Nepal Ambient Monitoring and Source Testing Experiment (NAMaSTE): Emissions of particulate matter and sulfur dioxide from vehicles and brick kilns and their impacts on air quality in the Kathmandu Valley, Nepal

Air pollution is one of the most pressing environmental issues in the Kathmandu Valley, where the capital city of Nepal is located. We estimated emissions from two of the major source types in the valley (vehicles and brick kilns) and analyzed the corresponding impacts on regional air quality. First, we estimated the on-road vehicle emissions in the valley using the International Vehicle Emissions (IVE) model with local emissions factors and the latest available data for vehicle registration. We also identified the locations of the brick kilns in the Kathmandu Valley and developed an emissions inventory for these kilns using emissions factors measured during the Nepal Ambient Monitoring and Source Testing Experiment (NAMaSTE) field campaign in April 2015. Our results indicate that the commonly used global emissions inventory, the Hemispheric Transport of Air Pollution (HTAP_v2.2), underestimates particulate matter emissions from vehicles in the Kathmandu Valley by a factor greater than 100. HTAP_v2.2 does not include the brick sector and we found that our sulfur dioxide (SO2) emissions estimates from brick kilns are comparable to 70 % of the total SO2 emissions considered in HTAP_v2.2. Next, we simulated air quality using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) for April 2015 based on three different emissions scenarios: HTAP only, HTAP with updated vehicle emissions, and HTAP with both updated vehicle and brick kilns emissions. Comparisons between simulated results and observations indicate that the model underestimates observed surface elemental carbon (EC) and SO2 concentrations under all emissions scenarios. However, our updated estimates of vehicle emissions significantly reduced model bias for EC, while updated emissions from brick kilns improved model performance in simulating SO2. These results highlight the importance of improving local emissions estimates for air quality modeling. We further find that model overestimation of surface wind leads to underestimated air pollutant concentrations in the Kathmandu Valley. Future work should focus on improving local emissions estimates for other major and underrepresented sources (e.g., crop residue burning and garbage burning) with a high spatial resolution, as well as the model\u27s boundary layer representation, to capture strong spatial gradients of air pollutant concentrations

A New Integer Linear Programming Formulation to the Inverse QSAR/QSPR for Acyclic Chemical Compounds Using Skeleton Trees

33rd International Conference on Industrial, Engineering and Other Applications of Applied Intelligent Systems, IEA/AIE 2020, Kitakyushu, Japan, September 22-25, 2020.Computer-aided drug design is one of important application areas of intelligent systems. Recently a novel method has been proposed for inverse QSAR/QSPR using both artificial neural networks (ANN) and mixed integer linear programming (MILP), where inverse QSAR/QSPR is a major approach for drug design. This method consists of two phases: In the first phase, a feature function f is defined so that each chemical compound G is converted into a vector f(G) of several descriptors of G, and a prediction function ψ is constructed with an ANN so that ψ(f(G)) takes a value nearly equal to a given chemical property π for many chemical compounds G in a data set. In the second phase, given a target value y∗ of the chemical property π , a chemical structure G∗ is inferred in the following way. An MILP M is formulated so that M admits a feasible solution (x∗, y∗) if and only if there exist vectors x∗, y∗ and a chemical compound G∗ such that ψ(x∗)=y∗ and f(G∗)=x∗. The method has been implemented for inferring acyclic chemical compounds. In this paper, we propose a new MILP for inferring acyclic chemical compounds by introducing a novel concept, skeleton tree, and conducted computational experiments. The results suggest that the proposed method outperforms the existing method when the diameter of graphs is up to around 6 to 8. For an instance for inferring acyclic chemical compounds with 38 non-hydrogen atoms from C, O and S and diameter 6, our method was 5×104 times faster

Ambient air quality in the Kathmandu Valley, Nepal, during the pre-monsoon: Concentrations and sources of particulate matter and trace gases

The Kathmandu Valley in Nepal is a bowl-shaped urban basin that experiences severe air pollution that poses health risks to its 3.5 million inhabitants. As part of the Nepal Ambient Monitoring and Source Testing Experiment (NAMaSTE), ambient air quality in the Kathmandu Valley was investigated from 11 to 24 April 2015, during the premonsoon season. Ambient concentrations of fine and coarse particulate matter (PM2:5 and PM10, respectively), online PM1, inorganic trace gases (NH3, HNO3, SO2, and HCl), and carbon-containing gases (CO2, CO, CH4, and 93 nonmethane volatile organic compounds; NMVOCs) were quantified at a semi-urban location near the center of the valley. Concentrations and ratios of NMVOC indicated origins primarily from poorly maintained vehicle emissions, biomass burning, and solvent/gasoline evaporation. During those 2 weeks, daily average PM2:5 concentrations ranged from 30 to 207 μ g m-3, which exceeded the World Health Organization 24 h guideline by factors of 1.2 to 8.3. On average, the nonwater mass of PM2:5 was composed of organic matter (48 %), elemental carbon (13 %), sulfate (16 %), nitrate (4 %), ammonium (9 %), chloride (2 %), calcium (1 %), magnesium (0.05 %), and potassium (1 %). Large diurnal variability in temperature and relative humidity drove corresponding variability in aerosol liquid water content, the gas-aerosol phase partitioning of NH3, HNO3, and HCl, and aerosol solution pH. The observed levels of gas-phase halogens suggest that multiphase halogen-radical chemistry involving both Cl and Br impacted regional air quality. To gain insight into the origins of organic carbon (OC), molecular markers for primary and secondary sources were quantified. Levoglucosan (averaging 1230±1154 ng m-3), 1,3,5-triphenylbenzene (0:8± 0:6 ng m-3), cholesterol (2:9±6:6 ng m-3), stigmastanol (1.0 ±0:8 ng m-3), and cis-pinonic acid (4:5 ± 1:9 ng m-3) indicate contributions from biomass burning, garbage burning, food cooking, cow dung burning, and monoterpene secondary organic aerosol, respectively. Drawing on source profiles developed in NAMaSTE, chemical mass balance (CMB) source apportionment modeling was used to estimate contributions to OC from major primary sources including garbage burning (18 ± 5 %), biomass burning (17 ± 10 %) inclusive of open burning and biomass-fueled cooking stoves, and internal-combustion (gasoline and diesel) engines (18±9 %). Model sensitivity tests with newly developed source profiles indicated contributions from biomass burning within a factor of 2 of previous estimates but greater contributions from garbage burning (up to three times), indicating large potential impacts of garbage burning on regional air quality and the need for further evaluation of this source. Contributions of secondary organic carbon (SOC) to PM2:5 OC included those originating from anthropogenic precursors such as naphthalene (10 ± 4 %) and methylnaphthalene (0:3 ± 0:1 %) and biogenic precursors for monoterpenes (0:13 ± 0:07 %) and sesquiterpenes (5 ± 2 %). An average of 25 % of the PM2.5 OC was unapportioned, indicating the presence of additional sources (e.g., evaporative and/or industrial emissions such as brick kilns, food cooking, and other types of SOC) and/or underestimation of the contributions from the identified source types. The source apportionment results indicate that anthropogenic combustion sources (including biomass burning, garbage burning, and fossil fuel combustion) were the greatest contributors to PM2:5 and, as such, should be considered primary targets for controlling ambient PM pollution

Variations in surface ozone and carbon monoxide in the Kathmandu Valley and surrounding broader regions during SusKat-ABC field campaign: role of local and regional sources

Air pollution resulting from rapid urbanization and associated human activities in the Kathmandu Valley of Nepal has been leading to serious public health concerns over the past 2 decades. These concerns led to a multinational field campaign SusKat-ABC (Sustainable atmosphere for the Kathmandu Valley – Atmospheric Brown Clouds) that measured different trace gases, aerosols and meteorological parameters in the Kathmandu Valley and surrounding regions during December 2012 to June 2013 to understand local- to regional-scale processes influencing air quality of the Kathmandu Valley. This study provides information about the regional distribution of ozone and some precursor gases using simultaneous in situ measurements from a SusKat-ABC supersite at Bode, Nepal, and two Indian sites: a high-altitude site, Nainital, located in the central Himalayan region and a low-altitude site, Pantnagar, located in the Indo-Gangetic Plain (IGP). The diurnal variations at Bode showed a daytime buildup in O3 while CO shows morning and evening peaks. Similar variations (with lower levels) were also observed at Pantnagar but not at Nainital. Several events of hourly ozone levels exceeding 80&thinsp;ppbv were also observed at Bode. The CO levels showed a decrease from their peak level of about 2000&thinsp;ppbv in January to about 680&thinsp;ppbv in June at Bode. The hourly mean ozone and CO levels showed a strong negative correlation during winter (r2 = 0.82 in January and r2 = 0.71 in February), but this negative correlation gradually becomes weaker, with the lowest value in May (r2 = 0.12). The background O3 and CO mixing ratios at Bode were estimated to be about 14 and 325&thinsp;ppbv, respectively. The rate of change of ozone at Bode showed a more rapid increase ( ∼ 17&thinsp;ppbv&thinsp;h−1) during morning than the decrease in the evening (5–6&thinsp;ppbv&thinsp;h−1), suggesting the prevalence of a semi-urban environ. The lower CO levels during spring suggest that regional transport also contributes appreciably to springtime ozone enhancement in the Kathmandu Valley on top of the local in situ ozone production. We show that regional pollution resulting from agricultural crop residue burning in northwestern IGP led to simultaneous increases in O3 and CO levels at Bode and Nainital during the first week of May 2013. A biomass-burning-induced increase in ozone and related gases was also confirmed by a global model and balloon-borne observations over Nainital. A comparison of surface ozone variations and composition of light non-methane hydrocarbons among different sites indicated the differences in emission sources of the Kathmandu Valley and the IGP. These results highlight that it is important to consider regional sources in air quality management of the Kathmandu Valley.</p

The impact of residential combustion emissions on atmospheric aerosol, human health, and climate

Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5) concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (>30 years of age) premature mortality (due to both cardiopulmonary disease and lung cancer) to be 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000–827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50% of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between −66 and +21 mW m−2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m−2, which is sensitive to the assumed size distribution of carbonaceous emissions. Overall, our results demonstrate that reducing residential combustion emissions would have substantial benefits for human health through reductions in ambient PM2.5 concentrations

Source apportionment of NMVOCs in the Kathmandu Valley during the SusKat-ABC international field campaign using positive matrix factorization

A positive matrix factorization model (US EPA PMF version 5.0) was applied for the source apportionment of the dataset of 37 non-methane volatile organic compounds (NMVOCs) measured from 19 December 2012 to 30 January 2013 during the SusKat-ABC international air pollution measurement campaign using a proton-transfer-reaction time-of-flight mass spectrometer in the Kathmandu Valley. In all, eight source categories were identified with the PMF model using the new constrained model operation mode. Unresolved industrial emissions and traffic source factors were the major contributors to the total measured NMVOC mass loading (17.9 and 16.8 %, respectively) followed by mixed industrial emissions (14.0 %), while the remainder of the source was split approximately evenly between residential biofuel use and waste disposal (10.9 %), solvent evaporation (10.8 %), biomass co-fired brick kilns (10.4 %), biogenic emissions (10.0 %) and mixed daytime factor (9.2 %). Conditional probability function (CPF) analyses were performed to identify the physical locations associated with different sources. Source contributions to individual NMVOCs showed that biomass co-fired brick kilns significantly contribute to the elevated concentrations of several health relevant NMVOCs such as benzene. Despite the highly polluted conditions, biogenic emissions had the largest contribution (24.2 %) to the total daytime ozone production potential, even in winter, followed by solvent evaporation (20.2 %), traffic (15.0 %) and unresolved industrial emissions (14.3 %). Secondary organic aerosol (SOA) production had approximately equal contributions from biomass co-fired brick kilns (28.9 %) and traffic (28.2 %). Comparison of PMF results based on the in situ data versus REAS v2.1 and EDGAR v4.2 emission inventories showed that both the inventories underestimate the contribution of traffic and do not take the contribution of brick kilns into account. In addition, the REAS inventory overestimates the contribution of residential biofuel use and underestimates the contribution of solvent use and industrial sources in the Kathmandu Valley. The quantitative source apportionment of major NMVOC sources in the Kathmandu Valley based on this study will aid in improving hitherto largely un-validated bottom-up NMVOC emission inventories, enabling more focused mitigation measures and improved parameterizations in chemical transport models

Overview of VOC emissions and chemistry from PTR-TOF-MS measurements during the SusKat-ABC campaign: high acetaldehyde, isoprene and isocyanic acid in wintertime air of the Kathmandu Valley

The Kathmandu Valley in Nepal suffers from severe wintertime air pollution. Volatile organic compounds (VOCs) are key constituents of air pollution, though their specific role in the valley is poorly understood due to insufficient data. During the SusKat-ABC (Sustainable Atmosphere for the Kathmandu Valley–Atmospheric Brown Clouds) field campaign conducted in Nepal in the winter of 2012&ndash;2013, a comprehensive study was carried out to characterise the chemical composition of ambient Kathmandu air, including the determination of speciated VOCs, by deploying a proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) &ndash; the first such deployment in South Asia. In the study, 71 ion peaks (for which measured ambient concentrations exceeded the 2<i>σ</i> detection limit) were detected in the PTR-TOF-MS mass scan data, highlighting the chemical complexity of ambient air in the valley. Of the 71 species, 37 were found to have campaign average concentrations greater than 200 ppt and were identified based on their spectral characteristics, ambient diel profiles and correlation with specific emission tracers as a result of the high mass resolution (<i>m</i> ∕ Δ<i>m</i>  &gt;  4200) and temporal resolution (1 min) of the PTR-TOF-MS. The concentration ranking in the average VOC mixing ratios during our wintertime deployment was acetaldehyde (8.8 ppb)  &gt;  methanol (7.4 ppb)  &gt;  acetone + propanal (4.2 ppb)  &gt;  benzene (2.7 ppb)  &gt;  toluene (1.5 ppb)  &gt;  isoprene (1.1 ppb)  &gt;  acetonitrile (1.1 ppb)  &gt;  C8-aromatics ( ∼ 1 ppb)  &gt;  furan ( ∼ 0.5 ppb)  &gt;  C9-aromatics (0.4 ppb). Distinct diel profiles were observed for the nominal isobaric compounds isoprene (<i>m</i> ∕ <i>z</i>  =  69.070) and furan (<i>m</i> ∕ <i>z</i>  =  69.033). Comparison with wintertime measurements from several locations elsewhere in the world showed mixing ratios of acetaldehyde ( ∼  9 ppb), acetonitrile ( ∼  1 ppb) and isoprene ( ∼  1 ppb) to be among the highest reported to date. Two "new" ambient compounds, namely formamide (<i>m</i> ∕ <i>z</i>  =  46.029) and acetamide (<i>m</i> ∕ <i>z</i>  =  60.051), which can photochemically produce isocyanic acid in the atmosphere, are reported in this study along with nitromethane (a tracer for diesel exhaust), which has only recently been detected in ambient studies. Two distinct periods were selected during the campaign for detailed analysis: the first was associated with high wintertime emissions of biogenic isoprene and the second with elevated levels of ambient acetonitrile, benzene and isocyanic acid from biomass burning activities. Emissions from biomass burning and biomass co-fired brick kilns were found to be the dominant sources for compounds such as propyne, propene, benzene and propanenitrile, which correlated strongly with acetonitrile (<i>r</i>² &gt; 0.7), a chemical tracer for biomass burning. The calculated total VOC OH reactivity was dominated by acetaldehyde (24.0 %), isoprene (20.2 %) and propene (18.7 %), while oxygenated VOCs and isoprene collectively contributed to more than 68 % of the total ozone production potential. Based on known secondary organic aerosol (SOA) yields and measured ambient concentrations in the Kathmandu Valley, the relative SOA production potential of VOCs were benzene  &gt;  naphthalene  &gt;  toluene  &gt;  xylenes  &gt;  monoterpenes  &gt;  trimethylbenzenes  &gt;  styrene  &gt;  isoprene. The first ambient measurements from any site in South Asia of compounds with significant health effects such as isocyanic acid, formamide, acetamide, naphthalene and nitromethane have been reported in this study. Our results suggest that mitigation of intense wintertime biomass burning activities, in particular point sources such biomass co-fired brick kilns, would be important to reduce the emission and formation of toxic VOCs (such as benzene and isocyanic acid) in the Kathmandu Valley

The seasonal cycle of the mixing layer height and its impact on black carbon concentrations in the Kathmandu Valley (Nepal)

The properties and the vertical structure of the mixing layer as part of the planetary boundary layer are of key importance for local air quality. They have a substantial impact on the vertical dispersion of pollutants in the lower atmosphere and thus on their concentrations near the surface. In this study, ceilometer measurements taken within the framework of the SusKat project (Sustainable Atmosphere for the Kathmandu Valley) are used to investigate the mixing layer height in the Kathmandu Valley, Nepal. The applied method is based on the assumption that the aerosol concentration is nearly constant in the vertical and distinctly higher within the mixing layer than in the air above. Thus, the height with the steepest gradient within the ceilometer backscatter profile marks the top of the mixing layer. Ceilometer and black carbon (BC) measurements conducted from March 2013 through February 2014 provide a unique and important dataset for the analysis of the meteorological and air quality conditions in the Kathmandu Valley. In this study the mean diurnal cycle of the mixing layer height in the Kathmandu Valley for each season (pre- monsoon, monsoon, post-monsoon and winter season) and its dependency on the meteorological situation is in- vestigated. In addition, the impact of the mixing layer height on the BC concentration is analyzed and compared to the relevance of other important processes such as emissions, horizontal advection and deposition. In all seasons the diurnal cycle is typically characterized by low mixing heights during the night, gradually increas- ing after sun rise reaching to maximum values in the afternoon before decreasing again. Seasonal differences can be seen particularly in the height of the mixing layer, e.g. from on average 153/1200 m (pre-monsoon) to 241/755 m (monsoon season) during the night/day, and the duration of enhanced mixing layer heights during daytime (around 12 hours (pre-monsoon season) to 8 hours (winter)). During the monsoon season, the observed diurnal cycle typ- ically shows the lowest amplitude and the lowest mixing height during the day and the highest in the night and morning hours of all seasons. These characteristics can mainly be explained with frequently present clouds and the associated lack of incoming solar radiation and outgoing longwave radiation. In general there is a clear anti-correlation of the BC concentration and the mixing layer height although this relation is less pronounced in the monsoon season. The shape and magnitude of the BC diurnal cycle differs between the seasons (e.g., daily maximum concentration from around 6 to 50 μg/m3 depending on the season). This is partly due to the different meteorological conditions including the mixing layer height but also caused by the different (seasonal and diurnal) time profiles of the main emission sources. From late December to April, for instance, brick kilns are major emitters of black carbon. The brick kilns emit continuously throughout the day whereas in the other months sources with more pronounced diurnal cycles, such as traffic and cooking activities, are dominating the total emissions

Wintertime aerosol optical and radiative properties in the Kathmandu Valley during the SusKat-ABC field campaign

Particulate air pollution in the Kathmandu Valley has reached severe levels that are mainly due to uncontrolled emissions and the location of the urban area in a bowl-shaped basin with associated local wind circulations. The AERONET measurements from December 2012 to August 2014 revealed a mean aerosol optical depth (AOD) of approximately 0.30 at 675 nm during winter, which is similar to that of the post-monsoon but half of that of the pre-monsoon AOD (0.63). The distinct seasonal variations are closely related to regional-scale monsoon circulations over South Asia and emissions in the Kathmandu Valley. During the SusKat-ABC campaign (December 2012&ndash;February 2013), a noticeable increase in both aerosol scattering (σs; 313  →  577 Mm−1 at 550 nm) and absorption (σa; 98  →  145 Mm−1 at 520 nm) coefficients occurred before and after 4 January 2013. This can be attributed to the increase in wood-burned fires due to a temperature drop and the start of firing at nearby brick kilns. The σs value in the Kathmandu Valley was a factor of 0.5 lower than that in polluted cities in India. The σa value in the Kathmandu Valley was approximately 2 times higher than that at severely polluted urban sites in India. The aerosol mass scattering efficiency of 2.6 m2 g−1 from PM10 measurements in the Kathmandu Valley is similar to that reported in urban areas. However, the aerosol mass absorption efficiency was determined to be 11 m2 g−1 from PM10 measurements, which is higher than that reported in the literature for pure soot particles (7.5 ± 1.2 m2 g−1). This might be due to the fact that most of the carbonaceous aerosols in the Kathmandu Valley were thought to be mostly externally mixed with other aerosols under dry conditions due to a short travel time from their sources. The σs and σa values and the equivalent black carbon (EBC) mass concentration reached up to 757 Mm−1, 224 Mm−1, and 29 µg m−3 at 08:00 LST (local standard time), respectively but decreased dramatically during the daytime (09:00&ndash;18:00 LST), to one-quarter of the morning average (06:00&ndash;09:00 LST) due to the development of valley winds and an atmospheric bounder layer. The σs and σa values and the EBC concentration remained almost constant during the night at the levels of 410 Mm−1, 130 Mm−1, and 17 µg m−3, respectively. The average aerosol direct radiative forcings over the intensive measurement period were estimated to be −6.9 ± 1.4 W m−2 (top of the atmosphere) and −20.8 ± 4.6 W m−2 (surface). Therefore, the high atmospheric forcing (i.e., 13.9 ± 3.6 W m−2) and forcing efficiency (74.8 ± 24.2 W m−2 τ−1) can be attributed to the high portion of light-absorbing aerosols in the Kathmandu Valley, as indicated by the high black carbon (or elemental carbon) to sulphate ratio (1.5 ± 1.1)