Light-absorbing carbon in Europe - measurement and modelling, with a focus on residential wood combustion emissions

被引:39
作者
Genberg, J. [1 ]
van der Gon, H. A. C. Denier [2 ]
Simpson, D. [3 ,4 ]
Swietlicki, E. [1 ]
Areskoug, H. [5 ]
Beddows, D. [6 ]
Ceburnis, D. [7 ,8 ]
Fiebig, M. [9 ]
Hansson, H. C. [5 ]
Harrison, R. M. [6 ,10 ]
Jennings, S. G. [7 ,8 ]
Saarikoski, S. [11 ]
Spindler, G. [12 ]
Visschedijk, A. J. H. [2 ]
Wiedensohler, A. [12 ]
Yttri, K. E. [9 ]
Bergstrom, R. [13 ,14 ]
机构
[1] Lund Univ, Dept Phys, Div Nucl Phys, S-22362 Lund, Sweden
[2] TNO Netherlands Org Appl Sci Res, Utrecht, Netherlands
[3] Norwegian Meteorol Inst, EMEP MSC W, Oslo, Norway
[4] Chalmers Univ Technol, Dept Earth & Space Sci, S-41296 Gothenburg, Sweden
[5] Stockholm Univ, Dept Appl Environm Sci ITM, S-10691 Stockholm, Sweden
[6] Univ Birmingham, Sch Geog Earth & Environm Sci, Natl Ctr Atmospher Sci, Div Environm Hlth & Risk Management, Birmingham B15 2TT, W Midlands, England
[7] Natl Univ Ireland Galway, Sch Phys, Galway, Ireland
[8] Natl Univ Ireland Galway, Ctr Climate & Air Pollut Studies, Ryan Inst, Galway, Ireland
[9] Norwegian Inst Air Res, NILU, Kjeller, Norway
[10] King Abdulaziz Univ, Ctr Excellence Environm Studies, Dept Environm Sci, Jeddah 21589, Saudi Arabia
[11] Finnish Meteorol Inst, Helsinki 00101, Finland
[12] Leibniz Inst Tropospharenforsch TROPOS, D-04318 Leipzig, Germany
[13] Univ Gothenburg, Dept Chem & Microbiol, S-41296 Gothenburg, Sweden
[14] Swedish Meteorol & Hydrol Inst, S-60176 Norrkoping, Sweden
基金
瑞典研究理事会;
关键词
SIZE-SEGREGATED CHARACTERIZATION; BLACK-CARBON; ELEMENTAL CARBON; ORGANIC-CARBON; AIR-POLLUTION; ABSORPTION-COEFFICIENT; SOURCE APPORTIONMENT; REACTIVE NITROGEN; AEROSOL; PM10;
D O I
10.5194/acp-13-8719-2013
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The atmospheric concentration of elemental carbon (EC) in Europe during the six-year period 2005-2010 has been simulated with the EMEP MSC-W model. The model bias compared to EC measurements was less than 20% for most of the examined sites. The model results suggest that fossil fuel combustion is the dominant source of EC in most of Europe but that there are important contributions also from residential wood burning during the cold seasons and, during certain episodes, also from open biomass burning (wildfires and agricultural fires). The modelled contributions from open biomass fires to ground level concentrations of EC were small at the sites included in the present study, <3% of the long-term average of EC in PM10. The modelling of this EC source is subject to many uncertainties, and it was likely underestimated for some episodes. EC measurements and modelled EC were also compared to optical measurements of black carbon (BC). The relationships between EC and BC (as given by mass absorption cross section, MAC, values) differed widely between the sites, and the correlation between observed EC and BC is sometimes poor, making it difficult to compare results using the two techniques and limiting the comparability of BC measurements to model EC results. A new bottom-up emission inventory for carbonaceous aerosol from residential wood combustion has been applied. For some countries the new inventory has substantially different EC emissions compared to earlier estimates. For northern Europe the most significant changes are much lower emissions in Norway and higher emissions in neighbouring Sweden and Finland. For Norway and Sweden, comparisons to source-apportionment data from winter campaigns indicate that the new inventory may improve model-calculated EC from wood burning. Finally, three different model setups were tested with variable atmospheric lifetimes of EC in order to evaluate the model sensitivity to the assumptions regarding hygroscopicity and atmospheric ageing of EC. The standard ageing scheme leads to a rapid transformation of the emitted hydrophobic EC to hygroscopic particles, and generates similar results when assuming that all EC is aged at the point of emission. Assuming hydrophobic emissions and no ageing leads to higher EC concentrations. For the more remote sites, the observed EC concentration was in between the modelled EC using standard ageing and the scenario treating EC as hydrophobic. This could indicate too-rapid EC ageing in the model in relatively clean parts of the atmosphere.
引用
收藏
页码:8719 / 8738
页数:20
相关论文
共 83 条
[1]   Lessons learnt from the first EMEP intensive measurement periods [J].
Aas, W. ;
Tsyro, S. ;
Bieber, E. ;
Bergstrom, R. ;
Ceburnis, D. ;
Ellermann, T. ;
Fagerli, H. ;
Froelich, M. ;
Gehrig, R. ;
Makkonen, U. ;
Nemitz, E. ;
Otjes, R. ;
Perez, N. ;
Perrino, C. ;
Prevot, A. S. H. ;
Putaud, J. -P. ;
Simpson, D. ;
Spindler, G. ;
Vana, M. ;
Yttri, K. E. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (17) :8073-8094
[2]   Black carbon or brown carbon?: The nature of light-absorbing carbonaceous aerosols [J].
Andreae, M. O. ;
Gelencser, A. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2006, 6 :3131-3148
[3]  
[Anonymous], 1999, VDI24652, V4
[4]  
Arnott WP, 1999, ATMOS ENVIRON, V33, P2845
[5]   Photoacoustic and filter-based ambient aerosol light absorption measurements:: Instrument comparisons and the role of relative humidity -: art. no. 4034 [J].
Arnott, WP ;
Moosmüller, H ;
Sheridan, PJ ;
Ogren, JA ;
Raspet, R ;
Slaton, WV ;
Hand, JL ;
Kreidenweis, SM ;
Collett, JL .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D1)
[6]   Carbonaceous aerosol at a forested and an urban background sites in Southern Finland [J].
Aurela, M. ;
Saarikoski, S. ;
Timonen, H. ;
Aalto, P. ;
Keronen, P. ;
Saarnio, K. ;
Teinila, K. ;
Kulmala, M. ;
Hillamo, R. .
ATMOSPHERIC ENVIRONMENT, 2011, 45 (07) :1394-1401
[7]  
Benedictow A., 2003, DOCUMENTATION VERIFI, P111
[8]   A regional scale multi-layer model for the calculation of long-term transport and deposition of air pollution in Europe [J].
Berge, E ;
Jakobsen, HA .
TELLUS SERIES B-CHEMICAL AND PHYSICAL METEOROLOGY, 1998, 50 (03) :205-223
[9]   Modelling of organic aerosols over Europe (2002-2007) using a volatility basis set (VBS) framework: application of different assumptions regarding the formation of secondary organic aerosol [J].
Bergstrom, R. ;
van der Gon, H. A. C. Denier ;
Prevot, A. S. H. ;
Yttri, K. E. ;
Simpson, D. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (18) :8499-8527
[10]   Regional modeling of carbonaceous aerosols over Europe-focus on secondary organic aerosols [J].
Bessagnet, Bertrand ;
Menut, Laurent ;
Curci, Gabriele ;
Hodzic, Alma ;
Guillaume, Bruno ;
Liousse, Catherine ;
Moukhtar, Sophie ;
Pun, Betty ;
Seigneur, Christian ;
Schulz, Michael .
JOURNAL OF ATMOSPHERIC CHEMISTRY, 2008, 61 (03) :175-202