The comprehensive fingerprints of VOCs from complex coking emissions and their temporal evolution in the atmosphere based on backward inference method

IF 4.4 2区 地球科学 Q1 METEOROLOGY & ATMOSPHERIC SCIENCES
Hongyan Li , Shidan Huang , Yuanchun Ren , Yanru Zhang , Jing'’ai Bai , Hongyu Li , Guozhong Zhang , Xueying Gao , Yang Cui , Lili Guo , Jie Fan , Yongchun Liu , Guo Fu , Zhentao Wang , Qiusheng He , Yang Yun
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Abstract

Coking industries are an important source of volatile organic compounds (VOCs). Coking emissions are characterized by diverse emission points, species and intensities, leading to inconsistencies in emission profiles. This complexity complicates the accurate identification of coking-related pollutants in the atmosphere. To obtain a distinct VOC fingerprint from coking emissions, 57 VOCs were detected based on a comprehensive sampling campaign conducted at three strategically placed sites (one in an area with intensive coking activity and two downwind sites) and one control site. We found a positive correlation between the contribution of coking emissions to total VOCs (TVOCs) (between 10.4 % and 44.2 %) and the severity of VOC pollution (TVOC content ranging from 28.75 to 49.28 ppbv). Furthermore, increases in the contribution of coking emissions to TVOC content resulted in increases in the proportions of alkenes (from 10 % to 19 % in summer and 13 % to 20 % in autumn) and aromatics (from 6 % to 18 % in autumn) in TVOCs. Ethane, ethene, propene, benzene, toluene, and acetylene were identified as dominant VOC species in coking emissions. Their concentrations increased as coking activity increased and were highly prevalent in the coking source profile, as indicated by positive matrix factorization analysis. The ratio of benzene to toluene, alongside the relative proportions of benzene, toluene, and ethylbenzene and of ethane, propane, and ethene was effective diagnostic indicators for identifying coking sources. The PMF-resolved factor profile from our field campaign could accurately represent coking emissions. Photochemical aging led to an underestimation of the coking-source contribution but had little effect on the ranges of the diagnostic indicators or the chemical profile of VOCs from coking sources.

Abstract Image

基于倒推法的复杂焦化排放VOCs综合指纹图谱及其在大气中的时间演化
焦化工业是挥发性有机化合物(VOCs)的重要来源。焦化排放具有不同的排放点、排放种类和排放强度的特点,导致焦化排放曲线的不一致性。这种复杂性使准确识别大气中与焦化有关的污染物变得复杂。为了从焦化排放中获得明显的挥发性有机化合物指纹,在三个战略地点(一个在焦化活动密集的地区,两个顺风地点)和一个控制地点进行了全面的采样活动,检测到57种挥发性有机化合物。我们发现焦化排放对总挥发性有机化合物(TVOCs)的贡献(10.4%至44.2%)与VOC污染的严重程度(TVOC含量范围为28.75至49.28 ppbv)呈正相关。此外,焦化排放对TVOC含量贡献的增加导致烯烃(夏季从10%增加到19%,秋季从13%增加到20%)和芳烃(秋季从6%增加到18%)在TVOC中的比例增加。乙烷、乙烯、丙烯、苯、甲苯和乙炔是焦化排放中主要的挥发性有机化合物。正矩阵分解分析表明,它们的浓度随着焦化活性的增加而增加,并且在焦化源剖面中非常普遍。苯与甲苯的比例,以及苯、甲苯和乙苯的相对比例,以及乙烷、丙烷和乙烯的相对比例是识别焦化源的有效诊断指标。从我们的现场活动中得到的pmf分解因子曲线可以准确地代表焦化排放。光化学老化导致对焦化源贡献的低估,但对焦化源挥发性有机化合物的诊断指标范围和化学特征影响不大。
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来源期刊
Atmospheric Research
Atmospheric Research 地学-气象与大气科学
CiteScore
9.40
自引率
10.90%
发文量
460
审稿时长
47 days
期刊介绍: The journal publishes scientific papers (research papers, review articles, letters and notes) dealing with the part of the atmosphere where meteorological events occur. Attention is given to all processes extending from the earth surface to the tropopause, but special emphasis continues to be devoted to the physics of clouds, mesoscale meteorology and air pollution, i.e. atmospheric aerosols; microphysical processes; cloud dynamics and thermodynamics; numerical simulation, climatology, climate change and weather modification.
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