Enhancements to the UK Photochemical Trajectory Model for simulation of secondary inorganic aerosol

Beddows, David C.S.; Hayman, Garry D.; Harrison, Roy M.. 2012 Enhancements to the UK Photochemical Trajectory Model for simulation of secondary inorganic aerosol. Atmospheric Environment, 57. 278-288.

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Particulate matter remains a challenging pollutant for air pollution control in the UK and across much of Europe. Particulate matter is a complex mixture of which secondary inorganic compounds (sulphates, nitrates) are a major component. This paper is concerned with taking a basic version of the UK Photochemical Trajectory Model and enhancing a number of features in the model in order to better represent boundary layer processes and to improve the description of secondary inorganic aerosol formation. The enhancements include an improved treatment of the boundary layer, deposition processes (both wet and dry), attenuation of photolysis rates by cloud cover, and inclusion of the aerosol thermodynamic model ISORROPIA II to account both for chemistry within the aerosol and between the particles and gas phase. Emissions inventories have been updated and are adjusted according to season, day of the week and hour of the day. Stack emissions from high level sources are now adjusted according to the height of the boundary layer and a scheme for generating marine aerosol has been included. The skill of the improved model has been evaluated through predictions of the concentrations of particulate chloride, nitrate and sulphate and the results show increased accuracy and lower mean bias. There is a much higher proportion of the values lying within a factor of 2 of the observed values compared to the basic model and Normalised Mean Bias has reduced by at least 89% for nitrate and sulphate. Similarly, the Index of Agreement between calculated and measured values has improved by ∼10%. Considering the contribution of each enhancement to the improvement in the performance metrics, the most significant enhancement was the replacement of the parameterisation of the boundary layer height, relative humidity and temperature by HYSPLIT values calculated for each trajectory. The second most significant enhancement was the parameterisation of the photolysis rates by values calculated by an off line database accounting for the dependence of photolysis rates on zenith angle, cloud cover, land surface type and column ozone. The inclusion of initial conditions which were dependent on the starting point of the trajectory and the modulation of stack emissions made the most significant improvement to sulphate. Furthermore, in order to assess the model's response to abatement scenarios, 30% abatements of either NH3, NOx or SO2 showed a reduction in the sum of chloride, nitrate and sulphate of between 3.1% and 8.5% (with a corresponding estimated reduction of 1.6–3.7% reduction in PM10). The largest reduction in this contribution is due to the abatement of NOx.

Item Type: Publication - Article
Digital Object Identifier (DOI):
Programmes: CEH Topics & Objectives 2009 - 2012 > Biogeochemistry
UKCEH and CEH Sections/Science Areas: Reynard
ISSN: 1352-2310
Additional Information. Not used in RCUK Gateway to Research.: NOTICE: this is the author’s version of a work that was accepted for publication in Atmospheric Environment. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Atmospheric Environment, 57. 278-288. 10.1016/j.atmosenv.2012.04.020.
Additional Keywords: Lagrangian model, sulphate, nitrate, chloride, Master Chemical Mechanism
NORA Subject Terms: Atmospheric Sciences
Date made live: 20 Sep 2012 13:50 +0 (UTC)

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