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Traditional combustion devices and fuels such as charcoal, wood and biomass, are widely utilised in rural and urban households in Africa. Incomplete combustion can generate air pollutants which are of human toxicological importance, including polycyclic aromatic hydrocarbons (PAHs). In this study, portable multi-channel polydimethylsiloxane rubber traps were used to sample gas phase emissions from cooking devices used in urban and rural households in Bomet and Narok counties of Kenya. A wide range of total PAH concentrations was found in samples collected (0.82 – 173.69 µg/m 3 ), which could be attributed to the differences in fuel type, combustion device, climate, and nature of households. Wood combustion using the 3-stone device had the highest average total PAH concentration of ~71 µg/m 3 . Narok had higher indoor total gas phase PAH concentrations averaging 35.88 µg/m 3 in urban and 70.84 µg/m 3 in rural households, compared to Bomet county (2.91 µg/m 3 in urban and 9.09 µg/m 3 in rural households). Ambient total gas phase PAH concentrations were more similar (Narok: 1.26 – 6.28 µg/m 3 and Bomet: 2.44 – 6.30 µg/m 3 ). Although the 3-stone device and burning of wood accounted for higher PAH emissions, the charcoal burning jiko stove produced the highest toxic equivalence quotient. Monitoring of PAHs emitted by these cooking devices and fuels is critical to public health and sustainable pollution mitigation.

This study employed an onboard emission measurement system to measure the real-world emission factors of particulate matter (PM), particle-bound polycyclic aromatic hydrocarbons (PAHs), and gaseous air pollutants for different types of diesel-fueled non-road construction machines operated inside confined spaces within a brick manufacturing factory located in Taiwan. To the best knowledge of the authors, this is the first study that reports real-world PM, PAH, and gaseous pollutant emission factors for non-road engines in Taiwan. The mean real-world fuel-specific emission factors of PM, carbon monoxide, total hydrocarbons, and nitric oxide were 0.712–1.17, 8.27–17.9, 3.04–5.77, and 38.1–96.8 g/kg-fuel, respectively, for the test machines. Likewise, mean ΣPAHs emission factors ranged from 157 to 230 μg/kg-fuel for three types of test machines. Further, the average emission of particle-bound PAH per unit PM emission ranged from 213 to 384 μg-PAH/g-PM. Among the analyzed PAHs, the medium-molecular weight (3- and 4-ring) compounds contributed to the largest share of particle-bound PAH emissions. However, in terms of Benzo[a]pyrene equivalent (BaPeq) toxicity, the high-molecular weight (5- and 6-ring) PAHs were more important, as they had the highest BaPeq toxic emission factors. This study provides detailed composition and emission factors of particle-bound PAHs in non-road diesel construction machine emissions, which may be useful as a chemical fingerprint for source apportionment studies.

The pollutants emitted during meal preparation in restaurants deteriorate the air quality. Thus, it is an environmental issue that needs to be addressed, especially in areas where these activities are densely located. The purpose of this study is to examine the impact on air quality from commercial cooking activities by performing a qualitative and quantitative analysis of the related parameters. The area of interest is located in the southeastern Mediterranean (Greater Athens area in Greece). Due to the lack of the necessary activity information, a survey was conducted. Emissions from the fuel burnt during the cooking procedures were calculated and it was found that, overall, 940.1 tonnes are attributed to commercial cooking activities annually (generated by classical pollutants, heavy metals, particulates and polycyclic aromatic hydrocarbon emissions). Comparing the contribution of different sources to the pollutants emitted, it was found that commercial cooking is responsible for about 0.6%, 0.8% and 1.0% of the total CO, NOx and PM10 values. Cooking organic aerosol (COA) and volatile organic compound (VOC) emissions from grilled meat were also calculated, accounting for 724.9 tonnes and 37.1 tonnes, respectively. Monthly, daily and hourly profiles of the cooking activities were developed and emissions were spatially disaggregated, indicating the city center as the area with higher values. Numerical simulations were performed with the WRF/CAMx modeling system and the results revealed a contribution of about 6% to the total PM10 concentrations in the urban center, where the majority of restaurants are located.

Among the biogenic volatile organic compounds (BVOCs) emitted by plant foliage, isoprene is by far the most important in terms of both global emission and atmospheric impact. It is highly reactive in the air, and its degradation favours the generation of ozone (in the presence of NOx) and secondary organic aerosols. A critical aspect of BVOC emission modelling is the representation of land use and land cover (LULC). The current emission inventories are usually based on land cover maps that are either modelled and dynamic or satellite-based and static. In this study, we use the state-of-the-art Model of Emissions of Gases and Aerosols from Nature (MEGAN) model coupled with the canopy model MOHYCAN (Model for Hydrocarbon emissions by the CANopy) to generate and evaluate emission inventories relying on satellite-based LULC maps at annual time steps. To this purpose, we first intercompare the distribution and evolution (2001–2016) of tree coverage from three global satellite-based datasets, MODerate resolution Imaging Spectroradiometer (MODIS), ESA Climate Change Initiative Land Cover (ESA CCI-LC), and the Global Forest Watch (GFW), and from national inventories. Substantial differences are found between the datasets; e.g. the global areal coverage of trees ranges from 30 to 50×106 km2, with trends spanning from −0.26 to +0.03 % yr−1 between 2001 and 2016. At the national level, the increasing trends in forest cover reported by some national inventories (in particular for the US) are contradicted by all remotely sensed datasets. To a great extent, these discrepancies stem from the plurality of definitions of forest used. According to some local censuses, clear cut areas and seedling or young trees are classified as forest, while satellite-based mappings of trees rely on a minimum height. Three inventories of isoprene emissions are generated, differing only in their LULC datasets used as input: (i) the static distribution of the stand-alone version of MEGAN, (ii) the time-dependent MODIS land cover dataset, and (iii) the MODIS dataset modified to match the tree cover distribution from the GFW database. The mean annual isoprene emissions (350–520 Tg yr−1) span a wide range due to differences in tree distributions, especially in isoprene-rich regions. The impact of LULC changes is a mitigating effect ranging from 0.04 to 0.33 % yr−1 on the positive trends (0.94 % yr−1) mainly driven by temperature and solar radiation. This study highlights the uncertainty in spatial distributions of and temporal variability in isoprene associated with remotely sensed LULC datasets. The interannual variability in the emissions is evaluated against spaceborne observations of formaldehyde (HCHO), a major isoprene oxidation product, through simulations using the global chemistry transport model (CTM) IMAGESv2. A high correlation (R > 0.8) is found between the observed and simulated interannual variability in HCHO columns in most forested regions. The implementation of LULC change has little impact on this correlation due to the dominance of meteorology as a driver of short-term interannual variability. Nevertheless, the simulation accounting for the large tree cover declines of the GFW database over several regions, notably Indonesia and Mato Grosso in Brazil, provides the best agreement with the HCHO column trends observed by the Ozone Monitoring Instrument (OMI). Overall, our study indicates that the continuous tree cover fields at fine resolution provided by the GFW database are our preferred choice for constraining LULC (in combination with discrete LULC maps such as those of MODIS) in biogenic isoprene emission models.

The effect of fuel ethanol content (10, 85 and 100 %) on primary emissions and on subsequent secondary aerosol formation was investigated for a Euro 5 flex-fuel gasoline vehicle. Emissions were characterized during a New European Driving Cycle (NEDC) using a comprehensive set-up of high time-resolution instruments. A detailed chemical composition of the exhaust particulate matter (PM) was studied using a soot particle aerosol mass spectrometer (SP-AMS), and secondary aerosol formation was studied using a potential aerosol mass (PAM) chamber. For the primary gaseous compounds, an increase in total hydrocarbon emissions and a decrease in aromatic BTEX (benzene, toluene, ethylbenzene and xylenes) compounds was observed when the amount of ethanol in the fuel increased. In regard to particles, the largest primary particulate matter concentrations and potential for secondary particle formation was measured for the E10 fuel (10 % ethanol). As the ethanol content of the fuel increased, a significant decrease in the average primary particulate matter concentrations over the NEDC was found. The PM emissions were 0.45, 0.25 and 0.15 mg m−3 for E10, E85 and E100, respectively. Similarly, a clear decrease in secondary aerosol formation potential was observed with a larger contribution of ethanol in the fuel. The secondary-to-primary PM ratios were 13.4 and 1.5 for E10 and E85, respectively. For E100, a slight decrease in PM mass was observed after the PAM chamber, indicating that the PM produced by secondary aerosol formation was less than the PM lost through wall losses or the degradation of the primary organic aerosol (POA) in the chamber. For all fuel blends, the formed secondary aerosol consisted mostly of organic compounds. For E10, the contribution of organic compounds containing oxygen increased from 35 %, measured for primary organics, to 62 % after the PAM chamber. For E85, the contribution of organic compounds containing oxygen increased from 42 % (primary) to 57 % (after the PAM chamber), whereas for E100 the amount of oxidized organics remained the same (approximately 62 %) with the PAM chamber when compared to the primary emissions.

Particulate matter (PM), of which a significant fraction is comprised of secondary organic aerosols (SOA), has received considerable attention due to its health implications. In this study, the water-soluble oxidative potential (OPWS) of SOA generated from the photooxidation of biogenic and anthropogenic hydrocarbon precursors (isoprene, α-pinene, β-caryophyllene, pentadecane, m-xylene, and naphthalene) under different reaction conditions (RO2+ HO2 vs. RO2+ NO dominant, dry vs. humid) was characterized using dithiothreitol (DTT) consumption. The measured intrinsic OPWS-DTT values ranged from 9 to 205 pmol min−1 µg−1 and were highly dependent on the specific hydrocarbon precursor, with naphthalene and isoprene SOA generating the highest and lowest OPWS-DTT values, respectively. Humidity and RO2 fate affected OPWS-DTT in a hydrocarbon-specific manner, with naphthalene SOA exhibiting the most pronounced effects, likely due to the formation of nitroaromatics. Together, these results suggest that precursor identity may be more influential than reaction condition in determining SOA oxidative potential, demonstrating the importance of sources, such as incomplete combustion, to aerosol toxicity. In the context of other PM sources, all SOA systems, with the exception of naphthalene SOA, were less DTT active than ambient sources related to incomplete combustion, including diesel and gasoline combustion as well as biomass burning. Finally, naphthalene SOA was as DTT active as biomass burning aerosol, which was found to be the most DTT-active OA source in a previous ambient study. These results highlight a need to consider SOA contributions (particularly from anthropogenic hydrocarbons) to health effects in the context of hydrocarbon emissions, SOA yields, and other PM sources.

As formaldehyde (HCHO) is a high-yield product in the oxidation of most volatile organic compounds (VOCs) emitted by fires, vegetation, and anthropogenic activities, satellite observations of HCHO are well-suited to inform us on the spatial and temporal variability of the underlying VOC sources. The long record of space-based HCHO column observations from the Ozone Monitoring Instrument (OMI) is used to infer emission flux estimates from pyrogenic and biogenic volatile organic compounds (VOCs) on the global scale over 2005–2013. This is realized through the method of source inverse modeling, which consists in the optimization of emissions in a chemistry-transport model (CTM) in order to minimize the discrepancy between the observed and modeled HCHO columns. The top–down fluxes are derived in the global CTM IMAGESv2 by an iterative minimization algorithm based on the full adjoint of IMAGESv2, starting from a priori emission estimates provided by the newly released GFED4s (Global Fire Emission Database, version 4s) inventory for fires, and by the MEGAN-MOHYCAN inventory for isoprene emissions. The top–down fluxes are compared to two independent inventories for fire (GFAS and FINNv1.5) and isoprene emissions (MEGAN-MACC and GUESS-ES). The inversion indicates a moderate decrease (ca. 20 %) in the average annual global fire and isoprene emissions, from 2028 Tg C in the a priori to 1653 Tg C for burned biomass, and from 343 to 272 Tg for isoprene fluxes. Those estimates are acknowledged to depend on the accuracy of formaldehyde data, as well as on the assumed fire emission factors and the oxidation mechanisms leading to HCHO production. Strongly decreased top–down fire fluxes (30–50 %) are inferred in the peak fire season in Africa and during years with strong a priori fluxes associated with forest fires in Amazonia (in 2005, 2007, and 2010), bushfires in Australia (in 2006 and 2011), and peat burning in Indonesia (in 2006 and 2009), whereas generally increased fluxes are suggested in Indochina and during the 2007 fires in southern Europe. Moreover, changes in fire seasonal patterns are suggested; e.g., the seasonal amplitude is reduced over southeast Asia. In Africa, the inversion indicates increased fluxes due to agricultural fires and decreased maxima when natural fires are dominant. The top–down fire emissions are much better correlated with MODIS fire counts than the a priori inventory in regions with small and agricultural fires, indicating that the OMI-based inversion is well-suited to assess the associated emissions. Regarding biogenic sources, significant reductions in isoprene fluxes are inferred in tropical ecosystems (30–40 %), suggesting overestimated basal emission rates in those areas in the bottom–up inventory, whereas strongly positive isoprene emission updates are derived over semiarid and desert areas, especially in southern Africa and Australia. This finding suggests that the parameterization of the soil moisture stress used in MEGAN greatly exaggerates the flux reduction due to drought in those regions. The isoprene emission trends over 2005–2013 are often enhanced after optimization, with positive top–down trends in Siberia (4.2 % year−1) and eastern Europe (3.9 % year−1), likely reflecting forest expansion and warming temperatures, and negative trends in Amazonia (−2.1 % year−1), south China (−1 % year−1), the United States (−3.7 % year−1), and western Europe (−3.3 % year−1), which are generally corroborated by independent studies, yet their interpretation warrants further investigation.

Measurements of isoprene concentration and flux were made at a mixed deciduous forest in southern Canada during 1995 to characterize diel and seasonal emissions and thus deduce annual inventories. Isoprene inventories are necessary for inputs to modeling systems to study atmospheric chemistry and carbon budgets. Despite adequate environmental conditions to promote emissions, the onset of isoprene emission occurred two weeks after full leaf expansion, and two additional weeks were required for plants to emit isoprene at the maximum capacity. Such maximum isoprene emission was measured during July when canopy isoprene fluxes reached 40-60 nmol (isoprene)·m-2(ground area)·s-1. Isoprene emission precipitously declined in concert with autumnal leaf senescence, with fluxes reaching the detection limit before the forest became leafless. In addition to plant development controls on emissions, temperatures below 10⚬C strongly modulated isoprene emission. After plants were exposed to low temperatures, isoprene emission remained suppressed and did not correspondingly increase in the manner that temperature is known to influence isoprene biosynthesis. Using a one-dimensional model to vertically adjust temperature and visible solar radiation with depth in the canopy, coupled with a seasonally adjusted emission rate, we estimated that the forest produced 71 mmol isoprene/m2during 1995. For a deciduous forest with final leaf-area index of 4.1 and active isoprene biomass of 75 g (dry mass)/m2, on average such isoprene source accounted for 2% of the carbon fixed through photosynthesis. The percentage of carbon entering the atmosphere in the form of isoprene became as high as 10% during warm (>30⚬C) and dry conditions. The data set reported here demonstrates that constant emission rates are inadequate to characterize emission rates for the entire growing season. Improved isoprene-emission inventories can be achieved if emission factors are seasonally adjusted. In this study we adopted a method to express the emission rates as a function of degree days.

The growth of the smallest atmospheric particles to sizes at which they may act as seeds for cloud droplets is a key step linking aerosols to clouds and climate. A synthesis of research indicates that the mechanisms controlling this growth depend on the size of the growing particle. Aerosols have a strong, yet poorly quantified, effect on climate. The growth of the smallest atmospheric particles from diameters in the nanometre range to sizes at which they may act as seeds for cloud droplets is a key step linking aerosols to clouds and climate. In many environments, atmospheric nanoparticles grow by taking up organic compounds that are derived from biogenic hydrocarbon emissions. Several mechanisms may control this uptake. Condensation of low-volatility vapours and formation of organic salts probably dominate the very first steps of growth in particles close to 1 nm in diameter. As the particles grow further, formation of organic polymers and effects related to the phase of the particle probably become increasingly important. We suggest that dependence of particle growth mechanisms on particle size needs to be investigated more systematically.

The vertical columns of formaldehyde (HCHO) retrieved from two satellite instruments, the Global Ozone Monitoring Instrument-2 (GOME-2) on Metop-A and the Ozone Monitoring Instrument (OMI) on Aura, are used to constrain global emissions of HCHO precursors from open fires, vegetation and human activities in the year 2010. To this end, the emissions are varied and optimized using the adjoint model technique in the IMAGESv2 global CTM (chemical transport model) on a monthly basis and at the model resolution. Given the different local overpass times of GOME-2 (09:30 LT) and OMI (13:30 LT), the simulated diurnal cycle of HCHO columns is investigated and evaluated against ground-based optical measurements at seven sites in Europe, China and Africa. The modeled diurnal cycle exhibits large variability, reflecting competition between photochemistry and emission variations, with noon or early afternoon maxima at remote locations (oceans) and in regions dominated by anthropogenic emissions, late afternoon or evening maxima over fire scenes, and midday minima in isoprene-rich regions. The agreement between simulated and ground-based columns is generally better in summer (with a clear afternoon maximum at mid-latitude sites) than in winter, and the annually averaged ratio of afternoon to morning columns is slightly higher in the model (1.126) than in the ground-based measurements (1.043). The anthropogenic VOC (volatile organic compound) sources are found to be weakly constrained by the inversions on the global scale, mainly owing to their generally minor contribution to the HCHO columns, except over strongly polluted regions, like China. The OMI-based inversion yields total flux estimates over China close to the bottom-up inventory (24.6 vs. 25.5 TgVOC yr−1 in the a priori) with, however, pronounced increases in the northeast of China and reductions in the south. Lower fluxes are estimated based on GOME-2 HCHO columns (20.6 TgVOC yr−1), in particular over the northeast, likely reflecting mismatches between the observed and the modeled diurnal cycle in this region. The resulting biogenic and pyrogenic flux estimates from both optimizations generally show a good degree of consistency. A reduction of the global annual biogenic emissions of isoprene is derived, of 9 and 13 % according to GOME-2 and OMI, respectively, compared to the a priori estimate of 363 Tg in 2010. The reduction is largest (up to 25–40 %) in the Southeastern US, in accordance with earlier studies. The GOME-2 and OMI satellite columns suggest a global pyrogenic flux decrease by 36 and 33 %, respectively, compared to the GFEDv3 (Global Fire Emissions Database) inventory. This decrease is especially pronounced over tropical forests, such as in Amazonia, Thailand and Myanmar, and is supported by comparisons with CO observations from IASI (Infrared Atmospheric Sounding Interferometer). In contrast to these flux reductions, the emissions due to harvest waste burning are strongly enhanced over the northeastern China plain in June (by ca. 70 % in June according to OMI) as well as over Indochina in March. Sensitivity inversions showed robustness of the inferred estimates, which were found to lie within 7 % of the standard inversion results at the global scale.