Characterization and source apportionment of organic aerosol at 260 m on a meteorological tower in Beijing, China
-
Published:2018-03-20
Issue:6
Volume:18
Page:3951-3968
-
ISSN:1680-7324
-
Container-title:Atmospheric Chemistry and Physics
-
language:en
-
Short-container-title:Atmos. Chem. Phys.
Author:
Zhou Wei, Wang Qingqing, Zhao Xiujuan, Xu Weiqi, Chen Chen, Du WeiORCID, Zhao Jian, Canonaco Francesco, Prévôt André S. H., Fu PingqingORCID, Wang Zifa, Worsnop Douglas R., Sun YeleORCID
Abstract
Abstract. Despite extensive efforts toward the
characterization of submicron aerosols at ground level in the megacity of
Beijing, our understanding of aerosol sources and processes at high altitudes
remains low. Here we conducted a 3-month real-time
measurement of non-refractory submicron aerosol (NR-PM1) species at
a height of 260 m from 10 October 2014 to 18 January 2015 using an
aerosol chemical speciation monitor. Our results showed a significant change
in aerosol composition from the non-heating period (NHP) to the heating period (HP).
Organics and chloride showed clear increases during HP due to coal combustion
emissions, while nitrate showed substantial decreases from 28 to
15–18 %. We also found that NR-PM1 species in the heating season
can have average mass differences of 30–44 % under similar emission
sources yet different meteorological conditions. Multi-linear engine 2 (ME-2)
using three primary organic aerosol (OA) factors as constraints, i.e., fossil-fuel-related
OA (FFOA) dominantly from coal combustion emissions, cooking OA (COA), and
biomass burning OA (BBOA) resolved from ground high-resolution aerosol mass
spectrometer measurements, was applied to OA mass spectra of
ACSM. Two types of secondary OA (SOA) that were well correlated with nitrate
and chloride–CO, respectively, were identified. SOA played a dominant role in
OA during all periods at 260 m although the contributions were
decreased from 72 % during NHP to 58–64 % during HP. The SOA
composition also changed significantly from NHP to HP. While the contribution
of oxygenated OA (OOA) was decreased from 56–63 to 32–40 %, less
oxidized OOA (LO-OOA) showed a large increase from 9–16 to
24–26 %. COA contributed a considerable fraction of OA at high altitude,
and the contribution was relatively similar across different periods
(10–13 %). In contrast, FFOA showed a large increase during HP due to
the influences of coal combustion emissions. We also observed very different
OA composition between ground level and 260 m. Particularly, the
contributions of COA and BBOA at the ground site were nearly twice those at
260 m, while SOA at 260 m was ∼ 15–34 % higher
than that at ground level. Bivariate polar plots and back-trajectory analysis
further illustrated the different source regions of OA factors in different
seasons.
Publisher
Copernicus GmbH
Subject
Atmospheric Science
Reference54 articles.
1. Aiken, A. C., DeCarlo, P. F., Kroll, J. H., Worsnop, D. R., Huffman, J. A.,
Docherty, K. S., Ulbrich, I. M., Mohr, C., Kimmel, J. R., Sueper, D.,
Sun, Y., Zhang, Q., Trimborn, A., Northway, M., Ziemann, P. J.,
Canagaratna, M. R., Onasch, T. B., Alfarra, M. R., Prevot, A. S. H.,
Dommen, J.,<span id="page3966"/> Duplissy, J., Metzger, A., Baltensperger, U., and Jimenez, J. L.:
O∕C and OM∕OC ratios of primary, secondary,
and ambient organic aerosols with high-resolution time-of-flight aerosol mass
spectrometry, Environ. Sci. Technol., 42, 4478–4485,
https://doi.org/10.1021/es703009q, 2008. 2. Aiken, A. C., Salcedo, D., Cubison, M. J., Huffman, J. A., DeCarlo, P. F.,
Ulbrich, I. M., Docherty, K. S., Sueper, D., Kimmel, J. R., Worsnop, D. R.,
Trimborn, A., Northway, M., Stone, E. A., Schauer, J. J., Volkamer, R. M.,
Fortner, E., de Foy, B., Wang, J., Laskin, A., Shutthanandan, V., Zheng, J.,
Zhang, R., Gaffney, J., Marley, N. A., Paredes-Miranda, G., Arnott, W. P.,
Molina, L. T., Sosa, G., and Jimenez, J. L.: Mexico City aerosol analysis
during MILAGRO using high resolution aerosol mass spectrometry at the urban
supersite (T0) – Part 1: Fine particle composition and organic source
apportionment, Atmos. Chem. Phys., 9, 6633–6653,
https://doi.org/10.5194/acp-9-6633-2009, 2009. 3. Allan, J. D., Williams, P. I., Morgan, W. T., Martin, C. L., Flynn, M. J.,
Lee, J., Nemitz, E., Phillips, G. J., Gallagher, M. W., and Coe, H.:
Contributions from transport, solid fuel burning and cooking to primary
organic aerosols in two UK cities, Atmos. Chem. Phys., 10, 647–668,
https://doi.org/10.5194/acp-10-647-2010, 2010. 4. Canonaco, F., Crippa, M., Slowik, J. G., Baltensperger, U., and
Prévôt, A. S. H.: SoFi, an IGOR-based interface for the efficient use
of the generalized multilinear engine (ME-2) for the source apportionment:
ME-2 application to aerosol mass spectrometer data, Atmos. Meas. Tech., 6,
3649–3661, https://doi.org/10.5194/amt-6-3649-2013, 2013. 5. Chen, C., Sun, Y. L., Xu, W. Q., Du, W., Zhou, L. B., Han, T. T.,
Wang, Q. Q., Fu, P. Q., Wang, Z. F., Gao, Z. Q., Zhang, Q., and
Worsnop, D. R.: Characteristics and sources of submicron aerosols above the
urban canopy (260 m) in Beijing, China, during the 2014 APEC summit, Atmos.
Chem. Phys., 15, 12879–12895, https://doi.org/10.5194/acp-15-12879-2015, 2015.
Cited by
27 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献
|
|