State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China; College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China.
Sci Total Environ. 2021 May 20;770:144821. doi: 10.1016/j.scitotenv.2020.144821. Epub 2021 Jan 27.
The light absorption black carbon (BC) and brown carbon (BrC) are two important sources of uncertainties in radiative forcing estimate. Here we investigated the light absorption enhancement (E) of BC due to coated materials at an urban (Beijing) and a rural site (Gucheng) in North China Plain (NCP) in winter 2019 by using a photoacoustic extinctiometer coupled with a thermodenuder. Our results showed that the average (±1σ) E was 1.32 (±0.15) at the rural site, which was slightly higher than that at the urban site (1.24 ± 0.15). The dependence of E on coating materials was found to be relatively limited at both sites. However, E presented considerable increases as a function of relative humidity below 70%. Further analysis showed that E during non-heating period in Beijing was mainly caused by secondary components, while it was dominantly contributed by enhanced primary emissions in heating season at both sites. In particular, aerosol particles mixed with coal combustion emissions had a large impact on E (>1.40), while the fresh traffic emissions and freshly oxidized secondary OA (SOA) had limited E (1.00-1.23). Although highly aged or aqueous-phase processed SOA coated on BC showed the largest E, their contributions to the bulk absorption enhancement were generally small. We also quantified the absorption of BrC and source contributions. The results showed the BrC absorption at the rural site was nearly twice that of urban site, yet absorption Ångström exponents were similar. Multiple linear regression analysis highlighted the major sources of BrC being coal combustion emissions and photochemical SOA at both sites with additional biomass burning at the rural site. Overall, our results demonstrated the relatively limited winter light absorption enhancement of BC in different chemical environments in NCP, which needs be considered in regional climate models to improve BC radiative forcing estimates.
光吸收黑碳 (BC) 和棕色碳 (BrC) 是辐射强迫估算中两个重要的不确定性来源。本研究利用光声消光光度计结合热脱附装置,于 2019 年冬季在中国华北平原 (NCP) 的城市 (北京) 和农村 (固城) 站点,考察了涂层物质对 BC 光吸收增强 (E) 的影响。结果表明,农村站点的平均 (±1σ) E 为 1.32 (±0.15),略高于城市站点 (1.24 ± 0.15)。E 对涂层物质的依赖性在两个站点都相对有限。然而,当相对湿度低于 70%时,E 会显著增加。进一步分析表明,北京非采暖期 E 的增加主要是由二次成分引起的,而在采暖季,两个站点的 E 主要是由增强的一次排放贡献的。特别是,混合有煤燃烧排放的气溶胶颗粒对 E 有较大影响 (>1.40),而新鲜交通排放和新鲜氧化的二次有机气溶胶 (SOA) 对 E 的影响有限 (1.00-1.23)。尽管涂覆在 BC 上的高度老化或水相处理的 SOA 具有最大的 E,但它们对整体吸收增强的贡献通常较小。我们还量化了 BrC 的吸收和来源贡献。结果表明,农村站点的 BrC 吸收几乎是城市站点的两倍,但吸收 Ångström 指数相似。多元线性回归分析突出了 BrC 的主要来源是两个站点的煤燃烧排放和光化学 SOA,农村站点还有生物质燃烧。总体而言,本研究结果表明,在不同的化学环境中,冬季 BC 的光吸收增强相对有限,这需要在区域气候模型中考虑,以提高 BC 辐射强迫估算的准确性。