Citation: ZOU Chan, WANG Chun-bo, XING Jia-ying. Reaction mechanism of arsenic and nitrous oxides during coal combustion[J]. Journal of Fuel Chemistry and Technology, ;2019, 47(2): 138-143. shu

Reaction mechanism of arsenic and nitrous oxides during coal combustion

School of Energy, Power Engineering and Mechanical Engineering, North China Electric Power University, Baoding 071003, China

Corresponding author: ZOU Chan, hbdlzch@163.com
Received Date: 11 September 2018
Revised Date: 29 November 2018

Fund Project: the National Key R & D Program of China 2016YFB0600701The project was supported by the National Key R & D Program of China (2016YFB0600701) and the Fundamental Research Funds for the Central Universities (2017XS122)the Fundamental Research Funds for the Central Universities 2017XS122

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The reaction mechanism between arsenic and nitrous oxides (N₂O, NO₂ and NO) was investigated by applying density functional theory in quantum chemistry. The geometries of reactants, intermediates, transition states and products for each reaction were optimized. Frequency analysis was applied to verify those geometries, and the authenticity of transition states were confirmed by intrinsic reaction coordinate analysis (IRC). The stationary points of the single point energy were calculated at B2PLYP level, and the kinetic analysis was conducted to further reveal the reaction mechanism. Results show that the energy barrier of the reactions between arsenic and nitrous oxides (N₂O, NO₂ and NO) is 78.45, 2.58 and 155.85 kJ/mol, respectively. The reaction rate increases in the range of 298-1800 K and keeps at a high level (>10¹² cm³/(mol·s)), although the temperature has a tiny impact on the reaction of arsenic with NO₂ as a result of a low energy barrier, indicating that the reaction is easy to take place. Furthermore, it is found that the rate of reaction between arsenic and N₂O or NO has a rapid increase at 298-900 K, and then the rate increment becomes less with the further increase of temperature.
- coal combustion,
- arsenic,
- nitrous oxides,
- density functional theory,
- kinetics
1. [1]
  LI Wen-xiu, WANG Bao-feng, REN Jie, ZHANG Kai, YANG Feng-ling, CHENG Fang-qin. Effect of mineral matter on emissions of SO₂ and NO_x during combustion of lean coal in O₂/CO₂ atmosphere[J]. J Fuel Chem Technol, 2017,45(10):1200-1208. doi: 10.3969/j.issn.0253-2409.2017.10.007
2. [2]
  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, 2018,68:1-28. doi: 10.1016/j.pecs.2018.04.001
3. [3]
  LIU H, PAN W, WANG C, ZHANG Y. Volatilization of arsenic during coal combustion based on isothermal thermogravimetric analysis at 600-1500℃[J]. Energy Fuels, 2016,30(8):6790-6798. doi: 10.1021/acs.energyfuels.6b00816
4. [4]
  LIU H, WANG C, ZOU C, ZHANG Y, WANG J. Simultaneous volatilization characteristics of arsenic and sulfur during isothermal coal combustion[J]. Fuel, 2017,203:152-161. doi: 10.1016/j.fuel.2017.04.101
5. [5]
  TANG Q, LIU G J, ZHOU C C, SUN R Y. Distribution of trace elements in feed coal and combustion residues from two coal-fired power plants at Huainan, Anhui, China[J]. Fuel, 2013,107:315-322. doi: 10.1016/j.fuel.2013.01.009
6. [6]
  ZHAO Y, ZHANG J, HUANG W, WANG Z, LI Y, SONG D, ZHAO F, ZHENG C. Arsenic emission during combustion of high arsenic coals from Southwestern Guizhou, China[J]. Energy Convers Manage, 2008,49(4):615-624. doi: 10.1016/j.enconman.2007.07.044
7. [7]
  ZIELINSKI R A, FOSTER A L, MEEKER G P, BROWNFIELD I K. Mode of occurrence of arsenic in feed coal and its derivative fly ash, Black Warrior Basin, Alabama[J]. Fuel, 2007,86(4):560-572. doi: 10.1016/j.fuel.2006.07.033
8. [8]
  CONTRERAS M L, AROSTEGUI J M, ARMESTO L. Arsenic interactions during co-combustion processes based on thermodynamic equilibrium calculations[J]. Fuel, 2009,88:539-546. doi: 10.1016/j.fuel.2008.09.028
9. [9]
  LIU Ying-hui, ZHENG Chu-guang, YOU Xiao-qing, GUO Xin. Interaction between most volatile toxic trace elements during coal combustion[J]. J Combust Sci Technol, 2001,7(4):243-247. doi: 10.3321/j.issn:1006-8740.2001.04.007
10. [10]
  URBAN D R, WILCOX J. A theoretical study of properties and reactions involving arsenic and selenium compounds present in coal combustion flue gases[J]. J Phys Chem A, 2006,110(17):5847-5852. doi: 10.1021/jp055564+
11. [11]
  MONAHAN-PENDERGAST M, PRZYBYLEK M, LINDBLAD M, WILCOX J. Theoretical predictions of arsenic and selenium species under atmospheric conditions[J]. Atmos Environ, 2008,42(10):2349-2357. doi: 10.1016/j.atmosenv.2007.12.028
12. [12]
  URBAN D R, WILCOX J. Theoretical study of the kinetics of the reactions Se + O₂ → Se + O and As + HCl → AsCl + H[J]. J Phys Chem A, 2006,110(28):8797-8801. doi: 10.1021/jp0628986
13. [13]
  LEI Ming, HUANG Xing-zhi, WANG Chun-bo. NO emission characteristics of typical coals under O₂/CO₂/H₂O atmosphere at intermediate and high temperatures[J]. J Chin Soc Power Eng, 2017,37(6):432-439.
14. [14]
  WANG Chun-bo, YUE Shuang, XU Xu-bin, LI Yi-peng. NO_x release of char in constant temperature combustion under O₂/CO₂ atmosphere[J]. J China Coal Soc, 2018,43(1):257-264.
15. [15]
  XIAO Hai-ping, ZHOU Jun-hu, LIU Jian-zhong, SUN Bao-ming, YE Li-ping. Effect mechanism of existence pattern of sulphur on reduction of NO[J]. J Fuel Chem Technol, 2008,36(3):381-384. doi: 10.3969/j.issn.0253-2409.2008.03.024
16. [16]
  LIU Jing, ZHENG Chu-guang, QIU Jian-rong. Study on quantum chemistry calculation method of mercury reactions in combustion flue gas[J]. J Eng Thermophys, 2007,28(3):519-522. doi: 10.3321/j.issn:0253-231X.2007.03.050
17. [17]
  AWUAHA J B, DZADE N Y, TIA R, ADEI E, KWAKYE-AWUAHAD B, CATLOW C R A, DE LEEUW N H. A density functional theory study of arsenic immobilization by the Al(iii)-modified zeolite clinoptilolite[J]. Phys Chem Chem Phys, 2016,18(16):11297-11305. doi: 10.1039/C6CP00190D
18. [18]
  FRISCH M J, TRUCKS G W, SCHLEGEL H B. Gaussian 09, Revision D.01[J]. Gaussian, Inc., Wallingford, CT, 2009.
19. [19]
  ZHANG H, LIU J, SHEN J, JIANG X. Thermodynamic and kinetic evaluation of the reaction between NO (nitric oxide) and char(N) (char bound nitrogen) in coal combustion[J]. Energy, 2015,82(C):312-321.
20. [20]
  SCHRÖDER B, SEBALD P, STEIN C, WESER O, BOTSCHWINA P. Challenging high-level ab initio rovibrational spectroscopy:The nitrous oxide molecule[J]. Z Phys Chem, 2015,229(10/12):1663-1690.
21. [21]
  BORISENKO K B, KOLONITS M, ROZSONDAI B, HARGITTAI I. Electron diffraction study of the nitrogen dioxide molecular structure at 294, 480, and 691 K[J]. J Mol Struct, 1997,413-414:121-131. doi: 10.1016/S0022-2860(96)09588-9
22. [22]
  MARSDEN C J, SMITH B J. AB initio force constants:A cautionary tale concerning nitrogen oxides[J]. J Mol Struct:Theochem, 1989,187:337-357. doi: 10.1016/0166-1280(89)85174-7
23. [23]
  EVENSON K M, WELLS J S, RADFORD H E. Infrared resonance of OH with the H₂O laser:A galactic maser pump?[J]. Phys Rev Lett, 1970,25(4):199-202. doi: 10.1103/PhysRevLett.25.199
24. [24]
  MIZUSHIMA M. Molecular parameters of OH free radical[J]. Phys Rev A, 1972,5(1):143-157. doi: 10.1103/PhysRevA.5.143
25. [25]
  WANG Peng-qian, WANG Chang-an, DU Yong-bo, ZHANG Long-fei, CHE De-fu. Experimental investigation on the NO₂ reduction property under O₂/CO₂ combustion condition[J]. J Xi'an Jiaotong Univ, 2017,51(5):16-22.
26. [26]
  JIAO A, ZHANG H, LIU J, SHEN J, JIANG X. The role of CO played in the nitric oxide heterogeneous reduction:A quantum chemistry study[J]. Energy, 2017,141:1538-1546. doi: 10.1016/j.energy.2017.11.115
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