Elemental carbon (EC), also known as black carbon, plays an important role in climate change. Accurately assessing EC concentration in aerosols remains challenging due to the overestimations caused by carbonates and organic carbon (OC) during thermal-optical measurement in the Tibetan Plateau (TP). This study evaluates the extent of EC overestimated by carbonates and OC at four remote sites (Nyalamu, Lulang, Everest and Ngari) in southern and western of the TP using different treatments. The average overestimation of EC concentration due to acid treatment was consistent across all sites (25.5 f 2.4 %). After correction, the proportion of EC overestimated by carbonates were approximately 8.5 f 7.3 %, 12.3 f 6.9 %, 18.1 f 11.8 % and 22.7 f 13.3 %, respectively, revealing an increasing trend from humid to arid regions. Methanol-soluble OC (MSOC) concentrations were significantly correlated with the reduction of EC concentrations, indicating that the methanol extraction effectively mitigates EC overestimation. Seasonal variation of carbonaceous aerosol concentrations was significantly affected by sources from South Asia. Despite the variations in climate and aerosol sources, the average overestimations of measured EC concentration by carbonates and OC were similar at Nyalamu (49.4 f 14.0 %), Lulang (47.8 f 8.4 %), Everest (48.7 f 15.9 %) and Ngari (49.3 f 13.7 %) sites. Therefore, the actual EC concentrations were only about 51.2 f 13.1 % of the original values. This estimation will significantly enhance the contribution of brown carbon (BrC) to radiative forcing relative to EC, highlighting a critical area for future research. Investigating the actual concentrations of EC in the TP provides critical data to support model simulation and validate model accuracy, further enhancing our understanding of EC's impacts on climate warming and glacier melting.
Brown carbon (BrC) represents not only a major component of haze pollution but also a non-negligible contributor to positive radiative forcing, making it a key species for coordinating air quality and climate policies. In China, field observations on BrC remain limited given the highly variable emission sources and meteorological conditions across different regions. Here we focused on the optical properties of BrC in a distinct but rarely studied megacity in Northeast China, which is within a major agricultural region and experiences extremely cold winter. Agricultural fires were evident in April of 2021 and the fall of 2020, although open burning was strictly prohibited. Such emissions enhanced BrC's mass absorption efficiency at 365 nm (MAE365), more efficiently by the fall fires which were inferred to have relatively high combustion efficiencies (CE). After taking CE into consideration, the relationships between MAE365 and the levoglucosan to organic carbon ratio (a measure of the significance of agricultural fire influence) roughly converged for the fire episodes in different seasons, including those identified in February and March of 2019 by a previous campaign. Agricultural fires also influenced the determination of absorption & ANGS;ngstrom exponent (AAE), by resulting in non-linearity for BrC's absorption spectra shown on ln-ln scale. Based on three indicators developed by this study, the non-linearity was inferred to be caused by similar chromophores although the fires were characterized by various CE levels in different seasons. In addition, for the samples without significant influence of open burning, coal combustion emissions were identified as the dominant influencing factor for MAE365, whereas none solid link was found between the solution-based AAE and aerosol source.
Biomass burning is a major source of Brown Carbon (BrC), strongly contributing to radiative forcing. In urban areas of the climate-sensitive Southeastern European region, where strong emissions from residential wood burning (RWB) are reported, radiative impacts of carbonaceous aerosols remain largely unknown. This study examines the absorption properties of water-and methanol-soluble organic carbon (WSOC, MeS_OC) in a city (Ioannina, Greece) heavily im-pacted by RWB. Measurements were performed during winter (December 2019 - February 2020) and summer (July - August 2019) periods, characterized by RWB and photochemical processing of organic aerosol (OA), respectively. PM2.5 filter extracts were analyzed spectrophotometrically for water-and methanol-soluble BrC (WS_BrC, MeS_BrC) absorption. WSOC concentrations were quantified using TOC analysis, while those of MeS_OC were determined using a newly developed direct quantification protocol, applied for the first time to an extended series of ambient sam-ples. The direct method led to a mean MeS_OC/OC of 0.68 and a more accurate subsequent estimation of absorption efficiencies. The mean winter WS_BrC and MeS_BrC absorptions at 365 nm were 13.9 Mm-1 and 21.9 Mm-1, respec-tively, suggesting an important fraction of water-insoluble OA. Mean winter WS_BrC and MeS_BrC absorptions were over 10 times those observed in summer. MeS_OC was more absorptive than WSOC in winter (mean mass absorption efficiencies - MAE365: 1.81 vs 1.15 m2 gC-1) and especially in summer (MAE: 1.12 vs 0.27 m2 gC-1) due to photo -dissociation and volatilization of BrC chromophores. The winter radiative forcing (RF) of WS_BrC and MeS_BrC rela-tive to elemental carbon (EC) was estimated at 8.7 % and 16.7 %, respectively, in the 300-2500 nm band. However, those values increased to 48.5 % and 60.2 % at 300-400 nm, indicating that, under intense RWB, BrC forcing becomes comparable to that of soot. The results highlight the consideration of urban BrC emissions in radiative transfer models, as a considerable climate forcing factor.
Black carbon plays an important role in climate change. Whereas, accurate measurement of black carbon (also known as elemental carbon (EC)) is still a challenging issue because portion of the pyrolytic carbon produced from the organic carbon (OC) can cause the overestimation of EC when measured by thermal-optical method. As one of the remote regions in the world, the Tibetan Plateau (TP) is characterized as high OC/EC ratio in its atmosphere. In this study, potential influence of relative high OC concentration to EC were investigated at three remote sites (Yaze, Everest and Nam Co) in the TP. The results showed that carbonaceous aerosols from different sources can affect the fraction of OC extracted by methanol. Concentration of OC extracted by methanol had a significantly positive correlation with the reduction of pyrolytic carbon and EC concentrations, indicating that part of OC extracted by methanol can decrease the production of pyrolytic carbon and then reduce the over-estimation of EC. After considering this effect, it is shown in this study that actual EC concentration at Yaze, Everest and Nam Co were overestimated by approximately 40.0 +/- 12.6%, 28.8 +/- 9.1% and 24.8 +/- 4.7%, respectively. Accordingly, combined with the overestimation of EC concentration by carbonates, actual ratios of solar energy absorbed by organic carbon to EC were 1.67, 2.33 and 2.78 times those of original ones at Yaze, Everest and Nam Co, respectively. Therefore, warming effect caused by EC on the TP should be lower than that previously estimated. This phenomenon needs to be considered for both in situ study and model simulation in the future.
As an important component of organic carbon (OC), brown carbon (BrC) plays a significant role in radiative forcing in the atmosphere. Water-insoluble OC (WIOC) generally has higher light absorption ability than water-soluble OC (WSOC). The mass absorption cross- (MAC) of WIOC is normally investigated by dissolving OC in methanol. However, all the current methods have shortcomings due to neglecting the methanol insoluble particulate carbon that is detached from the filter and suspended in methanol extracts, which results in MAC uncertainties of the methanol-soluble BrC and its climate warming estimation. In this study, by investigating typical biomass combustion sourced aerosols from the Tibetan Plateau and ambient aerosols from rural and urban areas in China, we evaluated the light absorption of extractable OC fraction for the existing methods. Moreover, a new method was developed to overcome the methanol insoluble particulate carbon detachment problem to achieve more reliable MAC values. We found that OC can be dissolved in methanol in a short time (e.g., 1 h) and ultrasonic treatment and long-term soaking do not significantly increase the extractable OC fraction. Additionally, we proved that methanol insoluble particulate carbon detachment in methanol does exist in previous methods, causing overestimation of the BrC mass extracted by methanol and thus the underestimation of MAC values. We therefore recommend the newly developed extraction method in this study to be utilized in future related studies to quantitatively obtain the light absorption property of methanol-soluble BrC. (C) 2020 Elsevier Ltd. All rights reserved.
Brown carbon (i.e., light-absorbing organic carbon, or BrC) exerts important effects on the environment and on climate in particular. Based on spectrophotometric absorption measurements on extracts of bulk aerosol samples, this study investigated the characteristics of BrC during winter in Beijing, China. Organic compounds extractable by methanol contributed approximately 85% to the organic carbon (OC) mass. Light absorption by the methanol extracts exhibited a strong wavelength dependence, with an average absorption Angstrom exponent of 7.10 (fitted between 310 and 450 nm). Normalizing the absorption coefficient (babs) measured at 365 nm to the extractable OC mass yielded an average mass absorption efficiency (MAE) of 1.45 m(2)/g for the methanol extracts. This study suggests that light absorption by BrC could be comparable with black carbon in the spectral range of near-ultraviolet light. Our results also indicate that BrC absorption and thus BrC radiative forcing could be largely underestimated when using water-soluble organic carbon (WSOC) as a surrogate for BrC. Compared to previous work relying only on WSOC, this study provides a more comprehensive understanding of BrC aerosol based on methanol extraction. (C) 2015 Elsevier Ltd. All rights reserved.