Response to referees

Abstract

Naturally and anthropogenically emitted aerosols, which are determined by their physical and chemical properties, have an impact on both air quality and the radiative properties of the earth. An important source of atmospheric particulate matter (PM) in South Africa is household combustion for space heating and cooking, which predominantly occurs in low-income urban settlements. The aim of this study was to conduct a detailed size-resolved assessment of chemical characteristics of aerosols associated with household combustion through the collection of particulates in low-income urban settlements in South Africa in order to quantify the extent of the impacts of atmospheric pollution within these settlements. Outdoor (ambient) and indoor aerosols in different size fractions were collected during summer and winter in four low-income urban settlements located in the north-eastern interior on the South African Highveld. The mass concentration and chemical composition was determined for three size fractions, namely, PM1, PM2.5 and PM2.5-10. The highest concentrations of particulates were measured indoors with the highest mass concentration determined in the indoor PM2.5-10 (coarse) size fraction. However, the highest mass concentrations were determined in PM1 in all outdoor aerosol samples collected during winter and summer, as well as in indoor samples collected during summer. Significantly higher concentrations were determined for SO4−2 in outdoor and indoor particulates compared to other ionic species, with NH4+ and NO3− being the second most abundant. SO4−2 and NH4+ almost exclusively occurred in the PM1 size fraction, while NO3− was the major constituent in the larger size fractions. The highest SO4−2 levels were recorded for the winter and summer outdoor campaigns conducted at Zamdela, while NO3− and NH4+ concentrations were higher during the winter outdoor campaign. The combined concentrations of trace elements were higher for indoor particulates compared to outdoor aerosols, while the total trace element concentrations in PM1 were substantially higher than levels thereof in the two larger size fractions of particulates collected during all sampling campaigns. No distinct seasonal trend was observed for the concentrations of trace elements. Na, Ca and Cr had the highest concentrations in particulates collected during outdoor and indoor sampling campaigns. Ni concentrations in outdoor and indoor aerosols exceeded the annual average European standard PM1 collected during all sampling campaigns in low-income urban settlements had the highest organic- and elemental carbon (OC and EC) concentrations. The highest OC and EC levels were determined in PM1 collected during the winter indoor campaign. OC and EC concentrations were highest during winter, which can be attributed to changes in meteorological patterns and increased household combustion during winter. Low OC / EC ratios determined for particulates collected in low-income urban settlements are indicative of OC and EC being mainly associated with local sources of these species. OC concentrations determined in this study were an order of magnitude lower than OC concentrations determined for ambient aerosols collected in the north-eastern interior of South Africa, while similar EC levels were measured. According to estimated dust concentrations, it was indicated that dust is the major constituent in all size ranges of particulates collected in this study, while trace elements were the second most abundant. However, trace elements made the highest contribution to indoor PM1 and PM1-2.5 mass. Mass concentrations and chemical concentrations determined for aerosols collected in low-income settlements reflects the regional impacts of anthropogenic sources in the north-eastern interior of South Africa, as well as the influence of local sources.