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Environmentally persistent free radicals (EPFRs) are an emerging class of environmental hazardous contaminants that extensively, stably exist in airborne particulate matter and pose harmful effects on human health. However, there was little research about the sources of EPFRs in actual atmospheric conditions. This study reported the occurrence, characteristics, and sources of EPFRs and polycyclic aromatic hydrocarbons (PAHs) in PM2.5 collected in Dalian, China. The concentrations of PM2.5-bound EPFRs ranged from 1.13 × 1013 to 8.97 × 1015 spins/m3 (mean value: 1.14 × 1015 spins/m3). Carbon-centered radicals and carbon-centered radicals with adjacent oxygen atoms were detected. The concentration of ∑PAHs ranged from 1.09 to 76.24 ng/m3, and PAHs with high molecular weight (HMW) were predominant species in PM2.5. Correlation of EPFRs with SO2, NO2, O3, and 12 kinds of PAHs indicated that both fuel (coal and biomass) combustion and photoreaction in atmosphere influenced the concentrations of EPFR. The positive matrix factorization (PMF) model results have shown that the primary sources contributed most of the EPFRs and those of secondary sources had a little proportion. Coal combustion (52.4%) was the primary contributor of EPFRs, followed by traffic emission (22.6%), industrial sources (9.6%), and secondary sources (9.2%) during the heating period, whereas industrial emission (39.2%) was the primary contributor, followed by coal combustion (38.1%), vehicular exhaust (23.5%), and secondary sources (9.6%) during the non-heating period. The finding of the present study provides an important evidence for further study on the formation mechanism of EPFRs in actual atmospheric to control the air pollution. [ABSTRACT FROM AUTHOR]