Abstract. 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 pre-monsoon 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 85 non-methane volatile organic compounds; NMVOC) were quantified at a semi-urban location near the center of the valley. Concentrations and ratios of NMVOC indicated that origins primarily from poorly-maintained vehicle emissions, biomass burning, and solvent/gasoline evaporation. During those two weeks, daily average PM2.5 concentrations ranged from 30 to 207 µg m−3, which exceeded the World Health Organization 24 hour guideline by factors of 1.2 to 8.3. On average, the non-water 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 (1230 ± 1153 ng m−3), 1,3,5-triphenylbenzene (0.8 ±0.5 ng m−3), cholesterol (3.0 ± 6.7 ng m−3), stigmastanol (1.4 ± 6.7 ng m−3), and cis-pinonic acid (4.5 ± 0.6 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 two of previous estimates, but relatively 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 for 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) 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.
Introduction and Application of the PMF Model to Estimate the Source Apportionment of PM2.5 at Various Sites
