Using advanced mass spectrometry techniques to fully characterize atmospheric organic carbon: current capabilities and remaining gaps
Using advanced mass spectrometry techniques to fully characterize atmospheric organic carbon: current capabilities and remaining gaps
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DOI：
10.1039/c7fd00021a
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发表时间：
2017-08-01
影响因子：
3.4
通讯作者：
Kroll, J. H.
中科院分区：
文献类型：
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作者：
Isaacman-VanWertz, G.;Massoli, P.;Kroll, J. H.
大气中的有机化合物在分子组成和化学性质上差异很大，因此没有一种仪器可以合理地测量环境化合物的整个范围。在过去的十年中，新一代的现场可部署质谱仪大大提高了我们检测、识别和量化这些有机化合物的能力，但还没有系统的方法来评估目前可用的工具在多大程度上捕获了大气中预期的化学特性和性质的整个空间。减少参数的框架，已经开发来描述大气混合物，在这里利用一套仪器访问的化学性质的范围内的特征。多个化学空间（例如，碳的氧化态与挥发性，和氧数与碳数）填充有通过几个质谱仪测量的离子，气相和颗粒相α-蒎烯氧化产物作为有机化合物的测试混合物。在这项工作中所采用的仪器的参数空间的覆盖范围内观察到的差距很少，但由于混合物成分的不确定性，难以评估全面测量的全部程度。在参数空间中的单个离子和区域之间的重叠被确定，无论是在气相和颗粒相的测量，并在每个阶段。保守地说，这些重叠部分几乎不占（
Organic compounds in the atmosphere vary widely in their molecular composition and chemical properties, so no single instrument can reasonably measure the entire range of ambient compounds. Over the past decade, a new generation of in situ, field-deployable mass spectrometers has dramatically improved our ability to detect, identify, and quantify these organic compounds, but no systematic approach has been developed to assess the extent to which currently available tools capture the entire space of chemical identity and properties that is expected in the atmosphere. Reduced-parameter frameworks that have been developed to describe atmospheric mixtures are exploited here to characterize the range of chemical properties accessed by a suite of instruments. Multiple chemical spaces (e.g. oxidation state of carbon vs. volatility, and oxygen number vs. carbon number) were populated with ions measured by several mass spectrometers, with gas- and particle-phase alpha-pinene oxidation products serving as the test mixture of organic compounds. Few gaps are observed in the coverage of the parameter spaces by the instruments employed in this work, though the full extent to which comprehensive measurement was achieved is difficult to assess due to uncertainty in the composition of the mixture. Overlaps between individual ions and regions in parameter space were identified, both between gas-and particle-phase measurements, and within each phase. These overlaps were conservatively found to account for little (