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在经历与大气相关的干燥过程的环境颗粒中,没有棕色碳形成的证据。

No evidence for brown carbon formation in ambient particles undergoing atmospherically relevant drying.

机构信息

Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, USA.

Department of Chemistry, University of California, Irvine, USA.

出版信息

Environ Sci Process Impacts. 2020 Feb 26;22(2):442-450. doi: 10.1039/c9em00457b.

Abstract

Recent laboratory studies have reported the formation of light-absorbing organic carbon compounds (brown carbon, BrC) in particles undergoing drying. Atmospheric particles undergo cycles of humidification and drying during vertical transport and through daily variations in temperature and humidity, which implies particle drying could potentially be an important source of BrC globally. In this work, we investigated BrC formation in ambient particles undergoing drying at a site in the eastern United States during summer. Aerosol BrC concentrations were linked to secondary organic aerosol (SOA) formation, consistent with seasonal expectations for this region. Measurements of water-soluble organic aerosol concentrations and light absorption (365 nm) were alternated between an unperturbed channel and a channel that dried particles to 41% or 35% relative humidity (RH), depending on the system configuration. The RH maintained in the dry channels was below most ambient RH levels observed throughout the study. We did not observe BrC formation in particles that were dried to either RH level. The results were consistent across two summers, spanning ∼5 weeks of measurements that included a wide range of RH conditions and organic and inorganic aerosol loadings. This work suggests that mechanisms aside from humidification-drying cycles are more important contributors to ambient particle BrC loadings. The implications of this work on the atmospheric budget of BrC are discussed.

摘要

最近的实验室研究报告称,在干燥过程中的颗粒中形成了吸光有机碳化合物(棕色碳,BrC)。大气颗粒在垂直传输过程中和通过温度和湿度的日常变化中经历着吸湿和干燥的循环,这意味着颗粒干燥可能是全球 BrC 的一个重要来源。在这项工作中,我们研究了在美国东部一个地点的环境颗粒在干燥过程中形成 BrC 的情况,在夏季。气溶胶 BrC 浓度与二次有机气溶胶(SOA)的形成有关,这与该地区的季节性预期一致。在一个未受干扰的通道和一个将颗粒干燥到 41%或 35%相对湿度(RH)的通道之间交替测量水溶性有机气溶胶浓度和光吸收(365nm),具体取决于系统配置。在干燥通道中保持的 RH 低于整个研究过程中观察到的大多数环境 RH 水平。我们没有观察到在任何 RH 水平下干燥的颗粒中形成 BrC。这一结果在两个夏季都得到了验证,跨越了约 5 周的测量,包括广泛的 RH 条件和有机和无机气溶胶负荷。这项工作表明,除了吸湿-干燥循环之外,其他机制对环境颗粒 BrC 负荷的贡献更为重要。讨论了这项工作对 BrC 大气预算的影响。

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