A chronology of global air quality.

Air pollution has been recognized as a threat to human health since the time of Hippocrates, ca 400 BC. Successive written accounts of air pollution occur in different countries through the following two millennia until measurements, from the eighteenth century onwards, show the growing scale of poor air quality in urban centres and close to industry, and the chemical characteristics of the gases and particulate matter. The industrial revolution accelerated both the magnitude of emissions of the primary pollutants and the geographical spread of contributing countries as highly polluted cities became the defining issue, culminating with the great smog of London in 1952. Europe and North America dominated emissions and suffered the majority of adverse effects until the latter decades of the twentieth century, by which time the transboundary issues of acid rain, forest decline and ground-level ozone became the main environmental and political air quality issues. As controls on emissions of sulfur and nitrogen oxides (SO2 and NOx) began to take effect in Europe and North America, emissions in East and South Asia grew strongly and dominated global emissions by the early years of the twenty-first century. The effects of air quality on human health had also returned to the top of the priorities by 2000 as new epidemiological evidence emerged. By this time, extensive networks of surface measurements and satellite remote sensing provided global measurements of both primary and secondary pollutants. Global emissions of SO2 and NOx peaked, respectively, in ca 1990 and 2018 and have since declined to 2020 as a result of widespread emission controls. By contrast, with a lack of actions to abate ammonia, global emissions have continued to grow. This article is part of a discussion meeting issue 'Air quality, past present and future'.

A chronology of ratios between black smoke and PM10 and PM2.5 in the context of comparison of air pollution epidemiology concentration-response functions.

BACKGROUND: For many air pollution epidemiological studies in Europe, 'black smoke' (BS) was the only measurement available to quantify ambient particulate matter (PM), particularly for exposures prior to the mid-1990s when quantification via the PM10 and/or PM2.5 metrics was introduced. The aim of this work was to review historic BS and PM measurements to allow comparison of health concentration-response functions (CRF) derived using BS as the measure of exposure with CRFs derived using PM10 or PM2.5. METHODS: The literature was searched for quantitative information on measured ratios of BS:PM10, BS:PM2.5, and chemical composition of PM; with specific focus on the United Kingdom (UK) between 1970 and the early 2000s when BS measurements were discontinued. RESULTS: The average BS:PM10 ratio in urban background air was just below unity at the start of the 1970s, decreased rapidly to ≈ 0.7 in the mid-1970s and to ≈ 0.5 at the end of the 1970s, with continued smaller declines in the 1980s, and was within the range 0.2-0.4 by the end of the 1990s. The limited data for the BS:PM2.5 ratio suggest it equalled or exceeded unity at the start of the 1970s, declined to ≈ 0.7 by the end of the 1970s, with slower decline thereafter to a range 0.4-0.65 by the end of the 1990s. For an epidemiological study that presents a CRF BS value, the corresponding CRF PM10 value can be estimated as R BS:PM10 × CRF BS where R BS:PM10 is the BS:PM10 concentration ratio, if the toxicity of PM10 is assumed due only to the component quantified by a BS measurement. In the general case of some (but unknown) contribution of toxicity from non-BS components of PM10 then CRF PM10 > R BS:PM10 × CRF BS, with CRF PM10 exceeding CRFBS if the toxicity of the other components in PM10 is greater than the toxicity of the component to which the BS metric is sensitive. Similar analyses were applied to relationships between CRF PM2.5 and CRF BS. CONCLUSIONS: Application of this analysis to example published CRF BS values for short and long-term health effects of PM suggest health effects from other components in the PM mixture in addition to the fine black particles characterised by BS.

Climate change impacts on human health over Europe through its effect on air quality.

This review examines the current literature on the effects of future emissions and climate change on particulate matter (PM) and O3 air quality and on the consequent health impacts, with a focus on Europe. There is considerable literature on the effects of climate change on O3 but fewer studies on the effects of climate change on PM concentrations. Under the latest Intergovernmental Panel on Climate Change (IPCC) 5th assessment report (AR5) Representative Concentration Pathways (RCPs), background O3 entering Europe is expected to decrease under most scenarios due to higher water vapour concentrations in a warmer climate. However, under the extreme pathway RCP8.5 higher (more than double) methane (CH4) abundances lead to increases in background O3 that offset the O3 decrease due to climate change especially for the 2100 period. Regionally, in polluted areas with high levels of nitrogen oxides (NOx), elevated surface temperatures and humidities yield increases in surface O3 - termed the O3 climate penalty - especially in southern Europe. The O3 response is larger for metrics that represent the higher end of the O3 distribution, such as daily maximum O3. Future changes in PM concentrations due to climate change are much less certain, although several recent studies also suggest a PM climate penalty due to high temperatures and humidity and reduced precipitation in northern mid-latitude land regions in 2100.A larger number of studies have examined both future climate and emissions changes under the RCP scenarios. Under these pathways the impact of emission changes on air quality out to the 2050s will be larger than that due to climate change, because of large reductions in emissions of O3 and PM pollutant precursor emissions and the more limited climate change response itself. Climate change will also affect climate extreme events such as heatwaves. Air pollution episodes are associated with stagnation events and sometimes heat waves. Air quality during the 2003 heatwave over Europe has been examined in numerous studies and mechanisms for enhancing O3 have been identified.There are few studies on health effects associated with climate change impacts alone on air quality, but these report higher O3-related health burdens in polluted populated regions and greater PM2.5 health burdens in these emission regions. Studies that examine the combined impacts of climate change and anthropogenic emissions change under the RCP scenarios report reductions in global and European premature O3-respiratory related and PM mortalities arising from the large decreases in precursor emissions. Under RCP 8.5 the large increase in CH4 leads to global and European excess O3-respiratory related mortalities in 2100. For future health effects, besides uncertainty in future O3 and particularly PM concentrations, there is also uncertainty in risk estimates such as effect modification by temperature on pollutant-response relationships and potential future adaptation that would alter exposure risk.

Insights into the composition and sources of rural, urban and roadside carbonaceous PM10.

Insights into the nature and sources of the urban and roadside increments in carbonaceous PM10 are gained from bulk chemical analyses on daily filter samples collected at a roadside, urban background and rural site in Edinburgh, UK (not all sampling contemporaneous). The concentrations of PM10 water-soluble organic matter (WSOM) at the three sites were similar, and (where measured concurrently) strongly correlated, indicating a uniform background source, in contrast to the black carbon component (quantified by filter optical reflectance) whose average concentrations at urban background and roadside were, respectively, about 3 and 7 times greater than at the rural site, indicating local urban sources. BC was not a major component of PM10 but was a major component of the urban and roadside PM10 increments (∼50% and ∼60% respectively). The roadside WSOM had greater hydrophobicity than the urban background WSOM. UV-vis spectra indicated increased prevalence of unsaturated bonds and conjugation in urban background WSOM in winter compared with summer. This is consistent with both summertime photochemical production of particle OM and maritime primary aliphatic WSOM. Raman microscopy of a small subset of samples indicated carbon functionality ranged between diesel-like material and more complex humic-like material. Results overall indicate the presence of a background functionalized carbonaceous material, with local BC sources superimposed.

The application of carbon-14 analyses to the source apportionment of atmospheric carbonaceous particulate matter: a review.

Organic carbon (OC) and elemental carbon (EC) together constitute a substantial proportion of airborne particulate matter (PM). Insight into the sources of this major contributor to PM is important for policies to mitigate the impact of PM on human health and climate change. In recent years measurement of the abundance of the radioisotope of carbon ((14)C) in samples of PM by accelerator mass spectrometry has been used to help quantify the relative contributions from sources of fossil carbon and contemporary carbon. This review provides an introduction to the different sources of carbon within PM and the role of (14)C measurements, a description of the preparation of PM samples and of the instrumentation used to quantify (14)C, and a summary of the results and source apportionment methods reported in published studies since 2004. All studies report a sizable fraction of the carbonaceous PM as of non-fossil origin. Even for PM collected in urban locations, the proportions of non-fossil carbon generally exceed 30%; typically the proportion in urban background locations is around 40-60% depending on the local influence of biomass burning. Where values have been measured directly, proportions of non-fossil carbon in EC are lower than in OC, reflecting the greater contribution of fossil-fuel combustion to EC and the generally small sources of contemporary EC. Detailed source apportionment studies point to important contributions from biogenic-derived secondary OC, consistent with other evidence of a ubiquitous presence of heavily oxidized background secondary OC. The review concludes with some comments on current issues and future prospects, including progress towards compound-class and individual-compound-specific (14)C analyses.

A low-tech, low-cost method to capture point-source ammonia emissions and their potential use as a nitrogen fertiliser.

Rising global energy prices have led to increased costs of nitrogen (N) fertilisers for farmers, but N pollution (losses) from agricultural activities can account for over 50% of the nitrogen applied. This study assesses the feasibility of a low-cost and low-tech method of NH3 emission capture from an agricultural point source (chicken manure) using a water column bubbling technique, and its application as a fertiliser to several plant types. Solutions of i) nitric acid (HNO3), ii) calcium nitrate (Ca(NO3)2), iii) a mixture of Ca(NO3)2 and HNO3 and iv) deionised H2O were used to scrub NH3 from air pumped from a storage container containing chicken manure. We conclude that NH3 can be captured from manure using low-tech methods, and that solutions of common fertiliser compounds such as ammonium nitrate and calcium ammonium nitrate can be replicated by binding captured NH3 to solutions of nitrate. Our results suggest that dissolved calcium nitrate is just as effective at scrubbing NH3 from the atmosphere as nitric acid at low concentrations, but could do so at a near neutral pH. For use on common silage grass for livestock feed, all of the captured ammonium solutions significantly increased yields, including the ammonium only solution. However, the aquatic plants (Taxiphyllum Barbieri and Salvinia auriculata) did not respond favourably to a high ratio of NH4+ in solution, and in the case of Salvinia auriculata, the plant was significantly damaged by the ammonium only solution. In conclusion, we highlight that the capture and utilisation of NH3 emissions from point sources is possible using very basic apparatus and that if used correctly, this captured nitrogen can be stored and applied to crops in a variety of forms which could reduce reliance and cost of mineral fertiliser use.

Measurement error in time-series analysis: a simulation study comparing modelled and monitored data.

BACKGROUND: Assessing health effects from background exposure to air pollution is often hampered by the sparseness of pollution monitoring networks. However, regional atmospheric chemistry-transport models (CTMs) can provide pollution data with national coverage at fine geographical and temporal resolution. We used statistical simulation to compare the impact on epidemiological time-series analysis of additive measurement error in sparse monitor data as opposed to geographically and temporally complete model data. METHODS: Statistical simulations were based on a theoretical area of 4 regions each consisting of twenty-five 5 km × 5 km grid-squares. In the context of a 3-year Poisson regression time-series analysis of the association between mortality and a single pollutant, we compared the error impact of using daily grid-specific model data as opposed to daily regional average monitor data. We investigated how this comparison was affected if we changed the number of grids per region containing a monitor. To inform simulations, estimates (e.g. of pollutant means) were obtained from observed monitor data for 2003-2006 for national network sites across the UK and corresponding model data that were generated by the EMEP-WRF CTM. Average within-site correlations between observed monitor and model data were 0.73 and 0.76 for rural and urban daily maximum 8-hour ozone respectively, and 0.67 and 0.61 for rural and urban loge(daily 1-hour maximum NO2). RESULTS: When regional averages were based on 5 or 10 monitors per region, health effect estimates exhibited little bias. However, with only 1 monitor per region, the regression coefficient in our time-series analysis was attenuated by an estimated 6% for urban background ozone, 13% for rural ozone, 29% for urban background loge(NO2) and 38% for rural loge(NO2). For grid-specific model data the corresponding figures were 19%, 22%, 54% and 44% respectively, i.e. similar for rural loge(NO2) but more marked for urban loge(NO2). CONCLUSION: Even if correlations between model and monitor data appear reasonably strong, additive classical measurement error in model data may lead to appreciable bias in health effect estimates. As process-based air pollution models become more widely used in epidemiological time-series analysis, assessments of error impact that include statistical simulation may be useful.

Particles, air quality, policy and health.

The diversity of ambient particle size and chemical composition considerably complicates pinpointing the specific causal associations between exposure to particles and adverse human health effects, the contribution of different sources to ambient particles at different locations, and the consequent formulation of policy action to most cost-effectively reduce harm caused by airborne particles. Nevertheless, the coupling of increasingly sophisticated measurements and models of particle composition and epidemiology continue to demonstrate associations between particle components and sources (and at lower concentrations) and a wide range of adverse health outcomes. This article reviews the current approaches to source apportionment of ambient particles and the latest evidence for their health effects, and describes the current metrics, policies and legislation for the protection of public health from ambient particles. A particular focus is placed on particles in the ultrafine fraction. The review concludes with an extended evaluation of emerging challenges and future requirements in methods, metrics and policy for understanding and abating adverse health outcomes from ambient particles.

Future impacts of O3 on respiratory hospital admission in the UK from current emissions policies.

Exposure to ambient ozone (O3) O3 is associated with impacts on human health. O3 is a secondary pollutant whose concentrations are determined inter alia by emissions of precursors such as oxides of nitrogen (NOx) and volatile organic compounds (VOCs), and thus future health burdens depend on policies relating to climate and air quality. While emission controls are expected to reduce levels of PM2.5 and NO2 and their associated mortality burdens, for secondary pollutants like O3 the picture is less clear. Detailed assessments are necessary to provide quantitative estimates of future impacts to support decision-makers. We simulate future O3 across the UK using a high spatial resolution atmospheric chemistry model with current UK and European policy projections for 2030, 2040 and 2050, and use UK regional population-weighting and latest recommendations on health impact assessment to quantify respiratory emergency hospital admissions associated with short-term effects of O3. We estimate 60,488 admissions in 2018, increasing by 4.2%, 4.5% and 4.6% by 2030, 2040 and 2050 respectively (assuming a fixed population). Including future population growth, estimated emergency respiratory hospital admissions are 8.3%, 10.3% and 11.7% higher by 2030, 2040 and 2050 respectively. Increasing O3 concentrations in future are driven by reduced nitric oxide (NO) in urban areas due to reduced emissions, with increases in O3 mainly occurring in areas with lowest O3 concentrations currently. Meteorology influences episodes of O3 on a day-to-day basis, although a sensitivity study indicates that annual totals of hospital admissions are only slightly impacted by meteorological year. While reducing emissions results in overall benefits to population health (through reduced mortality due to long-term exposure to PM2.5 and NO2), due to the complex chemistry, as NO emissions reduce there are associated local increases in O3 close to population centres that may increase harms to health.

Impacts of emissions policies on future UK mortality burdens associated with air pollution.

Air pollution is the greatest environmental risk to public health. Future air pollution concentrations are primarily determined by precursor emissions, which are driven by environmental policies relating to climate and air pollution. Detailed health impact assessments (HIA) are necessary to provide quantitative estimates of the impacts of future air pollution to support decision-makers developing environmental policy and targets. In this study we use high spatial resolution atmospheric chemistry modelling to simulate future air pollution concentrations across the UK for 2030, 2040 and 2050 based on current UK and European policy projections. We combine UK regional population-weighted concentrations with the latest epidemiological relationships to quantify mortality associated with changes in PM2.5 and NO2 air pollution. Our HIA suggests that by 2050, population-weighted exposure to PM2.5 will reduce by 28% to 36%, and for NO2 by 35% to 49%, depending on region. The HIA shows that for present day (2018), annual mortality attributable to the effects of long-term exposure to PM2.5 and NO2 is in the range 26,287 - 42,442, and that mortality burdens in future will be substantially reduced, being lower by 31%, 35%, and 37% in 2030, 2040 and 2050 respectively (relative to 2018) assuming no population changes. Including population projections (increases in all regions for 30+ years age group) slightly offsets these health benefits, resulting in reductions of 25%, 27%, and 26% in mortality burdens for 2030, 2040, 2050 respectively. Significant reductions in future mortality burdens are estimated and, importantly for public health, the majority of benefits are achieved early on in the future timeline simulated, though further efforts are likely needed to reduce impacts of air pollution to health.

Ammonia mitigation campaign with smallholder farmers improves air quality while ensuring high cereal production.

Reducing cropland ammonia (NH3) emissions while improving air quality and food supply is a challenge, particularly in China where there are millions of smallholder farmers. We tested the effectiveness of a tailored nitrogen (N) management strategy applied to wheat-maize cropping systems in 'demonstration squares' across Quzhou County in the North China Plain. The N-management techniques included optimal N rates, deep fertilizer placement and application of urease inhibitors, implemented through cooperation between government, researchers, businesses and smallholders. Compared with conventional local smallholder practice, our NH3 mitigation campaign reduced NH3 volatilization from wheat and maize by 49% and 39%, and increased N-use efficiency by 28% and 40% and farmers' profitability by 25% and 19%, respectively, with no detriment to crop yields. County-wide atmospheric NH3 and fine particulate matter (with aerodynamic diameter <2.5 µm) concentrations decreased by 40% and 8%, respectively. County-wide net benefits were estimated at US$7.0 million. Our demonstration-square approach shows that cropland NH3 mitigation and improved air quality and farm profitability can be achieved simultaneously by coordinated actions at the county level.

Association between long-term exposure to air pollution and specific causes of mortality in Scotland.

OBJECTIVE: This study investigated the association between long-term exposure to black smoke (BS) air pollution and mortality in two related Scottish cohorts with 25 years of follow-up. METHODS: Risk factors were collected during 1970-1976 for 15331 and 6680 participants in the Renfrew/Paisley and Collaborative cohorts respectively. Exposure to BS during 1970-1979 was estimated by inverse-distance weighted averages of observed concentrations at monitoring sites and by two alternative spatial modelling approaches which included local air quality predictors (LAQP). RESULTS: Consistent BS-mortality associations (per 10 µg m(-3) increment in 10-year average BS) were observed in the Renfrew/Paisley cohort using LAQP-based exposure models (all-cause mortality HR 1.10 (95% CI 1.04 to 1.17); cardiovascular HR 1.11 (1.01 to 1.22); ischaemic heart disease HR 1.13 (1.02 to 1.25); respiratory HR 1.26 (1.02 to 1.28)). The associations were largely unaffected by additional adjustment for area-level deprivation category. A less consistent and generally implausible pattern of cause-specific BS-mortality associations was found for inverse-distance averaging of BS concentrations at nearby monitoring sites. BS-mortality associations in the Collaborative cohort were weaker and not statistically significant. CONCLUSIONS: The association between mortality and long-term exposure to BS observed in the Renfrew/Paisley cohort is consistent with hypotheses of how air pollution may affect human health. The dissimilarity in pollution-mortality associations for different exposure models highlights the critical importance of reliable estimation of exposures on intraurban spatial scales to avoid potential misclassification bias.

Integrating life cycle assessment and a farmer survey of management practices to study environmental impacts of peach production in Beijing, China.

While intensive peach production has expanded rapidly in recent years, few studies have explored the environmental impacts associated with specific regional systems or the optimal management strategies to minimize associated environmental risks. Here, data from a survey of 290 native farmers were used to conduct a life cycle assessment to quantify the acidification potential (AP), global warming potential (GWP), eutrophication potential (EP), and reactive nitrogen (Nr) losses in peach production in Pinggu District, Beijing. Total annual Nr losses, and GWP, AP, and EP values for peach production in Pinggu District were respectively 10.7 kg N t-1, 857 kg CO2-eq t-1, 12.9 kg SO2-eq t-1, and 4.1 kg PO4-eq t-1. The principal driving factors were fertilizer production, transportation, and application, which together accounted for 94%, 67%, 75%, and 94% of Nr losses, GWP, AP, and EP, respectively. In the high yield, high nitrogen-use efficiency (HH) group, relative values of Nr losses, GWP, AP, and EP were respectively 33%, 25%, 39%, and 32% lower than the overall averages for 290 orchards. Further analyses indicate that improved farming practices such as decreasing application rates of fertilizers, increasing proportion of base fertilization rate, and proper fertilization frequency in the HH group were the main reasons for these orchards' better performance in peach yields and partial factor productivity of nitrogen fertilizer, and their reduced environmental impacts. These results highlight the need to optimize nutrient management in peach production in order simultaneously to realize both environmental sustainability and high productivity in the peach production system.

Ozone, heat and mortality: acute effects in 15 British conurbations.

BACKGROUND: Acute associations between mortality and ozone are largely accepted, though recent evidence is less conclusive. Evidence on ozone-heat interaction is sparse. We assess effects of ozone, heat, and their interaction, on mortality in Britain. METHODS: Acute effects of summer ozone on mortality were estimated using data from 15 conurbations in England and Wales (May-September, 1993-2003). 2-day means of daily maximum 8-h ozone were entered into case series analyses, controlling for particulate matter with aerodynamic diameter of <10 µm, natural cubic splines of temperature, and other factors. Heat effects were estimated, comparing adjusted mortality rates at 97.5th and 75th percentiles of 2-day mean temperature. A separate model employed interaction terms to assess whether ozone effects increased on 'hot days' (where 2-day mean temperature exceeded the whole-year 95th percentile). Other heat metrics, and non-linear ozone effects, were also examined. RESULTS: Adverse ozone and heat effects occurred in nearly all conurbations. The mean mortality rate ratio for heat effect across conurbations was 1.071 (1.050-1.093). The mean ozone rate ratio was 1.003 per 10 µg/m(3) ozone increase (95% CI 1.001 to 1.005). On 'hot days' the mean ozone effect reached 1.006 (1.002-1.009) per 10 µg/m(3), though ozone-heat interaction was significant in London only. On substituting maximum for mean temperature, the overall ozone effect reduced to null, though evidence remained of effects on hot days, particularly in London. An estimated ozone effect threshold was below current guidelines in 'mean temperature' models. CONCLUSION: While heat showed robust effects on summer mortality, estimates for ozone depended upon the modelling of temperature. However, there was some evidence that ozone effects were worse on hot days, whichever temperature measure was used.

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.

The relationship between personal exposure and ambient PM2.5 and black carbon in Beijing.

This study is part of the "Air Polluion Impacts on Cardiopulmonary disease in Beijing: an integrated study of Exposure Science, Toxicologenomics & Environmental Epidemiology (APIC-ESTEE)" project under the UK-China joint research programme "Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-China)". The aim is to capture the spatio-temporal variability in people's exposure to fine particles (PM2.5) and black carbon (BC) air pollution in Beijing, China. A total of 120 students were recruited for a panel study from ten universities in Haidian District in northwestern Beijing from December 2017 to June 2018. Real-time personal concentrations of PM2.5 and BC were measured over a 24-h period with two research-grade portable personal exposure monitors. Personal microenvironments (MEs) were determined by applying an algorithm to the handheld GPS unit data. On average, the participants spent the most time indoors (79% in Residence and 16% in Workplace), and much less time travelling by Walking, Cycling, Bus and Metro. Similar patterns were observed across participant gender and body-mass index classifications. The participants were exposed to 33.8 ± 27.8 µg m-3 PM2.5 and to 1.9 ± 1.2 µg m-3 BC over the 24-h monitoring period, on average 24.3 µg m-3 (42%) and 0.8 µg m-3 (28%) lower, respectively, than the concurrent fixed-site ambient measurements. Relative differences between personal and ambient BC concentrations showed greater variability across the MEs, highlighting significant contributions from Dining and travelling by Bus, which involve potential combustion of fuels. This study demonstrates the potential value of personal exposure monitoring in investigating air pollution related health effects, and in evaluating the effectiveness of pollution control and intervention measures.

Current and future climate- and air pollution-mediated impacts on human health.

BACKGROUND: We describe a project to quantify the burden of heat and ozone on mortality in the UK, both for the present-day and under future emission scenarios. METHODS: Mortality burdens attributable to heat and ozone exposure are estimated by combination of climate-chemistry modelling and epidemiological risk assessment. Weather forecasting models (WRF) are used to simulate the driving meteorology for the EMEP4UK chemistry transport model at 5 km by 5 km horizontal resolution across the UK; the coupled WRF-EMEP4UK model is used to simulate daily surface temperature and ozone concentrations for the years 2003, 2005 and 2006, and for future emission scenarios. The outputs of these models are combined with evidence on the ozone-mortality and heat-mortality relationships derived from epidemiological analyses (time series regressions) of daily mortality in 15 UK conurbations, 1993-2003, to quantify present-day health burdens. RESULTS: During the August 2003 heatwave period, elevated ozone concentrations > 200 microg m-3 were measured at sites in London and elsewhere. This and other ozone photochemical episodes cause breaches of the UK air quality objective for ozone. Simulations performed with WRF-EMEP4UK reproduce the August 2003 heatwave temperatures and ozone concentrations. There remains day-to-day variability in the high ozone concentrations during the heatwave period, which on some days may be explained by ozone import from the European continent.Preliminary calculations using extended time series of spatially-resolved WRF-EMEP4UK model output suggest that in the summers (May to September) of 2003, 2005 & 2006 over 6000 deaths were attributable to ozone and around 5000 to heat in England and Wales. The regional variation in these deaths appears greater for heat-related than for ozone-related burdens.Changes in UK health burdens due to a range of future emission scenarios will be quantified. These future emissions scenarios span a range of possible futures from assuming current air quality legislation is fully implemented, to a more optimistic case with maximum feasible reductions, through to a more pessimistic case with continued strong economic growth and minimal implementation of air quality legislation. CONCLUSION: Elevated surface ozone concentrations during the 2003 heatwave period led to exceedences of the current UK air quality objective standards. A coupled climate-chemistry model is able to reproduce these temperature and ozone extremes. By combining model simulations of surface temperature and ozone with ozone-heat-mortality relationships derived from an epidemiological regression model, we estimate present-day and future health burdens across the UK. Future air quality legislation may need to consider the risk of increases in future heatwaves.

Quantifying the spatial and temporal variation of ground-level ozone in the rural Annapolis Valley, Nova Scotia, Canada using nitrite-impregnated passive samplers.

The spatiotemporal variability of ground-level ozone (GLO) in the rural Annapolis Valley, Nova Scotia was investigated between August 29, 2006, and September 28, 2007, using Ogawa nitrite-impregnated passive diffusion samplers (PS). A total of 353 PS measurements were made at 17 ambient and 1 indoor locations over 18 sampling periods ranging from 2 to 4 weeks. The calculated PS detection limit was 0.8 +/- 0.02 parts per billion by volume (ppbv), for a 14-day sampling period. Duplicate samplers were routinely deployed at three sites and these showed excellent agreement (R2 values of 0.88 [n = 11], 0.95 [n = 17], and 0.96 [n = 17]), giving an overall PS imprecision value of 5.4%. Comparisons between PS and automated continuous ozone analyzers at three sites also demonstrated excellent agreement with R2 values of 0.82, 0.95, and 0.95, and gradients not significantly different from unity. The minimum, maximum, and mean (+/- 1 sigma) ambient annual GLO concentrations observed were 7.7, 72.1, and 34.3 +/- 10.1 ppbv, respectively. The three highest sampling sites had significantly greater (P = 0.032) GLO concentrations than three Valley floor sites, and there was a strong correlation between concentration and elevation (R2 = 0.82). Multivariate models were used to parameterize the observed GLO concentrations in terms of prevailing meteorology at an elevated site found at Kejimkujik National Park and also at a site on the Valley floor. Validation of the multivariate models using 30 months of historical meteorological data at these sites yielded R2 values of 0.70 (elevated site) and 0.61 (Valley floor). The mean indoor ozone concentration was 5.4 +/- 3.3 ppbv and related to ambient GLO concentration by the equation: indoor = 0.34 x ambient - 5.07. This study has demonstrated the suitability of PS for long-term studies of GLO over a wide geographic area and the effect of topographical and meteorological influences on GLO in this region.

Using mass reconstruction along a four-site transect as a method to interpret PM10 in west-central Scotland, United Kingdom.

Concurrent 24-hr samples of particulate matter of median aerodynamic diameter less than 10 microm (PM10) were collected over a 10-day period in August 2000 at four sites along a transect in west-central Scotland, UK (passing from the coast through the city of Glasgow) in line with the prevailing southwesterly wind. Each sample was analyzed for chloride (Cl(-)), nitrate (NO3(-)), sulfate (SO4(2-)), ammonium (NH4(+)), calcium (Ca(2+)), iron (Fe), and organic hydrocarbon material (OHM). The contribution from elemental carbon (EC) was estimated. Sampling days were categorized according to local wind direction, synoptic flow, and air mass back trajectories. Chemical mass balance (CMB) reconstruction of the following PM10 components was derived for each wind direction group and at each transect location: ammonium sulfate ((NH4)2SO4), ammonium nitrate (NH4NO3), sodium chloride (NaCl), gypsum (CaSO4), OHM, EC, soil/surface dusts, and particle-bound water. The results showed that PM10 at the coastal site was dominated by the marine background (NaCl) compared with the urban sites, which were dominated by local primary (EC and soil/resuspension) and secondary sources (NH4NO3, (NH4)2SO4, and OHM). There was evidence of Cl(-) depletion as NaCl aerosol passes over urban areas. There was also evidence of long-range transport of primary PM10 (EC and OHM); for example, at the coastal site from transport from Ireland. The work demonstrates how the general approach of combining mass reconstruction along a transect with other information such as wind/air-mass direction generates insight into the sources contributing to PM10 over a more extended spatial scale than at a single receptor.