The goals of the “dual carbon” program in China are to implement a series of air pollution policies to reduce the emission of carbon-bearing particulate matter (PM). Following improvements in the reduction in carbon emissions in Handan City, China, fine particulate matter (PM2.5) was collected in the winters from 2016 to 2020 to characterize the concentrations and sources of carbonaceous components in PM2.5. Trend analysis revealed that both organic carbon (OC) and elemental carbon (EC) concentrations significantly decreased. The proportion of total carbon aerosol (TCA) in PM2.5 decreased by 47.0%, highlighting the effective reduction in carbon emissions. Secondary organic carbon (SOC) concentrations increased from 2016 (12.86 ± 14.10 μg·m−3) to 2018 (36.76 ± 21.59 μg·m−3) and then declined gradually. SOC/OC was larger than 67.0% from 2018 to 2020, implying that more effective synergistic emission reduction measures for carbonaceous aerosol and volatile organic compounds (VOCs) were needed. In the winters from 2016 to 2020, primary organic carbon (POC) concentrations reduced by 76.1% and 87.6% under a light/moderate pollution period (LP) and heavy/severe pollution periods (HPs), respectively. The TCA/PM2.5 showed a decreasing trend under LP and HP conditions, decreasing by 42.1% and 54.7%, respectively. Source analysis revealed that carbonaceous components were mainly from biomass burning, coal combustion and automotive exhaust emissions in the winters of 2016 and 2020. OC/EC and K+/EC analysis pointed out that air pollutant reduction measurements should focus on rectification biomass fuels in the next stage. Compared with 2016, the contributions of automotive exhaust emissions decreased in 2020. OC and EC concentrations decreased due to control measures on automotive exhaust emissions.
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