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Monitoring urban-industrial emissions is often challenging because observations are scarce and regional atmospheric transport models are too coarse to represent the high spatiotemporal variability in the resulting concentrations. In this paper we apply a new combination of an Eulerian model (Weather Research and Forecast, WRF, with chemistry) and a Gaussian plume model (Operational Priority Substances - OPS). The modelled mixing ratios are compared to observed CO2 and CO mole fractions at four sites along a transect from an urban-industrial complex (Rotterdam, the Netherlands) towards rural conditions for October-December 2014. Urban plumes are well-mixed at our semi-urban location, making this location suited for an integrated emission estimate over the whole study area. The signals at our urban measurement site (with average enhancements of 11 ppm CO2 and 40 ppb CO over the baseline) are highly variable due to the presence of distinct source areas dominated by road traffic/residential heating emissions or industrial activities. This causes different emission signatures that are translated into a large variability in observed Delta CO : Delta CO2 ratios, which can be used to identify dominant source types. We find that WRF-Chem is able to represent synoptic variability in CO2 and CO (e.g. the median CO2 mixing ratio is 9.7 ppm, observed, against 8.8 ppm, modelled), but it fails to reproduce the hourly variability of daytime urban plumes at the urban site (R-2 up to 0.05). For the urban site, adding a plume model to the model framework is beneficial to adequately represent plume transport especially from stack emissions. The explained variance in hourly, daytime CO2 enhancements from point source emissions increases from 30% with WRF-Chem to 52% with WRF-Chem in combination with the most detailed OPS simulation. The simulated variability in Delta CO : Delta CO2 ratios decreases drastically from 1.5 to 0.6 ppb ppm(-1), which agrees better with the observed standard deviation of 0.4 ppb ppm(-1). This is partly due to improved wind fields (increase in R-2 of 0.10) but also due to improved point source representation (increase in R-2 of 0.05) and dilution (increase in R-2 of 0.07). Based on our analysis we conclude that a plume model with detailed and accurate dispersion parameters adds substantially to top-down monitoring of greenhouse gas emissions in urban environments with large point source contributions within a similar to 10 km radius from the observation sites.

Monitoring urban-industrial emissions is often challenging because observations are scarce and regional atmospheric transport models are too coarse to represent the high spatiotemporal variability in the resulting concentrations. In this paper we apply a new combination of an Eulerian model (Weather Research and Forecast, WRF, with chemistry) and a Gaussian plume model (Operational Priority Substances - OPS). The modelled mixing ratios are compared to observed CO2 and CO mole fractions at four sites along a transect from an urban-industrial complex (Rotterdam, the Netherlands) towards rural conditions for October-December 2014. Urban plumes are well-mixed at our semi-urban location, making this location suited for an integrated emission estimate over the whole study area. The signals at our urban measurement site (with average enhancements of 11 ppm CO2 and 40 ppb CO over the baseline) are highly variable due to the presence of distinct source areas dominated by road traffic/residential heating emissions or industrial activities. This causes different emission signatures that are translated into a large variability in observed Delta CO : Delta CO2 ratios, which can be used to identify dominant source types. We find that WRF-Chem is able to represent synoptic variability in CO2 and CO (e.g. the median CO2 mixing ratio is 9.7 ppm, observed, against 8.8 ppm, modelled), but it fails to reproduce the hourly variability of daytime urban plumes at the urban site (R-2 up to 0.05). For the urban site, adding a plume model to the model framework is beneficial to adequately represent plume transport especially from stack emissions. The explained variance in hourly, daytime CO2 enhancements from point source emissions increases from 30% with WRF-Chem to 52% with WRF-Chem in combination with the most detailed OPS simulation. The simulated variability in Delta CO : Delta CO2 ratios decreases drastically from 1.5 to 0.6 ppb ppm(-1), which agrees better with the observed standard deviation of 0.4 ppb ppm(-1). This is partly due to improved wind fields (increase in R-2 of 0.10) but also due to improved point source representation (increase in R-2 of 0.05) and dilution (increase in R-2 of 0.07). Based on our analysis we conclude that a plume model with detailed and accurate dispersion parameters adds substantially to top-down monitoring of greenhouse gas emissions in urban environments with large point source contributions within a similar to 10 km radius from the observation sites.