Green infrastructure can reduce PM2.5 traffic emissions on a city scale, by a combination of dispersion by trees and deposition on buildings, trees and grass. Simulations of PM2.5 concentrations were ...performed using a validated CFD model. A 2 × 2 km area has been reconstructed as a 3D representation of Leicester (UK) city centre which is on a scale larger than most of the other CFD studies. Combining both the effects of tree aerodynamics and the deposition capabilities of trees and grass is also something that has not yet been modelled at this scale. During summer time in Leicester City, the results show that the aerodynamic dispersive effect of trees on PM2.5 concentrations result in a 9.0% reduction. In contrast, a decrease of PM2.5, by 2.8% owing to deposition on trees (11.8 t year−1) and 0.6% owing to deposition on grass (2.5 t year−1), was also observed. Trees and grass are shown to have greater effects locally, as smaller decreases in PM2.5 were found when considering reduction across the whole boundary layer. Densely built areas like Leicester City centre have relatively less vegetation and subsequently have a smaller effect on PM2.5 concentration. It was found that particle deposition on buildings was negligible with less than 0.03%. An empirical equation was derived to describe the changes in PM2.5 based on ground surface fraction of trees and grass, and their deposition velocities.
•We model the effectiveness of trees and grass on traffic PM2.5 reduction.•City scale CFD simulations were performed under the OpenFOAM software.•Aerodynamics effect of tree prevails over deposition.•Tree are beneficial for wind speeds greater than 2 m s−1.•PM2.5 deposition on buildings is negligible with less than 0.03 %.
The COVID-19 pandemic forced governments around the world to impose restrictions on daily life to prevent the spread of the virus. This resulted in unprecedented reductions in anthropogenic activity, ...and reduced emissions of certain air pollutants, namely oxides of nitrogen. The UK ‘lockdown’ was enforced on 23/03/2020, which led to restrictions on movement, social interaction, and ‘non-essential’ businesses and services. This study employed an ensemble of measurement and modelling techniques to investigate changes in air quality, atmospheric composition and boundary layer reactivity in the South East of the UK post-lockdown. The techniques employed included in-situ gas- and particle-phase monitoring within central and local authority air quality monitoring networks, remote sensing by long path Differential Optical Absorption Spectroscopy and Sentinel-5P's TROPOMI, and detailed 0-D chemical box modelling. Findings showed that de-trended NO2 concentrations decreased by an average of 14–38% when compared to the mean of the same period over the preceding 5-years. We found that de-trended particulate matter concentrations had been influenced by interregional pollution episodes, and de-trended ozone concentrations had increased across most sites, by up to 15%, such that total Ox levels were roughly preserved. 0-D chemical box model simulations showed the observed increases in ozone concentrations during lockdown under the hydrocarbon-limited ozone production regime, where total NOx decreased proportionally greater than total non-methane hydrocarbons, which led to an increase in total hydroxyl, peroxy and organic peroxy radicals. These findings suggest a more complex scenario in terms of changes in air quality owing to the COVID-19 lockdown than originally reported and provide a window into the future to illustrate potential outcomes of policy interventions seeking large-scale NOx emissions reductions without due consideration of other reactive trace species.
Display omitted
•Boundary layer trace composition changed during the COVID-19 pandemic.•NO2 concentrations across measurement sites were down by ~14–38%.•PM10/PM2.5 concentrations were influenced by interregional pollution episodes.•O3 concentrations were up by as much as 15% and total Ox levels were ~ preserved.•Under HC limited regime, increased O3 led to increased radicals and reactivity.
This paper focuses on the effectiveness of trees at dispersing road traffic emissions on a city scale. CFD simulations of air-pollutant concentrations were performed using the OpenFOAM software ...platform using the k-ε model. Results were validated against the CODASC wind tunnel database before being applied to a LIDAR database of buildings and trees representing the City of Leicester (UK). Most other CFD models in the literature typically use idealised buildings to model wind flow and pollution dispersion. However, the methodology used in this study uses real buildings and trees data from LIDAR to reconstruct a 3D representation of Leicester City Centre. It focuses on a 2×2 km area which is on a scale larger than those usually used in other CFD studies. Furthermore, the primary focus of this study is on the interaction of trees with wind flow dynamics. It was found that in effect, trees have a regionally beneficial impact on road traffic emissions by increasing turbulence and reducing ambient concentrations of road traffic emissions by 7% at pedestrian height on average. This was an important result given that previous studies generally concluded that trees trapped pollution by obstructing wind flow in street canyons. Therefore, this study is novel both in its methodology and subsequent results, highlighting the importance of combining local and regional scale models for assessing the impact of trees in urban planning.
•We model the effectiveness of trees at dispersing road traffic emissions.•City scale CFD simulations were performed under the OpenFOAM software.•Trees increase turbulence and vertical velocity at pedestrian height.•Trees reduce concentrations of road traffic emissions by 7% at pedestrian height.•We propose combining local and regional scales for planting trees in city planning.
To gain a better understanding on the spatiotemporal variation of ultrafine particles (UFPs) in urban environments, this study reports on the first results of a long-term UFP monitoring network, set ...up in Amsterdam (NL), Antwerp (BE), Leicester (UK) and London (UK). Total number concentrations and size distributions were assessed during 1–2 years at four fixed urban background sites, supplemented with mobile trailer measurements for co-location monitoring and additional short-term monitoring sites. Intra- and interurban spatiotemporal UFP variation, associations with commonly-monitored pollutants (PM, NOx and BC) and impacts of wind fields were evaluated. Although comparable size distributions were observed between the four cities, source-related differences were demonstrated within specific particle size classes. Total and size-resolved particle number concentrations showed clear traffic-related temporal variation, confirming road traffic as the major UFP contributor in urban environments. New particle formation events were observed in all cities. Correlations with typical traffic-related pollutants (BC and NOx) were obtained for all monitoring stations, except for Amsterdam, which might be attributable to UFP emissions from Schiphol airport. The temporal variation in particle number concentration correlated fairly weakly between the four cities (rs = 0.28−0.50, COD = 0.28−0.37), yet improved significantly inside individual cities (rs = 0.59−0.77). Nevertheless, considerable differences were still obtained in terms of particle numbers (20–38% for total particle numbers and up to 49% for size-resolved particle numbers), confirming the importance of local source contributions and the need for careful consideration when allocating UFP monitoring stations in heterogeneous urban environments.
•We evaluated spatiotemporal UFP levels in Amsterdam, Antwerp, Leicester and London.•Size-resolved particle numbers provide valuable information on contributing sources.•Road traffic seems to be a major UFP contributor in the studied urban environments.•New particle formation (NPF) events were observed in all cities.•Consideration is needed when allocating UFP monitoring sites in urban environments.
National and European legislation over the past 20 yr, and the modernisation or removal of industrial sources, have significantly reduced European ozone precursor emissions. This study quantifies ...observed and modelled European ozone annual and seasonal linear trends from 158 harmonised rural background monitoring stations over a constant time period of a decade (1996–2005). Mean ozone concentrations are investigated, in addition to the ozone 5th percentiles as a measure of the baseline or background conditions, and the 95th percentiles that are representative of the peak concentration levels. This study aims to characterise and quantify surface European ozone concentrations and trends and assess the impact of the changing anthropogenic emission tracers on the observed and modelled trends. Significant (p<0.1) positive annual trends in ozone mean, 5th and 95th percentiles are observed at 54 %, 52 % and 45 % of sites respectively (85 sites, 82 sites and 71 sites). Spatially, sites in central and north-western Europe tend to display positive annual ozone trends in mean, 5th and 95th percentiles. Significant negative annual trends in ozone mean 5th and 95th percentiles are observed at 11 %, 12 % and 12 % of sites respectively (18 sites, 19 sites and 19 sites) which tend to be located in the eastern and south-western extremities of Europe. European-averaged annual trends have been calculated from the 158 sites in this study. Overall there is a net positive annual trend in observed ozone mean (0.16±0.02 ppbv yr−1 (2σ error)), 5th (0.13±0.02 ppbv yr−1) and 95th (0.16±0.03 ppbv yr−1) percentiles, representative of positive trends in mean, baseline and peak ozone. Assessing the sensitivity of the derived overall trends to the constituent years shows that the European heatwave year of 2003 has significant positive influence and 1998 the converse effect; demonstrating the masking effect of inter-annual variability on decadal based ozone trends. The European scale 3-D CTM CHIMERE was used to simulate hourly O3 concentrations for the period 1996–2005. Comparisons between the 158 observed ozone trends to those equivalent sites extracted from regional simulations by CHIMERE better match the observed increasing annual ozone (predominantly in central and north-western Europe) for 5th percentiles, than for mean or 95th ozone percentiles. The European-averaged annual ozone trend in CHIMERE 5th percentiles (0.13±0.01 ppbv yr−1) matches the corresponding observed trend extremely well, but displays a negative trend for the 95th percentile (−0.03±0.02 ppbv yr−1) where a positive ozone trend is observed. Inspection of the EU-averaged monthly means of ozone shows that the CHIMERE model is overestimating the summer month O3 levels. In comparison to trends in EMEP emissions inventories, with the exception of Austria-Hungary, we do not find that anthropogenic NOx and VOC reductions have a substantial effect on observed annual mean O3 trends in the rest of Europe. On a ten year time-scale presented in this study, O3 trends related to anthropogenic NOx and VOC reductions are being masked as a result of a number of factors including meteorological variability, changes in background ozone and shifts in source patterns.
Measurements of ozone throughout the troposphere clearly show an annual cycle. Over the last couple of decades it has become apparent that the measured annual cycle of ozone in certain locations ...shows a distinct maximum during spring and the magnitude of the maximum seems to have increased. There has been much debate as to the origins of this phenomenon. There is broad agreement that much of the ozone found in the troposphere is of photochemical origin. In contrast, there is still no over-arching consensus as to the mechanisms that lead to the formation of the spring ozone maximum. Part of the problem would seem to lie in the interpretation of measurements and the interactions of processes occurring on differing scales from the local to the global scale. This paper reviews both the experimental evidence concerning the origin of the spring ozone maximum and the supporting modelling studies. The roles of stratospheric–tropospheric exchange and photochemistry in the appearance of the spring ozone maximum are discussed; the evidence for various mechanisms for accumulation of ozone and its precursors are considered. The paper concludes with a summary of the state of the knowledge with respect to the spring ozone maximum and some possible areas for future consideration. The spring ozone phenomenon may well be a proxy for the continuing changes to the atmospheric composition owing to man's activities. Understanding the appearance of the spring ozone maximum and the mechanisms that lead to its formation therefore remains an issue fundamental to tropospheric chemistry.
Ecosystems and the atmosphere: This review describes the state of understanding the processes involved in the exchange of trace gases and aerosols between the earth's surface and the atmosphere. The ...gases covered include NO, NO2, HONO, HNO3, NH3, SO2, DMS, Biogenic VOC, O3, CH4, N2O and particles in the size range 1 nm–10 μm including organic and inorganic chemical species. The main focus of the review is on the exchange between terrestrial ecosystems, both managed and natural and the atmosphere, although some new developments in ocean–atmosphere exchange are included. The material presented is biased towards the last decade, but includes earlier work, where more recent developments are limited or absent.
New methodologies and instrumentation have enabled, if not driven technical advances in measurement. These developments have advanced the process understanding and upscaling of fluxes, especially for particles, VOC and NH3. Examples of these applications include mass spectrometric methods, such as Aerosol Mass Spectrometry (AMS) adapted for field measurement of atmosphere–surface fluxes using micrometeorological methods for chemically resolved aerosols. Also briefly described are some advances in theory and techniques in micrometeorology.
For some of the compounds there have been paradigm shifts in approach and application of both techniques and assessment. These include flux measurements over marine surfaces and urban areas using micrometeorological methods and the up-scaling of flux measurements using aircraft and satellite remote sensing. The application of a flux-based approach in assessment of O3 effects on vegetation at regional scales is an important policy linked development secured through improved quantification of fluxes. The coupling of monitoring, modelling and intensive flux measurement at a continental scale within the NitroEurope network represents a quantum development in the application of research teams to address the underpinning science of reactive nitrogen in the cycling between ecosystems and the atmosphere in Europe.
Some important developments of the science have been applied to assist in addressing policy questions, which have been the main driver of the research agenda, while other developments in understanding have not been applied to their wider field especially in chemistry-transport models through deficiencies in obtaining appropriate data to enable application or inertia within the modelling community. The paper identifies applications, gaps and research questions that have remained intractable at least since 2000 within the specialized sections of the paper, and where possible these have been focussed on research questions for the coming decade.
We demonstrate that the water uptake properties derived from sub- and super-saturated measurements of chamber-generated biogenic secondary organic aerosol (SOA) particles are independent of their ...degree of oxidation, determined using both online and offline methods. SOA particles are formed from the photooxidation of five structurally different biogenic VOCs, representing a broad range of emitted species and their corresponding range of chemical reactivity: α-pinene, β-caryophyllene, limonene, myrcene and linalool. The fractional contribution of mass fragment 44 to the total organic signal (f44) is used to characterise the extent of oxidation of the formed SOA as measured online by an aerosol mass spectrometer. Results illustrate that the values of f44 are dependent on the precursor, the extent of photochemical ageing as well as on the initial experimental conditions. SOA generated from a single biogenic precursor should therefore not be used as a general proxy for biogenic SOA. Similarly, the generated SOA particles exhibit a range of hygroscopic properties, depending on the precursor, its initial mixing ratio and photochemical ageing. The activation behaviour of the formed SOA particles show no temporal trends with photochemical ageing. The average κ values derived from the HTDMA and CCNc are generally found to cover the same range for each precursor under two different initial mixing ratio conditions. A positive correlation is observed between the hygroscopicity of particles of a single size and f44 for α-pinene, β-caryophyllene, linalool and myrcene, but not for limonene SOA. The investigation of the generality of this relationship reveals that α-pinene, limonene, linalool and myrcene are all able to generate particles with similar hygroscopicity (κHTDMA ~0.1) despite f44 exhibiting a relatively wide range of values (~4 to 11%). Similarly, κCCN is found to be independent of f44. The same findings are also true when sub- and super-saturated water uptake properties of SOA are compared to the averaged carbon oxidation state (OSC) determined using an offline method. These findings do not necessarily suggest that water uptake and chemical composition are not related. Instead, they suggest that either f44 and OSC do not represent the main dominant composition-related factors controlling water uptake of SOA particles, or they may emphasise the possible impact of semi-volatile compounds on limiting the ability of current state-of-the-art techniques to determine the chemical composition and water uptake properties of aerosol particles.
The lifetime of methane is controlled to a very large extent by the abundance of the OH radical. The tropics are a key region for methane removal, with oxidation in the lower tropical troposphere ...dominating the global methane removal budget (Bloss et al., 2005). In tropical forested environments where biogenic VOC emissions are high and NOx concentrations are low, OH concentrations are assumed to be low due to rapid reactions with sink species such as isoprene. New, simultaneous measurements of OH concentrations and OH reactivity, k'OH, in a Borneo rainforest are reported and show much higher OH than predicted, with mean peak concentrations of ~2.5×106 molecule cm−3 (10 min average) observed around solar noon. Whilst j(O1D) and humidity were high, low O3 concentrations limited the OH production from O3 photolysis. Measured OH reactivity was very high, peaking at a diurnal average of 29.1±8.5 s−1, corresponding to an OH lifetime of only 34 ms. To maintain the observed OH concentration given the measured OH reactivity requires a rate of OH production approximately 10 times greater than calculated using all measured OH sources. A test of our current understanding of the chemistry within a tropical rainforest was made using a detailed zero-dimensional model to compare with measurements. The model over-predicted the observed HO2 concentrations and significantly under-predicted OH concentrations. Inclusion of an additional OH source formed as a recycled product of OH initiated isoprene oxidation improved the modelled OH agreement but only served to worsen the HO2 model/measurement agreement. To replicate levels of both OH and HO2, a process that recycles HO2 to OH is required; equivalent to the OH recycling effect of 0.74 ppbv of NO. This recycling step increases OH concentrations by 88 % at noon and has wide implications, leading to much higher predicted OH over tropical forests, with a concomitant reduction in the CH4 lifetime and increase in the rate of VOC degradation.
Air pollution continues to be a problem in the urban environment. A range of different pollutant mitigation strategies that promote dispersion and deposition exist, but there is little evidence with ...respect to their comparative performance from both an environmental and economic perspective. This paper focuses on examining different NO2 mitigation strategies such as trees, buildings facades coated with photocatalytic paint and solid barriers in Oxford Street in London. The case study findings will support ranking the environmental and economic impacts of these different strategies to improve personal exposure conditions on the footpath and on the road in a real urban street canyon. CFD simulations of airflow and NO2 dispersion in Oxford Street in London were undertaken using the OpenFOAM software platform with the k-ε model, taking into account local prevailing wind conditions. Trees are shown to be the most cost-effective strategy, with a small reduction in NO2 concentrations of up to 0.7% on the road. However, solid barriers with and without the application of photocatalytic paint and an innovative material (20 times more expensive than trees) can improve air quality on the footpaths more substantially, up to 7.4%, yet this has a significant detrimental impact on NO2 concentrations (≤23.8%) on the road. Photocatalytic paint on building surfaces presented a minimal environmental reductions (1.2%) and economic (>100 times more expensive than trees) mitigation strategy. The findings recognised the differences between footpath and road concentrations occurred and that a focused examination of three pollution hotspots can provide more cost effective pollution mitigation. This study considers how a number of pollutant mitigation measures can be applied in a single street canyon and demonstrates the strengths and weaknesses of these strategies from economic and environmental perspectives. Further research is required to extrapolate the findings presented here to different street geometries.
Display omitted
•Several NO2 mitigation strategies were compared in Oxford Street, London.•Trees are the most cost-effective measure, with minimal reduction <1%.•Photocatalytic paint presented a reduction up to 1.2%, yet had a high maintenance cost.•Solid barriers combined aerodynamic and deposition effects had reductions up to 7.4%.•The urban background is decreasing the mitigation strategies dispersive effects.
This paper compares the environmental and economic performance of different NO2 mitigation strategies to improve air quality at street level in Oxford Street in London. Hotspot mitigation is presented as a cost-effective alternative to implementing mitigation strategies in the full street when budgets are limited.