Remarkable differences between copper-based sulfides and iron-based sulfides for the adsorption of high concentrations of gaseous elemental mercury: Mechanisms, kinetics, and significance

被引:24
作者
Hu, Qixing [1 ]
Wang, Chang [1 ]
Geng, Yang [1 ]
Zhang, Xufan [1 ]
Mei, Jian [1 ]
Yang, Shijian [1 ]
机构
[1] Jiangnan Univ, Sch Environm & Civil Engn, Wuxi 214122, Jiangsu, Peoples R China
关键词
Hg-0; adsorption; desorption; Cu-based sulfides; Fe-based sulfides; Kinetics; RECYCLABLE MAGNETIC SORBENT; FLUE-GAS; ATMOSPHERIC MERCURY; EMISSIONS; REMOVAL; HG(II); FLOW; XPS; FE; SPECIATION;
D O I
10.1016/j.jcis.2020.08.067
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Copper sulfides (CuSx) and iron sulfides (FeSx) have been developed to capture gaseous elemental mercury (Hg-0) originating from the smelting flue gas. However, these compounds exhibit different Hg-0 adsorption characteristics and Hg species adsorbed on CuSx can be spontaneously released as gaseous Hg-0. Following these findings, the adsorption/desorption kinetics of Hg-0 onto and from FeSx and CuSx were determined. After comparing the kinetic parameters, the mechanisms behind some of the remarkable differences between FeSx and CuSx with respect to Hg-0 adsorption were discovered. The Cu-S bond in CuSx was not completely broken during Hg-0 oxidation, but the S-S bond in FeSx was. Hence, the activation energy for the oxidation of Hg-0 physically adsorbed on CuSx was much lower than that for FeSx, resulting in a much higher efficiency of CuSx to oxidize Hg-0 than FeSx. However, the bond strength of Hg-S for HgS on CuSx was weaker due to the sharing of S2- in HgS with Cu+, resulting in a decrease in the thermal stability of HgS on CuSx. Therefore, HgS adsorbed on Cu-based sulfides was metastable, and could be spontaneously decomposed to release moderate concentrations of gaseous Hg-0, which was not preferable for capturing high concentrations of Hg-0. (C) 2020 Elsevier Inc. All rights reserved.
引用
收藏
页码:581 / 590
页数:10
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