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Black carbon (BC) is one important component contributing to global warming and its climate-related impacts strongly depend on mixing state. Previous observations at ground level indicated BC aging was at a fast rate in daytime with efficient photochemical reactions, while BC aging significantly weakened at night. Here we present evidences that BC aging still occurs efficiently at night in the residual layer (RL). The ratio of thickly coated refractory BC (rBC) in total rBC (f(BC)) increased from 51.3% at 00:00 LST to 61.5% at 07:00 LST at the CITIC station, which located in the RL at night, with an increasing rate of 1.4% per hour. Such an increasing rate was even higher than that during noontime (11:00 to 15:00 LST, 0.7% per hour). Similar trend also reflected in the coating thickness (Dp/Dc) of rBC particles, which increased from 1.52 at 00:00 LST to 1.63 at 07:00 LST. The aging of rBC in the RL at night enhances light absorption of rBC particles correspondingly; calculated absorption enhancement (E-abs) increased from 1.64 at 00:00 LST to 1.79 in at 07:00 LST. Further analysis indicated that the Eabs depends not only on the D-p/D-c of rBC particles, but also on its size. An increase in the size of rBC particles in polluted episode can also enhance the Eabs. Combined observations of development of boundary layer and pollutants at the CITIC station suggested that rBC particles were upwards transported in daytime and trapped in the RL at night, where they were aged efficiently. These results will improve our understanding on rBC aging in the atmosphere, and hence help to evaluate its radiative forcing.

期刊论文 2023-02-15 DOI: 10.1016/j.atmosenv.2022.119558 ISSN: 1352-2310

Due to the lack of black carbon (BC) measurement data in some cases, elemental carbon (EC) is often used as a surrogate of BC, with a simple assumption that they are interchangeable. Such assumption will inevitably lead to uncertainties in radiative forcing estimation and health impact assessment. In order to quantitatively and sys-tematically evaluate the relationship between BC and EC as well as factors responsible for their difference, 3-year collocated equivalent BC (eBC) and EC measurements with 1-h resolution were performed in Beijing, China continuously from 2016 to 2019. EBC concentration was measured by the multi-wavelength aethalometer (AE-33) based on optical analysis, while EC concentration was determined by semi-continuous OC/EC analyzer with thermal-optical method. The results showed that around 90% of eBC concentration was higher than that of EC, with average difference between eBC and EC as 1.21 mu g m(-3) (accounting for 33% of average eBC in Beijing). EBC and EC concentrations exhibited strong correlation (r = 0.90) during the whole study period, but the slopes (or eBC/EC ratio) and correlation coefficients varied across seasons (spring: 1.67 and 0.94; summer: 0.91 and 0.65; fall: 1.15 and 0.88; winter: 1.09 and 0.91, respectively). Based on the information from shell/core ratios by Single Particle Soot Photometer (SP2), source apportionment results by positive matrix factorization model, and chemical composition of PM2.5, the differences between eBC and EC concentrations were found to be primarily related to BC aging process and secondary components as evidenced by strong positive correlation with sec-ondary species (e.g., secondary organic carbon and nitrate). This study provided seasonal specific conversion factors of eBC and EC in Beijing and helpful reference for other areas, which will contribute new knowledge of carbonaceous aerosol and reduce uncertainty in assessing future climate change and health studies of BC.

期刊论文 2022-06-01 DOI: 10.1016/j.envres.2022.112791 ISSN: 0013-9351
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