Abstract. Humic-like substances (HULIS) are a mixture of high molecular weight, water-soluble organic compounds that are widely distributed in atmospheric aerosol. Their sources are rarely studied quantitatively. Biomass burning is generally accepted as a major primary source of ambient humic-like substances (HULIS) with additional secondary material formed in the atmosphere. However, the present study provides direct evidence that residential coal burning is also a significant source of ambient HULIS, especially in the heating season in northern China based on source measurements, ambient sampling and analysis, and apportionment with source-oriented CMAQ modeling. Emissions tests show that residential coal combustion produces 5 to 24 % of the emitted organic carbon (OC) as HULIS carbon (HULISc). Estimation of primary emissions of HULIS in Beijing indicated that residential biofuel and coal burning contribute about 70 % and 25 % of annual primary HULIS, respectively. Vehicle exhaust, industry, and power plants contributions are negligible. Average concentration of ambient HULIS was 7.5 μg/m3 in atmospheric PM2.5 in urban Beijing and HULIS exhibited obvious seasonal variations with the highest concentrations in winter. HULISc account for 7.2 % of PM2.5 mass, 24.5 % of OC, and 59.5 % of water-soluble organic carbon, respectively. HULIS are found to correlate well with K+, Cl−, sulfate, and secondary organic aerosol suggesting its sources include biomass burning, coal combustion and secondary aerosol formation. Source apportionment based on CMAQ modeling shows residential biofuel and coal burning, secondary formation are important annual sources of ambient HULIS, contributing 57.5 %, 12.3 %, and 25.8 %, respectively.
Reply to Hopke and Dai: The correlation between PM2.5 and combustion-derived water is unlikely driven by local residential coal combustion
