Please wait a minute...
Shopping Cart Email List Chinese
Advanced Search Fig/Tab
Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Featured Articles  |  Most Downloaded  |  Most Reading
Online Submission Subscribe to Our RSS Content Feed
Front. Environ. Sci. Eng.    2016, Vol. 10 Issue (5) : 12    https://doi.org/10.1007/s11783-016-0861-y
RESEARCH ARTICLE
Characteristics and mixing state of S-rich particles in haze episodes in Beijing
Jun Hu1,2,3,Fengkui Duan1,2,3,*(),Kebin He1,2,3,*(),Yongliang Ma1,2,3,Shuping Dong4,Xiande Liu5
1. State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
2. State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, Tsinghua University, Beijing 100084, China
3. Beijing Key Laboratory of Indoor Air Quality Evaluation and Control (Tsinghua University), Beijing 100084, China
4. Sino-Japan Friendship Environmental Protection Center, Beijing 100029, China
5. Chinese Research Academy of Environmental Sciences, Beijing 100029, China
 Download: PDF(1453 KB)   HTML
 Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
Abstract

Four types of S-rich particles are identified by SEM/FESEM-EDX

With on-line observation, characteristics of S-rich particles are discovered

Intensities of formation of S-rich particles are seasonally different

Direct individual analysis using Scanning Electron Microscopy combined with online observation was conducted to examine the S-rich particles in PM2.5 of two typical polluted haze episodes in summer and winter from 2014 to 2015 in Beijing. Four major types of S-rich particles, including secondary CaSO4 particles (mainly observed in summer), S-rich mineral particles (SRM), S-rich water droplets (SRW) and (C, O, S)-rich particles (COS) were identified. We found the different typical morphologies and element distributions of S-rich particles and considered that (C, O, S)-rich particles had two major mixing states in different seasons. On the basis of the S-rich particles’ relative abundances, S concentrations and their relationships with PM2.5 as well as the seasonal comparison, we revealed that the S-participated formation degrees of SRM and SRW would enhance with increasing PM2.5 concentration. Moreover, C-rich matter and sulfate had seasonally different but significant impacts on the formation of COS.
Keywords S-rich particles      Morphology      Element distribution      Mixing state     
PACS:     
Fund: 
Corresponding Author(s): Fengkui Duan,Kebin He   
Issue Date: 12 July 2016
 Cite this article:   
Jun Hu,Fengkui Duan,Kebin He, et al. Characteristics and mixing state of S-rich particles in haze episodes in Beijing[J]. Front. Environ. Sci. Eng., 2016, 10(5): 12.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-016-0861-y
https://academic.hep.com.cn/fese/EN/Y2016/V10/I5/12
season number sampling time AQI season number sampling time AQI
summer A 11:48–12:13, 28 June, 2014 34 winter a 15:18–15:4311 Jan., 2015 32
B 17:14–17:2830 June, 2014 156 b 9:13–9:1712 Jan., 2015 200
C 14:45–14:531 July, 2014 190 c 18:18–18:2412 Jan., 2015 167
D 9:30–9:422 July, 2014 63 d 23:56–23:59 12 Jan., 2015 270
E 14:00–14:102 July, 2014 99 e 8:30–8:34 13 Jan., 2015 208
F 17:30–17:392 July, 2014 109 f 15:43–15:4913 Jan., 2015 152
G 10:20–10:253 July, 2014 292 g 22:28–22:3213 Jan., 2015 197
H 14:18–14:233 July, 2014 245 h 8:39–8:4314 Jan., 2015 209
I 18:00–18:053 July, 2014 219 i 16:11–16:1414 Jan., 2015 303
j 22:33–22:3614 Jan., 2015 290
k 8:24–8:2615 Jan., 2015 358
l 15:09–15:1015 Jan., 2015 430
m 22:24–22:2515 Jan., 2015 487
n 8:21–8:5116 Jan., 2015 19
Tab.1  Information on filter sampling
Fig.1  Online observations of focus haze episodes in summer and winter. (a) Time series of PM2.5, sulfate in PM2.5, SOR and gas pollutants. (b) Water in PM2.5 and meteorological parameters
Fig.2  Frequency of elements in detected particles
Fig.3  Morphologies, chemical compositions and elements correlative analyses of secondary CaSO4 and SRM. (a) Two morphologies with different scanning time of one secondary CaSO4 in summer episode and its element distribution. Red arrows point to water parts. (b) Relationship between S at.% and Ca at.% of all secondary CaSO4 particles. (c) Morphology of one typical SRM in winter episode and its element distribution. Red arrows point to Ca/S. (d) Relationships between S at.% and Ca at.%, Mg at.%, Si at.% and Na at.% of all SRM particles in summer episode and winter episode, respectively
Fig.4  Morphologies, chemical compositions and elements correlative analyses of SRW and SRO. (a) Morphologies of two typical SRW particles in summer episode and winter episode, respectively. Corresponding elemental mapping pictures of S distribution are on the bottom right corners. (b) Relationship between S at.% and O at.% of all SRW particles in summer episode and winter episode, respectively. (c) Morphologies of two typical COS particles in summer episode and winter episode, respectively. Red arrows point to C-rich matter. Their elemental mapping pictures of C, O, S elements distribution are presented
Fig.5  Relative abundance (%) variation trend of three types of S-rich particles with PM2.5 concentration
Fig.6  Variation trend of S at.% and at.% ratios of S-rich particles in summer episode (a) and winter episode (b), respectively
1 Huang R J, Zhang Y, Bozzetti C, Ho K F, Cao J J, Han Y, Daellenbach K R, Slowik J G, Platt S M, Canonaco F, Zotter P, Wolf R, Pieber S M, Bruns E A, Crippa<?Pub Caret1?> M, Ciarelli G, Piazzalunga A, Schwikowski M, Abbaszade G, Schnelle-Kreis J, Zimmermann R, An Z, Szidat S, Baltensperger U, El Haddad I, Prévôt A S H. High secondary aerosol contribution to particulate pollution during haze events in China. Nature, 2014, 514(7521): 218–222
pmid: 25231863
2 Zheng G J, Duan F K, Su H, Ma Y L, Cheng Y, Zheng B, Zhang Q, Huang T, Kimoto T, Chang D, Poeschl U, Cheng Y F, He K B. Exploring the severe winter haze in Beijing: the impact of synoptic weather, regional transport and heterogeneous reactions. Atmospheric Chemistry and Physics, 2015, 15(6): 2969–2983
https://doi.org/10.5194/acp-15-2969-2015
3 Went F W. Blue hazes in the atmosphere. Nature, 1960, 187(4738): 641–643
https://doi.org/10.1038/187641a0
4 Yu L E, Shulman M L, Kopperud R, Hildemann L M. Characterization of organic compounds collected during southeastern aerosol and visibility study: water-soluble organic species. Environmental Science & Technology, 2005, 39(3): 707–715
https://doi.org/10.1021/es0489700 pmid: 15757330
5 Lu F, Xu D, Cheng Y, Dong S, Guo C, Jiang X, Zheng X. Systematic review and meta-analysis of the adverse health effects of ambient PM2.5 and PM10 pollution in the Chinese population. Environmental Research, 2015, 136: 196–204
https://doi.org/10.1016/j.envres.2014.06.029 pmid: 25460637
6 Clarke A, Kapustin V. Hemispheric aerosol vertical profiles: anthropogenic impacts on optical depth and cloud nuclei. Science, 2010, 329(5998): 1488–1492
https://doi.org/10.1126/science.1188838 pmid: 20847262
7 von Schneidemesser E, Monks P S, Allan J D, Bruhwiler L, Forster P, Fowler D, Lauer A, Morgan W T, Paasonen P, Righi M, Sindelarova K, Sutton M A. Chemistry and the linkages between air quality and climate change. Chemical Reviews, 2015, 115(10): 3856–3897
https://doi.org/10.1021/acs.chemrev.5b00089 pmid: 25926133
8 He K B, Yang F M, Ma Y L, Zhang Q, Yao X H, Chan C K, Cadle S, Chan T, Mulawa P. The characteristics of PM2.5 in Beijing, China. Atmospheric Environment, 2001, 35(29): 4959–4970
https://doi.org/10.1016/S1352-2310(01)00301-6
9 Markku K, Tuukka P, Veli-Matti K, Joni K, Taina R, Aijun DWei N, Min H, Zhibin W, Zhijun W, Lin W, Douglas R W.On secondary new particle formation in China. Frontiers of Environmental Science & Engineering, 2016, 10(5): 08
10 Xu L, Guo H, Boyd C M, Klein M, Bougiatioti A, Cerully K M, Hite J R, Isaacman-VanWertz G, Kreisberg N M, Knote C, Olson K, Koss A, Goldstein A H, Hering S V, de Gouw J, Baumann K, Lee S H, Nenes A, Weber R J, Ng N L. Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States. Proceedings of the National Academy of Sciences of the United States of America, 2015, 112(1): 37–42
https://doi.org/10.1073/pnas.1417609112 pmid: 25535345
11 Satsangi P G, Yadav S. Characterization of PM2.5 by X-ray diffraction and scanning electron microscopy-energy dispersive spectrometer: its relation with different pollution sources. International Journal of Environmental Science and Technology, 2014, 11(1): 217–232
https://doi.org/10.1007/s13762-012-0173-0
12 Liu X, Zhu J, Van Espen P, Adams F, Xiao R, Dong S, Li Y. Single particle characterization of spring and summer aerosols in Beijing: formation of composite sulfate of calcium and potassium. Atmospheric Environment, 2005, 39(36): 6909–6918
https://doi.org/10.1016/j.atmosenv.2005.08.007
13 Song Y C, Eom H J, Jung H J, Malek M A, Kim H K, Geng H, Ro C U. Investigation of aged Asian dust particles by the combined use of quantitative ED-EPMA and ATR-FTIR imaging. Atmospheric Chemistry and Physics, 2013, 13(6): 3463–3480
https://doi.org/10.5194/acp-13-3463-2013
14 Geng H, Ryu J Y, Maskey S, Jung H J, Ro C U. Characterisation of individual aerosol particles collected during a haze episode in Incheon, Korea using the quantitative ED-EPMA technique. Atmospheric Chemistry and Physics, 2011, 11(3): 1327–1337
https://doi.org/10.5194/acp-11-1327-2011
15 Li W, Shi Z, Yan C, Yang L, Dong C, Wang W. Individual metal-bearing particles in a regional haze caused by firecracker and firework emissions. Science of the Total Environment, 2013, 443: 464–469
https://doi.org/10.1016/j.scitotenv.2012.10.109 pmid: 23208278
16 Li W, Shao L, Shen R, Yang S, Wang Z, Tang U. Internally mixed sea salt, soot, and sulfates at Macao, a coastal city in South China. Journal of the Air & Waste Management Association, 2011, 61(11): 1166–1173
pmid: 22168100
17 Li W, Chi J, Shi Z, Wang X, Chen B, Wang Y, Li T, Chen J, Zhang D, Wang Z, Shi C, Liu L, Wang W. Composition and hygroscopicity of aerosol particles at Mt. Lu in South China: implications for acid precipitation. Atmospheric Environment, 2014, 94: 626–636
https://doi.org/10.1016/j.atmosenv.2014.06.003
18 Seinfeld J H, Pandis S N. Atomspheric Chemistry and Physics. Canada: John Wiley & Sons, Inc. 2006, 284–387
19 Hu G, Zhang Y, Sun J, Zhang L, Shen X, Lin W, Yang Y. Variability, formation and acidity of water-soluble ions in PM2.5 in Beijing based on the semi-continuous observations. Atmospheric Research, 2014, 145–146(0): 1–11
https://doi.org/10.1016/j.atmosres.2014.03.014
20 Duan F, He K, Ma Y, Jia Y, Yang F, Lei Y, Tanaka S, Okuta T. Characteristics of carbonaceous aerosols in Beijing, China. Chemosphere, 2005, 60(3): 355–364
https://doi.org/10.1016/j.chemosphere.2004.12.035 pmid: 15924954
21 Ianniello A, Spataro F, Esposito G, Allegrini I, Hu M, Zhu T. Chemical characteristics of inorganic ammonium salts in PM2.5 in the atmosphere of Beijing (China). Atmospheric Chemistry and Physics, 2011, 11(21): 10803–10822
https://doi.org/10.5194/acp-11-10803-2011
22 Yin H, Mu S Y, Zhao L, Qi X L, Pan X L. Microscopic morphology and elemental composition of size distributed atmospheric particulate matter in Urumqi, China. Environmental Earth Sciences, 2013, 69(7): 2139–2150
https://doi.org/10.1007/s12665-012-2043-y
23 Qu W J, Wang J, Zhang X Y, Wang D, Sheng L F. Influence of relative humidity on aerosol composition: impacts on light extinction and visibility impairment at two sites in coastal area of China. Atmospheric Research, 2015, 153: 500–511
https://doi.org/10.1016/j.atmosres.2014.10.009
24 Zhang Q, Geng G, Wang S, Richter A, He K. Satellite remote sensing of changes in NOx emissions over China during 1996–2010. Chinese Science Bulletin, 2012, 57(22): 2857–2864
https://doi.org/10.1007/s11434-012-5015-4
25 Xiao R, Liu X, Liang H, Dong S, Adams F. Analytical characterization of single particle of atmospheric aerosols in spring and summer seasons in Beijing. Rock and Mineral Analysis, 2004, 23(2): 125–131
26 Matsuki A, Iwasaka Y, Shi G Y, Zhang D Z, Trochkine D, Yamada M, Kim Y S, Chen B, Nagatani T, Miyazawa T, Nagatani M, Nakata H. Morphological and chemical modification of mineral dust: observational insight into the heterogeneous uptake of acidic gases. Geophysical Research Letters, 2005, 32(22), doi: 10.1029/2005GL024176
27 Zhang Y X, Yang Z H, Zhang Q X, Li R J, Geng H, Dong C. Chemical compositions and effects on chemiluminescence of AMs in vitro of chalk dusts. Chinese Chemical Letters, 2015, 26(1): 157–159
https://doi.org/10.1016/j.cclet.2014.08.004
28 Hwang H, Ro C U. Direct observation of nitrate and sulfate formations from mineral dust and sea-salts using low-Z particle electron probe X-ray microanalysis. Atmospheric Environment, 2006, 40(21): 3869–3880
https://doi.org/10.1016/j.atmosenv.2006.02.022
29 Geng H, Hwang H, Liu X, Dong S, Ro C U. Investigation of aged aerosols in size-resolved Asian dust storm particles transported from Beijing, China, to Incheon, Korea, using low-Z particle EPMA. Atmospheric Chemistry and Physics, 2014, 14(7): 3307–3323
https://doi.org/10.5194/acp-14-3307-2014
30 Marszałek M, Alexandrowicz Z, Rzepa G. Composition of weathering crusts on sandstones from natural outcrops and architectonic elements in an urban environment. Environmental Science and Pollution Research International, 2014, 21(24): 14023–14036
https://doi.org/10.1007/s11356-014-3312-y pmid: 25037099
31 Maskey S, Chong K Y, Kim G, Kim J S, Ali A, Park K. Effect of mixing structure on the hygroscopic behavior of ultrafine ammonium sulfate particles mixed with succinic acid and levoglucosan. Particuology, 2014, 13(0): 27–34
https://doi.org/10.1016/j.partic.2013.08.004
32 Denjean C, Formenti P, Picquet-Varrault B, Katrib Y, Pangui E, Zapf P, Doussin J F. A new experimental approach to study the hygroscopic and optical properties of aerosols: application to ammonium sulfate particles. Atmospheric Measurement Techniques, 2014, 7(1): 183–197
https://doi.org/10.5194/amt-7-183-2014
33 Li W, Shao L. Mixing and water-soluble characteristics of particulate organic compounds in individual urban aerosol particles. Journal of Geophysical Research, D, Atmospheres, 2010, 115,
https://doi.org/10.1029/2009JD012575
34 Li W J, Shao L Y, Buseck P R. Haze types in Beijing and the influence of agricultural biomass burning. Atmospheric Chemistry and Physics, 2010, 10(17): 8119–8130
https://doi.org/10.5194/acp-10-8119-2010
35 Zhou Q, Pang S F, Wang Y, Ma J B, Zhang Y H. Confocal Raman studies of the evolution of the physical state of mixed phthalic acid/ammonium sulfate aerosol droplets and the effect of substrates. Journal of Physical Chemistry B, 2014, 118(23): 6198–6205
https://doi.org/10.1021/jp5004598 pmid: 24839869
[1] Juntao HUO,Xiaohui LU,Xinning WANG,Hong CHEN,Xingnan YE,Song Gao,Deborah S. Gross,Jianmin CHEN,Xin YANG. Online single particle analysis of chemical composition and mixing state of crop straw burning particles: from laboratory study to field measurement[J]. Front. Environ. Sci. Eng., 2016, 10(2): 244-252.
[2] Yuankai ZHANG,Zhijiang HE,Hongchen WANG,Lu QI,Guohua LIU,Xiaojun ZHANG. Applications of hollow nanomaterials in environmental remediation and monitoring: A review[J]. Front. Environ. Sci. Eng., 2015, 9(5): 770-783.
[3] Jing FENG,Yili WANG,Xueyuan JI,Dongqin YUAN,Hui LI. Performance and bioparticle growth of anaerobic baffled reactor (ABR) fed with low-strength domestic sewage[J]. Front. Environ. Sci. Eng., 2015, 9(2): 352-364.
Viewed
Full text


Abstract

Cited
  Shared   
  Discussed