On the fossil and non-fossil fuel sources of carbonaceous aerosol with radiocarbon and AMS-PMF methods during winter hazy days in a rural area of North China plain

Regional transport is a key source of carbonaceous aerosol in many Chinese megacities including Beijing. The sources of carbonaceous aerosol in urban areas have been studied extensively but are poorly known in upwind rural areas. This work aims to quantify the contributions of fossil and non-fossil fuel emissions to carbonaceous aerosols at a rural site in North China Plain in winter 2016. We integrated online high resolution-time of flight-aerosol mass spectrometer (HR-TOF-AMS) observations and radiocarbon (C-14) measurements of fine particles with Positive Matrix Factorization (PMF) analysis as well as Extended Gelencser (EG) method. We found that fine particle concentration is much higher at the rural site than in Beijing during the campaign (Dec 7, 2016 to Jan 8, 2017). PMF analysis of the AMS data showed that coal-combustion related organic aerosol (CCOA + Oxidized CCOA) and more oxidized oxygenated organic aerosol (MO-OOA) contributed 48% and 30% of organic matter to non-refractory PM1 (NR-PM1) mass. About 2/3 of the OC and EC were from fossil-fuel combustion. The EG method, combining AMS-PMF and C-14 data, showed that primary and secondary OC from fossil fuel contribute 35% and 22% to total carbon (TC), coal combustion emission dominates the fossil fuel sources, and biomass burning accounted for 21% of carbonaceous aerosol. In summary, our results confirm that fossil fuel combustion was the dominant source of carbonaceous aerosol during heavy pollution events in the rural areas. Significant emissions of solid fuel carbonaceous aerosols at rural areas can affect air quality in downwind cities such as Beijing and Tianjin, highlighting the benefits of energy transition from solid fuels to cleaner energy in rural areas.