Eddy covariance emission and deposition flux measurements using proton transfer reaction-time of flight-mass spectrometry (PTR-TOF-MS): comparison with PTR-MS measured vertical gradients and fluxes-猫眼课题宝

DOI：

10.5194/acp-13-1439-2013

发表时间：

2012-08

期刊：

Atmospheric Chemistry and Physics

影响因子：

6.3

通讯作者：

中科院分区：

地球科学1区

文献类型：

作者：

J. Park;A. Goldstein;J. Timkovsky;S. Fares;R. Weber;J. Karlik;R. Holzinger

抽象。2010年夏季，在加州中央谷的一个橙子果园中同时部署了质子转移反应-飞行时间-质谱仪（PTR-TOF-MS）和四极杆质子转移反应质谱仪（PTR-MS），以收集适用于涡度相关（EC）通量计算的连续数据。PTR-TOF-MS的高时间分辨率（5 Hz）和高质量分辨率（高达5000 m/Δm）数据为计算各种挥发性有机化合物（VOC）的浓度和通量提供了基础。在整个活动中，在10和1278之间的质荷比中检测到664个质量峰。在这里，我们提出了27种离子种类的PTR-TOF-MS EC通量，其中垂直梯度通过PTR-MS同时测量。这些EC通量数据通过光谱分析进行验证（即，共谱、归一化共谱和卵形）。基于两种PTR仪器的相互比较，在混合比或通量方面均未发现显著的仪器偏差，并且数据显示甲醇和丙酮的平均一致性在5%以内。对于所测量的生物源挥发性有机化合物（BVOC），PTR-TOF-MS的EC通量与PTR-MS垂直梯度测量定性推断的通量方向一致。对于本文报告的27种选定离子，PTR-TOF-MS测量的总（24 h）平均净通量为299 μg C m −2 h −1。该站点的主要BVOC排放物为单萜（m/z 81.070 + m/z 137.131 + m/z 95.086，34%，102 μg C m −2 h −1）和甲醇（m/z 33.032，18%，72 μg C m −2 h −1）。下一个最大的通量检测在以下质量（括号中的属性）：m/z 59.048（主要是丙酮，12.2%，36.5 μg C m −2 h −1），m/z 61.027（主要是乙酸，11.9%，35.7 μg C m −2 h −1），m/z 93.069（对伞花烃+甲苯，4.1%，12.2 μg Cm −2 h −1），m/z 45.033（乙醛，3.8%，11.5 μg C m −2 h −1），m/z 71.048（甲基乙烯基酮+甲基丙烯醛，2.4%，7.1 μg C m −2 h −1）和m/z 69.071（异戊二烯+ 2-甲基-3-丁烯-2-醇，1.8%，5.3 μg C m −2 h −1）。低水平的排放和/或沉积（

Abstract. During summer 2010, a proton transfer reaction – time of flight – mass spectrometer (PTR-TOF-MS) and a quadrupole proton transfer reaction mass spectrometer (PTR-MS) were deployed simultaneously for one month in an orange orchard in the Central Valley of California to collect continuous data suitable for eddy covariance (EC) flux calculations. The high time resolution (5 Hz) and high mass resolution (up to 5000 m/Δm) data from the PTR-TOF-MS provided the basis for calculating the concentration and flux for a wide range of volatile organic compounds (VOC). Throughout the campaign, 664 mass peaks were detected in mass-to-charge ratios between 10 and 1278. Here we present PTR-TOF-MS EC fluxes of the 27 ion species for which the vertical gradient was simultaneously measured by PTR-MS. These EC flux data were validated through spectral analysis (i.e., co-spectrum, normalized co-spectrum, and ogive). Based on inter-comparison of the two PTR instruments, no significant instrumental biases were found in either mixing ratios or fluxes, and the data showed agreement within 5% on average for methanol and acetone. For the measured biogenic volatile organic compounds (BVOC), the EC fluxes from PTR-TOF-MS were in agreement with the qualitatively inferred flux directions from vertical gradient measurements by PTR-MS. For the 27 selected ion species reported here, the PTR-TOF-MS measured total (24 h) mean net flux of 299 μg C m −2 h −1 . The dominant BVOC emissions from this site were monoterpenes ( m/z 81.070 + m/z 137.131 + m/z 95.086, 34%, 102 μg C m −2 h −1 ) and methanol ( m/z 33.032, 18%, 72 μg C m −2 h −1 ). The next largest fluxes were detected at the following masses (attribution in parenthesis): m/z 59.048 (mostly acetone, 12.2%, 36.5 μg C m −2 h −1 ), m/z 61.027 (mostly acetic acid, 11.9%, 35.7 μg C m −2 h −1 ), m/z 93.069 (para-cymene + toluene, 4.1%, 12.2 μg C m −2 h −1 ), m/z 45.033 (acetaldehyde, 3.8%, 11.5 μg C m −2 h −1 ), m/z 71.048 (methylvinylketone + methacrolein, 2.4%, 7.1 μg C m −2 h −1 ), and m/z 69.071 (isoprene + 2-methyl-3-butene-2-ol, 1.8%, 5.3 μg C m −2 h −1 ). Low levels of emission and/or deposition (

Eddy covariance emission and deposition flux measurements using proton transfer reaction-time of flight-mass spectrometry (PTR-TOF-MS): comparison with PTR-MS measured vertical gradients and fluxes

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