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中国车辆排放的元素碳粒径分布特征:隧道研究结果及大气影响

Size distribution characteristics of elemental carbon emitted from Chinese vehicles: results of a tunnel study and atmospheric implications.

作者信息

Huang Xiao-Feng, Yu Jian Zhen, He Ling-Yan, Hu Min

机构信息

Atmospheric, Marine and Coastal Environment Program, Department of Chemistry, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.

出版信息

Environ Sci Technol. 2006 Sep 1;40(17):5355-60. doi: 10.1021/es0607281.

Abstract

The size distribution characteristics of elemental carbon (EC) emissions from Chinese vehicles have not been previously described. In this study, we collected size-segregated aerosol samples using a 10-stage MOUDI sampler (0.056-18 microm) in the Zhujiang tunnel, a roadway tunnel in the urban area of Guangzhou, China. The samples were analyzed for EC, organic carbon (OC), and inorganic ions. Fine particles had an OC/EC ratio of 0.57, indicating a dominant contribution of EC from diesel vehicles. Both EC and OC showed a dominant accumulation mode with a mass median aerodynamic diameter (MMAD) of 0.42 microm. In comparison, studies available in the literature typically reported a much lower MMAD for EC (approximately 0.1 microm) in vehicular emissions in North America. A theoretical analysis indicated that the larger EC particles observed in this study could not have resulted from after-emission growth processes (i.e., water accretion, coagulation, and vapor condensation). This leaves operating conditions such as high engine loads and low combustion efficiencies, which are more prevalent in diesel-fueled Chinese vehicles, as a more plausible inherent reason for producing the larger EC agglomerates. While fresh 0.1 microm EC particles are unlikely to act as cloud condensation nuclei (CCN), calculations showed that EC particles as large as 0.42 microm are effective CCN at atmospherically relevant critical supersaturation values of less than 1%. As a result, fresh EC particles from Chinese vehicle emissions could readily undergo cloud processing and form internal mixtures with sulfate in the residue droplet mode particles. This prediction is consistent with observations that EC frequently showed a dominant droplet mode in urban atmospheres in this region. The internal mixing of EC with highly hygroscopic sulfate would facilitate its removal by wet deposition and shorten its lifetime in the atmosphere. In addition, the light-absorbing capabilities of EC particles could also be enhanced due to their internal mixing with sulfate. Numerical aerosol models need to take these factors into consideration for better predictions of the behaviors and effects of urban aerosols in China.

摘要

中国车辆排放的元素碳(EC)的粒径分布特征此前尚未有过描述。在本研究中,我们在中国广州城区的一条道路隧道——珠江隧道中,使用一台十阶MOUDI采样器(0.056 - 18微米)采集了按粒径分类的气溶胶样本。对样本进行了元素碳、有机碳(OC)和无机离子分析。细颗粒物的有机碳/元素碳比值为0.57,表明柴油车辆排放的元素碳占主导。元素碳和有机碳均呈现出以质量中位空气动力学直径(MMAD)为0.42微米的主导积聚模态。相比之下,文献中现有研究报道北美车辆排放中元素碳的质量中位空气动力学直径通常要低得多(约0.1微米)。理论分析表明,本研究中观测到的较大元素碳颗粒并非后排放增长过程(即水吸附、凝聚和蒸汽凝结)所致。这使得诸如高发动机负荷和低燃烧效率等运行条件成为产生更大元素碳团聚体的更合理内在原因(这些运行条件在中国柴油车辆中更为普遍)。虽然新鲜生成的0.1微米元素碳颗粒不太可能充当云凝结核(CCN),但计算表明,粒径达0.42微米的元素碳颗粒在大气相关临界过饱和度值小于1%时是有效的云凝结核。因此,来自中国车辆排放的新鲜元素碳颗粒很容易经历云过程,并以残留液滴模态颗粒与硫酸盐形成内部混合物。这一预测与该地区城市大气中元素碳常呈现主导液滴模态的观测结果一致。元素碳与高吸湿性硫酸盐的内部混合将有助于其通过湿沉降去除,并缩短其在大气中的寿命。此外,元素碳颗粒与硫酸盐的内部混合还可能增强其光吸收能力。数值气溶胶模型需要考虑这些因素,以便更好地预测中国城市气溶胶的行为和影响。

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