Development of an automatic linear calibration method for high-resolution single-particle mass spectrometry: improved chemical species identification for atmospheric aerosols

Zhu, Shengqiang1; Li, Lei2; Wang, Shurong1; Li, Mei2; Liu, Yaxi1; Lu, Xiaohui1; Chen, Hong1; Wang, Lin1,3; Chen, Jianmin1,3; Zhou, Zhen2; Yang, Xin1,3,4; Wang, Xiaofei1,3

2020-08-03

10.5194/amt-13-4111-2020

Atmospheric Measurement Techniques   影响因子和分区

1867-1381

1867-8548

The mass resolution of laser desorption ionization (LDI) single-particle aerosol mass spectrometry (SPAMS) is usually low (similar to 500), which has been greatly improved by the recent development of the delayed ion extraction technique. However, due to large fluctuations among LDI processes during each laser shot, accurate calibration of the mass-to-charge ratio for high-resolution SPAMS (HR-SPAMS) spectra is challenging. Here we developed an automatic linear calibration method to improve the accuracy of mass-to-charge (m/z) measurement for single atmospheric aerosol particles. Laboratory-generated sea spray aerosol and atmospheric ambient aerosol were tested. After the calibration, the fluctuation ranges of the reference ions' (e.g., Pb+ and SO4+) m/z reaches +/- 0.018 for sea spray aerosol and +/- 0.024 for ambient aerosol in average mass spectra. With such m/z accuracy, the HR-SPAMS spectra of sea spray aerosol can easily identify elemental compositions of organic peaks, such as C-x, CxHy and CxHyOz. While the chemical compositions of ambient aerosols are more complicated, CxHy, CxHyOz, and CNO peaks can also be identified based on their accurate mass. With the improved resolution, the time series of peaks with small m/z differences can be separated and measured. In addition, it is also found that applying high-resolution data with enhanced mass calibration can significantly affect particle classification (identification) using the ART-2a algorithm, which classify particles based on similarities among single-particle mass spectra.

SCI

英语

通讯

National Natural Science Foundation of China[41827804][41775150][21906024][91544224] ; Shanghai Natural Science Foundation[19ZR1404000]

Meteorology & Atmospheric Sciences

Meteorology & Atmospheric Sciences

WOS:000558715500002

COPERNICUS GESELLSCHAFT MBH

Web of Science

1.Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China
2.Jinan Univ, Inst Mass Spectrometer & Atmospher Environm, Guangzhou 510632, Peoples R China
3.Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China
4.Southern Univ Sci & Technol, Sch Environm Sci & Engn, Shenzhen 518055, Peoples R China

Zhu, Shengqiang,Li, Lei,Wang, Shurong,et al. Development of an automatic linear calibration method for high-resolution single-particle mass spectrometry: improved chemical species identification for atmospheric aerosols[J]. Atmospheric Measurement Techniques,2020,13(8):4111-4121.

Zhu, Shengqiang.,Li, Lei.,Wang, Shurong.,Li, Mei.,Liu, Yaxi.,...&Wang, Xiaofei.(2020).Development of an automatic linear calibration method for high-resolution single-particle mass spectrometry: improved chemical species identification for atmospheric aerosols.Atmospheric Measurement Techniques,13(8),4111-4121.

Zhu, Shengqiang,et al."Development of an automatic linear calibration method for high-resolution single-particle mass spectrometry: improved chemical species identification for atmospheric aerosols".Atmospheric Measurement Techniques 13.8(2020):4111-4121.