SO2-Driven In Situ Formation of Superstable Hg3Se2Cl2 for Effective Flue Gas Mercury Removal.

Abstract

Flue gas mercury removal is mandatory for decreasing global mercury background concentration and ecosystem protection, but it severely suffers from the instability of traditional demercury products (e.g., HgCl2, HgO, HgS, and HgSe). Herein, we demonstrate a superstable Hg3Se2Cl2 compound, which offers a promising next-generation flue gas mercury removal strategy. Theoretical calculations revealed a superstable Hg bonding structure in Hg3Se2Cl2, with the highest mercury dissociation energy (4.71 eV) among all known mercury compounds. Experiments demonstrate its unprecedentedly high thermal stability (>400 °C) and strong acid resistance (5% H2SO4). The Hg3Se2Cl2 compound could be produced via the reduction of SeO32- to nascent active Se0 by the flue gas component SO2 and the subsequent combination of Se0 with Hg0 and Cl- ions or HgCl2. During a laboratory-simulated experiment, this Hg3Se2Cl2-based strategy achieves >96% removal efficiencies of both Hg0 and HgCl2 enabling nearly zero Hg0 re-emission. As expected, real mercury removal efficiency under Se-rich industrial flue gas conditions is much more efficient than Se-poor counterparts, confirming the feasibility of this Hg3Se2Cl2-based strategy for practical applications. This study sheds light on the importance of stable demercury products in flue gas mercury treatment and also provides a highly efficient and safe flue gas demercury strategy.