Investigations of primary and secondary particulate matter of different wood combustion appliances with a high-resolution time-of-flight aerosol mass spectrometer

被引:159
作者
Heringa, M. F. [1 ]
DeCarlo, P. F. [1 ]
Chirico, R. [1 ]
Tritscher, T. [1 ]
Dommen, J. [1 ]
Weingartner, E. [1 ]
Richter, R. [1 ]
Wehrle, G. [1 ]
Prevot, A. S. H. [1 ]
Baltensperger, U. [1 ]
机构
[1] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland
基金
美国国家科学基金会; 瑞士国家科学基金会;
关键词
ORGANIC AEROSOL; FINE-PARTICLE; AIR-POLLUTION; PHOTOCHEMICAL OXIDATION; LIGHT-ABSORPTION; BLACK CARBON; MEXICO-CITY; EMISSIONS; LEVOGLUCOSAN; URBAN;
D O I
10.5194/acp-11-5945-2011
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A series of photo-oxidation smog chamber experiments were performed to investigate the primary emissions and secondary aerosol formation from two different log wood burners and a residential pellet burner under different burning conditions: starting and flaming phase. Emissions were sampled from the chimney and injected into the smog chamber leading to primary organic aerosol (POA) concentrations comparable to ambient levels. The composition of the aerosol was measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and black carbon (BC) instrumentation. The primary emissions were then exposed to xenon light to initiate photo-chemistry and subsequent secondary organic aerosol (SOA) production. After correcting for wall losses, the average increase in organic matter (OM) concentrations by SOA formation for the starting and flaming phase experiments with the two log wood burners was found to be a factor of 4.1 +/- 1.4 after five hours of aging. No SOA formation was observed for the stable burning phase of the pellet burner. The startup emissions of the pellet burner showed an increase in OM concentration by a factor of 3.3. Including the measured SOA formation potential, average emission factors of BC+POA+SOA, calculated from CO2 emission, were found to be in the range of 0.04 to 3.9 g/kg wood for the stable burning pellet burner and an old log wood burner during startup respectively. SOA contributed significantly to the ion C2H4O2+ at mass to charge ratio m/z 60, a commonly used marker for primary emissions of wood burning. This contribution at m/z 60 can overcompensate for the degradation of levoglucosan leading to an overestimation of the contribution of wood burning or biomass burning to the total OM. The primary organic emissions from the three different burners showed a wide range in O:C atomic ratio (0.19-0.60) for the starting and flaming conditions, which also increased during aging. Primary wood burning emissions have a rather low relative contribution at m/z 43 (f43) to the total organic mass spectrum. The non-oxidized fragment C3H7+ has a considerable contribution at m/z 43 for the fresh OA with an increasing contribution of the oxygenated ion C2H3O+ during aging. After five hours of aging, the OA has a rather low C2H3O+ signal for a given CO2+ fraction, possibly indicating a higher ratio of acid to non-acid oxygenated compounds in wood burning OA compared to other oxygenated organic aerosol (OOA).
引用
收藏
页码:5945 / 5957
页数:13
相关论文
共 46 条
[21]  
Hennigan C.J., 2011, ATMOS CHEM PHYS, V11, P7669, DOI [DOI 10.5194/ACP-11-7669-2011, DOI 10.5194/ACPD-11-11995-2011]
[22]   Levoglucosan stability in biomass burning particles exposed to hydroxyl radicals [J].
Hennigan, Christopher J. ;
Sullivan, Amy P. ;
Collett, Jeffrey L., Jr. ;
Robinson, Allen L. .
GEOPHYSICAL RESEARCH LETTERS, 2010, 37
[23]   Atmospheric Stability of Levoglucosan: A Detailed Laboratory and Modeling Study [J].
Hoffmann, D. ;
Tilgner, A. ;
Iinuma, Y. ;
Herrmann, H. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2010, 44 (02) :694-699
[24]   Evolution of Organic Aerosols in the Atmosphere [J].
Jimenez, J. L. ;
Canagaratna, M. R. ;
Donahue, N. M. ;
Prevot, A. S. H. ;
Zhang, Q. ;
Kroll, J. H. ;
DeCarlo, P. F. ;
Allan, J. D. ;
Coe, H. ;
Ng, N. L. ;
Aiken, A. C. ;
Docherty, K. S. ;
Ulbrich, I. M. ;
Grieshop, A. P. ;
Robinson, A. L. ;
Duplissy, J. ;
Smith, J. D. ;
Wilson, K. R. ;
Lanz, V. A. ;
Hueglin, C. ;
Sun, Y. L. ;
Tian, J. ;
Laaksonen, A. ;
Raatikainen, T. ;
Rautiainen, J. ;
Vaattovaara, P. ;
Ehn, M. ;
Kulmala, M. ;
Tomlinson, J. M. ;
Collins, D. R. ;
Cubison, M. J. ;
Dunlea, E. J. ;
Huffman, J. A. ;
Onasch, T. B. ;
Alfarra, M. R. ;
Williams, P. I. ;
Bower, K. ;
Kondo, Y. ;
Schneider, J. ;
Drewnick, F. ;
Borrmann, S. ;
Weimer, S. ;
Demerjian, K. ;
Salcedo, D. ;
Cottrell, L. ;
Griffin, R. ;
Takami, A. ;
Miyoshi, T. ;
Hatakeyama, S. ;
Shimono, A. .
SCIENCE, 2009, 326 (5959) :1525-1529
[25]   Evaluating tree carbon predictions for beech (Fagus sylvatica L.) in western Germany [J].
Joosten, R ;
Schumacher, J ;
Wirth, C ;
Schulte, A .
FOREST ECOLOGY AND MANAGEMENT, 2004, 189 (1-3) :87-96
[26]   Source apportionment of submicron organic aerosols at an urban site by factor analytical modelling of aerosol mass spectra [J].
Lanz, V. A. ;
Alfarra, M. R. ;
Baltensperger, U. ;
Buchmann, B. ;
Hueglin, C. ;
Prevot, A. S. H. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2007, 7 (06) :1503-1522
[27]   Characterization of aerosol chemical composition with aerosol mass spectrometry in Central Europe: an overview [J].
Lanz, V. A. ;
Prevot, A. S. H. ;
Alfarra, M. R. ;
Weimer, S. ;
Mohr, C. ;
DeCarlo, P. F. ;
Gianini, M. F. D. ;
Hueglin, C. ;
Schneider, J. ;
Favez, O. ;
D'Anna, B. ;
George, C. ;
Baltensperger, U. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (21) :10453-10471
[28]   Chemical Smoke Marker Emissions During Flaming and Smoldering Phases of Laboratory Open Burning of Wildland Fuels [J].
Lee, Taehyoung ;
Sullivan, Amy P. ;
Mack, Laura ;
Jimenez, Jose L. ;
Kreidenweis, Sonia M. ;
Onasch, Timothy B. ;
Worsnop, Douglas R. ;
Malm, William ;
Wold, Cyle E. ;
Hao, Wei Min ;
Collett, Jeffrey L., Jr. .
AEROSOL SCIENCE AND TECHNOLOGY, 2010, 44 (09) :I-V
[29]   Effects of dilution on fine particle mass and partitioning of semivolatile organics in diesel exhaust and wood smoke [J].
Lipsky, EM ;
Robinson, AL .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (01) :155-162
[30]   Fine particle and gaseous emission rates from residential wood combustion [J].
McDonald, JD ;
Zielinska, B ;
Fujita, EM ;
Sagebiel, JC ;
Chow, JC ;
Watson, JG .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2000, 34 (11) :2080-2091