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美国倍半萜烯和单萜烯排放产生的二次有机气溶胶

Secondary organic aerosol from sesquiterpene and monoterpene emissions in the United States.

作者信息

Sakulyanontvittaya Tanarit, Guenther Alex, Helmig Detlev, Milford Jana, Wiedinmyer Christine

机构信息

Mechanical Engineering Department, University of Colorado, Boulder, Colorado 80309, USA.

出版信息

Environ Sci Technol. 2008 Dec 1;42(23):8784-90. doi: 10.1021/es800817r.

Abstract

Emissions of volatile organic compounds (VOC) from vegetation are believed to be a major source of secondary organic aerosol (SOA), which in turn comprises a large fraction of fine particulate matter in many areas. Sesquiterpenes are a class of biogenic VOC with high chemical reactivity and SOA yields. Sesquiterpenes have only recently been quantified in emissions from a wide variety of plants. In this study, a new sesquiterpene emission inventory is used to provide input to the Models-3 Community Multiscale Air Quality (CMAQ) model. CMAQ is used to estimate the contribution of sesquiterpenes and monoterpenes to SOA concentrations over the contiguous United States. The gas-particle partitioning module of CMAQ was modified to include condensable products of sesquiterpene oxidation and to update values of the enthalpy of vaporization. The resulting model predicts July monthly average surface concentrations of total SOA in the eastern U.S. ranging from about 0.2-0.8 microg m(-3). This is roughly double the amount of SOA produced in this region when sesquiterpenes are not included. Even with sesquiterpenes included, however, the model significantly underpredicts surface concentrations of particle-phase organic matter compared to observed values. Treating all SOA as capable of undergoing polymerization increases predicted monthly average surface concentrations in July to 0.4-1.2 microg m(-3), in closer agreement with observations. Using the original enthalpy of vaporization value in CMAQ in place of the values estimated from the recent literature results in predicted SOA concentrations of about 0.3-1.3 microg m(-3).

摘要

植被排放的挥发性有机化合物(VOC)被认为是二次有机气溶胶(SOA)的主要来源,而二次有机气溶胶在许多地区的细颗粒物中占很大比例。倍半萜是一类具有高化学反应性和SOA生成率的生物源VOC。直到最近才对多种植物排放的倍半萜进行了量化。在本研究中,一个新的倍半萜排放清单被用于为Models-3社区多尺度空气质量(CMAQ)模型提供输入。CMAQ用于估算倍半萜和单萜对美国本土SOA浓度的贡献。对CMAQ的气粒分配模块进行了修改,以纳入倍半萜氧化的可凝产物,并更新汽化焓值。结果模型预测美国东部7月总SOA的月平均地表浓度范围约为0.2 - 0.8微克/立方米。这大约是不包括倍半萜时该地区产生的SOA量的两倍。然而,即使纳入了倍半萜,该模型预测的颗粒相有机物地表浓度仍比观测值显著偏低。将所有SOA视为能够发生聚合反应,会使7月预测的月平均地表浓度增加到0.4 - 1.2微克/立方米,与观测结果更接近。在CMAQ中使用原始的汽化焓值代替根据近期文献估算的值,得到的SOA浓度预测值约为0.3 - 1.3微克/立方米。

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