Abstract. The methanol extraction method was widely applied to isolate organic carbon(OC) from ambient aerosols, followed by measurements of brown carbon (BrC)absorption. However, undissolved OC fractions will lead to underestimatedBrC absorption. In this work, water, methanol (MeOH), MeOH / dichloromethane(MeOH / DCM, 1:1, v/v), MeOH / DCM (1:2, v/v), tetrahydrofuran (THF), andN,N-dimethylformamide (DMF) were tested for extraction efficiencies ofambient OC, and the light absorption of individual solvent extracts wasdetermined. Among the five solvents and solvent mixtures, DMF dissolved thehighest fractions of ambient OC (up to ∼95 %), followed byMeOH and MeOH / DCM mixtures (<90 %), and the DMF extracts hadsignificantly (p<0.05) higher light absorption than other solventextracts. This is because the OC fractions evaporating at highertemperatures (>280∘) are less soluble in MeOH(∼80 %) than in DMF (∼90 %) and containstronger light-absorbing chromophores. Moreover, the light absorption of DMFand MeOH extracts of collocated aerosol samples in Nanjing showed consistenttemporal variations in winter when biomass burning dominated BrC absorption, while the average light absorption of DMF extracts was more than 2 timesgreater than the MeOH extracts in late spring and summer. The average lightabsorption coefficient at 365 nm of DMF extracts was 30.7 % higher (p<0.01) than that of MeOH extracts. Source apportionment resultsindicated that the MeOH solubility of BrC associated with biomass burning,lubricating oil combustion, and coal combustion is similar to their DMFsolubility. The BrC linked with unburned fossil fuels and polymerizationprocesses of aerosol organics was less soluble in MeOH than in DMF, whichwas likely the main reason for the large difference in time series betweenMeOH and DMF extract absorption. These results highlight the importance oftesting different solvents to investigate the structures and lightabsorption of BrC, particularly for the low-volatility fraction potentiallyoriginating from non-combustion sources.
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Highly time-resolved characterization of carbonaceous aerosols using a two-wavelength Sunset thermal–optical carbon analyzer
Abstract. Carbonaceous aerosols have great influence on the air quality, human healthand climate change. Except for organic carbon (OC) and elemental carbon (EC), brown carbon (BrC) mainly originates from biomass burning as a group of OC, with strong absorption from the visible to near-ultravioletwavelengths, and makes a considerable contribution to global warming. Largenumbers of studies have reported long-term observation of OC and ECconcentrations throughout the world, but studies of BrC based on long-termobservations are rather limited. In this study, we established atwo-wavelength method (658 and 405 nm) applied in the Sunset thermal–optical carbon analyzer. Based on a 1-year observation, we firstly investigated the characteristics, meteorological impact and transport process of OC and EC. Since BrC absorbs light at 405 nm more effectively than 658 nm, we defined the enhanced concentrations (dEC = EC405 nm − EC658 nm) and gave the possibility of providing an indicator of BrC. The receptor model and MODIS fire information were used to identify the presence of BrC aerosols. Our results showed that the carbonaceous aerosol concentrations were the highest in winter and lowest in summer. Traffic emission was an important source of carbonaceous aerosols in Nanjing. Receptor model results showed that strong local emissions were found for OC and EC; however, dEC was significantly affected by regional or long-range transport.The dEC/OC and OC/EC ratios showed similar diurnal patterns, and the dEC/OC increased when the OC/EC ratios increased, indicating strong secondarysources or biomass burning contributions to dEC. A total of two biomass burning events both in summer and winter were analyzed, and the results showed that the dEC concentrations were obviously higher on biomass burning days; however, no similar levels of the OC and EC concentrations were found both in biomass burning days and normal days in summer, suggesting that biomass burning emissions made a great contribution to dEC, and the sources of OC and EC were more complicated. Large number of open fire counts from the northwestern and southwestern areas of the study site were observed in winter and significantly contributed to OC, EC and dEC. In addition, the nearby Yangtze River Deltaarea was one of the main potential source areas of dEC, suggesting thatanthropogenic emissions could also be important sources of dEC. The resultsproved that dEC can be an indicator of BrC on biomass burning days. Ourmodified two-wavelength instrument provided more information than thetraditional single-wavelength thermal–optical carbon analyzer and gave a new idea about the measurement of BrC; the application of dEC data needs to be further investigated.
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- Award ID(s):
- 1743401
- PAR ID:
- 10315318
- Date Published:
- Journal Name:
- Atmospheric Measurement Techniques
- Volume:
- 14
- Issue:
- 6
- ISSN:
- 1867-8548
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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