O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry

被引：1195

作者：

Aiken, Allison C. ^{[1
,2
]}

Decarlo, Peter F. ^{[2
,3
]}

Kroll, Jesse H. ^{[4
]}

Worsnop, Douglas R. ^{[4
]}

Huffman, J. Alex ^{[1
,2
]}

Docherty, Kenneth S. ^{[2
]}

Ulbrich, Ingrid M. ^{[1
,2
]}

Mohr, Claudia ^{[2
]}

Kimmel, Joel R. ^{[2
]}

Sueper, Donna ^{[2
]}

Sun, Yele ^{[5
]}

Zhang, Qi ^{[5
]}

Trimborn, Achim ^{[4
]}

Northway, Megan ^{[4
]}

Ziemann, Paul J. ^{[6
]}

Canagaratna, Manjula R. ^{[4
]}

Onasch, Timothy B. ^{[4
]}

Alfarra, M. Rami ^{[7
]}

Prevot, Andre S. H. ^{[7
]}

Dommen, Josef ^{[7
]}

Duplissy, Jonathan ^{[7
]}

Metzger, Axel ^{[7
]}

Baltensperger, Urs ^{[7
]}

Jimenez, Jose L. ^{[1
,2
]}

机构：

[1] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA

[2] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA

[3] Univ Colorado, Dept Atmospher & Ocean Sci ATOC, Boulder, CO 80309 USA

[4] Aerodyne Res Inc, Billerica, MA 01821 USA

[5] SUNY Albany, Atmospher Sci Res Ctr, Albany, NY 12222 USA

[6] Univ Calif Riverside, Dept Environm Sci, Riverside, CA 92521 USA

[7] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland

来源：

ENVIRONMENTAL SCIENCE & TECHNOLOGY | 2008年 / 42卷 / 12期

基金：

英国自然环境研究理事会;

关键词：

D O I：

10.1021/es703009q

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

A recently developed method to rapidly quantify the elemental composition of bulk organic aerosols (OA) using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is improved and applied to ambient measurements. Atomic oxygen-to-carbon (O/C) ratios characterize the oxidation state of OA, and O/C from ambient urban OA ranges from 0.2 to 0.8 with a diurnal cycle that decreases with primary emissions and increases because of photochemical processing and secondary OA (SOA) production. Regional O/C approaches similar to 0.9. The hydrogen-to-carbon (H/C, 1.4-1.9) urban diurnal profile increases with primary CIA (POA) as does the nitrogen-to-carbon WC, similar to 0.02). Ambient organic-mass-to-organic-carbon ratios (OM/OC) are directly quantified and correlate well with O/C (R-2 = 0.997) for ambient OA because of low N/C. Ambient O/C and OWN have values consistent with those recently reported from other techniques. Positive matrix factorization applied to ambient OA identifies factors with distinct O/C and OM/OC trends. The highest O/C and OM/OC (1.0 and 2.5, respectively) are observed for aged ambient oxygenated OA, significantly exceeding values for traditional chamber SOA, while laboratory-produced primary biomass burning OA (BBOA) is similar to ambient BBOA, O/C of 0.3-0.4. Hydrocarbon-like OA (HOA), a surrogate for urban combustion POA, has the lowest O/C (0.06-0.10), similar to vehicle exhaust. An approximation for predicting O/C from unit mass resolution data is also presented.

引用

页码：4478 / 4485

页数：8

共 30 条

[1] 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

[2] A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data [J].

Allan, JD ;

Delia, AE ;

Coe, H ;

Bower, KN ;

Alfarra, MR ;

Jimenez, JL ;

Middlebrook, AM ;

Drewnick, F ;

Onasch, TB ;

Canagaratna, MR ;

Jayne, JT ;

Worsnop, DR .

JOURNAL OF AEROSOL SCIENCE, 2004, 35 (07) :909-922

[3] Secondary formation and the Smoky Mountain organic aerosol: An examination of aerosol polarity and functional group composition during SEAVS [J].

Blando, JD ;

Porcja, RJ ;

Li, TH ;

Bowman, D ;

Lioy, PJ ;

Turpin, BJ .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1998, 32 (05) :604-613

[4] Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer [J].

Canagaratna, M. R. ;

Jayne, J. T. ;

Jimenez, J. L. ;

Allan, J. D. ;

Alfarra, M. R. ;

Zhang, Q. ;

Onasch, T. B. ;

Drewnick, F. ;

Coe, H. ;

Middlebrook, A. ;

Delia, A. ;

Williams, L. R. ;

Trimborn, A. M. ;

Northway, M. J. ;

DeCarlo, P. F. ;

Kolb, C. E. ;

Davidovits, P. ;

Worsnop, D. R. .

MASS SPECTROMETRY REVIEWS, 2007, 26 (02) :185-222

[5] Fast airborne aerosol size and chemistry measurements above Mexico City and Central Mexico during the MILAGRO campaign [J].

DeCarlo, P. F. ;

Dunlea, E. J. ;

Kimmel, J. R. ;

Aiken, A. C. ;

Sueper, D. ;

Crounse, J. ;

Wennberg, P. O. ;

Emmons, L. ;

Shinozuka, Y. ;

Clarke, A. ;

Zhou, J. ;

Tomlinson, J. ;

Collins, D. R. ;

Knapp, D. ;

Weinheimer, A. J. ;

Montzka, D. D. ;

Campos, T. ;

Jimenez, J. L. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2008, 8 (14) :4027-4048

[6] 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

[7] Water soluble organic compounds formed by oxidation of soot [J].

Decesari, S ;

Facchini, MC ;

Matta, E ;

Mircea, M ;

Fuzzi, S ;

Chughtai, AR ;

Smith, DM .

ATMOSPHERIC ENVIRONMENT, 2002, 36 (11) :1827-1832

[8] Cloud forming potential of secondary organic aerosol under near atmospheric conditions [J].

Duplissy, J. ;

Gysel, Martin ;

Alfarra, M.R. ;

Dommen, J. ;

Metzger, A. ;

Prevot, A.S.H. ;

Weingartner, E. ;

Laaksonen, A. ;

Raatikainen, T. ;

Good, N. ;

Turner, S.F. ;

McFiggans, G. ;

Baltensperger, U. .

Geophysical Research Letters, 2008, 35 (02)

[9] Oligomers in the early stage of biogenic secondary organic aerosol formation and growth [J].

Heaton, Katherine J. ;

Dreyfus, Matthew A. ;

Wang, Shenyi ;

Johnston, Murray V. .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2007, 41 (17) :6129-6136

[10]

HUFFMAN JA, 2008, VOLATILITY PRI UNPUB

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