Online gas- and particle-phase measurements of organosulfates, organosulfonates and nitrooxy organosulfates in Beijing utilizing a FIGAERO ToF-CIMS
Online gas- and particle-phase measurements of organosulfates, organosulfonates and nitrooxy organosulfates in Beijing utilizing a FIGAERO ToF-CIMS
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在北京使用 FigAERO ToF-CIMS 对有机硫酸盐、有机磺酸盐和硝氧基有机硫酸盐进行在线气相和颗粒相测量
DOI：
10.5194/acp-18-10355-2018
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发表时间：
2017-11
影响因子：
6.3
通讯作者：
Guo So
中科院分区：
文献类型：
--
作者：
Le Breton Michael;Wang Yujue;Hallquist Asa M.;Pathak Ravi Kant;Zheng Jing;Yang Yudong;Shang Dongjie;Glasius Marianne;Bannan Thomas J.;Liu Qianyun;Chan Chak K.;Percival Carl J.;Zhu Wenfei;Lou Shengrong;Topping David;Wang Yuchen;Yu Jianzhen;Lu Keding;Guo So
.飞行时间化学电离质谱仪
利用气体和气溶胶过滤器入口（FIGAERO）部署在
北京西北40公里的区域站点，并成功确定和
测量了17种含硫有机物（SCO是有机/硝基氧基有机硫酸盐和磺酸盐）与生物和人为前体。SCO
使用实验室合成的乳酸硫酸盐标准品进行定量
和硝基苯酚有机硫酸盐（NP OS）。实地观察的变化
通过与离线测量技术（轨道阱和
高效液相色谱法，HPLC）。平均
总的（由CIMS鉴定的17个）SCO颗粒质量浓度为
210 ± 110 ng m−3，最大值为540 ng m−3，
尽管它仅占有机气溶胶（OA）的2 ± 1%。
CIMS确定了环境中持续存在的SCO气相
空气，这进一步支持了单独的蒸汽压力测量，
NP OS通过克努森效应质谱仪（KEMS）测定。增加
相对湿度（RH）促进SCO向颗粒相的分配，
而较高的温度有利于较高的气相浓度。生物源排放量仅占本研究中测量的SCO总量的19%。
study.这里，C10 H16 NSO 7，一种单萜衍生的SCO，
代表最高的分数（10%），随后是异戊二烯衍生的
上合组织多环芳烃（PAH）和
芳族前体占主导地位的SCO质量负载（51%），
C11 H11 SO 7，来自甲基萘氧化，
贡献40 ng m−3和0.3%的OA质量。与人类有关的SCOs与苯相关性很好，尽管它们的丰度取决于
高度依赖于空气质量的光化学年龄，
之间的pinonic酸及其氧化产物，作为定性
光化学钟除了典型的人为和生物
前体生物质燃烧前体硝基苯酚（NP）提供了一种
NP OS的显著水平。必须指出，
这里仅代表检测到的SCO。很可能
有更多的SCO存在，但CIMS没有识别。乙醇酸的气相和颗粒相测量表明，
向颗粒相的分配促进乙醇酸硫酸盐
生产，与目前的形成机制建议，
文学此外，HSO_4·H_2SO_4 ~-团簇的测量结果表明，
CIMS被用作酸度的定性标记，并表明
总SCOs的产生在高酸性气溶胶中是有效的，
SO 42-和有机物含量。这种依赖关系变得更加复杂
由于特定VOC前体的可变性，
. A time-of-flight chemical ionization mass spectrometer (CIMS)
utilizing the Filter Inlet for Gas and Aerosol (FIGAERO) was deployed at a
regional site 40 km north-west of Beijing and successfully identified and
measured 17 sulfur-containing organics (SCOs are organo/nitrooxy organosulfates and sulfonates) with biogenic and anthropogenic precursors. The SCOs
were quantified using laboratory-synthesized standards of lactic acid sulfate
and nitrophenol organosulfate (NP OS). The variation in field observations
was confirmed by comparison to offline measurement techniques (orbitrap and
high-performance liquid chromatography, HPLC) using daily averages. The mean
total (of the 17 identified by CIMS) SCO particle mass concentration was
210 ± 110 ng m−3 and had a maximum of 540 ng m−3,
although it contributed to only 2 ± 1 % of the organic aerosol (OA).
The CIMS identified a persistent gas-phase presence of SCOs in the ambient
air, which was further supported by separate vapour-pressure measurements of
NP OS by a Knudsen Effusion Mass Spectrometer (KEMS). An increase in
relative humidity (RH) promoted partitioning of SCO to the particle phase,
whereas higher temperatures favoured higher gas-phase concentrations. Biogenic emissions contributed to only 19 % of total SCOs measured in this
study. Here, C10H16NSO7, a monoterpene-derived SCO,
represented the highest fraction (10 %) followed by an isoprene-derived
SCO. The anthropogenic SCOs with polycyclic aromatic hydrocarbon (PAH) and
aromatic precursors dominated the SCO mass loading (51 %) with
C11H11SO7, derived from methyl naphthalene oxidation,
contributing to 40 ng m−3 and 0.3 % of the OA mass. Anthropogenic-related SCOs correlated well with benzene, although their abundance depended
highly on the photochemical age of the air mass, tracked using the ratio
between pinonic acid and its oxidation product, acting as a qualitative
photochemical clock. In addition to typical anthropogenic and biogenic
precursors the biomass-burning precursor nitrophenol (NP) provided a
significant level of NP OS. It must be noted that the contribution analysis
here is only representative of the detected SCOs. There are likely to
be many more SCOs present which the CIMS has not identified. Gas- and particle-phase measurements of glycolic acid suggest that
partitioning towards the particle phase promotes glycolic acid sulfate
production, contrary to the current formation mechanism suggested in the
literature. Furthermore, the HSO4⋅H2SO4- cluster measured by the
CIMS was utilized as a qualitative marker for acidity and indicates that the
production of total SCOs is efficient in highly acidic aerosols with high
SO42- and organic content. This dependency becomes more complex
when observing individual SCOs due to variability of specific VOC precursors.
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影响因子：
11.4
作者：
T. Bannan;A. M. Booth;Benjamin T. Jones;S. O'Meara;M. Barley;I. Riipinen;Carl J. Percival;D. Topping
通讯作者：
T. Bannan;A. M. Booth;Benjamin T. Jones;S. O'Meara;M. Barley;I. Riipinen;Carl J. Percival;D. Topping
DOI：
10.1002/chin.201528326
发表时间：
2015-07
期刊：
ChemInform
影响因子：
--
作者：
M. Bilde;K. Barsanti;Murray Booth;C. Cappa;N. Donahue;E. Emanuelsson;G. Mcfiggans;U. Krieger;C. Marcolli;D. Topping
通讯作者：
M. Bilde;K. Barsanti;Murray Booth;C. Cappa;N. Donahue;E. Emanuelsson;G. Mcfiggans;U. Krieger;C. Marcolli;D. Topping
影响因子：
5.2
作者：
B. Nozière;S. Ekström;T. Alsberg;S. Holmström
通讯作者：
B. Nozière;S. Ekström;T. Alsberg;S. Holmström
DOI：
10.1021/es061812j.s001
发表时间：
2007
期刊：
--
影响因子：
--
作者：
Q. I Z H A N G;E. L. J I M E N E Z-E.-L.-J-I-M-E-N-E-Z-2082909205;D. O U G L A;S. R. W. O R S N O P, § A N D M A N J U L A C A N A G A R A-S.-R.-W.-O-R-S-N-O-P,-§-A-N-D-M-A-N-J-U-L-A-C-A-N-A-2096364242
通讯作者：
Q. I Z H A N G;E. L. J I M E N E Z-E.-L.-J-I-M-E-N-E-Z-2082909205;D. O U G L A;S. R. W. O R S N O P, § A N D M A N J U L A C A N A G A R A-S.-R.-W.-O-R-S-N-O-P,-§-A-N-D-M-A-N-J-U-L-A-C-A-N-A-2096364242
影响因子：
11.4
作者：
Iinuma, Yoshiteru;Muller, Conny;Herrmann, Hartmut
通讯作者：
Herrmann, Hartmut