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Simultaneous Aerosol Mass Spectrometry and Chemical Ionisation Mass Spectrometry measurements during a biomass burning event in the UK: Insights into nitrate chemistry

机译:同时气溶胶质谱和化学电离 生物质燃烧过程中的质谱测量 英国:硝酸盐化学的见解

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摘要

Over the past decade, there has been an increasing interest in short-term events that negatively affect air quality such as bonfires and fireworks. High aerosol and gas concentrations generated from public bonfires/fireworks were measured in order to understand the night-time chemical processes and their atmospheric implications. Nitrate chemistry was observed during the bonfire night with nitrogen containing compounds in both gas and aerosol phase and further NO and ClNO concentrations, which depleted early next morning due to photolysis of NO radicals, ceasing production. Particulate organic nitrate (PON) concentrations of 2.8 μg.m were estimated using the m/z 46:30 ratios from AMS measurements, according to previously published methods. ME-2 source apportionment was performed to determine organic aerosol concentrations from different sources after modifying the fragmentation table and it was possible to identify two PON factors representing primary (pPON_ME2) and secondary (sPON_ME2) contributions. A slight improvement in the agreement between the source apportionment of the AMS and a collocated AE-31 Aethalometer was observed after modifying the prescribed fragmentation in the AMS organic spectrum (the fragmentation table) to determine PON sources, which resulted in an r = 0.865 between BBOA and compared to an r = 0.819 obtained without the modification. Correlations between OA sources and measurements made using Time of Flight Chemical Ionization Mass Spectrometry with an iodide adduct ion were performed in order to determine possible gas tracers to be used in future ME-2 analyses to constrain solutions. During bonfire night, high correlations (r) were observed between BBOA and methacrylic acid (0.915), Acrylic acid (0.901), nitrous acid (0.864), propionic acid, (0.851) and Hydrogen cyanide (0.755). A series of oxygenated species, chlorine compounds as well as cresol showed good correlations with sPON_ME2 and the low volatility oxygenated organic aerosol (LVOOA) factor during an episode with low pollutant concentrations. Further analysis of pPON_ME2 and sPON_ME2 was performed in order to determine whether these PON sources absorb light near the UV region using an Aethalometer. This hypothesis was tested by doing multilinear regressions between and BBOA, sPON_ME2 and pPON_ME2. Our results suggest that sPON_ME2 does not absorb light at 470 nm while pPON_ME2 and LVOOA absorb light at 470 nm over that of black carbon. This may inform black carbon (BC) source apportionment studies from Aethalometer measurements, through investigation of the brown carbon contribution to .
机译:在过去的十年中,人们越来越关注对篝火和烟花等空气质量产生负面影响的短期事件。为了了解夜间化学过程及其对大气的影响,对公共篝火/焰火产生的高浓度气溶胶和气体进行了测量。在篝火之夜观察到硝酸盐化学反应,气相和气溶胶相中都含有含氮化合物,并且NO和ClNO的浓度进一步增加,由于NO自由基的光解作用,第二天清晨耗尽了氮,停止了生产。根据以前公布的方法,使用AMS测量的m / z 46:30比率估算出2.8μg.m的颗粒状有机硝酸盐(PON)浓度。修改碎片表后,执行ME-2源分配以确定不同来源的有机气溶胶浓度,并且有可能识别出代表主要(pPON_ME2)和次要(sPON_ME2)的两个PON因子。在修改了AMS有机光谱中规定的碎片(碎片表)以确定PON来源后,观察到AMS的来源分配和并置的AE-31测湿仪之间的协议略有改善,这导致r = 0.865 BBOA并与未经修改获得的r = 0.819进行比较。进行了OA源与使用飞行时间化学电离质谱与碘化物加成离子进行的测量之间的相关性,以确定可能的气体示踪剂,以用于将来的ME-2分析来限制溶液。在篝火之夜,观察到BBOA与甲基丙烯酸(0.915),丙烯酸(0.901),亚硝酸(0.864),丙酸(0.851)和氰化氢(0.755)之间的高度相关性(r)。在污染物浓度低的情况下,一系列含氧物质,氯化合物以及甲酚与sPON_ME2和低挥发性含氧有机气溶胶(LVOOA)因子显示出良好的相关性。为了确定这些PON源是否使用Aethalometer探测UV区附近的光,对pPON_ME2和sPON_ME2进行了进一步分析。通过在BBOA,sPON_ME2和pPON_ME2之间进行多元线性回归,检验了该假设。我们的结果表明,sPON_ME2不会吸收470 nm的光,而pPON_ME2和LVOOA会吸收470 nm以上的黑碳。通过调查棕色碳对的贡献,这可能有助于从烟度计测量中获取黑碳(BC)源分配研究。

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