Prediction of total oxides of nitrogen and nitrogen dioxide concentrations in a large urban area using a new generation urban scale dispersion model with integral chemistry model

Abstract. The quality of the Nimbus 7 Limb Infrared Monitor of the Stratosphere (LIMS) nitric acid (HNO3) and nitrogen dioxide (NO2) profiles and distributions of 1978/1979 are described after their processing with an updated, Version 6 (V6) algorithm and subsequent archival in 2002. Estimates of the precision and accuracy of both of those species are developed and provided herein. The character of the V6 HNO3 profiles is relatively unchanged from that of the earlier LIMS Version 5 (V5) profiles, except in the upper stratosphere where the interfering effects of CO2 are accounted for better with V6. The accuracy of the retrieved V6 NO2 is also significantly better in the middle and upper stratosphere, due to improvements in its spectral line parameters and in the reduced biases for the accompanying V6 temperature and water vapor profiles. As a result of these important updates, there is better agreement with theoretical calculations for profiles of the HNO3/NO2 ratio, day-to-night NO2 ratio, and with estimates of the production of NO2 in the mesosphere and its descent to the upper stratosphere during polar night. In particular, the findings for middle and upper stratospheric NO2 should also be more compatible with those obtained from more recent satellite sensors because the effects of the spin-splitting of the NO2 lines are accounted for now with the LIMS V6 algorithm. The improved precisions and more frequent retrievals of the LIMS profiles along their orbit tracks provide for better continuity and detail in map analyses of these two species on pressure surfaces. It is judged that the chemical effects of the oxides of nitrogen on ozone can be studied quantitatively throughout the stratosphere with the LIMS V6 data.

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Development of the city-scale chemistry transport model CityChem-EPISODE and its application to the city of Hamburg

10.5194/gmd-2018-8 ◽

2018 ◽

Cited By ~ 2

Author(s):

Matthias Karl

Keyword(s):

Air Quality ◽

Urban Area ◽

Transport Model ◽

Dispersion Model ◽

Temporal Correlation ◽

Urban Atmosphere ◽

Aerosol Formation ◽

Urban Background ◽

New Model ◽

The City

Abstract. This paper describes the City-scale Chemistry (CityChem) extension of the urban dispersion model EPISODE with the aim to enable chemistry/transport simulations of multiple reactive pollutants on urban scales. The new model is called CityChem-EPISODE. The primary focus is on the simulation of urban ozone concentrations. Ozone is produced in photochemical reaction cycles involving nitrogen oxides (NOx) and volatile organic compounds (VOC) emitted by various anthropogenic activities in the urban area. The performance of the new model was evaluated with a series of synthetic tests and with a first application to the air quality situation in the city of Hamburg, Germany. The model performs fairly well for ozone in terms of temporal correlation and bias at the air quality monitoring stations in Hamburg. In summer afternoons, when photochemical activity is highest, modelled median ozone at an inner-city urban background station was about 30 % lower than the observed median ozone. Inaccuracy of the computed photolysis frequency of nitrogen dioxide (NO2) is the most probable explanation for this. CityChem-EPISODE reproduces the spatial variation of annual mean NO2 concentrations between urban background, traffic and industrial stations. However, the temporal correlation between modelled and observed hourly NO2 concentrations is weak for some of the stations. For daily mean PM10, the performance of CityChem-EPISODE is moderate due to low temporal correlation. The low correlation is linked to uncertainties in the seasonal cycle of the anthropogenic particulate matter (PM) emissions within the urban area. Missing emissions from domestic heating might be an explanation for the too low modelled PM10 in winter months. Four areas of need for improvement have been identified: (1) dry and wet deposition fluxes; (2) treatment of photochemistry in the urban atmosphere; (3) formation of secondary inorganic aerosol (SIA); and (4) formation of biogenic and anthropogenic secondary organic aerosol (SOA). The inclusion of secondary aerosol formation will allow for a better sectorial attribution of observed PM levels. Envisaged applications of the CityChem-EPISODE model are urban air quality studies, environmental impact assessment, sensitivity analysis of sector-specific emission and the assessment of local and regional emission abatement policy options.

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