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Urban conurbations of East Africa are affected by harmful levels of air pollution. The paucity of local air quality networks and the absence of capacity to forecast air quality make difficult to quantify the real level of air pollution in this area. The chemistry-transport model CHIMERE has been coupled with the meteorological model WRF and used to simulate hourly concentrations of Particulate Matter PM2.5 for three East African urban conurbations: Addis Ababa in Ethiopia, Nairobi in Kenya, and Kampala in Uganda. Two existing emission inventories were combined to test the performance of CHIMERE as an air quality tool for a target monthly period of 2017 and the results compared against observed data from urban and rural sites. The results show that the model is able to reproduce hourly and daily temporal variability of aerosol concentrations close to observations both in urban and in rural environments. CHIMERE's performance as a tool for managing air quality was also assessed. The analysis demonstrated that despite the absence of high-resolution data and up-to-date biogenic and anthropogenic emissions, the model was able to reproduce 66-99% of the daily PM2.5 exceedances above the WHO 24-hour mean PM2.5 guideline (25 μg m-3) in the three cities. An analysis of the 24-hour mean levels of PM2.5 was also carried out for 17 constituencies in the vicinity of Nairobi. This showed that 47% of the constituencies in the area exhibited a low air quality index for PM2.5 in the unhealthy category for human health exposing between 10000 to 30000 people/km2 to harmful level of air contamination. [ABSTRACT FROM AUTHOR]

Nitrous acid, HONO, is a key net photolytic precursor to OH radicals in the atmospheric boundary later. As OH is the dominant atmospheric oxidant, driving the removal of many primary pollutants and the formation of secondary species, a quantitative understanding of HONO sources is important to predict atmospheric oxidising capacity. While a number of HONO formation mechanisms have been identified, recent work has ascribed significant importance to the dark, oceansurface mediated conversion of NO2 to HONO in the coastal marine boundary layer. In order to evaluate the role of this mechanism, here we analyse measurements of HONO and related species obtained at two contrasting coastal locations - Cape Verde (Atlantic Ocean), representative of the clean remote tropical marine boundary layer, and Weybourne (United Kingdom), representative of semi-polluted Northern European coastal waters. As expected, higher average concentrations of HONO (70 ppt) were observed in marine air for the more anthropogenically influenced Weybourne location compared to Cape Verde (HONO <5 ppt). At both sites, the approximately constant HONO/NO 2 ratio at night pointed to a low importance for the dark ocean-surface mediated conversion of NO2 into HONO, whereas the midday maximum in the HONO/NO2 ratios indicated significant contributions from photo-enhanced HONO formation mechanisms (or other sources). We obtained an upper limit to the rate coefficient of dark ocean-surface HONO-to-NO2 conversion of CHONO = 0.0011 ppb hr-1 from the Cape Verde observations; this is a factor of 5 lower than the slowest rate reported previously. These results point to significant geographical variation in the predominant HONO formation mechanisms in marine environments and indicate that caution is required when extrapolating the importance of such mechanisms from individual study locations to assess regional and/or global impacts on oxidising capacity. As a significant fraction of atmospheric processing occurs in the marine boundary layer, particularly in the tropics, better constraint of the possible ocean surface source of HONO is important for a quantitative understanding of chemical processing of primary trace gases in the global atmospheric boundary layer and associated impacts upon air pollution and climate. [ABSTRACT FROM AUTHOR]

New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially and this variability is yet to be fully understood. In the present study, long term particle size distribution datasets (minimum of three years) from thirteen sites of various land uses and climates from across Europe were studied and NPF events, deriving from secondary formation and not traffic related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides, underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found even at sites in close proximity (< 200 km) due to the different local conditions at each site. Region-wide events were also studied and were found to be associated with the same conditions as local events, although some variability was found which was associated with the different seasonality of the events at two neighbouring sites. NPF events were responsible for an increase in the number concentration of ultrafine particles of more than 400% at rural background sites on the day of their occurrence. The degree of enhancement was less at urban sites due to the increased contribution of other sources within the urban environment. It is evident that, while some variables (such as solar radiation intensity, relative humidity or the concentrations of specific pollutants) appear to have a similar influence on NPF events across all sites, it is impossible to predict the characteristics of NPF events at a site using just these variables, due to the crucial role of local conditions. [ABSTRACT FROM AUTHOR]

Measurements of atmospheric boundary layer nitrous acid (HONO) and nitrogen oxides (NOx) were performed in summer 2016 inside a city centre road tunnel in Birmingham, United Kingdom. HONO and NOx mixing ratios were strongly correlated with traffic density, with peak levels observed during the early evening rush hour as a result of traffic congestion in the tunnel. A daytime ΔHONO / ΔNOx ratio of 0.85 % (0.72–1.01 %, 95 % CI) was calculated using reduced major axis regression as the overall fleet-average (comprising 59 % diesel-fuelled vehicles). A comparison with previous tunnel studies and analysis on composition of the fleet suggest that goods-vehicles have a large impact on the overall HONO vehicle emissions; however, new technologies aimed at reducing exhaust emissions, particularly for diesel vehicles, may have reduced the overall direct HONO emission in the UK. This result suggests that in order to accurately represent urban atmospheric emissions and OH radical budget, fleet-weighted HONO / NOx ratios may better quantify HONO vehicle emissions in models, compared with use of a single emissions ratio for all vehicles. The contribution of the direct vehicular source of HONO to total ambient HONO concentrations is also investigated and results show that, in areas with high traffic density, vehicle exhaust emissions are likely to be the dominant HONO source to the boundary layer. [ABSTRACT FROM AUTHOR]

NPF events have different patterns of development depending on the conditions of the area in which they occur. In this study, NPF events occurring at three sites of differing characteristics (rural Harwell (HAR), urban background North Kensington (NK), urban roadside Marylebone Road (MR), London, UK) were studied (seven years of data). The different atmospheric conditions in each study area not only have an effect on the frequency of the events, but also affect their development. The frequency of NPF events is similar at the rural and urban background locations (about 7% of days), with a high proportion of events occurring at both sites on the same day (45%). The frequency of NPF events at the urban roadside site is slightly less (6% of days), and higher particle growth rates (average 5.5nmh−1 at MR compared to 3.4nmh−1 and 4.2nmh−1 at HAR and NK respectively) must result from rapid gas to particle conversion of traffic-generated pollutants. A general pattern is found in which the condensation sink increases with the degree of pollution of the site, but this is counteracted by increased particle growth rates at the more polluted location. A key finding of this study is that the role of the urban environment leads to an increment of 20% in N16–20nm in the urban background compared to that of the rural area in NPF events occurring at both sites. The relationship of the origin of incoming air masses is also considered and an association of regional events with cleaner air masses is found. Due to lower availability of condensable species, NPF events that are associated with cleaner atmospheric conditions have lower growth rates of the newly formed particles. The decisive effect of the condensation sink in the development of NPF events and the survivability of the newly formed particles is underlined, and influences the overall contribution of NPF events to the number of ultrafine particles in an area. The other key factor identified by this study is the important role that urban pollution plays in new particle formation events. [ABSTRACT FROM AUTHOR]

East African countries face an increasing threat from poor air quality, stemming from rapid urbanisation, population growth and a steep rise in fuel use and motorization rates. With few air quality monitoring systems available, this study provides the much needed high temporal resolution data to investigate the concentrations of particulate matter (PM) air pollution in Kenya. Calibrated low cost optical particle counters (OPCs) were deployed in Kenya in three locations: two in the capital of Nairobi and one in a rural location in the outskirts of Nanyuki, which is upwind of Nairobi. The two Nairobi sites consist of an urban background site and a roadside site. The instruments were composed of an Alphasense OPC-N2 optical particle counter (OPC) ran with a raspberry pi low cost microcomputer, packaged in a weather proof box. Measurements were conducted over a two-month period (February–March 2017) with an intensive study period when all measurements were active at all sites lasting two weeks. When collocated, the three OPC-N2 instruments demonstrated good inter-instrument precision with a coefficient of variance of 8.8 ± 2.0 % in the PM2.5 fraction. The low cost sensors had an absolute PM mass concentration calibration using a collocated gravimetric measurement at the urban background site in Nairobi. The mean daily PM1 mass concentration measured at the urban roadside, urban background and rural background sites were 23.9, 16.1, 8.8 µg m−3. The mean daily PM2.5 mass concentration measured at the urban roadside, urban background and rural background sites were 36.6, 24.8, 13.0 µg m−3. The mean daily PM10 mass concentration measured at the urban roadside, urban background and rural background sites were 93.7, 53.0, 19.5 µg m−3. The urban measurements in Nairobi showed that particulate matter concentrations regularly exceed WHO guidelines in both the PM10 and PM2.5 size ranges. Following a Lenschow type approach we can estimate the urban and roadside increments that are applicable to Nairobi. Median urban and roadside increments are 33.1 and 43.3 µg m−3 for PM10, respectively, the median urban and roadside increments are 7.1 and 18.3 µg m−3 for PM2.5, respectively, and the median urban and roadside increments are 4.7 and 12.6 µg m−3 for PM1, respectively. These increments highlight the importance of both the urban and roadside increments to urban air pollution in Nairobi. A clear diurnal behaviour in PM mass concentration was observed at both urban sites, which peaks during the morning and evening Nairobi rush hours; this was consistent with the high measured roadside increment indicating vehicular traffic being a dominant source of particulate matter in the city, accounting for approximately 48.1, 47.5, and 57.2 % of the total particulate matter loading in the PM10, PM2.5 and PM1 size ranges, respectively. Collocated meteorological measurements at the urban sites were collected, allowing for an understanding of the location of major sources of particulate matter at the two sites. The potential problems of using low cost sensors for PM measurement without gravimetric calibration available at all sites are discussed. This study shows that calibrated low cost sensors can be used successfully to measure air pollution in cities like Nairobi. It demonstrates that low cost sensors could be used to create an affordable and reliable network to monitor air quality in cities. [ABSTRACT FROM AUTHOR]

Reduced visibility is an indicator of poor air quality. Moreover, degradation in visibility can be hazardous to human safety; for example, low visibility can lead to road, rail, sea and air accidents. In this paper, we explore the combined influence of atmospheric aerosol particle and gas characteristics, and meteorology, on long-term visibility. We use visibility data from eight meteorological stations, situated in the UK, which have been running since the 1950s. The site locations include urban, rural and marine environments. Most stations show a long term trend of increasing visibility which is indicative of reductions in air pollution, especially in urban areas. Additionally, the visibility at all sites show a very clear dependence on relative humidity indicating the importance of aerosol hygroscopicity on the ability of aerosol particles to scatter radiation. The dependence of visibility on other meteorological parameters, such as wind speed and wind direction is also investigated. Most stations show long term increases in temperature which can be ascribed to either climate change, land-use changes (e.g. urban heat island effects) or a combination of both; the observed effect is greatest in urban areas. The impact of this temperature change upon local relative humidity is discussed. To explain the long term visibility trends and their dependence on meteorological conditions, the measured data were fitted to a newly developed light extinction model to generate predictions of historic aerosol and gas scattering and absorbing properties. In general, an excellent fit was achieved between measured and modelled visibility for all 8 sites. The model incorporates parameterizations of aerosol hygroscopicity, particle concentration, particle scattering, and particle and gas absorption. This new model should be applicable and is easily transferrable to other data sets worldwide. Hence, historical visibility data can be used to assess trends in aerosol particle properties. This approach may help constrain global model simulations which attempt to generate aerosol fields for time periods when observational data are scarce or non-existent. Both the measured visibility and the modelled aerosol properties reported in this paper highlight the success of the UK's Clean Air Act, which was passed in 1956, in cleaning the atmosphere of visibility reducing pollutants. [ABSTRACT FROM AUTHOR]

A chemical reaction chamber system has been developed for the processing of oleic acid aerosol particles with ozone under two relative humidity conditions: dry and humidified to 65% R.H.. The apparatus consists of an aerosol flow tube, in which the ozonolysis occurs, coupled to a scanning mobility particle sizer (SMPS) and an aerosol time-of-flight mass spectrometer (ATOFMS) which measure the evolving particle size and composition. Under both relative humidity conditions, ozonolysis results in a significant decrease in particle size and mass which is consistent with the formation of volatile products that partition from the particle to the gas phase. Mass spectra derived from the ATOFMS reveal the presence of the typically observed reaction products: azaleic acid, nonanal, oxononanoic acid and nonanoic acid, as well as a range of higher molecular weight products deriving from the reactions of reaction intermediates with oleic acid and its oxidation products. These include octanoic acid, and 9- and 10-oxooctadecanoic acid, as well as products of considerably higher molecular weight. Quantitative evaluation of product yields with the ATOFMS shows a marked dependence upon both particle size association (from 0.3 to 2.1 μm diameter) and relative humidity. Under dry conditions, the percentage residual oleic acid increases with increasing particle size, as does the percentage of higher molecular weight products, due to the poorer internal mixing of the larger particles. The main lower molecular weight products are nonanal and oxonononic acid. Under humidified conditions, the percentage unreacted oleic acid is greater, except in the smallest particle fraction, and oxononanoic acid dominates the product distribution, with little formation of high molecular weight products relative to the dry particles. It is postulated that water reacts with reactive intermediates, competing with the processes which produce high molecular weight products. Whilst the oleic acid model aerosol system is of limited relevance to complex internally mixed atmospheric aerosol, the generic findings presented in this paper give useful insights into the nature of heterogeneous chemical processes. [ABSTRACT FROM AUTHOR]

A chemical reaction chamber system has been developed for the processing of oleic acid aerosol particles with ozone under two relative humidity conditions: dry and humidified to 65% R.H. The apparatus consists of an aerosol flow tube, in which the ozonolysis occurs, coupled to a scanning mobility particle sizer (SMPS) and an aerosol time-of-flight mass spectrometer (ATOFMS) which measure the evolving particle size and composition. Under both relative humidity conditions, ozonolysis results in a significant decrease in particle size and mass which is consistent with the formation of volatile products that partition from the particle to the gas phase. Mass spectra derived from the ATOFMS reveal the presence of the typically observed reaction products: azaleic acid, nonanal, oxononanoic acid and nonanoic acid, as well as a range of higher molecular weight products deriving from the reactions of reaction intermediates with oleic acid and its oxidation products. These include octanoic acid, and 9- and 10-oxooctadecanoic acid, as well as products of considerably higher molecular weight. Quantitative evaluation of product yields with the ATOFMS shows a marked dependence upon both particle size association (from 0.3 to 2.1 µm diameter) and relative humidity. Under dry conditions, the percentage residual oleic acid increases with increasing particle size, as does the percentage of higher molecular weight products, due to the poorer internal mixing of the larger particles. The main lower molecular weight products are nonanal and oxonononic acid. Under humidified conditions, the percentage unreacted oleic acid is greater, except in the smallest particle fraction, and oxononanoic acid dominates the product distribution, with little formation of high molecular weight products relative to the dry particles. It is postulated that water reacts with reactive intermediates, competing with the processes which produce high molecular weight products. Whilst the oleic acid model aerosol system is of limited relevance to complex internally mixed atmospheric aerosol, the generic findings presented in this paper give useful insights into the nature of heterogeneous chemical processes. [ABSTRACT FROM AUTHOR]