Abstract
Enhancement of the formation of unsaturated short-chain sulfur represents the key point in enhancing the gaseous elemental mercury (Hg0) capture by sulfur-based sorbents, and yet the sulfur often agglomerates into long-chain species. Herein, by doping with iron cation as the regulator of the coordination environment of sulfur, the long-chain sulfur was successfully converted into short-chain sulfur on carbon. The iron-sulfur loaded carbon shows a high Hg0 adsorption capacity of 72.8 mg·g−1 (80 % breakthrough) and a low cost of $42.09/kg Hg, which are superior to various sulfur modified carbons and metal sulfides. The iron can not only immobilize more amount of sulfur on carbon surface, but also break the S-S bonds. The double interaction of iron and carbon with sulfur facilitates the formation of short-chain sulfur species for Hg0 adsorption. Density functional calculations suggest that S, Fe and C sites on surface are active centers for Hg adsorption. The Hg can tri-coordinate with S, Fe and C sites, which gives a high adsorption energy of − 219.3 kJ‧mol−1, confirming the strong reaction. This work provides a new in insights into the regulation of the coordination environment of sulfur, which allows the designing of high-capacity and low-cost sorbents for gaseous Hg0 removal.
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