Imperial College London

DrDavidGreen

Faculty of MedicineSchool of Public Health

Senior Research Fellow
 
 
 
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d.green

 
 
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Sir Michael Uren HubWhite City Campus

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Summary

 

Publications

Publication Type
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86 results found

Barratt BM, Fuller GW, Kelly FJ, Priestman M, Tremper AH, Green DCet al., 2020, PM2.5 on the London Underground, Environment International, Vol: 134, ISSN: 0160-4120

Introduction: Despite the London Underground (LU) handling on average 2.8 million passenger journeys per day, the characteristics and potential health effects of the elevated concentrations of metal-rich PM2.5 found in this subway system are not well understood. Methods: Spatial monitoring campaigns were carried out to characterise the health-relevant chemical and physical properties of PM2.5 across the LU network, including diurnal and day-to-day variability and spatial distribution (above ground, depth below ground and subway line). Population-weighted station PM2.5 rankings were produced to understand the relative importance of concentrations at different stations and on different lines. Results: The PM2.5 mass in the LU (mean 88 μg m−3, median 28 μg m−3) was greater than at ambient background locations (mean 19 μg m−3, median 14 μg m−3) and roadside environments in central London (mean 22 μg m−3, median 14 μg m−3). Concentrations varied between lines and locations, with the deepest and shallowest submerged lines being the District (median 4 μg m−3) and Victoria (median 361 μg m−3 but up to 885 μg m−3). Broadly in agreement with other subway systems around the world, sampled LU PM2.5 comprised 47% iron oxide, 7% elemental carbon, 11% organic carbon, and 14% metallic and mineral oxides. Although a relationship between line depth and air quality inside the tube trains was evident, there were clear influences relating to the distance from cleaner outside air and the exchange with cabin air when the doors open. The passenger population-weighted exposure analysis demonstrated a method to identify stations that should be prioritised for remediation to improve air quality. Conclusion: PM2.5 concentrations in the LU are many times higher than in other London transport Environments. Failure to include this environment in epidemiological studies of the relationship between PM2.5 and health in

Journal article

Saunders BM, Smith JD, Smith TEL, Green DC, Barratt Bet al., 2019, Spatial variability of fine particulate matter pollution (PM2.5) on the London Underground network, URBAN CLIMATE, Vol: 30, ISSN: 2212-0955

Journal article

Freney E, Zhang Y, Croteau P, Amodeo T, Williams L, Truong F, Petit J-E, Sciare J, Sarda-Esteve R, Bonnaire N, Arumae T, Aurela M, Bougiatioti A, Mihalopoulos N, Coz E, Artinano B, Crenn V, Elste T, Heikkinen L, Poulain L, Wiedensohler A, Herrmann H, Priestman M, Alastuey A, Stavroulas I, Tobler A, Vasilescu J, Zanca N, Canagaratna M, Carbone C, Flentje H, Green D, Maasikmets M, Marmureanu L, Minguillon MC, Prevot ASH, Gros V, Jayne J, Favez Oet al., 2019, The second ACTRIS inter-comparison (2016) for Aerosol Chemical Speciation Monitors (ACSM): Calibration protocols and instrument performance evaluations, AEROSOL SCIENCE AND TECHNOLOGY, ISSN: 0278-6826

Journal article

Warren E, Charlton-perez C, Kotthaus S, Marenco F, Ryder C, Johnson B, Green D, Lean H, Ballard S, Grimmond Set al., 2019, Observed aerosol characteristics to improve forward-modelled attenuated backscatter in urban areas, ATMOSPHERIC ENVIRONMENT, ISSN: 1352-2310

Numerical weather prediction (NWP) models often parameterise aerosols to reduce computational needs, while aiming to accurately capture their impact adequately. Increasingly, aerosols are monitored in-situ directly and/or indirectly (e.g. by automatic lidars and ceilometers, ALC). ALC measure the aerosol optical characteristic of attenuated backscatter. This can also be estimated using forward models that combine forecast aerosol and relative humidity to parameterise aerosol physical and optical characteristics. The aerFO is one such forward model, designed to use Met Office NWP model output and parameterisations from the MURK visibility scheme. Given the aerFO-MURK scheme link, assessing the aerFO and its output could therefore be used to inform future developments of the MURK scheme. To identify which parameterised physical and optical aerosol characteristics in the scheme are the most critical in urban settings, aerFO is driven with different in-situ aerosol observations at a background site in central London. Estimated attenuated backscatter is then assessed against ALC observations. It is shown that the original MURK scheme parameterisation underestimates the variance of both dry mean volume radius and total number concentration. Representing both the accumulation and coarse mode aerosols in the aerFO reduces the median bias error of estimated attenuated backscatter by 69.1%. Providing more realistic temporal (monthly to hourly) variability of relative mass for different species leads to little improvement, compared to using monthly climatological means. Numerical experiments show that having more realistic estimates of number concentration is more important than providing more accurate values of the dry mean volume radius for the accumulation mode. Hence, improving the parameterisations for number concentration should be a main focus for further development of the MURK scheme. To estimate aerosol attenuated backscatter, the aerFO requires an extinction to back

Journal article

Green DC, Fuller GW, 2019, Evaluation of tire wear contribution to PM2.5 in urban environments, Atmosphere, Vol: 10

Vehicle-related particulate matter (PM) emissions may arise from both exhaust andnon-exhaust mechanisms, such as brake wear, tire wear, and road pavement abrasion, each ofwhich may be emitted directly and indirectly through resuspension of settled road dust. Severalresearchers have indicated that the proportion of PM2.5 attributable to vehicle traffic will increasingly come from non-exhaust sources. Currently, very little empirical data is available to characterize tire and road wear particles (TRWP) in the PM2.5 fraction. As such, this study was undertaken to quantify TRWP in PM2.5 at roadside locations in urban centers including London, Tokyo and Los Angeles, where vehicle traffic is an important contributor to ambient air PM. The samples were analyzed using validated chemical markers for tire tread polymer based on a pyrolysis technique. Results indicated that TRWP concentrations in the PM2.5 fraction were low, with averages ranging from < 0.004 to 0.10 g/m3, representing an average contribution to total PM2.5 of 0.27%. The TRWP levels in PM2.5 were significantly different between the three cities, with significant differences between London and Los Angeles and Tokyo and Los Angeles. There was no significant correlation between TRWP in PM2.5 and traffic count. This study provides an initial dataset to understand potential human exposure to airborne TRWP and the potential contribution of this non-exhaust emission source to total PM2.5.

Journal article

Tremper AH, Font A, Priestman M, Hamad SH, Chung T-C, Pribadi A, Brown RJC, Goddard SL, Grassineau N, Petterson K, Kelly FJ, Green DCet al., 2018, Field and laboratory evaluation of a high time resolution x-ray fluorescence instrument for determining the elemental composition of ambient aerosols, Atmospheric Measurement Techniques, Vol: 11, Pages: 3541-3557, ISSN: 1867-1381

Measuring the chemical composition of airborne particulate matter (PM) can provide valuable information on the concentration of regulated toxic metals, support modelling approaches for source detection and assist in the identification and validation of abatement techniques. Undertaking these at a high time resolution (1 h or less) enables receptor modelling techniques to be more robustly linked to emission processes. This study describes a comprehensive laboratory and field evaluation of a high time resolution x-ray fluorescence (XRF) instrument (CES XACT 625) for a range of elements (As, Ba, Ca, Cd, Ce, Cl, Cr, Cu, Fe, K, Mn, Mo, Ni, Pb, Pt, S, Sb, Se, Si, Sr, Ti, V and Zn) against alternative techniques: high time resolution mass measurements, high time resolution ion chromatography, aerosol mass spectrometry, and established filter-based, laboratory analysis using inductively coupled plasma mass spectrometry (ICP-MS).Laboratory evaluation was carried out using a novel mass-based calibration technique to independently assess the accuracy of the XRF against laboratory generated aerosols, which resulted in slopes that were not significantly different from unity. This demonstrated that generated particles can serve as an alternative calibration method for this instrument.The XACT was evaluated in three contrasting field deployments; a heavily trafficked roadside site (PM10 and PM2.5), an industrial location downwind of a nickel refinery (PM10) and an urban background location influenced by nearby industries and motorways (PM10). The XRF technique agreed well with the ICP-MS measurements of daily filter samples in all cases with a median R2 of 0.93 and a median slope of 1.07 for the elements As, Ba, Ca, Cr, Cu, Fe, K, Mn, Ni, Pb, Se, Sr, Ti, V and Zn. Differences in the results were attributed to a combination of inlet location and sampling temperature, variable blank levels in filter paper and recovery rates from acid digestion. The XRF technique also agreed well wit

Journal article

McEneff GL, Richardson A, Webb T, Wood D, Murphy B, Irlam R, Mills J, Green D, Barron LPet al., 2018, Sorbent film-coated passive samplers for explosives vapour detection Part B, Deployment in Semi-Operational Environments and Alternative Applications, Vol: 8, Pages: 1-13, ISSN: 2045-2322

The application of new sorbent-film coated passive samplers for capture of bulk commercial and military explosives vapours in operationally relevant spaces such as luggage, rooms, vehicles and shipping containers is presented. Samplers were easily integrated with in-service detection technologies with little/no sample preparation required. Ethylene glycol dinitrate (EGDN) was detected within 4 h in a container holding a suitcase packed with 0.2 kg Perunit 28E. Within a 22,000 dm3 room, 1 kg of concealed Seguridad was detected within 24 h and in an adjoining room within 7 days. Exposed samplers also successfully captured components of 1 kg TNT after 72 h and 1 kg concealed Perunit 28E after 6 h in both a furnished room and a large, partially filled shipping container. For the latter, samplers captured detectable residues outside the container after 24 h and were stable during wet weather for 72 h. A one-week trial at three operationally relevant venues including a university, a theatre and a government building revealed a nuisance positive rate of <1.4% (n = 72). Finally, two alternative applications are presented for extraction of liquid samples and use a particulate contact swab showing flexibility for a range of different search activities.

Journal article

McEneff GL, Murphy B, Webb T, Wood D, Irlam R, Mills J, Green D, Barron LPet al., 2018, Sorbent film-coated passive samplers for explosives vapour detection Part A, Materials Optimisation and Integration with Analytical Technologies, Vol: 8, Pages: 1-13, ISSN: 2045-2322

A new thin-film passive sampler is presented as a low resource dependent and discrete continuous monitoring solution for explosives-related vapours. Using 15 mid-high vapour pressure explosives-related compounds as probes, combinations of four thermally stable substrates and six film-based sorbents were evaluated. Meta-aramid and phenylene oxide-based materials showed the best recoveries from small voids (~70%). Analysis was performed using liquid chromatography-high resolution accurate mass spectrometry which also enabled tentative identification of new targets from the acquired data. Preliminary uptake kinetics experiments revealed plateau concentrations on the device were reached between 3–5 days. Compounds used in improvised explosive devices, such as triacetone triperoxide, were detected within 1 hour and were stably retained by the sampler for up to 7 days. Sampler performance was consistent for 22 months after manufacture. Lastly, its direct integration with currently in-service explosives screening equipment including ion mobility spectrometry and thermal desorption mass spectrometry is presented. Following exposure to several open environments and targeted interferences, sampler performance was subsequently assessed and potential interferences identified. High-security building and area monitoring for concealed explosives using such cost-effective and discrete passive samplers can add extra assurance to search routines while minimising any additional burden on personnel or everyday site operation.

Journal article

Ots R, Heal MR, Young DE, Williams LR, Allan JD, Nemitz E, Di Marco C, Detournay A, Xu L, Ng NL, Coe H, Herndon SC, Mackenzie IA, Green DC, Kuenen JJP, Reis S, Vieno Met al., 2018, Modelling carbonaceous aerosol from residential solid fuel burning with different assumptions for emissions, ATMOSPHERIC CHEMISTRY AND PHYSICS, Vol: 18, Pages: 4497-4518, ISSN: 1680-7316

Journal article

Wooster MJ, Gaveau DLA, Salim MA, Zhang T, Xu W, Green DC, Huijnen V, Murdiyarso D, Gunawan D, Borchard N, Schirrmann M, Main B, Sepriando Aet al., 2018, New Tropical Peatland Gas and Particulate Emissions Factors Indicate 2015 Indonesian Fires Released Far More Particulate Matter (but Less Methane) than Current Inventories Imply, REMOTE SENSING, Vol: 10

Journal article

Dong S, Ochoa Gonzalez R, Harrison RM, Green D, North R, Fowler G, Weiss Det al., 2017, Isotopic signatures in atmospheric particulate matter suggest important contributions from recycled gasoline for lead and non-exhaust traffic sources for copper and zinc in aerosols in London, United Kingdom, ATMOSPHERIC ENVIRONMENT, ISSN: 1352-2310

The aim of this study was to improve our understanding of what controls the isotope composition of Cu, Zn and Pb in particulate matter (PM) in the urban environment and to develop these isotope systems as possible source tracers. To this end, isotope ratios (Cu, Zn and Pb) and trace element concentrations (Fe, Al, Cu, Zn, Sb, Ba, Pb, Cr, Ni and V) were determined in PM10 collected at two road sites with contrasting traffic densities in central London, UK, during two weeks in summer 2010, and in potential sources, including non-combustion traffic emissions (tires and brakes), road furniture (road paint, manhole cover and road tarmac surface) and road dust. The isotope signatures of other important sources (gasoline and exhaust emissions) were taken from previous published data. Iron, Ba and Sb were used as proxies for emissions derived from brake pads, and Ni, and V for emissions derived from fossil fuel oil. The isotopic composition of Pb (expressed using 206Pb/207Pb) ranged between 1.1137 and 1.1364. The isotope ratios of Cu and Zn expressed as δ65CuNIST976 and δ66ZnLyon ranged between -0.01‰ and +0.51‰ and between -0.21‰ and +0.33‰, respectively. We did not find significant differences in the isotope signatures in PM10 over the two weeks sampling period and between the two sites, suggesting similar sources for each metal at both sites despite their different traffic densities. The stable isotope composition of Pb suggests significant contribution from road dust resuspension and from recycled leaded gasoline. The Cu and Zn isotope signatures of tires, brakes and road dust overlap with those of PM10. The correlation between the enrichments of Sb, Cu, Ba and Fe in PM10 support the previously established hypothesis that Cu isotope ratios are controlled by non-exhaust traffic emission sources in urban environments (Ochoa Gonzalez et al., 2016). Analysis of the Zn isotope signatures in PM10 and possible sources at the two sites su

Journal article

Ropkins K, DeFries TH, Pope F, Green DC, Kemper J, Kishan S, Fuller GW, Li H, Sidebottom J, Crilley LR, Kramer L, Bloss WJ, Stewart Hager Jet al., 2017, Evaluation of EDAR vehicle emissions remote sensing technology, Science of the Total Environment, Vol: 609, Pages: 1464-1474, ISSN: 0048-9697

Despite much work in recent years, vehicle emissions remain a significant contributor in many areas where air quality standards are under threat. Policy-makers are actively exploring options for next generation vehicle emission control and local fleet management policies, and new monitoring technologies to aid these activities. Therefore, we report here on findings from two separate but complementary blind evaluation studies of one new-to-market real-world monitoring option, HEAT LLC's Emission Detection And Reporting system or EDAR, an above-road open path instrument that uses Differential Absorption LIDAR to provide a highly sensitive and selective measure of passing vehicle emissions. The first study, by Colorado Department of Public Health and Environment and Eastern Research Group, was a simulated exhaust gas test exercise used to investigate the instrumental accuracy of the EDAR. Here, CO, NO, CH4 and C3H8 measurements were found to exhibit high linearity, low bias, and low drift over a wide range of concentrations and vehicle speeds. Instrument accuracy was high (R2 0.996 for CO, 0.998 for NO; 0.983 for CH4; and 0.976 for C3H8) and detection limits were 50 to 100 ppm for CO, 10 to 30 ppm for NO, 15 to 35 ppmC for CH4, and, depending on vehicle speed, 100 to 400 ppmC3 for C3H8. The second study, by the Universities of Birmingham and Leeds and King's College London, used the comparison of EDAR, on-board Portable Emissions Measurement System (PEMS) and car chaser (SNIFFER) system measurements collected under real-world conditions to investigate in situ EDAR performance. Given the analytical challenges associated with aligning these very different measurements, the observed agreements (e.g. EDAR versus PEMS R2 0.92 for CO/CO2; 0.97 for NO/CO2; ca. 0.82 for NO2/CO2; and, 0.94 for PM/CO2) were all highly encouraging and indicate that EDAR also provides a representative measure of vehicle emissions under real-world conditions.

Journal article

Reyes-Villegas E, Green DC, Priestman M, Canonaco F, Coe H, Prevot ASH, Allan JDet al., 2016, Organic aerosol source apportionment in London 2013 with ME-2: exploring the solution space with annual and seasonal analysis, ATMOSPHERIC CHEMISTRY AND PHYSICS, Vol: 16, Pages: 15545-15559, ISSN: 1680-7316

Journal article

Camina N, Green DC, Kelly FJ, Mudway ISet al., 2016, LOCAL SOURCES RATHER THAN INTERACTIONS WITH OXIDISING CO-POLLUTANT GASES DETERMINE THE GEOGRAPHICAL AND SEASONAL VARIATION IN PARTICULATE MATTER OXIDATIVE POTENTIAL, Publisher: BMJ PUBLISHING GROUP, Pages: A149-A149, ISSN: 0040-6376

Conference paper

Balducci C, Green DC, Romagnoli P, Perilli M, Johansson C, Panteliadis P, Cecinato Aet al., 2016, Cocaine and cannabinoids in the atmosphere of Northern Europe cities, comparison with Southern Europe and wastewater analysis, ENVIRONMENT INTERNATIONAL, Vol: 97, Pages: 187-194, ISSN: 0160-4120

Journal article

Ots R, Vieno M, Allan JD, Reis S, Nemitz E, Young DE, Coe H, Di Marco C, Detournay A, Mackenzie IA, Green DC, Heal MRet al., 2016, Model simulations of cooking organic aerosol (COA) over the UK using estimates of emissions based on measurements at two sites in London, ATMOSPHERIC CHEMISTRY AND PHYSICS, Vol: 16, Pages: 13773-13789, ISSN: 1680-7316

Journal article

Wragg FPH, Fuller SJ, Freshwater R, Green DC, Kelly FJ, Kalberer Met al., 2016, An automated online instrument to quantify aerosol-bound reactive oxygen species (ROS) for ambient measurement and health-relevant aerosol studies, ATMOSPHERIC MEASUREMENT TECHNIQUES, Vol: 9, Pages: 4891-4900, ISSN: 1867-1381

Journal article

Twigg MM, Ilyinskaya E, Beccaceci S, Green DC, Jones MR, Langford B, Leeson SR, Lingard JJN, Pereira GM, Carter H, Poskitt J, Richter A, Ritchie S, Simmons I, Smith RI, Tang YS, Van Dijk N, Vincent K, Nemitz E, Vieno M, Braban CFet al., 2016, Impacts of the 2014-2015 Holuhraun eruption on the UK atmosphere, ATMOSPHERIC CHEMISTRY AND PHYSICS, Vol: 16, Pages: 11415-11431, ISSN: 1680-7316

Journal article

Wragg FPH, Fuller SJ, Freshwater R, Green DC, Kelly FJ, Kalberer Met al., 2016, An Automated On-line Instrument to Quantify Aerosol-Bound Reactive Oxygen Species (ROS) for Ambient Measurement and Health Relevant Aerosol Studies

<jats:p>Abstract. The adverse health effects associated with ambient aerosol particles have been well documented, but it is still unclear which aerosol properties are most important for their negative health impact. Some studies suggest the oxidative effects of particle bound reactive oxygen species (ROS) are potential major contributors to the toxicity of particles. Traditional ROS measurement techniques are labour intense, give poor temporal resolution, and generally have significant delays between aerosol sampling and ROS analysis. However, many oxidizing particle components are reactive and thus potentially short lived. Thus, a technique to quantify particle-bound ROS online would be beneficial to quantify also the short-lived ROS components. We introduce a new portable instrument to allow on-line, continuous measurement of particle-bound ROS using a chemical assay of 2'7'-dichlorofluorescein (DCFH) with horseradish peroxidase (HRP), via fluorescence spectroscopy. All components of the new instrument are attached to a containing shell, resulting in a compact system capable of automated continuous field deployment over many hours to days. From laboratory measurements, the instrument was found to have a detection limit of ~4 nmol[H2O2]equivalents per m3 air, a dynamic range up to at least ~2000 nmol[H2O2]equivalents per m3 air, and a time resolution under 12 minutes. The instrument allows for ~12 hours automated measurement if unattended, and shows a fast response to changes in concentrations of laboratory-generated oxidised organic aerosol. The instrument was deployed at an urban site in London and particulate ROS levels of up to 24 nmol[H2O2]equivalents per m3 air were detected with PM2.5 concentrations up to 28 μg m-3. The new and portable On-line Particle-bound ROS Instrument (OPROSI) allows fast-response quantification; this is important due to the potentially short-lived nature of particle-bound ROS as well as fast changing atmospheric onditions

Journal article

Ots R, Vieno M, Allan JD, Reis S, Nemitz E, Young DE, Coe H, Di Marco C, Detournay A, Mackenzie IA, Green DC, Heal MRet al., 2016, Model simulations of cooking organic aerosol (COA) over the UK using estimates of emissions based on measurements at two sites in London

<jats:p>Abstract. Cooking organic aerosol (COA) is currently not included in European emission inventories. However, recent positive matrix factorization (PMF) analyses of aerosol mass spectrometer (AMS) measurements have suggested important contributions of COA in several European cities. In this study, emissions of COA were estimated for the UK, based on hourly AMS measurements of COA made at two sites in London (a kerbside site in central London and an urban background site in a residential area close to central London) for the full calendar year of 2012 during the Clean Air for London (ClearfLo) campaign. Iteration of COA emissions estimates and subsequent evaluation and sensitivity experiments were conducted with the EMEP4UK atmospheric chemistry transport modelling system with a horizontal resolution of 5 km × 5 km. The spatial distribution of these emissions was based on workday population density derived from the 2011 census data. The estimated UK annual COA emission was 7.4 Gg per year, which is an almost 10 % addition to the officially reported UK national total anthropogenic emissions of PM2.5 (82 Gg in 2012), corresponding to 320 mg person−1 day−1 on average. Weekday and weekend diurnal variation in COA emissions were also based on the AMS measurements. Modelled concentrations of COA were then independently evaluated against AMS-derived COA measurements from another city and time period (Manchester, Jan–Feb 2007), as well as with COA estimated by a chemical mass balance model of measurements for a two-week period at the Harwell rural site (~ 80 km west of central London). The modelled annual average contribution of COA to ambient particulate matter (PM) in central London was between 1–2 μg m−3, and between 0.5–0.7 μg m−3 in other major cities in England (Manchester, Birmingham, Leeds). It was also shown that cities smaller than London can have a central hot-spot of population density of smalle

Journal article

Reyes-Villegas E, Green DC, Priestman M, Canonaco F, Coe H, Prévôt ASH, Allan JDet al., 2016, Organic Aerosol source apportionment in London 2013 with ME-2: exploring the solution space with annual and seasonal analysis

<jats:p>Abstract. The Multilinear Engine (ME-2) factorisation tool is being widely used following the recent development of the Source Finder (SoFi) interphase at PSI. However, the success of this tool, when using the a-value approach, largely depends on the inputs (i.e. target profiles) applied as well as the experience of the user. A strategy to explore the solution space is proposed to objectively determine the solution that best deconvolves the organic aerosol (OA) sources where trilinear regression has proven to be a useful tool to compare different ME-2 solutions. Aerosol Chemical Speciation Monitor (ACSM) measurements were carried out at the urban-background site of North Kensington, London from March to December 2013, where for the first time the behaviour of OA sources and their possible environmental implications are studied using an ACSM. Five OA sources were identified: biomass burning OA (BBOA), hydrocarbon-like OA (HOA), cooking OA (COA), semivolatile oxygenated OA (SVOOA) and low-volatility oxygenated OA (LVOOA). ME-2 analysis of the seasonal datasets (spring, summer and autumn) showed a higher seasonal variability in the OA sources that was not detected when the March-December dataset was analysed; this variability was explored with the triangle plots f44 : f43 f44 : f60, with HOA and COA being the most suitable sources to constrain. Further analysis on the atmospheric implications of these OA sources was carried out, identifying evidence of the possible contribution of heavy-duty diesel vehicles to air pollution during weekdays compared to those fuelled by petrol. </jats:p>

Journal article

Ots R, Young DE, Vieno M, Xu L, Dunmore RE, Allan JD, Coe H, Williams LR, Herndon SC, Ng NL, Hamilton JF, Bergström R, Di Marco C, Nemitz E, Mackenzie IA, Kuenen JJP, Green DC, Reis S, Heal MRet al., 2016, Simulating secondary organic aerosol from missing diesel-related intermediate-volatility organic compound emissions during the Clean Air for London (ClearfLo) campaign, Atmospheric Chemistry and Physics Discussions, Vol: 2016, ISSN: 1680-7367

We present high-resolution atmospheric chemistry transport model (ACTM) simulations of secondary organic aerosol (SOA) formation over the UK for 2012. Our simulations include additional diesel-related intermediate volatility organic compound (IVOC) emissions derived directly from comprehensive field measurements at an urban background site in London during the 2012 Clean Air for London (ClearfLo) campaign. Our IVOC emissions are added proportionally to VOC emissions, as opposed to proportionally to primary organic aerosol (POA) as has been done by previous ACTM studies seeking to simulate the effects of these missing emissions. Modelled concentrations are evaluated against hourly and daily measurements of organic aerosol (OA) components derived from aerosol mass spectrometer (AMS) measurements also made during the ClearfLo campaign at three sites in the London area. Good hourly performance in comparison to the measurements was shown, giving confidence in the SOA prediction skill of the ACTM system used. According to the model simulations, diesel-related IVOCs can explain on average ∼30% of the annual SOA in and around London. Furthermore, the 90-th percentile of modelled daily SOA concentrations for the whole year is 3.8 μg m-3 (more than 40% of which is produced from the missing diesel precursors), constituting a notable addition to total particulate matter. More measurements of these precursors (currently not included in official emissions inventories) is recommended. During the period of concurrent measurements, SOA concentrations at the Detling rural background location east of London were greater than at the central London location. The model shows that this was caused by an intense pollution plume with a strong gradient of imported SOA passing over the rural location. This demonstrates the value of modelling for supporting the interpretation of measurements taken at different sites or for short durations.

Journal article

Samoli E, Atkinson RW, Analitis A, Fuller GW, Beddows D, Green DC, Mudway IS, Harrison RM, Anderson HR, Kelly FJet al., 2016, Differential health effects of short-term exposure to source-specific particles in London, U.K, Environment International, Vol: 97, Pages: 246-253, ISSN: 0160-4120

BackgroundThere is ample evidence of adverse associations between short-term exposure to ambient particle mass concentrations and health but little is known about the relative contribution from various sources.MethodsWe used air particle composition and number networks in London between 2011 and 2012 to derive six source-related factors for PM10 and four factors for size distributions of ultrafine particles (NSD). We assessed the associations of these factors, at pre-specified lags, with daily total, cardiovascular (CVD) and respiratory mortality and hospitalizations using Poisson regression. Relative risks and 95% confidence intervals (CI) were expressed as percentage change per interquartile range increment in source-factor mass or number concentration. We evaluated the sensitivity of associations to adjustment for multiple other factors and by season.ResultsWe found no evidence of associations between PM10 or NSD source-related factors and daily mortality, as the direction of the estimates were variable with 95% CI spanning 0%. Traffic-related PM10 and NSD displayed consistent associations with CVD admissions aged 15–64 years (1.01% (95%CI: 0.03%, 2.00%) and 1.04% (95%CI: − 0.62%, 2.72%) respectively) as did particles from background urban sources (0.36% for PM10 and 0.81% for NSD). Most sources were positively associated with pediatric (0–14 years) respiratory hospitalizations, with stronger evidence for fuel oil PM10 (3.43%, 95%CI: 1.26%, 5.65%). Our results did not suggest associations with cardiovascular admissions in 65 + or respiratory admissions in 15 + age groups. Effect estimates were generally robust to adjustment for other factors and by season.ConclusionsOur findings are broadly consistent with the growing evidence of the toxicity of traffic and combustion particles, particularly in relation to respiratory morbidity in children and cardiovascular morbidity in younger adults.

Journal article

Samoli E, Atkinson RW, Analitis A, Fuller GW, Green DC, Mudway I, Anderson HR, Kelly FJet al., 2016, Associations of short-term exposure to traffic-related air pollution with cardiovascular and respiratory hospital admissions in London, UK, Occupational and Environmental Medicine, ISSN: 1351-0711

Objectives There is evidence of adverse associations between short-term exposure to traffic-related pollution and health, but little is known about the relative contribution of the various sources and particulate constituents.Methods For each day for 2011–2012 in London, UK over 100 air pollutant metrics were assembled using monitors, modelling and chemical analyses. We selected a priori metrics indicative of traffic sources: general traffic, petrol exhaust, diesel exhaust and non-exhaust (mineral dust, brake and tyre wear). Using Poisson regression models, controlling for time-varying confounders, we derived effect estimates for cardiovascular and respiratory hospital admissions at prespecified lags and evaluated the sensitivity of estimates to multipollutant modelling and effect modification by season.Results For single day exposure, we found consistent associations between adult (15–64 years) cardiovascular and paediatric (0–14 years) respiratory admissions with elemental and black carbon (EC/BC), ranging from 0.56% to 1.65% increase per IQR change, and to a lesser degree with carbon monoxide (CO) and aluminium (Al). The average of past 7 days EC/BC exposure was associated with elderly (65+ years) cardiovascular admissions. Indicated associations were higher during the warm period of the year. Although effect estimates were sensitive to the adjustment for other pollutants they remained consistent in direction, indicating independence of associations from different sources, especially between diesel and petrol engines, as well as mineral dust.Conclusions Our results suggest that exhaust related pollutants are associated with increased numbers of adult cardiovascular and paediatric respiratory hospitalisations. More extensive monitoring in urban centres is required to further elucidate the associations.

Journal article

Ots R, Young DE, Vieno M, Xu L, Dunmore RE, Allan JD, Coe H, Williams LR, Herndon SC, Ng NL, Hamilton JF, Bergstrom R, Di Marco C, Nemitz E, Mackenzie IA, Kuenen JJP, Green DC, Reis S, Heal MRet al., 2016, Simulating secondary organic aerosol from missing diesel-related intermediate-volatility organic compound emissions during the Clean Air for London (ClearfLo) campaign, ATMOSPHERIC CHEMISTRY AND PHYSICS, Vol: 16, Pages: 6453-6473, ISSN: 1680-7316

Journal article

Atkinson RW, Samoli E, Analitis A, Fuller GW, Green DC, Anderson HR, Purdie E, Dunster C, Aitlhadj L, Kelly FJ, Mudway ISet al., 2016, Short-term associations between particle oxidative potential and daily mortality and hospital admissions in London, INTERNATIONAL JOURNAL OF HYGIENE AND ENVIRONMENTAL HEALTH, Vol: 219, Pages: 566-572, ISSN: 1438-4639

Background:Particulate matter (PM) from traffic and other sources has been associated with adverse health effects. One unifying theory is that PM, whatever its source, acts on the human body via their capacity to cause damaging oxidation reactions related to their content of pro-oxidants components. Few epidemiological studies have investigated particle oxidative potential (OP) metrics and health. We conducted a time series analysis to assess associations between daily particle OP measures and numbers of deaths and hospital admissions for cardiovascular and respiratory diseases.Methods:During 2011 and 2012 particles with an aerodynamic diameter less than 2.5 and 10 microns (PM2.5 and PM10 respectively) were collected daily on Partisol filters located at an urban background monitoring station in Central London. Particulate OP was assessed based on the capacity of the particles to oxidize ascorbate (OPAA) and glutathione (OPGSH) from a simple chemical model reflecting the antioxidant composition of human respiratory tract lining fluid. Particulate OP, expressed as % loss of antioxidant per μg of PM, was then multiplied by the daily concentrations of PM to derive the daily OP of PM mass concentrations (% loss per m3). Daily numbers of deaths and age- and cause-specific hospital admissions in London were obtained from national registries. Poisson regression accounting for seasonality and meteorology was used to estimate the percentage change in risk of death or admission associated with an interquartile increment in particle OP.Results:We found little evidence for adverse associations between OPAA and OPGSH and mortality. Associations with cardiovascular admissions were generally positive in younger adults and negative in older adults with confidence intervals including 0%. For respiratory admissions there was a trend, from positive to negative associations, with increasing age although confidence intervals generally included 0%.Conclusions:Our study, the first to an

Journal article

Crenn V, Sciare J, Croteau PL, Verlhac S, Froehlich R, Belis CA, Aas W, Aijala M, Alastuey A, Artinano B, Baisnee D, Bonnaire N, Bressi M, Canagaratna M, Canonaco F, Carbone C, Cavalli F, Coz E, Cubison MJ, Esser-Gietl JK, Green DC, Gros V, Heikkinen L, Herrmann H, Lunder C, Minguillon MC, Mocnik G, O'Dowd CD, Ovadnevaite J, Petit J-E, Petralia E, Poulain L, Priestman M, Riffault V, Ripoll A, Sarda-Esteve R, Slowik JG, Setyan A, Wiedensohler A, Baltensperger U, Prevot ASH, Jayne JT, Favez Oet al., 2015, ACTRIS ACSM intercomparison - Part 1: Reproducibility of concentration and fragment results from 13 individual Quadrupole Aerosol Chemical Speciation Monitors (Q-ACSM) and consistency with co-located instruments, Atmospheric Measurement Techniques, Vol: 8, Pages: 5063-5087, ISSN: 1867-1381

As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for 3 weeks during the late-fall – early-winter period (November–December 2013). The first week was dedicated to the tuning and calibration of each instrument, whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical, and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium, and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r2 > 0.9) were observed systematically for each individual Q-ACSM across all chemical families except for chloride for which three Q-ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025, 1999) and were found to be 9, 15, 19, 28, and 36 % for NR-PM1, nitrate, organic matter, sulfate, and ammonium, respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of Q-ACSMs, detailed intercomparison results are presented, along with a discuss

Journal article

Zhang T, Wooster MJ, Green DC, Main Bet al., 2015, New field-based agricultural biomass burning trace gas, PM2.5, and black carbon emission ratios and factors measured in situ at crop residue fires in Eastern China, Atmospheric Environment, Vol: 121, Pages: 22-34, ISSN: 1352-2310

Despite policy attempts to limit or prevent agricultural burning, its use to remove crop residues either immediately after harvest (e.g. field burning of wheat stubble) or after subsequent crop processing (e.g. “bonfires” of rice straw and rapeseed residues) appears to remain widespread across parts of China. Emission factors for these types of small but highly numerous fire are therefore required to fully assess their impact on atmospheric composition and air pollution. Here we describe the design and deployment of a new smoke measurement system for the close-range sampling of key gases and particles within smoke from crop residue fires, using it to assess instantaneous mixing ratios of CO and CO2 and mass concentrations of black carbon (BC) and PM2.5 from wheat stubble, rice straw, and rapeseed residue fires. Using data of our new smoke sampling system, we find a strong linear correlation between the PM2.5 mass and BC, with very high PM2.5 to BC emission ratios found in the smouldering phase (up to 80.7 mg m−3.(mg m−3)−1) compared to the flaming phase (2.0 mg m−3.(mg m−3)−1). We conclude that the contribution of BC to PM2.5 mass was as high as 50% in the flaming phase of some burns, whilst during smouldering it sometimes decreased to little over one percent. A linear mixing model is used to quantify the relative contribution of each combustion phase to the overall measured smoke composition, and we find that flaming combustion dominated the total emission of most species assessed. Using time series of trace gas concentrations from different fire cases, we calculated ‘fire integrated’ trace gas emission factors (EFs) for wheat, rice and rapeseed residue burns as 1739 ± 19 g kg−1, 1761 ± 30 g kg−1and 1704 ± 27 g kg−1 respectively for CO2, and 60 ± 12 g kg−1, 47 ± 19 g kg−1 and 82 ± 17 g kg−1 respectively for CO. Where comparisons

Journal article

Visser S, Slowik JG, Furger M, Zotter P, Bukowiecki N, Dressler R, Flechsig U, Appel K, Green DC, Tremper AH, Young DE, Williams PI, Allan JD, Herndon SC, Williams LR, Mohr C, Xu L, Ng NL, Detournay A, Barlow JF, Halios CH, Fleming ZL, Baltensperger U, Prevot ASHet al., 2015, Kerb and urban increment of highly time-resolved trace elements in PM<sub>10</sub>, PM<sub>2.5</sub> and PM<sub>1.0</sub> winter aerosol in London during ClearfLo 2012, ATMOSPHERIC CHEMISTRY AND PHYSICS, Vol: 15, Pages: 2367-2386, ISSN: 1680-7316

Journal article

Beccaceci S, McGhee EA, Brown RJC, Green DCet al., 2015, A Comparison Between a Semi-Continuous Analyzer and Filter-Based Method for Measuring Anion and Cation Concentrations in PM<sub>10</sub> at an Urban Background Site in London, AEROSOL SCIENCE AND TECHNOLOGY, Vol: 49, Pages: 793-801, ISSN: 0278-6826

Journal article

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