Analysis of the chemical composition of organic aerosol at the Mt. Sonnblick observatory using a novel high mass resolution thermal-desorption proton-transfer-reaction mass-spectrometer (hr-TD-PTR-MS)

被引:71
作者
Holzinger, R. [1 ]
Kasper-Giebl, A. [2 ]
Staudinger, M. [3 ]
Schauer, G. [3 ]
Rockmann, T. [1 ]
机构
[1] Inst Marine & Atmospher Res Utrecht, NL-3584 CC Utrecht, Netherlands
[2] Vienna Univ Technol, Inst Chem Technol Analyt, A-1040 Vienna, Austria
[3] Cent Inst Meteorol & Geodynam, Vienna, Austria
关键词
ATMOSPHERIC AEROSOLS; ONLINE ANALYSIS; BLACK CARBON; CLIMATE; SECONDARY; PRECIPITATION; RATIOS; PPTV;
D O I
10.5194/acp-10-10111-2010
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
For the first time a high mass resolution thermal desorption proton transfer reaction mass spectrometer (hr-TD-PTR-MS) was deployed in the field to analyze the composition of the organic fraction of aerosols. We report on measurements from the remote Mt. Sonnblick observatory in the Austrian alps (3108 ma.s.l.) during a 7 week period in summer 2009. A total of 638 mass peaks in the range 18-392 Da were detected and quantified in aerosols. An empirical formula was tentatively attributed to 464 of these compounds by custom-made data analysis routines which consider compounds containing C, H, O, N, and S atoms. Most of the other (unidentified) compounds must contain other elements - most likely halogenated compounds. The mean total concentration of all detected compounds was 1.1 mu g m(-3). Oxygenated hydrocarbons constitute the bulk of the aerosol mass (75%) followed by organic nitrogen compounds (9%), inorganic compounds (mostly NH3, 8%), unidentified/halogenated (3.8%), hydrocarbons (2.7%), and organic sulfur compounds (0.8%). The measured O/C ratios are lower than expected and suggest a significant effect from charring. Organic carbon concentrations measured with TD-PTR-MS were about 25% lower than measurements on high volume filter samples.
引用
收藏
页码:10111 / 10128
页数:18
相关论文
共 36 条
[1]   O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry [J].
Aiken, Allison C. ;
Decarlo, Peter F. ;
Kroll, Jesse H. ;
Worsnop, Douglas R. ;
Huffman, J. Alex ;
Docherty, Kenneth S. ;
Ulbrich, Ingrid M. ;
Mohr, Claudia ;
Kimmel, Joel R. ;
Sueper, Donna ;
Sun, Yele ;
Zhang, Qi ;
Trimborn, Achim ;
Northway, Megan ;
Ziemann, Paul J. ;
Canagaratna, Manjula R. ;
Onasch, Timothy B. ;
Alfarra, M. Rami ;
Prevot, Andre S. H. ;
Dommen, Josef ;
Duplissy, Jonathan ;
Metzger, Axel ;
Baltensperger, Urs ;
Jimenez, Jose L. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (12) :4478-4485
[2]   Elemental analysis of organic species with electron ionization high-resolution mass spectrometry [J].
Aiken, Allison. C. ;
DeCarlo, Peter F. ;
Jimenez, Jose L. .
ANALYTICAL CHEMISTRY, 2007, 79 (21) :8350-8358
[3]   Aerosol-cloud-precipitation interactions. Part 1. The nature and sources of cloud-active aerosols [J].
Andreae, M. O. ;
Rosenfeld, D. .
EARTH-SCIENCE REVIEWS, 2008, 89 (1-2) :13-41
[4]   Atmospheric aerosols: Biogeochemical sources and role in atmospheric chemistry [J].
Andreae, MO ;
Crutzen, PJ .
SCIENCE, 1997, 276 (5315) :1052-1058
[5]  
Bascom R, 1996, AM J RESP CRIT CARE, V153, P3, DOI [10.1164/ajrccm.153.2.8564086, 10.1164/ajrccm.153.1.8542133]
[6]   Determination of atmospheric soot carbon with a simple thermal method [J].
Cachier, Helene ;
Bremond, Marie-Pierre ;
Buat-Menard, Patrick .
TELLUS SERIES B-CHEMICAL AND PHYSICAL METEOROLOGY, 1989, 41 (03) :379-390
[7]   CLIMATE FORCING BY ANTHROPOGENIC AEROSOLS [J].
CHARLSON, RJ ;
SCHWARTZ, SE ;
HALES, JM ;
CESS, RD ;
COAKLEY, JA ;
HANSEN, JE ;
HOFMANN, DJ .
SCIENCE, 1992, 255 (5043) :423-430
[8]   Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer [J].
DeCarlo, Peter F. ;
Kimmel, Joel R. ;
Trimborn, Achim ;
Northway, Megan J. ;
Jayne, John T. ;
Aiken, Allison C. ;
Gonin, Marc ;
Fuhrer, Katrin ;
Horvath, Thomas ;
Docherty, Kenneth S. ;
Worsnop, Doug R. ;
Jimenez, Jose L. .
ANALYTICAL CHEMISTRY, 2006, 78 (24) :8281-8289
[9]   Coupled partitioning, dilution, and chemical aging of semivolatile organics [J].
Donahue, NM ;
Robinson, AL ;
Stanier, CO ;
Pandis, SN .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (08) :2635-2643
[10]   Known and unexplored organic constituents in the earth's atmosphere [J].
Goldstein, Allen H. ;
Galbally, Ian E. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2007, 41 (05) :1514-1521