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:22
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
  • [21] Study on the regenerable sulfur-resistant sorbent for mercury removal from nonferrous metal smelting flue gas
    Quan, Zongwen
    Huang, Wenjun
    Liao, Yong
    Liu, Wei
    Xu, Haomiao
    Yan, Naiqiang
    Qu, Zan
    [J]. FUEL, 2019, 241 : 451 - 458
  • [22] An X-ray Photoelectron Spectroscopy Study of Surface Changes on Brominated and Sulfur-Treated Activated Carbon Sorbents during Mercury Capture: Performance of Pellet versus Fiber Sorbents
    Saha, Arindom
    Abram, David N.
    Kuhl, Kendra P.
    Paradis, Jennifer
    Crawford, Jenni L.
    Sasmaz, Erdem
    Chang, Ramsay
    Jaramillo, Thomas F.
    Wilcox, Jennifer
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (23) : 13695 - 13701
  • [23] XPS identification of bulk hole defects and itinerant Fe 3d electrons in natural troilite (FeS)
    Skinner, WM
    Nesbitt, HW
    Pratt, AR
    [J]. GEOCHIMICA ET COSMOCHIMICA ACTA, 2004, 68 (10) : 2259 - 2263
  • [24] Projections of Global Mercury Emissions in 2050
    Streets, David G.
    Zhang, Qiang
    Wu, Ye
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2009, 43 (08) : 2983 - 2988
  • [25] Mercury speciation and emissions from coal combustion in Guiyang, southwest China
    Tang, Shunlin
    Feng, Xinbin
    Qiu, Hanrong
    Yin, Guoxun
    Yang, Zaichan
    [J]. ENVIRONMENTAL RESEARCH, 2007, 105 (02) : 175 - 182
  • [26] Outstanding Performance of Magnetically Separable Sulfureted MoO3/Fe-Ti Spinel for Gaseous Hg0 Recovery from Smelting Flue Gas: Mechanism and Adsorption Kinetics
    Wang, Chang
    Zhang, Xufan
    Mei, Jian
    Hu, Qixing
    Yang, Shijian
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2020, 54 (12) : 7659 - 7668
  • [27] Novel Synergetic Effect of Fe and W in FeWx/TiO2 on Capturing High Concentrations of Gaseous Hg0 from Smelting Flue Gas: Adsorption Kinetics and Structure-Activity Relationship
    Wang, Chang
    Hu, Qixing
    Zhang, Qi
    Mei, Jian
    Yang, Shijian
    [J]. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2020, 59 (07) : 2745 - 2753
  • [28] Novel Synergistic Effect of Fe and Mo in FeMoSx/TiO2 for Recovering High Concentrations of Gaseous Hg0 from Smelting Flue Gas: Reaction Mechanism and Kinetics
    Wang, Chang
    Zhang, Xufan
    Mei, Jian
    Hu, Qixing
    Yang, Shijian
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2020, 54 (01) : 586 - 594
  • [29] Mercury emission and speciation of coal-fired power plants in China
    Wang, S. X.
    Zhang, L.
    Li, G. H.
    Wu, Y.
    Hao, J. M.
    Pirrone, N.
    Sprovieri, F.
    Ancora, M. P.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (03) : 1183 - 1192
  • [30] Update of mercury emissions from China's primary zinc, lead and copper smelters, 2000-2010
    Wu, Q. R.
    Wang, S. X.
    Zhang, L.
    Song, J. X.
    Yang, H.
    Meng, Y.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (22) : 11153 - 11163