UPDATE OF THE ROMBERG-APPROACH AND SIMPLIFIED NO / NO 2 CONVERSION MODEL UNDER CONSIDERATION OF DIRECT NO 2 - EMISSIONS

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1 UPDATE OF THE ROMBERG-APPROACH AND SIMPLIFIED NO / NO 2 CONVERSION MODEL UNDER CONSIDERATION OF DIRECT NO 2 - EMISSIONS I. Düring 1, W. Bächlin 2, M. Ketzel 3, A. Baum 4, S. Wurzler 5 1, Mohrenstraße 14, D Radebeul 2, An der Roßweid 3, D Karlsruhe 3 Department of Atmospheric Environment, Research Institute, Aarhus, Frederiksborgvej 399, DK-4 Roskilde, Denmark 4 Bundesanstalt für Straßenwesen, Brüderstraße 53, D Bergisch Gladbach 5 Landesamt für Natur, Umwelt und Verbraucherschutz NRW, Wallneyer Straße 6, D Essen June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 1 Outline 1. Motivation 2. The Romberg approach 3. Updating the Romberg approach 4. OSPM Chemistry Model 5. Simplified chemistry model based on annual average values 6. Conclusions June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 2 1

2 Motivation NO 2 -limit value: 4µg/m³ (annual mean) Jagtvej NOX (µg/m 3 ) urban background (measured) measured Jagtvej modelled with COPERT4 emissions Air quality measurements at street stations show often reduction in NO x levels, but no significant reduction in NO 2 NO x = NO + NO 2 [ppb] NO + O 3 => NO 2 +O 2 more chemistry Jagtvej NO2 (µg/m 3 ) urban background NO2 (measured) urban background O3 (measured) measured Jagtvej modelled with COPERT4 emissions limit value June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 3 Motivation According to the EU directive the EPA in co-operation with local authorities has to prepare action plans to assure compliance by 21 Concentration-annual mean [µg/m³] Concentration and Emission Frankfurt-Leipziger Straße year NO2-concentration (annual mean) NO2-emission NO-concentration (annual mean) NOx-emission Emission [mg/(mh)] June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 4 2

3 NO x - chemistry Formation of NO 2 from NO is a complex photochemical process. Mainly depending on the total amount of available NO x and ozone. NO 2 concentration is also depending on the primarily emitted NO 2. Besides NO-emission, ozone concentrations as well as primary NO 2 emission are changing from year to year. (Platt U., 28 ) June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 5 Updating the Romberg approach A [ NOx ] [ NO2 ] = + C [ NOx] [ NO ] + B x The new constants for the given period of 24 to 26 (German measurement sites) along with the earlier parameters from 1996: Statistical concentration parameters parameter of function Romberg et al. (1996) A B C annual average percentile Bächlin et al. (28) A B C annual average percentile highest hourly value June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 6 3

4 Comparison old / new measurements Romberg et al. (1996) Bächlin et al. (28) NO 2 = f (NO x p, O 3 ) 28 NO 2 [µg/m 3 ] limit value 2 81 µg/m³ 88 µg/m³ NO x [µg/m 3 ] The approach by Romberg et al. (1996) results in too low NO 2 -values for high NO x -values. The annual average value of 4 µg NO 2 /m 3 would be reached by an annual mean NO x -concentration of approx. 88 µg/m 3 with the new approach June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 7 OSPM Chemistry Model More realistic conversions can be obtained using a chemistry model. A simplified relation scheme is often used to describe the chemical conversion in the equilibrium state of NO 2, NO, and ozone. The considered reactions are: NO + O 3 => NO 2 + O 2 (k) NO 2 + hv => NO + O 3 (J) k (ppb -1 s -1 ) is the reaction coefficient J (s -1 ) is the photolytic frequency of NO 2, June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 8 4

5 OSPM Chemistry Model Assuming that the equilibrium is quickly reached, the differential equations have an analytical solution for the concentration: ( ( x 2 2 / τ) ) 2 [ NO ].5 B- B - 4 [ NO ] [ NO ] + [ NO ] With the variables : [ NO2 ] O = [ NO2 ] n + [ O3 ] B 2 = k B = June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 9 O [ NO ] + [ NO ] + J + x 2 O [ NO 2 ] n = [ NO 2 ] V + [ NO 2 ] B The two terms [NO] V and [NO 2 ] V are the amount being produced by traffic emissions as an increase of concentration above the background concentration. [NOx] V is calculated from the difference in NOx between the traffic station and the background station as [ NO ] = p( [ NO ]- [ ] ) 2 V x NOx B [ NO ] = ([ NO] - [ ] ) V NO B with p = NO 2 /NOx being the fraction of NO 2 in the direct traffic emissions and [NO x ] the concentration, which is estimated at the traffic station by measurements or dispersion model. n 1 k 1 τ NO 2 = f (NO x, p, O 3 B, NO x B, NO 2 B k, J, τ) OSPM Chemistry Model Used in OSPM for hourly time series. The parameter τ is calculated from meteorological values (e.g. wind speed and turbulence) as well as the road geometry (height of the street canyon) and represents the typical residence time the pollution is trapped inside the street canyon and is available for chemical reactions (see Berkowicz et al., 1997). Typical values for are in the range of 8s to 15s. NO 2 modelled (based on measured NO x!) NO2-1h-mean modelled [µg/m³] τ y = 1.1x -.3 R 2 = NO2-1h-mean measured [µg/m³] Comparison of hourly mean NO 2 -concentrations, calculated with the OSPM chemistry model from observed NOx data, and values from the measurement site Corneliusstraße in Duesseldorf for the year June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 1 5

6 Simplified chemistry model based on annual average values Strictly speaking, the above equations of the chemistry model can only be used in time series calculations, because the parameters J and k are dependent on meteorological parameters. However, based on several research projects, these equations can also be applied for annual mean concentrations using the following parameters: J =.45 s -1 k =.39 m³ (ppb s) -1 τ = 1 s (street canyons) or 4 s (free dispersion) The input data is the same as for the Romberg approach: NOx- annual mean at traffic station (observed value or estimated by dispersion model) NOx- annual mean at background station NO 2 = f (NO x, p, O 3 B, NO 2 - annual mean at background station NO x B, NO 2 B k, J, τ) as well as two additional values: Ozone- annual mean at background station p = share of primary NO 2 emissions for all NOx emissions June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 11 Cottbus-Bahnhofstraße C_Bhf_1997 C_Bhf_1998 C_Bhf_1999 C_Bhf_2 C_Bhf_21 C_Bhf_22 C_Bhf_23 C_Bhf_24 NO2-GB C_Bhf_25 C_Bhf_26 C_Bhf_27 NO2-GB (measured) NO2-GB (Romberg '96) NO2-VB simplified chemistry model NO2-GB (Bächlin '8) June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 12 6

7 Düsseldorf- Corneliusstraße 8 7 D-Corneliusstraße 6 NO2-GB DDC-1997 DDC-1998 DDC-1999 DDC-2 DDC-21 DDC-22 DDC-23 DDC-24 DDC-25 DDC-26 NO2-GB (measured) NO2-GB (Romberg '96) NO2-VB simplified chemistry model NO2-GB (Bächlin '8) June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 13 Comparision (Data ; 3 German measurement sites) Romberg (1996) Bächlin (28) Simplified chemistry model June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 14 7

8 Conclusions The approach by Romberg et al. (1996) is often conservative for existing data up to the year 23; however, it cannot reproduce the long term trends. The approach by Bächlin and Bösinger (28) reproduces the existing measured data better than the approach by Romberg, but it cannot reproduce the long term tendencies very well, either. The simplified chemistry model can best reproduce the tendencies and the absolute values. The main reason for the good fit for trends in the NO 2 /NOx ratios is the explicit incorporation of the share of primary NO 2 emissions. Better NO 2 -prognosis possible, especially if primary NO 2 - emission changes (e.g. change of the vehicle fleet mix due to environmental zone, future fleet trend etc.) June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 15 Acknowledgements Bundesanstalt für Straßenwesen, Bergisch Gladbach Landesamt für Natur, Umwelt und Verbraucherschutz NRW, Essen Ministerium für Ländliche Entwicklung, Umwelt und Verbraucherschutz des Landes Brandenburg, Potsdam June 21 HARMO13 in Paris- NO / NO 2 CONVERSION MODEL 16 8

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