2020 Volume 39 Issue 5
Article Contents

LI Xiaohang, TENG Yang, WANG Pengcheng, LI Lifeng, ZHANG Kai. Release characteristics of mercury in fly ashes collected from coal-fired CFB power units during thermal treatment[J]. Environmental Chemistry, 2020, (5): 1375-1383. doi: 10.7524/j.issn.0254-6108.2020010702
Citation: LI Xiaohang, TENG Yang, WANG Pengcheng, LI Lifeng, ZHANG Kai. Release characteristics of mercury in fly ashes collected from coal-fired CFB power units during thermal treatment[J]. Environmental Chemistry, 2020, (5): 1375-1383. doi: 10.7524/j.issn.0254-6108.2020010702

Release characteristics of mercury in fly ashes collected from coal-fired CFB power units during thermal treatment

  • Corresponding author: ZHANG Kai, kzhang@ncepu.edu.cn
  • Received Date: 07/01/2020
    Fund Project: Supported by the National Natural Science Foundation of China (U1610254), Major Special Project of Shanxi Province (MD2015-01) and Fundamental Research Funds for the Central Universities (2017MS020).
  • In order to investigate release characteristics of mercury in fly ashes collected from a coal-fired CFB power unit, the effect of temperature and time on mercury release characteristics of fly ash samples as well as release rules of mercury in fly ash samples were analyzed through the heat treatment experiments and temperature-programmed pyrolysis experiments. Moreover, the mechanism of mercury adsorption was examined based on the fitting results of first order kinetic model, Elovich kinetic model, Freundlich kinetic model and parabolic diffusion kinetic model. The results of heat treatment experiments showed that mercury release rate of the CFB fly ash was closely related to the heating temperature and time. The release rate of mercury in the CFB fly ash was lower than 0.2 at temperature below 200 ℃, while the release rate of mercury in the CFB fly ash was no less than 0.935 at the temperature over 300 ℃. The results of temperature-programmed pyrolysis experiments suggested that Mercury species present in the fly ash include HgCl2, Hg2Cl2, HgO, HgSO4, HgS (black) and HgS (red). HgS (black) and HgS (red) were the main mercury species present in the fly ash. The fitting results of kinetic equation showed that Elovich kinetic model was more applicable to reflect the Hg release from the fly ash, while the correlation coefficient R2 between the experimental and calculated data was greater than 0.95. It is indicated that this process controlled by multiple reaction mechanisms, and the activation energy changes greatly.
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  • [1] UNEP. Mercury fate and transport in the global atmosphere:Measurement, models and policy implication report[R]. Geneva:UNEP, 2008.

    Google Scholar Pub Med

    [2] UNEP. Global mercury assessment 2013:Sources, emissions, releases and environmental transport[R]. Geneva, Switzerland:UNEP Chemicals Branch, 2013.

    Google Scholar Pub Med

    [3] 孙淑静, 刘学敏. 我国粉煤灰资源化利用现状、问题及对策分析[J]. 粉煤灰综合利用, 2015(3):49-52. SUN S J, LIU X M. Recycling utilization of fly ash in china:Situations, problems and countermeasures[J]. Fly Ash Comprehensive Utilization, 2015 (3):49-52(in Chinese).

    Google Scholar Pub Med

    [4] 任建莉, 周劲松, 骆仲泱, 等. 燃煤电站汞排放分布及控制研究的进展[J]. 电站系统工程, 2006, 22(1):44-46. REN J L, ZHOU J S, LUO Z Y, et al. A review of mercury speciation and control for coal-fired power plants[J]. Power System Engineering, 2006, 22(1):44-46(in Chinese).

    Google Scholar Pub Med

    [5] PAVLISH J H, SONDREAL E A, MANN M D, et al. Status review of mercury control options for coal-fired power plants[J]. Fuel Processing Technology, 2003, 82(2):89-165.

    Google Scholar Pub Med

    [6] 姚多喜, 支霞臣, 郑宝山. 煤燃烧过程中5种微量元素的迁移和富集[J]. 环境化学, 2004, 23(1):31-37. YAO D X, ZHI X C, ZHENG B S. The transformation and concentration of 5 trace elements during coal combustion[J]. Environmental Chemistry, 2004, 23(1):31-37(in Chinese).

    Google Scholar Pub Med

    [7] 孟阳, 王书肖. 粉煤灰综合利用过程中汞的二次释放规律研究[J]. 环境科学, 2012, 33(9):2993-2999. MENG Y, WANG S X. Study on mercury re-emissions during fly ash utilization[J]. Environmental Science, 2012, 33(9):2993-2999(in Chinese).

    Google Scholar Pub Med

    [8] 张淼, 张梦泽, 董勇. 燃煤电厂固废利用过程中汞的二次污染分析[J]. 节能技术, 2014, 32(1):45-47. ZHANG M, ZHANG M Z, DONG Y. Analyze of mercury re-emission during the utilization of coal-fired power plant solid wastes[J]. Energy Conservation Technology, 2014, 32(1):45-47(in Chinese).

    Google Scholar Pub Med

    [9] RUBEL A M, HOWER J C, MARDON S M, et al. Thermal stability of mercury captured by ash[J]. Fuel, 2006, 85(17-18):2509-2515.

    Google Scholar Pub Med

    [10] 武成利, 陈晨, 田梦琦, 等. 燃煤电厂粉煤灰中汞的稳定性研究[J]. 环境污染与防治, 2016, 38(6):20-23. WU C L, CHEN C, TIAN M Q, et al. Study on the stability of mercury in fly ash at coal-fired power plant[J]. Environmental Pollution and Prevention, 2016,38(6):20-23(in Chinese).

    Google Scholar Pub Med

    [11] 高正阳, 吕少昆, 陈嵩涛, 等. ESP对燃煤电站锅炉颗粒汞形态及热稳定性的影响[J]. 华北电力大学学报:自然科学版, 2015, 42(1):63-68. GAO Z Y, LV S K, CHEN S T, et al. ESP effects on particulate mercury speciation and thermal stability in coal-fired utility boiler[J]. Journal of North China Electric Power University, 2015, 42(1):63-68(in Chinese).

    Google Scholar Pub Med

    [12] 程乐鸣, 岑可法, 倪明江, 等.循环流化床锅炉炉膛热力计算[J].中国电机工程学报,2002,22(12):146-151. CHENG L M, CEN K F, NI M J, et al. Thermal calculation of a circulating fluidized bed boiler furnace[J]. Proceedings of the CSEE, 2002, 22(12):146-151(in Chinese).

    Google Scholar Pub Med

    [13] 姜秀民, 孙东红, 闫澈, 等. 65t/h示范性油页岩循环流化床电厂锅炉运行实践[J].中国电机工程学报,2001,21(2):69-73. JIANG X M, SUN D H, YAN C, et al. Performance characteristics of 65t/h oil shale-fired circulating fluidized bed demonstration utility boiler[J].Proceedings of the CSEE,2001,21(2):69-73(in Chinese).

    Google Scholar Pub Med

    [14] 谢磊, 毛国明, 金晓明,等. 循环流化床锅炉燃烧过程预测控制与经济性能优化[J]. 化工学报, 2016, 67(3):695-700. XIE L, MAO G M, JIN X M, et.al. Predictive control and economic performance optimization of CFBB combustion process[J]. CIESC Journal, 2016, 67(3):695-700(in Chinese).

    Google Scholar Pub Med

    [15] WANG S, ZHANG Y, GU Y, et al. Using modified fly ash for mercury emissions control for coal-fired power plant applications in China[J]. Fuel, 2016, 16; 1230-1237.

    Google Scholar Pub Med

    [16] 段钰锋, 江贻满, 杨立国,等. 循环流化床锅炉汞排放和吸附实验研究[J]. 中国电机工程学报, 2008, 28(32):1-5. DUAN Y F, JIANG Y M, YANG L G, et.al. Experimental study on mercury emission and adsorption in circulating fluidized bed boiler[J]. Proceedings of the CSEE, 2008, 28(32):1-5(in Chinese).

    Google Scholar Pub Med

    [17] 樊保国, 贾里, 李晓栋, 等. 电站燃煤锅炉飞灰特性对其吸附汞能力的影响[J]. 动力工程学报, 2016, 36(8):621-628. FAN B G, JIA L, LI X D, et.al. Study on mercury adsorption by fly ash form coal-fired coilers of power plants[J]. Journal of Chinese Society of Power Engineering, 2016, 36(8):621-628(in Chinese).

    Google Scholar Pub Med

    [18] 李晓航, 刘芸, 苏银皎, 等. 煤粉炉和循环流化床锅炉飞灰特性对其汞吸附能力的影响[J]. 化工学报, 2019, 70(3):295-302. LI X H, LIU Y, SU Y J, et al. Difference of fly ash characteristics from PC and CFB boilers and its effect on mercury adsorption capability[J]. CIESC Journal, 2019, 70(3):295-302(in Chinese).

    Google Scholar Pub Med

    [19] 李晓航,刘红刚,路建洲,等.煤粉炉和循环流化床锅炉飞灰吸附汞动力学及其吸附机制[J]. 化工学报, 2019,70(11):4397-4409. LI X H, LIU H G, LU J Z, et al. Kinetics and mechanism of mercury adsorption on fly ashes from pulverized coal boiler and circulating fluidized bed boiler[J]. CIESC Journal, 2019, 70(11):4397-4409(in Chinese).

    Google Scholar Pub Med

    [20] 苏银皎, 刘轩, 李丽锋, 等. 三类煤阶煤中汞的赋存形态分布特征[J]. 化工学报, 2019, 70(4):324-331. SU Y J, LI X H, LI L F, et al. Distribution characteristics of mercury speciation in coals with three different ranks[J]. CIESC Journal, 2019, 70(4):324-331(in Chinese).

    Google Scholar Pub Med

    [21] LOPZE-ANTON M A, YUAN Y, PERRY R, et al. Analysis of mercury species present during coal combustion by thermal desorption[J]. Fuel, 2010, 89(3):629-634.

    Google Scholar Pub Med

    [22] 于颖, 邵子婴, 刘靓,等. 热强化气相抽提法修复半挥发性石油烃污染土壤的影响因素[J]. 环境工程学报, 2017, 11(4):2252-2257. YU Y, SHAO Z Y, LIU L, et al. Factors influencing remediation of semi-volatile petroleum hydrocarbon-contaminated soil by thermally enhanced soil vapor extraction[J]. Chinese Journal of Environmental Engineering, 2017,11(4):2252-2257(in Chinese).

    Google Scholar Pub Med

    [23] 涂从. 土壤体系中的化学动力学方程及其应用[J]. 热带亚热带土壤科学, 1994, 3(3):175-182. TU C. Equations of chemical kineties and their application to soil system[J]. Tropical and Subtropical Soil Science, 1994,3(3):175-182(in Chinese).

    Google Scholar Pub Med

    [24] 许端平, 何依琳, 庄相宁, 等. 热解吸修复污染土壤过程中DDTs的去除动力学[J]. 环境科学研究, 2013, 26(2):202-207. XU D P, HE Y L, ZHUANG X Y, et al. Desorption kinetics of DDTs from contaminated soil during processes of thermal desorption[J]. Research of Environmental Sciences, 2013, 26(2):202-207(in Chinese).

    Google Scholar Pub Med

    [25] COURCHESNE F, HENDERSHOT W H. Kinetics of sulfate of desorption from two spodosols of the laurentians, quebec1[J]. Soil Science, 1990, 150(6):858-866.

    Google Scholar Pub Med

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Release characteristics of mercury in fly ashes collected from coal-fired CFB power units during thermal treatment

Fund Project: Supported by the National Natural Science Foundation of China (U1610254), Major Special Project of Shanxi Province (MD2015-01) and Fundamental Research Funds for the Central Universities (2017MS020).

Abstract: In order to investigate release characteristics of mercury in fly ashes collected from a coal-fired CFB power unit, the effect of temperature and time on mercury release characteristics of fly ash samples as well as release rules of mercury in fly ash samples were analyzed through the heat treatment experiments and temperature-programmed pyrolysis experiments. Moreover, the mechanism of mercury adsorption was examined based on the fitting results of first order kinetic model, Elovich kinetic model, Freundlich kinetic model and parabolic diffusion kinetic model. The results of heat treatment experiments showed that mercury release rate of the CFB fly ash was closely related to the heating temperature and time. The release rate of mercury in the CFB fly ash was lower than 0.2 at temperature below 200 ℃, while the release rate of mercury in the CFB fly ash was no less than 0.935 at the temperature over 300 ℃. The results of temperature-programmed pyrolysis experiments suggested that Mercury species present in the fly ash include HgCl2, Hg2Cl2, HgO, HgSO4, HgS (black) and HgS (red). HgS (black) and HgS (red) were the main mercury species present in the fly ash. The fitting results of kinetic equation showed that Elovich kinetic model was more applicable to reflect the Hg release from the fly ash, while the correlation coefficient R2 between the experimental and calculated data was greater than 0.95. It is indicated that this process controlled by multiple reaction mechanisms, and the activation energy changes greatly.

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