Energy Technology & Innovation Initiative FACULTY OF ENGINEERING. Mercury oxidation. Alastair Clements 13/06/2012
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1 Energy Technology & Innovation Initiative FACULTY OF ENGINEERING Mercury oxidation Alastair Clements 13/06/2012
2 Outline Introduction to mercury Mercury oxidation Oxidation modelling Summary Further work
3 Mercury Toxicity Methyl mercury ([HgCH 3 ] + ) forms in the environment. Potent neurotoxin; RfD = µg/kg per day. Bioaccumulates through the food web into lethal doses. Transport 6-18 months atmospheric lifetime. Global distribution from source. Corrosion Mercury forms amalgams with many metals, including aluminium. Alastair Clements Mercury oxidation 3/18
4 Mercury oxidation Elemental Hg thermodynamically favoured at high temperatures. Hg is volatile, relatively inert and has low solubility. Oxidised at moderate temperatures by halides. Oxidised to HgCl2 or HgBr 2. Mercuric halides are soluble and so can be captured. Alastair Clements Mercury oxidation 4/18
5 Relative abundance of Cl Chlorine Bromine 3500 Coal content (ppmw ) Bulgaria Ukraine Australia USA Canada Japan China South Africa UK [Vassilev et al. 2000] [Spears and Zheng 1999] Alastair Clements Mercury oxidation 5/18
6 Correlation of Hg 2+ and HCl Hg E (µg/dscm) / Hg T (ppmw ) Chlorine (ppm w ) [EPA 2011] Alastair Clements Mercury oxidation 6/18
7 Oxidation pathways Gas-phase Focus of early work. Unable to model in all situations. Paricle-bound Activated carbon and fly ash. Influenced by O/S/halogen species. Surface-catalysed Uncoated surface effects observed. Speculative mechanisms. Alastair Clements Mercury oxidation 7/18
8 Gas phase oxidation Widmer et al. mechanism: Hg + Cl + M HgCl + M (R 1) Hg + Cl 2 HgCl + Cl (R 2) Hg + HCl HgCl + H (R 3) Hg + HOCl HgCl + OH (R 4) HgCl + Cl + M HgCl 2 + M (R 5) HgCl + Cl 2 HgCl 2 + Cl (R 6) HgCl + HCl HgCl 2 + H (R 7) HgCl + HOCl HgCl 2 + OH (R 8) Reaction R 1-R 4 produce the unstable HgCl intermediate. Only R 1 can proceed at an appreciable rate. Reactions R 5-R 8 complete mercury oxidation and occur much faster. [Widmer et al. 2000] Alastair Clements Mercury oxidation 8/18
9 Oxidation levels 100 Percentage Hg oxidation HCl (400ppm) HCl (100ppm) HBr (25ppm) HBr (50ppm) + HCl (100ppm) HBr (50ppm) HBr (25ppm) + HCl (400ppm) HBr (50ppm) + HCl (400ppm) HCl (100ppm) HCl (400ppm) HBr (50ppm) HBr (25ppm) HBr (25ppm) + HCl (100ppm) Air firing Oxy-firing [Buitrago 2011] Alastair Clements Mercury oxidation 9/18
10 Chlorine modelling Leeds mercury-chlorine model: Reaction Ref. Method Hg + Cl + M HgCl + M Donohoue et al. PLP/PLIF Hg + Cl 2 HgCl + Cl Widmer et al. TST/ab initio Hg + HCl HgCl + H Wilcox TST/ab initio Hg + HOCl HgCl + OH Wilcox TST/ab initio HgCl + Cl + M HgCl 2 + M Niksa et al. Collision limited HgCl + Cl 2 HgCl 2 + Cl Wilcox TST/ab initio HgCl + HCl HgCl 2 + H Wilcox TST/ab initio HgCl + HOCl HgCl 2 + OH Wilcox TST/ab initio [Gharabaghi et al. 2011] Alastair Clements Mercury oxidation 10/18
11 Chlorine modelling results 10 Percentage Hg oxidation Experimental 440K/s Experimental 220 K/s Model 440 K/s Model 220 K/s HCl concentration (ppm v ) Experimental data from [Cauch 2008] Alastair Clements Mercury oxidation 11/18
12 Bromine modelling Leeds mercury-bromine model: Reaction Ref. Method Hg + Br + M HgBr + M Donohoue et al. PLP/PLIF Hg + Br 2 HgBr + Br Okano TST/ab initio Hg + HBr HgBr + H Okano TST/ab initio Hg + HOBr HgBr + OH Niksa et al. Collision limited HgBr + Br + M HgBr 2 + M Goodsite et al. TST/ab initio HgBr + Br 2 HgBr 2 + Br Niksa et al. Collision limited HgBr + HBr HgBr 2 + H Okano TST/ab initio HgBr + HOBr HgBr 2 + OH Niksa et al. Collision limited [Hughes et al. 2011] Alastair Clements Mercury oxidation 12/18
13 Bromine modelling results Percentage Hg oxidation Experimental 440K/s Experimental 220 K/s Model 440 K/s Model 220 K/s HBr concentration (ppm v ) Experimental data from [van Otten et al. 2011] Alastair Clements Mercury oxidation 13/18
14 Summary Mercury oxidation chemistry has proven challenging for modellers. Existing gas-phase oxidation models have failed to be validated across datasets. Experimental data only covers the atomic recombination reactions. Not all potential gas-phase pathways have been fully investigated. Work has also started on identifying surface-catalysed and particle-bound mechanisms. Alastair Clements Mercury oxidation 14/18
15 Further work Continue to improve and validate current model. Measure reaction rates under flue gas temperatures. Using flash photolysis and adsorption spectroscopy. Analyse and integrate models for heterogeneous reactions. Alastair Clements Mercury oxidation 15/18
16 References Buitrago, P. A. Gas-phase mercury oxidation: effects of bromine, chlorine and SO2 under air firing and oxy-fuel conditions, experimental and modeling study The University of Utah, 2011 Cauch, B. Experimental Investigation And Kinetic Modeling Of Homogeneous Mercury Oxidation By Halogens The University of Utah, 2008 Donohoue, D. L.; Bauer, D. & Hynes, A. J. Temperature and Pressure Dependent Rate Coefficients for the Reaction of Hg with Cl and the Reaction of Cl with Cl: A Pulsed Laser Photolysis-Pulsed Laser Induced Fluorescence Study The Journal of Physical Chemistry A, 2005, 109, Donohoue, D. L.; Bauer, D.; Cossairt, B. & Hynes, A. J. Temperature and Pressure Dependent Rate Coefficients for the Reaction of Hg with Br and the Reaction of Br with Br: A Pulsed Laser Photolysis-Pulsed Laser Induced Fluorescence Study The Journal of Physical Chemistry A, 2006, 110, Donohoue, D. L. Kinetic Studies of the Oxidation Pathways of Gaseous Elemental Mercury University of Miami, 2008 Environmental Protection Agency, accessed 11/06/2012 Alastair Clements Mercury oxidation 16/18
17 References Gharebaghi, M.; Hughes, K.; Porter, R.; Pourkashanian, M. & Williams, A. Mercury speciation in air-coal and oxy-coal combustion: A modelling approach Proceedings of the Combustion Institute, 2011, 33, Goodsite, M. E.; Plane, J. M. C. & Skov, H. A Theoretical Study of the Oxidation of Hg0 to HgBr2 in the Troposphere Environmental Science & Technology, 2004, 38, Hughes, K. J.; Ma, L.; Porter, R. T. & Pourkashanian, M. E.N. Pistikopoulos, M. G. & Kokossis, A. (Eds.) Mercury Transformation Modelling with Bromine Addition in Coal Derived Flue Gases 21st European Symposium on Computer Aided Process Engineering, Elsevier, 2011, 29, Niksa, S.; Helble, J. & Fujiwara, N. Kinetic modeling of homogeneous mercury/oxidation: The importance of NO and H2O in predicting oxidation in coal-derived systems Environmental Science and Technology, 2001, 35, Niksa, S.; Padak, B.; Krishnakumar, B. & Naik, C. V. Process Chemistry of Br Addition to Utility Flue Gas for Hg Emissions Control Energy & Fuels, 2010, 24, Okano, T. High Temperature Mercury Oxidation Kinetics via Bromine Mechanisms Worcester Polytechnic Institute, 2009 van Otten, B.; Buitrago, P. A.; Senior, C. L. & Silcox, G. D. Gas-Phase Oxidation of Mercury by Bromine and Chlorine in Flue Gas Energy & Fuels, 2011, 25, Alastair Clements Mercury oxidation 17/18
18 References Spears, D. & Zheng, Y. Geochemistry and origin of elements in some UK coals International Journal of Coal Geology, 1999, 38, Vassilev, S.; Eskenazy, G. & Vassileva, C. Contents, modes of occurrence and origin of chlorine and bromine in coal Fuel, 2000, 79, Widmer, N. C.; West, J. & Cole, J. A. Proceedings of the Air & Waste Management Association Annual Conference, 2000 Wilcox, J. A kinetic investigation of high-temperature mercury oxidation by chlorine Journal of Physical Chemistry A, 2009, 113, Alastair Clements Mercury oxidation 18/18
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