Analysis of dispersion and propagation of fine and ultra fine particle aerosols from a busy road

Queensland University of Technology School of Physical and Chemical Sciences Analysis of Dispersion and Propagation of Fine and Ultra Fine Particle Aerosols from a Busy Road Submitted by Galina GRAMOTNEV, School of Physical and Chemical Sciences, Queensland University of Technology in partial fulfilment of the requirements of the degree of Doctor of Philosophy January 2007 Keywords Combustion aerosols, urban aerosols, outdoor aerosols, background aerosols, nanoparticles, ultra-fine particles, particle formation, aerosol evolution, busy road, aerosol dispersion, air quality, transport emissions, emission factors, canonical correlations analysis, multi-variate analysis, degradation processes, turbulent diffusion, atmospheric monitoring, hydrodynamics, statistical mechanics, probability, particle deposition ii Statement of original authorship The work contained in this Thesis has not been previously submitted for a degree or diploma at any other higher education institution To the best of my knowledge and belief, the Thesis contains no material previously published or written by another persons except where due reference is made Galina Gramotnev iii Acknowledgements I note my appreciation of financial support for this research from the Queensland University of Technology (QUT), Faculty of Science, School of Physical and Chemical Sciences, and QUT Office of Research I would like to express my sincere gratitude and appreciation to Dr Richard J Brown for very helpful discussions, support, useful directions, and introduction to the theory of turbulent atmospheric processes I also thank Mr Pierre Madl and Ms Maricella Yip for their substantial help and consultations with respect to monitoring equipment, and all my friends from the International Laboratory for Air Quality and Health for their support during my PhD studies Special thanks go to my husband, Dr Dmitri K Gramotnev, for the comprehensive support during my studies and suggested ideas iv Abstract Nano-particle aerosols are one of the major types of air pollutants in the urban indoor and outdoor environments Therefore, determination of mechanisms of formation, dispersion, evolution, and transformation of combustion aerosols near the major source of this type of air pollution – busy roads and road networks – is one of the most essential and urgent goals This Thesis addresses this particular direction of research by filling in gaps in the existing physical understanding of aerosol behaviour and evolution The applicability of the Gaussian plume model to combustion aerosols near busy roads is discussed and used for the numerical analysis of aerosol dispersion New methods of determination of emission factors from the average fleet on a road and from different types of vehicles are developed Strong and fast evolution processes in combustion aerosols near busy roads are discovered experimentally, interpreted, modelled, and statistically analysed A new major mechanism of aerosol evolution based on the intensive thermal fragmentation of nano-particles is proposed, discussed and modelled A comprehensive interpretation of mutual transformations of particle modes, a strong maximum of the total number concentration at an optimal distance from the road, increase of the proportion of small nano-particles far from the road is suggested Modelling of the new mechanism is developed on the basis of the theory of turbulent diffusion, kinetic equations, and theory of stochastic evaporation/degradation v processes Several new powerful statistical methods of analysis are developed for comprehensive data analysis in the presence of strong turbulent mixing and stochastic fluctuations of environmental factors and parameters These methods are based upon the moving average approach, multi-variate and canonical correlation analyses As a result, an important new physical insight into the relationships/interactions between particle modes, atmospheric parameters and traffic conditions is presented In particular, a new definition of particle modes as groups of particles with similar diameters, characterised by strong mutual correlations, is introduced Likely sources of different particle modes near a busy road are identified and investigated Strong anti-correlations between some of the particle modes are discovered and interpreted using the derived fragmentation theorem The results obtained in this thesis will be important for accurate prediction of aerosol pollution levels in the outdoor and indoor environments, for the reliable determination of human exposure and impact of transport emissions on the environment on local and possibly global scales This work will also be important for the development of reliable and scientifically-based national and international standards for nano-particle emissions vi LIST OF AUTHOR PUBLICATIONS Refereed journal papers [A1] Gramotnev, G., Brown, R., Ristovski, Z, Hitchins, J., Morawska, L 2003 Determination of emission factors for vehicles on a busy road Atmospheric Environment, 37, pp 465-474 (Number 13 out of 25 most downloaded papers in 2004) [A2] Gramotnev, G., Ristovski Z., Brown, R., Madl, P 2004 New methods of determination of emission factors for two groups of vehicles on a busy road, Atmospheric Environment, vol.38, pp.2607-2610 [A3] Gramotnev, G., Ristovski, Z 2004 Experimental investigation of ultra fine particle size distribution near a busy road, Atmospheric Environment, vol.38, pp.1767-1776 [A4] Gramotnev, D.K., Gramotnev, G 2005 A new mechanism of aerosol evolution near a busy road: fragmentation of nano-particles, Journal of Aerosol Science, vol.36, pp.323-340 (Number out of 25 most downloaded papers in 2005) [A5] Gramotnev, D.K., Gramotnev, G 2005 Modelling of aerosol dispersion from a busy road in the presence of nanoparticle fragmentation, Journal of Applied Meteorology, vol.44, pp.888–899 [A6] Gramotnev, G., Gramotnev, D.K Multi-channel statistical analysis of combustion aerosols Part I: Canonical correlations and sources of particle modes Atmospheric Environment (accepted January 2007) [A7] Gramotnev, D.K., Gramotnev, G Multi-channel statistical analysis of combustion aerosols Part II: Anti-correlations of particle modes and fragmentation theorem Atmospheric Environment (accepted January 2007) [A8] Gramotnev, D.K., Gramotnev, G Kinetics of stochastic degradation / vii evaporation processes in polymer-like systems with multiple bonds, J Appl Phys (submitted) [A9] Gramotnev, D K., Mason, D R., Gramotnev, G., Rasmussen A J Thermal tweezers for surface manipulation with nano-scale resolution Appl Phys Lett (accepted January 2007) [A10] Gramotnev, G., Madl, P., Gramotnev, D K., Urban background aerosols: Anti-correlations of particle modes and fragmentation mechanism Geophysical Research Letters (submitted) Full-length refereed conference papers [A11] Gramotnev, G., Brown, R., Ristovski, Z., Hitchins, J., Morawska, L 2002 Estimation of fine particles emission factors for vehicles on a road using Caline4 program Proceedings of 4th Queensland Environmental Conference, Brisbane, Australia, 30 & 31 May 2002, pp 43-48 [A12] Gramotnev, G., Ristovski, Z., Brown, R., Morawska, L, Jamriska, M., Agranovski, V 2003 A new method for obtaining fine particles emission factors with validation from measurements near a busy road in Brisbane Proceedings of National Environmental Conference, Brisbane, Australia, 18 & 20 June 2003, pp 206-211 Conference papers in refereed journals [A13] Gramotnev, G., Ristovski, Z., Brown, R., Morawska, L., Madl, P 2003 New method of determination of emission factors for different types of vehicles on a busy road Journal of Aerosol Science, EAC 2003, vol.34s, S259-S260 [A14] Gramotnev, G., Ristovski, Z 2003 Nanoparticles near a busy road: experimental observation of the effect of formation of a new mode of particles Journal of Aerosol Science, EAC 2003, vol.34s, S255-S256 viii [A15] Gramotnev, G., Ristovski, Z and Gramotnev, A 2003 Dependence of concentration of nanoparticles near a busy road on meteorological parameters: canonical correlation analysis Journal of Aerosol Science, EAC 2003, vol.34s, S257-S258 [A16] Gramotnev, G., Ristovski, Z., Morawska, L., Thomas, S 2003 Statistical analysis of correlations between air pollution in the city area and temperature and humidity Journal of Aerosol Science, EAC 2003, vol.34s, S715-S716 [A17] Gramotnev, G 2004 Determination of the average emission factors for three different types of vehicles on a busy road Journal of Aerosol Science, EAC 2004, vol.35, S1089-S1090 [A18] Gramotnev, D.K., Gramotnev, G 2004 A new mechanism of aerosol evolution near a busy road: fragmentation of nanoparticles Journal of Aerosol Science, EAC 2004, vol.35, S221-S222 [A19] Gramotnev, D.K., Gramotnev, G 2004 Modelling of aerosol dispersion from a busy road in the presence of nano-particle fragmentation Journal of Aerosol Science, EAC 2004, vol.35, S925-S926 Other conference publications [A20] Gramotnev, G., Brown, R., Ristovski, Z, Hitchins, J., Morawska, L 2002 Dispersion of fine and ultra fine particles from busy road: the comparison of experimental and theoretical results, in Chiu-Sen Wang (Ed) Proc of Sixth International Aerosol Conference, Taipei, Taiwan (September – 13, 2002), pp 839-840 [A21] Gramotnev, G., Thomas, S., Morawska, L., Ristovski, Z 2002 Canonical correlation analysis of fine particle and gaseous pollution in the city area, in ChiuSen Wang (Ed) Proc of Sixth International Aerosol Conference, Taipei, Taiwan (September – 13, 2002), pp 873-874 [A22] Gramotnev, D.K., Gramotnev, G 2004 Fragmentation of nanoparticles near ix a busy road: Justification and modelling Proceedings of 8th International Conference on Carbonaceous Particles in the Atmosphere, Vienna, Austria, 14-16 September 2004, H3 [A23] Gramotnev, G., Gramotnev, D.K 2004 New statistical method of determination of particle modes in the presence of strong turbulent mixing Proceedings of 8th International Conference on Carbonaceous Particles in the Atmosphere, Vienna, Austria, 14-16 September 2004, H4 [A24] Gramotnev, G., Gramotnev, D K 2005 Theoretical analysis of multiple thermal fragmentation of aerosol nanoparticles from a line source: Evolution of particle modes Biannual AIP Congress, Canberra, Australia, February, 2005, p.210 [A25] Gramotnev, G., Gramotnev, D K 2005 Numerical and experimental investigation of thermal fragmentation of aerosol nano-particles from vehicle exhaust Biannual AIP Congress, Canberra, Australia, February, 2005, p.210 [A26] Gramotnev, D K., Gramotnev, G 2005 Combustion nano-particle aerosols: Mechanisms of evolution and modelling, Aerosol Workshop, 30 March – April 2005, Sydney, Australia (invited talk) [A27] Gramotnev, D K., Gramotnev, G 2005 Time delays during multiple thermal fragmentation of nanoparticles: evolution of particle modes European Aerosol Conference (EAC 2005), Ghent, Belgium, p 690 [A28] Gramotnev, G., Madl, P 2005 Multi-channel statistical analysis of background fine particle aerosols, European Aerosol Conference (EAC 2005), Ghent, Belgium, p 697 [A29] Gramotnev, D K., Bostrom, T E., Devine, N., Gramotnev, G 2005 Experimental investigation of deposition of aerosol particles near a busy road European Aerosol Conference (EAC 2005), Ghent, Belgium, p 696 [A30] Mason, D.R., Gramotnev, D.K., Rasmussen, A., Gramotnev, G 2005 Feasibility of thermal tweezers for effective manipulation of nano-particles on surfaces ACOLS’05, December, Christchurch, New Zealand, ThC6 x CHAPTER 12 CONCLUSIONS This thesis was focused at gaining better understanding of fundamental and applied aspects of evolution and dispersion of combustion aerosols near busy roads in the urban environment, and development of practical methods and techniques for the identification and investigation of the main physical mechanisms of behavior of airborne nano-particles from vehicle exhaust with the ultimate aim of accurate prediction of human exposure and environmental impact of combustion aerosols The research was based on a natural combination of experimental monitoring of combustion aerosols and air quality in the urban environment, theoretical and numerical modelling of aerosol dispersion and mechanisms of evolution of nano-particles, and development and application of new statistical methods of data analysis in the presence of strong turbulent mixing and stochastic variations of atmospheric and environmental parameters in real-world situations One of the major fundamental achievements of this thesis is the suggestion, experimental investigation, and theoretical modelling of a radically new mechanism of aerosol evolution based on intensive thermal fragmentation of nano-particles The significance of this new mechanism may be far beyond evolution and transformation of combustion aerosols near busy roads (which is demonstrated by this thesis) It may also play a major role in shaping patterns of atmospheric aerosols on the global and local scales At the same time, it is important to understand that the presented theory and models will certainly need further extensive experimental and theoretical confirmation/validation under different conditions For example, at this stage little is known about the actual types of volatile compounds that may be responsible for the fragmentation mechanisms of aerosol evolution Direct observations of solid 239 primary nano-particles and laboratory investigations of their possible interaction/fragmentation would also be of a significant benefit in future Therefore, this thesis presents the first major step towards the further important research in this area The thesis has also developed several specific methods and approaches for the accurate prediction of aerosol pollution levels in the urban environment, and techniques for the determination and analysis of vehicle emissions under field conditions Several unique and powerful statistical methods for the investigation of dispersion, evolution processes, and possible sources of nano-particle aerosols have been successfully developed and applied for the analysis of combustion and background aerosols All these findings and methods will be important for the development of workable and scientifically-based national and international standards for nano-particle emissions, accurate prediction of human exposure to combustion aerosols, determination and reduction of the environmental impact of aerosols and other types of air pollutants in the indoor and outdoor environments List of main results Adjustment of the software package CALINE4 (from the California Transport) for prediction and modelling of aerosol pollution from busy roads in the Gaussian plume approximation Development of a new method for the determination of the average emission factors per vehicle on a road, based on the experimental measurements of particle concentration at one point near the road Determination of the average emission factors for Gateway Motorway, Brisbane, Australia Development of two new methods of determination of average emission factors from different types of vehicles (cars, light trucks, heavy-duty diesels) on a road 240 Detailed experimental investigation of evolution of particle modes near a busy road Discovery of strong variations in the size distribution, including a maximum of the total number concentration at an “optimal” distance from the road Development of a new mechanism of evolution of combustion aerosols, based on intensive thermal fragmentation of nano-particles Its theoretical justification and experimental confirmed by means of several independent sets of data Development of a new model of dispersion of combustion aerosols near busy roads, based on intensive particle fragmentation Determination of the typical fragmentation rate coefficient and existence conditions for a maximum of the total number concentration at an optimal distance from the road Development of three major new methods of statistical analysis of mode evolution and experimental data in the presence of strong stochastic fluctuations of external and meteorological parameters, based on the moving average approach, simple and canonical correlation analyses Re-definition of particle modes as groups of particles of similar dimensions and strong mutual correlations Statistical identification of particle modes emitted by cars and heavy diesels In particular, determination of a volatile ~ nm mode that exists at earlier stages of aerosol evolution and is strongly related to heavy-duty diesel trucks Detailed canonical correlation analysis of the relationships between particle modes and external atmospheric conditions 10 Derivation and proof of the fragmentation theorem that provides further strong confirmation of the fragmentation mechanism of evolution of combustion aerosols 241 11 Development of a theory of probabilistic time delays during stochastic degradation/evaporation processes and their relationship to 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III: biological responses Journal of Aerosol Science, 29 (Suppl 2), S995-S996 253 ... Combustion aerosols, urban aerosols, outdoor aerosols, background aerosols, nanoparticles, ultra -fine particles, particle formation, aerosol evolution, busy road, aerosol dispersion, air quality, transport... Multi-channel statistical analysis of aerosol particle modes near a busy road 155 8.1 Introduction 155 8.2 Experimental data and particle modes 156 8.3 Moving average approach and the canonical correlation... mixing and stochastic fluctuations of environmental factors and parameters These methods are based upon the moving average approach, multi-variate and canonical correlation analyses As a result, an