Strong evidence for the continued contribution of lead deposited during the 20th century to the atmospheric environment in London of today.

Although leaded gasoline was banned at the end of the last century, lead (Pb) remains significantly enriched in airborne particles in large cities. The remobilization of historical Pb deposited in soils from atmospheric removal has been suggested as an important source providing evidence for the hypothetical long-term persistency of lead, and possibly other pollutants, in the urban environment. Here, we present data on Pb isotopic composition in airborne particles collected in London (2014 to 2018), which provide strong support that lead deposited via gasoline combustion still contributes significantly to the lead burden in present-day London. Lead concentration and isotopic signature of airborne particles collected at a heavily trafficked site did not vary significantly over the last decade, suggesting that sources remained unchanged. Lead isotopic composition of airborne particles matches that of road dust and topsoils and can only be explained with a significant contribution (estimate of 32 ± 10 to 43 ± 9% based on a binary mixing model) of Pb from leaded gasoline. The lead isotopes furthermore suggest significant contributions from nonexhaust traffic emissions, even though isotopic signatures of anthropogenic sources are increasingly overlapping. Lead isotopic composition of airborne particles collected at building height shows a similar signature to that collected at street level, suggesting effective mixing of lead within the urban street canyon. Our results have important implications on the persistence of Pb in urban environments and suggest that atmospheric Pb reached a baseline in London that is difficult to decrease further with present policy measures.

A dependent Bayesian Dirichlet process model for source apportionment of particle number size distribution.

The relationship between particle exposure and health risks has been well established in recent years. Particulate matter (PM) is made up of different components coming from several sources, which might have different level of toxicity. Hence, identifying these sources is an important task in order to implement effective policies to improve air quality and population health. The problem of identifying sources of particulate pollution has already been studied in the literature. However, current methods require an a priori specification of the number of sources and do not include information on covariates in the source allocations. Here, we propose a novel Bayesian nonparametric approach to overcome these limitations. In particular, we model source contribution using a Dirichlet process as a prior for source profiles, which allows us to estimate the number of components that contribute to particle concentration rather than fixing this number beforehand. To better characterize them we also include meteorological variables (wind speed and direction) as covariates within the allocation process via a flexible Gaussian kernel. We apply the model to apportion particle number size distribution measured near London Gatwick Airport (UK) in 2019. When analyzing this data, we are able to identify the most common PM sources, as well as new sources that have not been identified with the commonly used methods.

Measurement of NO(x) fluxes from a tall tower in Central London, UK and comparison with emissions inventories.

Direct measurements of NOx concentration and flux were made from a tall tower in central London, UK as part of the Clean Air for London (ClearfLo) project. Fast time resolution (10 Hz) NO and NO2 concentrations were measured and combined with fast vertical wind measurements to provide top-down flux estimates using the eddy covariance technique. Measured NOx fluxes were usually positive and ranged from close to zero at night to 2000-8000 ng m(-2) s(-1) during the day. Peak fluxes were usually observed in the morning, coincident with the maximum traffic flow. Measurements of the NOx flux have been scaled and compared to the UK National Atmospheric Emissions Inventory (NAEI) estimate of NOx emission for the measurement footprint. The measurements are on average 80% higher than the NAEI emission inventory for all of London. Observations made in westerly airflow (from parts of London where traffic is a smaller fraction of the NOx source) showed a better agreement on average with the inventory. The observations suggest that the emissions inventory is poorest at estimating NOx when traffic is the dominant source, in this case from an easterly direction from the BT Tower. Agreement between the measurements and the London Atmospheric Emissions Inventory (LAEI) are better, due to the more explicit treatment of traffic flow by this more detailed inventory. The flux observations support previous tailpipe observations of higher NOx emitted from the London vehicle diesel fleet than is represented in the NAEI or predicted for several EURO emission control technologies. Higher-than-anticipated vehicle NOx is likely responsible for the significant discrepancies that exist in London between observed NOx and long-term NOx projections.

Air quality on UK diesel and hybrid trains.

Concentrations of particulate matter (PM10, PM2.5), ultrafine (UFP), particle number (PNC), black carbon (BC), nitrogen dioxide (NO2) and nitrogen oxides (NOX) were measured in train carriages on diesel and bi-mode trains on inter-city and long-distance journeys in the United Kingdom (UK) using a high-quality mobile measurement system. Air quality on 15 different routes was measured using highly-time resolved data on a total of 119 journeys during three campaigns in winter 2020 and summer 2021; this included 13 different train classes. Each journey was sampled 4-10 times with approximatively 11,000 min of in-train concentrations in total. Mean-journey concentrations were 7.552 µg m-3 (PM10); 3.936 µg m-3 (PM2.5); 333-11,300 # cm-3 (PNC); 225-9,131 # cm-3 (UFP); 0.6-11 µg m-3 (BC); 28-201 µg m-3 (NO2); and 130-3,456 µg m-3 (NOX). The impact of different factors on in-train concentrations was evaluated. The presence of tunnels was the factor with the largest impact on the in-train particle concentrations with enhancements by a factor of 40 greater than baseline for BC, and a factor 6 to 7 for PM and PNC. The engine fuel mode was the factor with the largest impact on NO2 with enhancements of up to 14-times larger when the train run on diesel compared to the times running on electric on hybrid trains. Train classes with an age < 10 years observed the lowest in-train PM, BC and NOX concentrations reflecting improvements in aspects of rail technology in recent years. Air quality on UK diesel trains is higher than ambient concentrations but has lower PM2.5 and PNC than most other transport modes, including subway systems, diesel and petrol cars. This paper adds significantly to the evidence on exposure to poor air quality in transport micro-environments and provides the industry and regulatory bodies with reference-grade measurements on which to establish in-train air quality guidelines.

Associations between short-term exposure to airborne carbonaceous particles and mortality: A time-series study in London during 2010-2019.

Exposure to ambient particulate matter (PM) has been identified as a major global health concern; however, the importance of specific chemical PM components remains uncertain. Recent studies have suggested that carbonaceous aerosols are important detrimental components of the particle mixture. Using time-series methods, we investigated associations between short-term exposure to carbonaceous particles and mortality in London, UK. Daily counts of non-accidental, respiratory, and cardiovascular deaths were obtained between 2010 and 2019. For the same period, daily concentrations of carbonaceous particles: organic (OC), elemental (EC), wood-burning (WC), total carbon (TC) and equivalent black carbon (eBC) were sourced from two centrally located monitoring sites (one urban-traffic and one urban-background). Generalized additive models were used to estimate the percentage change in mortality risk associated with interquartile range increases in particulate concentrations. Lagged effects up to 3 days were examined. Stratified analyses were conducted by age, sex, and season, separate analyses were also performed by site-type. For non-accidental mortality, positive associations were observed for all particle species at lag1, including statistically significant percentage risk changes in WC (0.51% (95%CI: 0.19%, 0.82%) per IQR (0.68 µg/m3)) and OC (0.45% (95%CI: 0.04%, 0.87% per IQR (2.36 µg/m3)). For respiratory deaths, associations were greatest for particulate concentrations averaged over the current and previous 3 days, with increases in risk of 1.70% (95%CI: 0.64%, 2.77%) for WC and 1.31% (95%CI: -0.08%, 2.71%) for OC. No associations were found with cardiovascular mortality. Results were robust to adjustment for particle mass concentrations. Stratified analyses suggested particulate effects were greatest in the summer and respiratory associations more pronounced in females. Our findings are supportive of an association between carbonaceous particles and non-accidental and respiratory mortality. The strongest evidence of an effect was for WC; this is of significance given the rising popularity of wood-burning for residential space heating and energy production across Europe.

Assessing the Impact of Non-Exhaust Emissions on the Asthmatic Airway (IONA) Protocol for a Randomised Three-Exposure Crossover Study.

BACKGROUND: People living with asthma are disproportionately affected by air pollution, with increased symptoms, medication usage, hospital admissions, and the risk of death. To date, there has been a focus on exhaust emissions, but traffic-related air pollution (TRAP) can also arise from the mechanical abrasion of tyres, brakes, and road surfaces. We therefore created a study with the aim of investigating the acute impacts of non-exhaust emissions (NEEs) on the lung function and airway immune status of asthmatic adults. METHODS: A randomised three-condition crossover panel design will expose adults with asthma using a 2.5 h intermittent cycling protocol in a random order at three locations in London, selected to provide the greatest contrast in the NEE components within TRAP. Lung function will be monitored using oscillometry, fractional exhaled nitric oxide, and spirometry (the primary outcome is the forced expiratory volume in one second). Biomarkers of inflammation and airborne metal exposure will be measured in the upper airway using nasal lavage. Symptom responses will be monitored using questionnaires. Sources of exhaust and non-exhaust concentrations will be established using source apportionment via the positive matrix factorisation of high-time resolution chemical measures conducted at the exposure sites. DISCUSSION: Collectively, this study will provide us with valuable information on the health effects of NEE components within ambient PM2.5 and PM10, whilst establishing a biological mechanism to help contextualise current epidemiological observations.

Recommendations for reporting equivalent black carbon (eBC) mass concentrations based on long-term pan-European in-situ observations.

A reliable determination of equivalent black carbon (eBC) mass concentrations derived from filter absorption photometers (FAPs) measurements depends on the appropriate quantification of the mass absorption cross-section (MAC) for converting the absorption coefficient (babs) to eBC. This study investigates the spatial-temporal variability of the MAC obtained from simultaneous elemental carbon (EC) and babs measurements performed at 22 sites. We compared different methodologies for retrieving eBC integrating different options for calculating MAC including: locally derived, median value calculated from 22 sites, and site-specific rolling MAC. The eBC concentrations that underwent correction using these methods were identified as LeBC (local MAC), MeBC (median MAC), and ReBC (Rolling MAC) respectively. Pronounced differences (up to more than 50 %) were observed between eBC as directly provided by FAPs (NeBC; Nominal instrumental MAC) and ReBC due to the differences observed between the experimental and nominal MAC values. The median MAC was 7.8 ± 3.4 m2 g-1 from 12 aethalometers at 880 nm, and 10.6 ± 4.7 m2 g-1 from 10 MAAPs at 637 nm. The experimental MAC showed significant site and seasonal dependencies, with heterogeneous patterns between summer and winter in different regions. In addition, long-term trend analysis revealed statistically significant (s.s.) decreasing trends in EC. Interestingly, we showed that the corresponding corrected eBC trends are not independent of the way eBC is calculated due to the variability of MAC. NeBC and EC decreasing trends were consistent at sites with no significant trend in experimental MAC. Conversely, where MAC showed s.s. trend, the NeBC and EC trends were not consistent while ReBC concentration followed the same pattern as EC. These results underscore the importance of accounting for MAC variations when deriving eBC measurements from FAPs and emphasize the necessity of incorporating EC observations to constrain the uncertainty associated with eBC.

Inter-annual trends of ultrafine particles in urban Europe.

Ultrafine particles (UFP, those with diameters ≤ 100 nm), have been reported to potentially penetrate deeply into the respiratory system, translocate through the alveoli, and affect various organs, potentially correlating with increased mortality. The aim of this study is to assess long-term trends (5-11 years) in mostly urban UFP concentrations based on measurements of particle number size distributions (PNSD). Additionally, concentrations of other pollutants and meteorological variables were evaluated to support the interpretations. PNSD datasets from 12 urban background (UB), 5 traffic (TR), 3 suburban background (SUB) and 1 regional background (RB) sites in 15 European cities and 1 in the USA were evaluated. The non-parametric Theil-Sen's method was used to detect monotonic trends. Meta-analyses were carried out to assess the overall trends and those for different environments. The results showed significant decreases in NO, NO2, BC, CO, and particle concentrations in the Aitken (25-100 nm) and the Accumulation (100-800 nm) modes, suggesting a positive impact of the implementation of EURO 5/V and 6/VI vehicle standards on European air quality. The growing use of Diesel Particle Filters (DPFs) might also have clearly reduced exhaust emissions of BC, PM, and the Aitken and Accumulation mode particles. However, as reported by prior studies, there remains an issue of poor control of Nucleation mode particles (smaller than 25 nm), which are not fully reduced with current DPFs, without emission controls for semi-volatile organic compounds, and might have different origins than road traffic. Thus, contrasting trends for Nucleation mode particles were obtained across the cities studied. This mode also affected the UFP and total PNC trends because of the high proportion of Nucleation mode particles in both concentration ranges. It was also found that the urban temperature increasing trends might have also influenced those of PNC, Nucleation and Aitken modes.

The variability of mass concentrations and source apportionment analysis of equivalent black carbon across urban Europe.

This study analyzed the variability of equivalent black carbon (eBC) mass concentrations and their sources in urban Europe to provide insights into the use of eBC as an advanced air quality (AQ) parameter for AQ standards. This study compiled eBC mass concentration datasets covering the period between 2006 and 2022 from 50 measurement stations, including 23 urban background (UB), 18 traffic (TR), 7 suburban (SUB), and 2 regional background (RB) sites. The results highlighted the need for the harmonization of eBC measurements to allow for direct comparisons between eBC mass concentrations measured across urban Europe. The eBC mass concentrations exhibited a decreasing trend as follows: TR > UB > SUB > RB. Furthermore, a clear decreasing trend in eBC concentrations was observed in the UB sites moving from Southern to Northern Europe. The eBC mass concentrations exhibited significant spatiotemporal heterogeneity, including marked differences in eBC mass concentration and variable contributions of pollution sources to bulk eBC between different cities. Seasonal patterns in eBC concentrations were also evident, with higher winter concentrations observed in a large proportion of cities, especially at UB and SUB sites. The contribution of eBC from fossil fuel combustion, mostly traffic (eBCT) was higher than that of residential and commercial sources (eBCRC) in all European sites studied. Nevertheless, eBCRC still had a substantial contribution to total eBC mass concentrations at a majority of the sites. eBC trend analysis revealed decreasing trends for eBCT over the last decade, while eBCRC remained relatively constant or even increased slightly in some cities.

Ambient air particulate total lung deposited surface area (LDSA) levels in urban Europe.

This study aims to picture the phenomenology of urban ambient total lung deposited surface area (LDSA) (including head/throat (HA), tracheobronchial (TB), and alveolar (ALV) regions) based on multiple path particle dosimetry (MPPD) model during 2017-2019 period collected from urban background (UB, n = 15), traffic (TR, n = 6), suburban background (SUB, n = 4), and regional background (RB, n = 1) monitoring sites in Europe (25) and USA (1). Briefly, the spatial-temporal distribution characteristics of the deposition of LDSA, including diel, weekly, and seasonal patterns, were analyzed. Then, the relationship between LDSA and other air quality metrics at each monitoring site was investigated. The result showed that the peak concentrations of LDSA at UB and TR sites are commonly observed in the morning (06:00-8:00 UTC) and late evening (19:00-22:00 UTC), coinciding with traffic rush hours, biomass burning, and atmospheric stagnation periods. The only LDSA night-time peaks are observed on weekends. Due to the variability of emission sources and meteorology, the seasonal variability of the LDSA concentration revealed significant differences (p = 0.01) between the four seasons at all monitoring sites. Meanwhile, the correlations of LDSA with other pollutant metrics suggested that Aitken and accumulation mode particles play a significant role in the total LDSA concentration. The results also indicated that the main proportion of total LDSA is attributed to the ALV fraction (50 %), followed by the TB (34 %) and HA (16 %). Overall, this study provides valuable information of LDSA as a predictor in epidemiological studies and for the first time presenting total LDSA in a variety of European urban environments.

Phenomenology of ultrafine particle concentrations and size distribution across urban Europe.

The 2017-2019 hourly particle number size distributions (PNSD) from 26 sites in Europe and 1 in the US were evaluated focusing on 16 urban background (UB) and 6 traffic (TR) sites in the framework of Research Infrastructures services reinforcing air quality monitoring capacities in European URBAN & industrial areaS (RI-URBANS) project. The main objective was to describe the phenomenology of urban ultrafine particles (UFP) in Europe with a significant air quality focus. The varying lower size detection limits made it difficult to compare PN concentrations (PNC), particularly PN10-25, from different cities. PNCs follow a TR > UB > Suburban (SUB) order. PNC and Black Carbon (BC) progressively increase from Northern Europe to Southern Europe and from Western to Eastern Europe. At the UB sites, typical traffic rush hour PNC peaks are evident, many also showing midday-morning PNC peaks anti-correlated with BC. These peaks result from increased PN10-25, suggesting significant PNC contributions from nucleation, fumigation and shipping. Site types to be identified by daily and seasonal PNC and BC patterns are: (i) PNC mainly driven by traffic emissions, with marked correlations with BC on different time scales; (ii) marked midday/morning PNC peaks and a seasonal anti-correlation with PNC/BC; (iii) both traffic peaks and midday peaks without marked seasonal patterns. Groups (ii) and (iii) included cities with high insolation. PNC, especially PN25-800, was positively correlated with BC, NO2, CO and PM for several sites. The variable correlation of PNSD with different urban pollutants demonstrates that these do not reflect the variability of UFP in urban environments. Specific monitoring of PNSD is needed if nanoparticles and their associated health impacts are to be assessed. Implementation of the CEN-ACTRIS recommendations for PNSD measurements would provide comparable measurements, and measurements of <10 nm PNC are needed for full evaluation of the health effects of this size fraction.

Sources of particle number concentration and noise near London Gatwick Airport.

There is increasing evidence of potential health impacts from both aircraft noise and aircraft-associated ultrafine particles (UFP). Measurements of noise and UFP are however scarce near airports and so their variability and relationship are not well understood. Particle number size distributions and noise levels were measured at two locations near Gatwick airport (UK) in 2018-19 with the aim to characterize particle number concentrations (PNC) and link PNC sources, especially UFP, with noise. Positive Matrix Factorization was used on particle number size distribution to identify these sources. Mean PNC (7500-12,000 p cm-3) were similar to those measured close to a highly trafficked road in central London. Peak PNC (94,000 p cm-3) were highest at the site closer to the runway. The airport source factor contributed 17% to the PNC at both sites and the concentrations were greatest when the respective sites were downwind of the runway. However, the main source of PNC was associated with traffic emissions. At both sites noise levels were above the recommendations by the WHO (World Health Organisation). Regression models of identified UFP sources and noise suggested that the largest source of noise (LAeq-1hr) above background was associated with sources of fresh traffic and urban UFP depending on the site. Noise and UFP correlations were moderate to low suggesting that UFP are unlikely to be an important confounder in epidemiological studies of aircraft noise and health. Correlations between UFP and noise were affected by meteorological factors, which need to be considered in studies of short-term associations between aircraft noise and health.

Source attribution and quantification of atmospheric nickel concentrations in an industrial area in the United Kingdom (UK).

Pontardawe in South Wales, United Kingdom (UK), consistently has the highest concentrations of nickel (Ni) in PM10 in the UK and repeatedly breaches the 20 ng m-3 annual mean EU target value. Several local industries use Ni in their processes. To assist policy makers and regulators in quantifying the relative Ni contributions of these industries and developing appropriate emission reduction approaches, the hourly concentrations of 23 elements were measured using X-ray fluorescence alongside meteorological variables and black carbon during a four-week campaign in November-December 2015. Concentrations of Ni ranged between 0 and 2480 ng m-3 as hourly means. Positive Matrix Factorization (PMF) was used to identify sources contributing to measured elements. Cluster analysis of bivariate polar plots of those factors containing Ni in their profile was further used to quantify the industrial processes contributing to ambient PM10 concentrations. Two sources were identified to contribute to Ni concentrations, stainless-steel (which contributed to 10% of the Ni burden) and the Ni refinery (contributing 90%). From the stainless-steel process, melting activities were responsible for 66% of the stainless-steel factor contribution.

Air quality in enclosed railway stations: Quantifying the impact of diesel trains through deployment of multi-site measurement and random forest modelling.

Concentrations of the air pollutants (NO2 and particulate matter) were measured for several months and at multiple locations inside and outside two enclosed railway stations in the United Kingdom - Edinburgh Waverly (EDB) and London King's Cross (KGX) - which, respectively, had at the time 59% and 18% of their train services powered by diesel engines. Average concentrations of NO2 were above the 40 µg m-3 annual limit value outside the stations and were further elevated inside, especially at EDB. Concentrations of PM2.5 inside the stations were 30-40% higher at EDB than outside and up to 20% higher at KGX. Concentrations of both NO2 and PM2.5 were highest closer to the platforms, especially those with a higher frequency of diesel services. A random-forest regression model was used to quantify the impact of numbers of different types of diesel trains on measured concentrations allowing prediction of the impact of individual diesel-powered rolling stock.