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null (Ed.)Abstract. Flux measurements of nitrogen oxides (NOx) were made over London usingairborne eddy covariance from a low-flying aircraft. Seven low-altitude flights were conducted over Greater London, performing multiple overpasses across the city during eight days in July 2014. NOx fluxes across theGreater London region (GLR) exhibited high heterogeneity and strong diurnalvariability, with central areas responsible for the highest emission rates(20–30 mg m−2 h−1). Other high-emission areas included the M25 orbital motorway. The complexity of London's emission characteristics makes it challenging to pinpoint single emissions sources definitively usingairborne measurements. Multiple sources, including road transport andresidential, commercial and industrial combustion sources, are all likely to contribute to measured fluxes. Measured flux estimates were compared toscaled National Atmospheric Emissions Inventory (NAEI) estimates, accountingfor monthly, daily and hourly variability. Significant differences were found between the flux-driven emissions and the NAEI estimates acrossGreater London, with measured values up to 2 times higher in Central London than those predicted by the inventory. To overcome the limitations ofusing the national inventory to contextualise measured fluxes, we usedphysics-guided flux data fusion to train environmental response functions(ERFs) between measured flux and environmental drivers (meteorological and surface). The aim was to generate time-of-day emission surfaces usingcalculated ERF relationships for the entire GLR; 98 % spatial coverage was achieved across the GLR at 400 m2 spatial resolution. All flight legprojections showed substantial heterogeneity across the domain, with highemissions emanating from Central London and major road infrastructure. Thediurnal emission structure of the GLR was also investigated, through ERF,with the morning rush hour distinguished from lower emissions during the early afternoon. Overall, the integration of airborne fluxes with anERF-driven strategy enabled the first independent generation of surfaceNOx emissions, at high resolution using an eddy-covariance approach,for an entire city region.more » « less
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null (Ed.)Abstract. Mixing ratios of volatile organic compounds (VOCs) were recordedin two field campaigns in central Beijing as part of the Air Pollution andHuman Health in a Chinese Megacity (APHH) project. These data were used tocalculate, for the first time in Beijing, the surface–atmosphere fluxes ofVOCs using eddy covariance, giving a top-down estimation of VOC emissionsfrom a central area of the city. The results were then used to evaluate theaccuracy of the Multi-resolution Emission Inventory for China (MEIC). TheAPHH winter and summer campaigns took place in November and December 2016and May and June 2017, respectively. The largest VOC fluxes observed were ofsmall oxygenated compounds such as methanol, ethanol + formic acid andacetaldehyde, with average emission rates of 8.31 ± 8.5, 3.97 ± 3.9 and 1.83 ± 2.0 nmol m−2 s−1, respectively, in the summer.A large flux of isoprene was observed in the summer, with an average emissionrate of 5.31 ± 7.7 nmol m−2 s−1. While oxygenated VOCs madeup 60 % of the molar VOC flux measured, when fluxes were scaled by ozoneformation potential and peroxyacyl nitrate (PAN) formation potential thehigh reactivity of isoprene and monoterpenes meant that these speciesrepresented 30 % and 28 % of the flux contribution to ozone and PANformation potential, respectively. Comparison of measured fluxes with theemission inventory showed that the inventory failed to capture the magnitudeof VOC emissions at the local scale.more » « less
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