Citation: LING Yang, WU Jiang. Interaction mechanism between unburned carbon in coal-fired fly ash and arsenic in flue gas based on the density functional theory[J]. Journal of Fuel Chemistry and Technology, ;2020, 48(11): 1365-1377. shu

Interaction mechanism between unburned carbon in coal-fired fly ash and arsenic in flue gas based on the density functional theory

LING Yang ^1,2 ,
WU Jiang ^1,,

1.
College of Energy and Mechanical Engineering, Shanghai University of Electric Power, Shanghai 200090, China
2.
School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China

Corresponding author: WU Jiang, wjcfd2002@163.com
Received Date: 10 September 2020
Revised Date: 21 October 2020

Fund Project: National Natural Science Foundation of China 52076126The project was supported by National Key Research and Development Program (2018YFB0605103), National Natural Science Foundation of China (52076126), and Natural Science Foundation of Shanghai (18ZR1416200)National Key Research and Development Program 2018YFB0605103Natural Science Foundation of Shanghai 18ZR1416200

Figures(13)

The interaction mechanism between the unburned carbon in fly ash and the arsenic pollutants in flue gas such as As, AsO, AsO₂ and As₂O₃ was studied based on the density functional theory. The results show that the elemental arsenic is preferentially adsorbed at the carbon bridge site, with an adsorption energy in the range (-5.95)-(-5.88) eV; the AsO molecule preferentially combines with the unburned carbon in a way that the arsenic and oxygen atoms are bound with the surface carbon atoms respectively, forming a most stable configuration with an adsorption energy of -7.87 eV. When AsO₂ is dissociated on the unburned carbon surface and form an AsO molecule and a surface reactive oxygen species, the system is the most stable, possessing an adsorption energy of -10.65 eV. While once the two oxygen atoms in a trigonal bipyramid As₂O₃ molecule first collide with the unburned carbon surface, it will be dissociated to small molecules of AsO and AsO₂, forming a covalent bond with surface carbon. The adsorption energy is significantly reduced to -10.64 eV, compared with the undissociated case. The unburned carbon in fly ash is easy to bind with AsO or AsO₂ small molecules, which locally tends to form a special five-member ring structure. Compared with As, AsO and AsO₂, the most toxic trivalent arsenic As₂O₃ is chemically stable and not easy to adsorb. Catalytic pyrolysis of As₂O₃ into small molecules of AsO and AsO₂ is expected to be a feasible measure to control the arsenic pollution in coal-fired power plants flue gas.
- coal-firedfly ash,
- unburned carbon,
- flue gas arsenic,
- density functional theory
1. [1]
  WANG C, LIU H, ZHANG Y, ZOU C, ANTHONY E J. Review of arsenic behavior during coal combustion: Volatilization, transformation, emission and removal technologies[J]. Prog Energy Combust Sci, 2018,68:1-28.
2. [2]
  YANG W, GAP Z, LIU X, DING X, YAN W. The adsorption characteristics of As₂O₃, Pb⁰, PbO and PbCl₂ on single atom iron adsorbent with graphene-based substrates[J]. Chem Eng J, 2019,361:304-313.
3. [3]
  ZHOU Qiang, DUAN Yu-feng, LU Ping. Research progress on in-duct mercury removal by sorbent injection in power plant[J]. Chem Ind Eng Prog, 2018,37(11):4460-4467.
4. [4]
  SUN X, WU J, LI Q, LIU Q, QI Y, YOU L, JI Z, HE P, SHENG P, REN J, ZHANG W, LU J, ZHANG J. Fabrication of BiOIO₃ with induced oxygen vacancies for efficient separation of the electron-hole pairs[J]. Appl Catal B: Environ, 2017,218:80-90.
5. [5]
  WANG J, ZHANG Y, WANG T, XU H, PAN W-P. Effect of modified fly ash injection on As, Se, and Pb emissions in coal-fired power plant[J]. Chem Eng J, 2020,380122561.
6. [6]
  WANG Yong-xing, HUANG Ya-ji, DONG Lu, YUAN Qi, DING Shou-yi, CHENG Hao-qiang, WANG Sheng, DUAN Yu-feng. 掺杂铁基氧化物吸附剂燃煤烟气脱汞实验研究[J]. J. Fuel Chem Technol, 2020,48(7):785-794.
7. [7]
  XU Ming-hou, WANG Wen-yu, WEN Chang, YU Dun-xi, LIU Xiao-wei. Research development of precipitation technology to accomplish the ultra-low emission from coal-fired power plants[J]. Proc CSEE, 2019,39(22):6627-6639.
8. [8]
  SHAH P, STREZOV V, PRINCE K, NELSON P F. Speciation of As, Cr, Se and Hg under coal fired power station conditions[J]. Fuel, 2008,87(10):1859-1869.
9. [9]
  TIAN C, GUPTA R, ZHAO Y, ZHANG J. Release behaviors of arsenic in fine particles generated from a typical high-arsenic coal at a high temperature[J]. Energy Fuels, 2016,30(8):6201-6209.
10. [10]
  SHEN F, LIU J, ZHANG Z, DAI J. On-line analysis and kinetic behavior of arsenic release during coal combustion and pyrolysis[J]. Environ Sci Technol, 2015,49(22):13716-13723.
11. [11]
  WINTER R M, MALLEPALLI R R, HELLEM K P, SZYDLO S W. Determination of As, Cd, Cr, and Pb species formed in a combustion environment[J]. Combust Sci Technol, 1994,101(1/6):45-58.
12. [12]
  YAN Ao, ZHANG Yue, WANG Chun-bo, BAI Tao, ZHAO Bin. Influence of O₂ on the formation of As₂O₃ by homogeneous reaction with As and AsO in the coal-fired flue gas[J]. J Fuel Chem Technol, 2020,48(1):11-17.
13. [13]
  ZHANF H, KONG M, CAI Z, JIANG L, LIU Q, YANG J, REN S, LI J, DUAN M. Synergistic effect of arsenic and different potassium species on V₂O₅-WO₃/TiO₂ catalyst poisoning: Comparison of Cl^-, SO₄^2- and NO₃^- anions[J]. Catal Commun, 2020,144106069.
14. [14]
  YUN Duan, SONG Qiang, YAO Qiang. Mechanism and analysis of SCR catalyst deactivation[J]. Coal Convers, 2009,32(1):91-96.
15. [15]
  YUN Duan, DENG Si-li, SONG Qiang, YAO Qiang. Potassium deactivation and regeneration method of V₂O₅-WO₃/TiO₂ SCR catalyst[J]. Res Environ Sci, 2009,22(6):730-735.
16. [16]
  LU Q, PEI X Q, WU Y W, XU M X, LIU D J, ZHAO L. Deactivation mechanism of the commercial v₂o₅-moo₃/tio₂ selective catalytic reduction catalyst by arsenic poisoning in coal-fired power plants[J]. Energy Fuels, 2020,34(4):4865-4873.
17. [17]
  LIU C, ZHAO Q, WANG Y, SHI P, JIANG M. Hydrothermal synthesis of calcium sulfate whisker from flue gas desulfurization gypsum[J]. Chin J Chem Eng, 2016,24(11):1552-1560.
18. [18]
  YANG P, LI X, TONG Z J, LI Q S, HE B Y, WANG L L, GUO S H, XU Z M. Use of flue gas desulfurization gypsum for leaching Cd and Pb in reclaimed tidal flat soil[J]. Environ Sci Pollut Res Int, 2016,23(8):7840-7848.
19. [19]
  CAO Z, CAO Y D, ZHANG J S, SUN C B, LI X L. Preparation and characterization of high-strength calcium silicate boards from coal-fired industrial solid wastes[J]. Int J Min Met Mater, 2015,22(8):892-900.
20. [20]
  LIU Z, HAO Y, ZHANG J, WU S, PAN Y, ZHOU J, QIAN G. The characteristics of arsenic in Chinese coal-fired power plant flue gas desulphurisation gypsum[J]. Fuel, 2020,271117515.
21. [21]
  HE X, YAO B, XIA Y, HUANG H, GAN Y, ZHANG W. Coal fly ash derived zeolite for highly efficient removal of Ni²⁺ inwaste water[J]. Powder Technol, 2020,367:40-46.
22. [22]
  LI Y, DANG L, YANG H, LI J, HU H. Removal of elemental mercury in flue gas by Cu-Fe modified magnetosphere from coal combustion fly ash[J]. Fuel, 2020,271117668.
23. [23]
  CHEN Ming-ming, DUAN Yu-feng, LI Jia-chen, ZHOU Qiang, LIU Shuai, LIU Meng. Experimental study of mercury removal mechanism by bromine-modified fly ash[J]. Proc CSEE, 2017,37(11):3207-3215.
24. [24]
  LI S, GONG H, HU H, LIU H, HUANG Y, FU B, WANG L, YAO H. Re-using of coal-fired fly ash for arsenic vapors in-situ retention before SCR catalyst: Experiments and mechanisms[J]. Chemosphere, 2020,254126700.
25. [25]
  GUEDES A, VALENTIM B, PRIETO A C, SANZ A, FLORES D, NORONHA F. Characterization of fly ash from a power plant and surroundings by micro-Raman spectroscopy[J]. Int J Coal Geol, 2008,73(3/4):359-370.
26. [26]
  BHARDWAJ R, CHEN X, VIDIC R D. Impact of fly ash composition on mercury speciation in simulated flue gas[J]. J Air Waste Manag Assoc, 2009,59(11):1331-1338.
27. [27]
  HOWER J C, SENIOR C L, SUUBERG E M, HURT R H, WILCOX J L, OLSON E S. Mercury capture by native fly ash carbons in coal-fired power plants[J]. Prog Energy Combust Sci, 2010,36(4):510-529.
28. [28]
  HE P, ZHANG X, PENG X, JIANG X, WU J, CHEN N. Interaction of elemental mercury with defective carbonaceous cluster[J]. J Hazard Mater, 2015,300:289-297.
29. [29]
  HE P, WU J, JIANG X, PAN W, REN J. Effect of SO₃ on elemental mercury adsorption on a carbonaceous surface[J]. Appl Surf Sci, 2012,258(22):8853-8860.
30. [30]
  QIN H, HE P, WU J, CHEN N. Theoretical study of hydrocarbon functional groups on elemental mercury adsorption on carbonaceous surface[J]. Chem Eng J, 2020,380122505.
31. [31]
  ZHU B, ZHANG J, JIANG C, CHENG B, YU J. First principle investigation of halogen-doped monolayer g-C₃N₄ photocatalyst[J]. Appl Catal B: Environ, 2017,207:27-34.
32. [32]
  LIU J, QU W, JOO S W, Chuguang Zheng. Effect of SO₂ on mercury binding on carbonaceous surfaces[J]. Chem Eng J, 2012,184:163-167.
33. [33]
  JUNGSUTTIWONG S, WONGNONGWA Y, NAMUANGRUK S, KUNGWAN N, PROMARAK V, KUNASETH M. Density functional theory study of elemental mercury adsorption on boron doped graphene surface decorated by transition metals[J]. Appl Surf Sci, 2016,362:140-145.
34. [34]
  LIU X, GAO Z, HUANG H, YAN G, HUANG T, CHEN C, YANG W, DING X-L. Simultaneous catalytic oxidation of nitric oxide and elemental mercury by single-atom Pd/g-C₃N₄ catalyst: A DFT study[J]. Mol Catal, 2020,488110901.
35. [35]
  LING L, FAN M, WANG B, ZHANG R. Application of computational chemistry in understanding the mechanisms of mercury removal technologies: a review[J]. Energy Environ Sci, 2015,8(11):3109-3133.
36. [36]
  YANG Tao, LIU Jin-jia, WANG Yan-dan, WEN Xiao-dong, SHEN Bao-jian. Structures and energetics of CO₂ adsorption on the Fe₃O₄ (111) surface[J]. J Fuel Chem Technol, 2018,46(9):1113-1120.
1. [1]
  Hao XU , Ruopeng LI , Peixia YANG , Anmin LIU , Jie BAI . Regulation mechanism of halogen axial coordination atoms on the oxygen reduction activity of Fe-N₄ site: A density functional theory study. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 695-701. doi: 10.11862/CJIC.20240302
2. [2]
  Kaifu Zhang , Shan Gao , Bin Yang . Application of Theoretical Calculation with Fun Practice in Raman Spectroscopy Experimental Teaching. University Chemistry, 2025, 40(3): 62-67. doi: 10.12461/PKU.DXHX202404045
3. [3]
  Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO₂ by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
4. [4]
  Jie ZHAO , Huili ZHANG , Xiaoqing LU , Zhaojie WANG . Theoretical calculations of CO₂ capture and separation by functional groups modified 2D covalent organic framework. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 275-283. doi: 10.11862/CJIC.20240213
5. [5]
  Xiaochen Zhang , Fei Yu , Jie Ma . 多角度数理模拟在电容去离子中的前沿应用. Acta Physico-Chimica Sinica, 2024, 40(11): 2311026-. doi: 10.3866/PKU.WHXB202311026
6. [6]
  Weina Wang , Lixia Feng , Fengyi Liu , Wenliang Wang . Computational Chemistry Experiments in Facilitating the Study of Organic Reaction Mechanism: A Case Study of Electrophilic Addition of HCl to Asymmetric Alkenes. University Chemistry, 2025, 40(3): 206-214. doi: 10.12461/PKU.DXHX202407022
7. [7]
  Meifeng Zhu , Jin Cheng , Kai Huang , Cheng Lian , Shouhong Xu , Honglai Liu . Classical Density Functional Theory for Understanding Electrochemical Interface. University Chemistry, 2025, 40(3): 148-152. doi: 10.12461/PKU.DXHX202405166
8. [8]
  Maitri Bhattacharjee , Rekha Boruah Smriti , R. N. Dutta Purkayastha , Waldemar Maniukiewicz , Shubhamoy Chowdhury , Debasish Maiti , Tamanna Akhtar . Synthesis, structural characterization, bio-activity, and density functional theory calculation on Cu(Ⅱ) complexes with hydrazone-based Schiff base ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1409-1422. doi: 10.11862/CJIC.20240007
9. [9]
  Zhengkun QIN , Zicong PAN , Hui TIAN , Wanyi ZHANG , Mingxing SONG . A series of iridium(Ⅲ) complexes with fluorophenyl isoquinoline ligand and low-efficiency roll-off properties: A density functional theory study. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1235-1244. doi: 10.11862/CJIC.20240429
10. [10]
  Yutao Lu , Jing Wu . Rebirth from the Flames: Unveiling the “Chemical Secrets” of Fire Smoke. University Chemistry, 2024, 39(9): 208-213. doi: 10.12461/PKU.DXHX202401001
11. [11]
  Xiangli Wang , Yuanfu Deng . Teaching Design of Elemental Chemistry from the Perspective of “Curriculum Ideology and Politics”: Taking Arsenic as an Example. University Chemistry, 2024, 39(2): 270-279. doi: 10.3866/PKU.DXHX202308092
12. [12]
  Mengyao Shi , Kangle Su , Qingming Lu , Bin Zhang , Xiaowen Xu . Determination of Potassium Content in Tobacco Stem Ash by Flame Atomic Absorption Spectroscopy. University Chemistry, 2024, 39(10): 255-260. doi: 10.12461/PKU.DXHX202404105
13. [13]
  Yueguang Chen , Wenqiang Sun . “Carbon” Adventures. University Chemistry, 2024, 39(9): 248-253. doi: 10.3866/PKU.DXHX202308074
14. [14]
  Jizhou Liu , Chenbin Ai , Chenrui Hu , Bei Cheng , Jianjun Zhang . 六氯锡酸铵促进钙钛矿太阳能电池界面电子转移及其飞秒瞬态吸收光谱研究. Acta Physico-Chimica Sinica, 2024, 40(11): 2402006-. doi: 10.3866/PKU.WHXB202402006
15. [15]
  Lei Shu , Zimin Duan , Yushen Kang , Zijian Zhao , Hong Wang , Lihua Zhu , Hui Xiong , Nan Wang . An Exploration of the CO₂-Involved Carbon Cycle World. University Chemistry, 2024, 39(5): 144-153. doi: 10.3866/PKU.DXHX202309084
16. [16]
  Shu'e Song , Xiaokui Wang , Yongmei Liu , Wanchun Zhu , Hong Yuan , Fuping Tian , Yunshan Bai , Yunchao Li , Li Wang , Zhongyun Wu , Yuan Chun , Jianrong Zhang , Shuyong Zhang . Suggestions on Operating Specifications of Physical Chemistry Experiment: Measurement of Viscosity, Density and Optical Properties. University Chemistry, 2025, 40(5): 148-156. doi: 10.12461/PKU.DXHX202503026
17. [17]
  Yi Yang , Xin Zhou , Miaoli Gu , Bei Cheng , Zhen Wu , Jianjun Zhang . Femtosecond transient absorption spectroscopy investigation on ultrafast electron transfer in S-scheme ZnO/CdIn₂S₄ photocatalyst for H₂O₂ production and benzylamine oxidation. Acta Physico-Chimica Sinica, 2025, 41(6): 100064-. doi: 10.1016/j.actphy.2025.100064
18. [18]
  Lei Shu , Zhengqing Hao , Kai Yan , Hong Wang , Lihua Zhu , Fang Chen , Nan Wang . Development of a Double-Carbon Related Experiment: Preparation, Characterization and Carbon-Capture Ability of Eggshell-Derived CaO. University Chemistry, 2024, 39(4): 149-156. doi: 10.3866/PKU.DXHX202310134
19. [19]
  Yanhui XUE , Shaofei CHAO , Man XU , Qiong WU , Fufa WU , Sufyan Javed Muhammad . Construction of high energy density hexagonal hole MXene aqueous supercapacitor by vacancy defect control strategy. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1640-1652. doi: 10.11862/CJIC.20240183
20. [20]
  Qiqi Li , Su Zhang , Yuting Jiang , Linna Zhu , Nannan Guo , Jing Zhang , Yutong Li , Tong Wei , Zhuangjun Fan . 前驱体机械压实制备高密度活性炭及其致密电容储能性能. Acta Physico-Chimica Sinica, 2025, 41(3): 2406009-. doi: 10.3866/PKU.WHXB202406009

Get Citation

PDF

XML

Metrics

PDF Downloads(4)
Abstract views(553)
HTML views(146)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142