Subscriber access provided by SWINBURNE UNIV OF TECHNOLOGY
Article
Source Impact Determination using Airborne and Ground Measurements of Industrial Plumes Cecilia Leoni, Jan Hovorka, Veronika Docekalova, Tomas Cajthaml, and Sona Marvanova Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.6b02304 • Publication Date (Web): 22 Aug 2016 Downloaded from http://pubs.acs.org on August 24, 2016
Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.
Environmental Science & Technology is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.
Page 1 of 26
Environmental Science & Technology
1
Source Impact Determination using Airborne and Ground Measurements of
2
Industrial Plumes
3
Cecilia Leoni1, Jan Hovorka*1, Veronika Dočekalová1, Tomáš Cajthaml1, Soňa Marvanová2
4
1
5
128 01 Prague 2, Czech Republic.
6
2
7
Brno, Czech Republic.
8
Corresponding author: Jan Hovorka, Institute for Environmental Studies, Faculty of Science, Charles
9
University in Prague, Benátská 2, 128 01 Prague 2, Czech Republic
10
Institute for Environmental Studies, Faculty of Science, Charles University in Prague, Benátská 2,
Department of Chemistry and Toxicology, Veterinary Research Institute, Hudcova 296/70, 621 00
T: +420 221951910, Fax: +420 224914803; e-mail:
[email protected] 11 12
Abstract
13
Industrial particulate matter (PM) air pollution exposing nearby residential areas forms several
14
European air pollution hot-spots. One of these hot-spot is the residential district of Ostrava Radvanice-
15
Bartovice with frequent exceedances for PM and benzo[a]pyrene B[a]P, a carcinogenic polycyclic
16
aromatic hydrocarbon (PAH) of MW>228 amu. Such PAHs are highly bonded to the ultrafine particles
17
(UFPs), the smallest PM size fraction, which deposits most efficiently in the alveolar region of human
18
lungs. Airborne measurements identified UFP point sources in the adjacent metallurgical complex and
19
mapped limited horizontal and vertical dispersion of industrial plumes enriched with UFPs
20
(3.2x105cm-3). The plumes, episodes of simultaneous peaks of UFPs (1.4 x105cm-3), SO2 (88.2ppb),
21
and CO (11.3ppm), were recorded on the ground downwind in the residential district when wind
22
speeds >1ms-1. In the plumes, UFPs were mostly 19-44 nm in diameter, enriched with PAHs / B[a]P 1 ACS Paragon Plus Environment
Environmental Science & Technology
Page 2 of 26
23
up to 43.8 / 3.5 mg.g-1. Electron microscopy showed that these plume UFPs were mostly agglomerates
24
of spherules of 30–50 nm in diameter. These source impact measurements, that combine airborne and
25
ground-level measurements, are applicable to clearly identify specific industrial air pollution sources
26
and provide information to assess their possible impact to human health in similar hot-spots
27
worldwide.
28 29
Keywords: ultrafine aerosol, coarse aerosol, carcinogenic polycyclic aromatic hydrocarbons, airship,
30
metallurgy
31
Graphical abstract
32 33
2 ACS Paragon Plus Environment
Page 3 of 26
Environmental Science & Technology
34
Introduction
35
In recent years, studies of the atmospheric aerosol have acquired major importance due to the relevance
36
to climate and to human health. The adverse health effects of aerosol particles have been demonstrated
37
by toxicological and epidemiological studies.1,2 Atmospheric particles include also ultrafine particles
38
(UFPs). The UFPs are the smallest aerosol particles in the atmosphere, with an aerodynamic diameter
39
(dae) of approximately < 0.150 nm. The high particle number concentration in the air and the high lung
40
deposition efficiency make UFPs particularly hazardous to human health.3
41
The UFPs can be either directly emitted from the combustion processes (primary particles) or formed
42
by nucleation from precursor vapors (secondary particles). Emissions of stationary combustion
43
sources such as industrial stack plumes can contain a high UFPs number. Depending on the plume
44
characteristics and the meteorological conditions, the particles can be spread from the stack to the
45
nearby areas. Studies performed at a receptor site in the vicinity of industrial plants have observed the
46
presence of UFPs when downwind from the emission source.4,5,6 The UFPs concentration and the size
47
distribution evolve very quickly once emitted into the atmosphere, influenced by numerous
48
parameters: meteorology (wind speed/direction, boundary layer height) concentration of precursor
49
gases (SO2 and NOx) and concentration of pre-existing particles.7 The fast changes and the transient
50
nature of the plumes require high time-resolved measurements, which can reveal short pollution events
51
in the atmosphere.
52
Evidence now shows that UFPs carry considerable amount of toxics, and also polycyclic aromatic
53
hydrocarbons (PAHs).3,8, 9,10 PAHs are persistent organic pollutants originated from the incomplete
54
combustion of fossil fuels and wood, and they have been associated with respiratory diseases and
55
cancer.11,12 PAHs are present in various size fractions in the particulate matter. Close to the emission
3 ACS Paragon Plus Environment
Environmental Science & Technology
Page 4 of 26
56
source the PAHs’ mass size distribution peaks in the ultrafine (