Molecular characterization of ultrafine particles using extractive electrospray time-of-flight mass spectrometry.
Molecular characterization of ultrafine particles using extractive electrospray time-of-flight mass spectrometry.
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DOI：
10.1039/d1ea00050k
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发表时间：
2021-09-23
期刊：
影响因子：
--
通讯作者：
El Haddad I
中科院分区：
文献类型：
--
作者：
Surdu M;Pospisilova V;Xiao M;Wang M;Mentler B;Simon M;Stolzenburg D;Hoyle CR;Bell DM;Lee CP;Lamkaddam H;Lopez-Hilfiker F;Ahonen LR;Amorim A;Baccarini A;Chen D;Dada L;Duplissy J;Finkenzeller H;He XC;Hofbauer V;Kim C;Kürten A;Kvashnin A;Lehtipalo K;Makhmutov V;Molteni U;Nie W;Onnela A;Petäjä T;Quéléver LLJ;Tauber C;Tomé A;Wagner R;Yan C;Prevot ASH;Dommen J;Donahue NM;Hansel A;Curtius J;Winkler PM;Kulmala M;Volkamer R;Flagan RC;Kirkby J;Worsnop DR;Slowik JG;Wang DS;Baltensperger U;El Haddad I
气溶胶颗粒对人类健康产生负面影响，同时由于其作为云凝结核的能力，也具有气候相关性。超细颗粒（直径Dp < 100 nm）通常占总数浓度的最大部分，然而，由于它们的质量低，它们的化学表征是困难的。使用萃取电喷雾飞行时间质谱仪（EESI-TOF），我们在欧洲核子研究中心的CLOUD室中表征了萘和β-卡烯氧化产物的新成核粒子的分子组成。我们进行了详细的相互比较的有机气溶胶的化学成分测量的EESI-TOF和碘加合物化学电离质谱仪配备了一个过滤器的气体和气溶胶的入口（FIGAERO-I-CIMS）。我们还使用了一个气溶胶增长模型的基础上的有机蒸汽的冷凝，表明EESI-TOF测量的化学成分是一致的，与预期的冷凝氧化产物。通过限制EESI-TOF化合物特定的灵敏度或考虑凝相过程，可以进一步改善这种一致性。我们的研究结果表明，EESI-TOF可以在真实的时间内获得直径小至20 nm的颗粒的化学组成，质量负载低至数百ng m−3。这是迄今为止难以实现的，因为其他在线仪器通常受到尺寸截止、电离/热碎裂和/或半连续采样的限制。利用实时同步的气相和颗粒相数据，我们讨论了萘氧化产物在分子水平上的缩合反应。利用实时的气相和颗粒相数据，在分子水平上讨论了萘和β-卡勒烯氧化产物的缩合反应。
Aerosol particles negatively affect human health while also having climatic relevance due to, for example, their ability to act as cloud condensation nuclei. Ultrafine particles (diameter Dp < 100 nm) typically comprise the largest fraction of the total number concentration, however, their chemical characterization is difficult because of their low mass. Using an extractive electrospray time-of-flight mass spectrometer (EESI-TOF), we characterize the molecular composition of freshly nucleated particles from naphthalene and β-caryophyllene oxidation products at the CLOUD chamber at CERN. We perform a detailed intercomparison of the organic aerosol chemical composition measured by the EESI-TOF and an iodide adduct chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols (FIGAERO-I-CIMS). We also use an aerosol growth model based on the condensation of organic vapors to show that the chemical composition measured by the EESI-TOF is consistent with the expected condensed oxidation products. This agreement could be further improved by constraining the EESI-TOF compound-specific sensitivity or considering condensed-phase processes. Our results show that the EESI-TOF can obtain the chemical composition of particles as small as 20 nm in diameter with mass loadings as low as hundreds of ng m−3 in real time. This was until now difficult to achieve, as other online instruments are often limited by size cutoffs, ionization/thermal fragmentation and/or semi-continuous sampling. Using real-time simultaneous gas- and particle-phase data, we discuss the condensation of naphthalene oxidation products on a molecular level. Using real-time simultaneous gas- and particle-phase data, the condensation of naphthalene and β-caryophyllene oxidation products on a molecular level is discussed.
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DOI：
10.1073/pnas.1900125116
发表时间：
2019-04-30
影响因子：
11.1
作者：
An, Zhisheng;Huang, Ru-Jin;Ji, Yuemeng
通讯作者：
Ji, Yuemeng
DOI：
10.1073/pnas.1404853111
发表时间：
2014-10-21
影响因子：
11.1
作者：
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通讯作者：
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影响因子：
6.3
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Merikanto, J.;Spracklen, D. V.;Carslaw, K. S.
通讯作者：
Carslaw, K. S.
影响因子：
6.3
作者：
Garmash, Olga;Rissanen, Matti P.;Ehn, Mikael
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Ehn, Mikael
影响因子：
7.4
作者：
Giannoukos, Stamatios;Lee, Chuan Ping;Slowik, Jay
通讯作者：
Slowik, Jay