Skip to main content

Advertisement

SpringerLink
Log in

Theoretical study of the reactions between arsenic and nitrogen oxides during coal combustion

  • Original Paper
  • Published:
Journal of Molecular Modeling Aims and scope Submit manuscript

Abstract

The reactions between arsenic and nitrogen oxides (N2O, NO2, and NO) were investigated using density functional theory. The geometries of the reactants, intermediates, transition states, and products in each reaction were optimized. Frequency analysis was applied to verify those geometries, and the authenticity of each transition state was checked using intrinsic reaction coordinate analysis (IRC). The single point energy of each stationary point was calculated at the B2PLYP level, and kinetic analysis was conducted to explore each reaction mechanism in more detail. Results showed that the energy barriers to the reactions of As with N2O, NO2, and NO were 78.45, 2.58, and 155.85 kJ mol−1, respectively. For each reaction, the rate increased as the temperature was increased from 298 to 1800 K. However, temperature had only a tiny impact on the reaction of As with NO2 due to the low energy barrier involved, and the reaction rate was consistently high (>1012 cm3 mol−1 s−1), which indicates that this reaction occurs readily. On the other hand, the rate of the reaction between As and N2O or NO increased rapidly between 298 and 900 K, and then increased more gradually upon further increasing the temperature.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  1. Liu G, Zheng L, Duzgoren-Aydin NS, Gao L, Liu J, Peng Z (2007) Health effects of arsenic, fluorine, and selenium from indoor burning of Chinese coal. Rev Environ Contam Toxicol 189:89–106

    CAS  Google Scholar 

  2. Zhao Y, Zhang J, Huang W, Wang Z, Li Y, Song D, Zhao F, Zheng C (2008) Arsenic emission during combustion of high arsenic coals from southwestern Guizhou, China. Energy Convers Manag 49(4):615–624

    Article  CAS  Google Scholar 

  3. Jiao F, Ninomiya Y, Zhang L, Yamada N, Sato A (2013) Effect of coal blending on the leaching characteristics of arsenic in fly ash from fluidized bed coal combustion. Fuel Process Technol 106:769–775

    Article  CAS  Google Scholar 

  4. Shah P, Strezov V, Prince K, Nelson PF (2008) Speciation of As, Cr, Se and Hg under coal fired power station conditions. Fuel 87(10-11):1859–1869

    Article  CAS  Google Scholar 

  5. Wang C, Liu H, Zhang Y, Zou C, Anthony EJ (2018) Review of arsenic behavior during coal combustion: volatilization, transformation, emission and removal technologies. Prog Energy Combust Sci 68:1–28

    Article  Google Scholar 

  6. Tang Q, Liu G, Yan Z, Sun R (2012) Distribution and fate of environmentally sensitive elements (arsenic, mercury, stibium and selenium) in coal-fired power plants at Huainan, Anhui, China. Fuel 95:334–339

    Article  CAS  Google Scholar 

  7. Liu H, Pan W, Wang C, Zhang Y (2016) Volatilization of arsenic during coal combustion based on isothermal thermogravimetric analysis at 600–1500 °C. Energy Fuel 30(8):6790–6798

  8. Liu H, Wang C, Sun X, Zhang Y, Zou C (2016) Volatilization of arsenic in coal during isothermal oxy-fuel combustion. Energy Fuel 30(4):3479–3487

    Article  CAS  Google Scholar 

  9. Contreras ML, Arostegui JM, Armesto L (2009) Arsenic interactions during co-combustion processes based on thermodynamic equilibrium calculations. Fuel 88(3):539–546

    Article  CAS  Google Scholar 

  10. Frandsen F, Johansen D, Rasmussen P (1994) Trace elements from combustion and gasification of coal—an equilibrium approach. Prog Energy Combust Sci 20(2):115–138

    Article  CAS  Google Scholar 

  11. Urban DR, Wilcox J (2006) A theoretical study of properties and reactions involving arsenic and selenium compounds present in coal combustion flue gases. J Phys Chem A 110(17):5847–5852

    Article  CAS  PubMed  Google Scholar 

  12. Monahan-Pendergast M, Przybylek M, Lindblad M, Wilcox J (2008) Theoretical predictions of arsenic and selenium species under atmospheric conditions. Atmos Environ 42(10):2349–2357

    Article  CAS  Google Scholar 

  13. Xu J, Sun R, Ismail TM, Sun S, Wang Z (2017) Effect of char particle size on NO release during coal char combustion. Energy Fuel 31(12):13406–13415

    Article  CAS  Google Scholar 

  14. Wang Z, Xu J, Sun R, Zhao Y, Li Y, Ismail TM (2017) Investigation of the NO reduction characteristics of coal char at different conversion degrees under an NO atmosphere. Energy Fuel 31:8722–8732

    Article  CAS  Google Scholar 

  15. Zhang H, Liu J, Shen J, Jiang X (2015) Thermodynamic and kinetic evaluation of the reaction between NO (nitric oxide) and char(N) (char bound nitrogen) in coal combustion. Energy 82:312–321

    Article  CAS  Google Scholar 

  16. Liu J, Qu W, Yuan J, Wang S, Qiu J, Zheng C (2010) Theoretical studies of properties and reactions involving mercury species present in combustion flue gases. Energy Fuel 24(1):117–122

    Article  CAS  Google Scholar 

  17. Peng Y, Li J, Si W, Luo J, Dai Q, Luo X, Liu X, Hao J (2014) Insight into deactivation of commercial SCR catalyst by arsenic: an experiment and DFT study. Environ Sci Technol 48(23):13895–13900. https://doi.org/10.1021/es503486w

  18. Liu J, Qu W, Zheng C (2013) Theoretical studies of mercury–bromine species adsorption mechanism on carbonaceous surface. Proc Combust Inst 34(2):2811–2819

    Article  CAS  Google Scholar 

  19. Lu T, Chen F (2012) Multiwfn: a multifunctional wavefunction analyzer. J Comput Chem 33(5):580–592

    Article  Google Scholar 

  20. Du X, Tang J, Gao X, Chen Y, Ran J, Zhang L (2016) Molecular transformations of arsenic species in the flue gas of typical power plants: a density functional theory study. Energy Fuel 30(5):4209–4214

    Article  CAS  Google Scholar 

  21. Awuaha JB, Dzade NY, Tiac R, Adeic E, Kwakye-Awuahad B, Catlowe CRA, Leeuwbde NH (2016) A density functional theory study of arsenic immobilization by the Al(III)-modified zeolite clinoptilolite. Phys Chem Chem Phys 18(16):11297–11305

  22. Gao Z, Yang W (2016) Effects of CO/CO2/NO on elemental lead adsorption on carbonaceous surfaces. J Mol Model 22:166

    Article  PubMed  Google Scholar 

  23. Ye S, Neese F (2010) Accurate modeling of spin-state energetics in spin-crossover systems with modern density functional theory. Inorg Chem 49:772–774

    Article  CAS  PubMed  Google Scholar 

  24. Frisch MJ, Trucks GW, Schlegel HB, Scuseria GE, Robb MA, Cheeseman JR, Scalmani G, Barone V, Mennucci B, Petersson GA, Nakatsuji H, Caricato M, Li X, Hratchian HP, Izmaylov AF, Bloino J, Zheng G, Sonnenberg JL, Hada M, Ehara M, Toyota K, Fukuda R, Hasegawa J, Ishida M, Nakajima T, Honda Y, Kitao O, Nakai H, Vreven T, Montgomery Jr JA, Peralta JE, Ogliaro F, Bearpark M, Heyd JJ, Brothers E, Kudin KN, Staroverov VN, Keith T, Kobayashi R, Normand J, Raghavachari K, Rendell A, Burant JC, Iyengar SS, Tomasi J, Cossi M, Rega N, Millam JM, Klene M, Knox JE, Cross JB, Bakken V, Adamo C, Jaramillo J, Gomperts R, Stratmann RE, Yazyev O, Austin AJ, Cammi R, Pomelli C, Ochterski JW, Martin RL, Morokuma K, Zakrzewski VG, Voth GA, Salvador P, Dannenberg JJ, Dapprich S, Daniels AD, Farkas O, Foresman JB, Ortiz JV, Cioslowski J, Fox DJ (2013) Gaussian 09, revision D.01. Gaussian, Inc., Wallingford

  25. Gao Z, Lv S, Yang W, Yang P, Ji S, Meng X (2015) Quantum chemistry investigation on the reaction mechanism of the elemental mercury, chlorine, bromine and ozone system. J Mol Model 21:160

    Article  PubMed  Google Scholar 

  26. Schröder B, Sebald P, Stein C, Weser O, Botschwina P (2015) Challenging high-level ab initio rovibrational spectroscopy: the nitrous oxide molecule. Z Phys Chem 229(10-12):1663–1690

    Article  Google Scholar 

  27. Borisenko KB, Kolonits R, Rozsondai B, Hargittai I (1997) Electron diffraction study of the nitrogen dioxide molecular structure at 294, 480, and 691 K. J Mol Struct 413-414:121–131

    Article  Google Scholar 

  28. Marsden CJ, Smith BJ (1989) Ab initio force constants: a cautionary tale concerning nitrogen oxides. J Mol Struct THEOCHEM 187:337–357

  29. Evenson KM, Wells JS, Radford HE (1970) Infrared resonance of OH with the H2O laser: a galactic maser pump? Phys Rev Lett 25(4):199–202

    Article  CAS  Google Scholar 

  30. Mizushima M (1972) Molecular parameters of OH free radical. Phys Rev A 5(1):143–157

Download references

Acknowledgements

Financial support was provided by the National Key R&D Program of China (no. 2016YFB0600701).

Author information

Authors and Affiliations

  1. Department of Energy Power & Mechanical Engineering, North China Electric Power University, Baoding, 071003, China

    Chan Zou & Chunbo Wang

Authors
  1. Chan Zou
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Chunbo Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Chunbo Wang.

Additional information

Publisher’s Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zou, C., Wang, C. Theoretical study of the reactions between arsenic and nitrogen oxides during coal combustion. J Mol Model 25, 30 (2019). https://doi.org/10.1007/s00894-018-3916-0

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s00894-018-3916-0

Keywords

Search

Navigation