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
相关论文
共 41 条
[1]   XPS and XAS study of the sorption of Hg(II) onto pyrite [J].
Behra, P ;
Bonnissel-Gissinger, P ;
Alnot, M ;
Revel, R ;
Ehrhardt, JJ .
LANGMUIR, 2001, 17 (13) :3970-3979
[2]  
Ehrhardt JJ, 2000, SURF INTERFACE ANAL, V30, P269, DOI 10.1002/1096-9918(200008)30:1<269::AID-SIA758>3.0.CO
[3]  
2-N
[4]   Three-Dimensionally Ordered Macroporous Iron Oxide for Removal of H2S at Medium Temperatures [J].
Fan, Hui-Ling ;
Sun, Ting ;
Zhao, Yan-Peng ;
Ju Shangguan ;
Lin, Jian-Ying .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (09) :4859-4865
[5]   Novel sorbents for mercury removal from flue gas [J].
Granite, EJ ;
Pennline, HW ;
Hargis, RA .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2000, 39 (04) :1020-1029
[6]   Reactive iron sulfide (FeS)-supported ultrafiltration for removal of mercury (Hg(II)) from water [J].
Han, Dong Suk ;
Orillano, Maria ;
Khodary, Ahmed ;
Duan, Yuhang ;
Batchelor, Bill ;
Abdel-Wahab, Ahmed .
WATER RESEARCH, 2014, 53 :310-321
[7]   Adsorption and Oxidation of Elemental Mercury over Ce-MnOx/Ti-PILCs [J].
He, Chuan ;
Shen, Boxiong ;
Chen, Jianhong ;
Cai, Ji .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2014, 48 (14) :7891-7898
[8]   Mercury pollution in China [J].
Jiang, Gui-Bin ;
Shi, Jian-Bo ;
Feng, Xin-Bin .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (12) :3672-3678
[9]   DOE/NETL's phase II mercury control technology field testing program: Preliminary economic analysis of activated carbon injection [J].
Jones, Andrew P. ;
Hoffmann, Jeffrey W. ;
Smith, Dennis N. ;
Feeley, Thomas J., III ;
Murphy, James T. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2007, 41 (04) :1365-1371
[10]   Outstanding Resistance of H2S-Modified Cu/TiO2 to SO2 for Capturing Gaseous Hg0 from Nonferrous Metal Smelting Flue Gas: Performance and Reaction Mechanism [J].
Kong, Lingnan ;
Zou, Sijie ;
Mei, Jian ;
Geng, Yang ;
Zhao, Hui ;
Yang, Shijian .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2018, 52 (17) :10003-10010