Oxygenated fraction and mass of organic aerosol from direct emission and atmospheric processing measured on the R/V Ronald Brown during TEXAQS/GoMACCS 2006
Oxygenated fraction and mass of organic aerosol from direct emission and atmospheric processing measured on the R/V Ronald Brown during TEXAQS/GoMACCS 2006
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DOI：
10.1029/2008jd011275
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发表时间：
2009-04
影响因子：
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通讯作者：
L. Russell;S. Takahama;Shang Liu;L. Hawkins;D. Covert;P. Quinn;T. Bates
中科院分区：
文献类型：
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作者：
L. Russell;S. Takahama;Shang Liu;L. Hawkins;D. Covert;P. Quinn;T. Bates
2006年德克萨斯州休斯顿港及其周围的德克萨斯州空气质量研究和墨西哥湾大气成分和气候研究（TexAQS/GoMACCS）期间，R/V罗纳德布朗号上的特氟隆过滤器收集的亚微米颗粒物通过傅里叶变换红外（FTIR）和X射线荧光法测量有机官能团和元素组成。有机质量（OM）浓度（1-25 μ g m（-3））的环境颗粒样品测量FTIR显示出良好的协议与气溶胶质谱仪的测量。有机质的烷烃和羧酸基团的馏分分别为47%和32%。三种不同类型的空气质量的基础上确定的空气质量的起源和氡浓度，与显着较高的羧酸基团质量分数从北部（35%）比南部（29%）或墨西哥湾（26%）的空气质量。正矩阵因子分解分析将30-35%的羧酸部分归因于与油燃烧的元素特征具有轻度或强相关性（r > 0.5）的因素，9-24%归因于木材烟雾，表明OM的部分羧酸部分由控制金属排放的相同来源形成，即油和木材燃烧活动。这意味着，所测量的羧酸贡献的很大一部分是独立于传统的“二次”过程形成的，这将受到大气（光化学和气象）条件和其他排放源的影响。墨西哥湾和南气团（分别为GAM和SAM）中的羧酸基团组分主要是来自船舶的石油燃烧排放物以及背景海洋来源，最近陆地影响有限（基于氡浓度）。在所有气团中，醇类占OM的14%（主要与石油燃烧排放和背景源有关），胺类占OM的4%。在GAM和SAM中发现了有机硫酸酯基团，分别占OM的1%和3%。三分之二的有机物和氧碳比（O/C）的测量可以归因于石油和木材燃烧源的基础上温和或强烈的相关性，共同排放，非挥发性微量金属，其余三分之一与大气处理的有机气溶胶。云凝结核（CCN）含量（以总凝结核归一化）与醇类和胺类含量相关性较弱，与O/C相关性较弱，与烷烃类含量呈负相关。影响f（RH）的化学成分是硫酸盐，有机物和硝酸盐馏分，但这种对比是一致的CCN计数器和浊度计的尺寸分布依赖。
Submicron particles collected on Teflon filters aboard the R/V Ronald Brown during the Texas Air Quality Study and Gulf of Mexico Atmospheric Composition and Climate Study (TexAQS/GoMACCS) 2006 in and around the port of Houston, Texas, were measured by Fourier transform infrared (FTIR) and X-ray fluorescence for organic functional groups and elemental composition. Organic mass (OM) concentrations (1-25 mu g m(-3)) for ambient particle samples measured by FTIR showed good agreement with measurements made with an aerosol mass spectrometer. The fractions of organic mass identified as alkane and carboxylic acid groups were 47% and 32%, respectively. Three different types of air masses were identified on the basis of the air mass origin and the radon concentration, with significantly higher carboxylic acid group mass fractions in air masses from the north (35%) than the south (29%) or Gulf of Mexico (26%). Positive matrix factorization analysis attributed carboxylic acid fractions of 30-35% to factors with mild or strong correlations (r > 0.5) to elemental signatures of oil combustion and 9-24% to wood smoke, indicating that part of the carboxylic acid fraction of OM was formed by the same sources that controlled the metal emissions, namely the oil and wood combustion activities. The implication is that a substantial part of the measured carboxylic acid contribution was formed independently of traditionally "secondary" processes, which would be affected by atmospheric (both photochemical and meteorological) conditions and other emission sources. The carboxylic acid group fractions in the Gulf of Mexico and south air masses (GAM and SAM, respectively) were largely oil combustion emissions from ships as well as background marine sources, with only limited recent land influences (based on radon concentrations). Alcohol groups accounted for 14% of OM (mostly associated with oil combustion emissions and background sources), and amine groups accounted for 4% of OM in all air masses. Organosulfate groups were found in GAM and SAM, accounting for 1% and 3% of OM, respectively. Two thirds of the OM and oxygen-to-carbon (O/C) measured could be attributed to oil and wood combustion sources on the basis of mild or strong correlations to coemitted, nonvolatile trace metals, with the remaining one third being associated with atmospherically processed organic aerosol. The cloud condensation nuclei (CCN) fraction (normalized by total condensation nuclei) had weak correlations to the alcohol and amine group fractions and mild correlation with O/C, also varying inversely with alkane group fraction. The chemical components that influenced f(RH) were sulfate, organic, and nitrate fraction, but this contrast is consistent with the size-distribution dependence of CCN counters and nephelometers.