valence state metal cations (Ni3+, Co3+, Mn4+, Cu2+ and Ce4+) and unsaturated Sx2− and S22− species can directly oxidize Hg0 and convert it into HgS. In comparison, the quaternary sulfide counterpart (NiCoMnCuSx) cannot form a main phase structure, and has obviously lower percentages of high valence state metal cations and unsaturated sulfur species. This work provides a new space for developing metal sulfides for Hg0 adsorption.