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Key Laboratory of Vegetation Restoration and Management of Degraded Ecosystems, South China Botanical Garden, Chinese
Academy of Sciences, Xingke Road 723, Guangzhou 510650, P.R. China
2
University of Chinese Academy of Sciences, Beijing 100049, P.R. China
3
Institute of Soil Ecology, Helmholtz Zentrum Mnchen, German Research Center for Environmental Health (GmbH), 85764
Neuherberg, Germany
RATIONALE: Aerosols play an important role in depositing metals into forest ecosystems. Better understanding of forest
aerosols with regard to their metal content and their possible sources is of great signicance for air quality and forest
health.
METHODS: Particulate matter with an aerodynamic diameter less than 2.5 m (PM2.5) in aerosols was collected every
month for 20 months using moderate-volume samplers in the Dinghushan (DHS) nature reserve in southern China.
The concentrations of metals (Al, Cd, Mn, Ni, Pb, and Zn) as well as the Pb isotopic ratios in the PM2.5 samples were
measured by inductively coupled plasma mass spectrometry (ICP-MS).
RESULTS: Moderate pollution with aerosol PM2.5 was detected at the DHS nature reserve with the air mass from
mainland China being the predominant PM2.5 source. The high enrichment factors (EFs) for the heavy metals Pb, Cd,
and Zn, as well as the PM2.5 mass concentrations, coupled with backward trajectory analysis, indicated the
anthropogenic origins of the PM2.5 and of the heavy metals in the PM2.5. The Pb isotopic ratios revealed the contributions
from various Pb sources, which varied between seasons.
CONCLUSIONS: Industrial emissions and automobile exhaust from the Pearl River Delta (PRD) primarily contributed to
the anthropogenic Pb in PM2.5, although there was occasionally a contribution from coal combustion during the wet
season. Pb isotopic ratios analyses are helpful for air quality assessment and Pb source tracing. Copyright 2015 John
Wiley & Sons, Ltd.
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EXPERIMENTAL
Site description
The Dinghushan (DHS) nature reserve (11230391123341E,
230921231130N) is located on the northwestern edge of
the PRD (Fig. 1) and has a monsoon-inuenced humid
subtropical climate according to the updated word map of
the Kppen-Geiger climate classication (with symbols
Cwa in which C, w, and a, respectively, represent
temperate, with dry winter, and with hot summer).[29] The
annual average temperature, precipitation and relative
humidity at DHS are 20.9 C, 1956 mm and 81.5%,
respectively, with a distinct dry season (from October to
March) and a distinct wet season (from April to September,
when approximately 70% of the precipitation occurs).[30]
Except for the wind speed, the meteorological conditions
including the temperature, relative humidity, precipitation
and barometric pressure at DHS showed signicant variations
(one-way analysis of variance (ANOVA), P <0.05) between
the dry and wet seasons from 2005 to 2011.[31] The Asian
monsoon appears from the southwest (South China Sea and
Pacic Ocean) in the wet season and from the northeast
(mainland of China) in the dry season.[25] This nature reserve
has experienced long-term (more than three decades)
exposure to atmospheric pollutants (e.g., atmospheric
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Data analysis
The seasonal variances of aerosol mass concentrations, heavy
metal concentrations, and Pb isotopic ratios in PM2.5 samples
between the dry and wet seasons and between air ow
categories were determined via one-way ANOVA using SPSS
18.0 software (IBM Corporation, Armonk, NY, USA). The
gures were drawn using SigmaPlot 10.0 software (Systat
Software GmbH, Erkrath, Germany).
Table 1. The mass concentrations of PM2.5 (g m3) at Dinghushan and their comparison with other regions (data in parentheses
indicate the average)
Site
Dinghushan
Changbai Mountain
Jianfengling
Guangzhou
Hong Kong
Zhongshan
Yangtze River Delta
Yangtze River Delta
Yangtze River Delta
Shanghai
Chongming Island
Nature Reserve
Feb. 2010-Sep.2011 (dry season)
Feb. 2010-Sep. 2011 (wet season)
Feb. 2010-Sep. 2011 (annual mean)
2-10 Aug. 2006
23-28 Jul. 2007
20-26 Nov. 2007
Pearl River Delta
Summer
Nov. 2000- Feb. 2001
27-29 Nov. 2009 haze period
Yangtze River Delta
Winter
Summer
Summer 2011
Sep. 2003 to Jan. 2005
13-15 Jun. 2006
Beijing
Summer 2009
Winter 2009
Mass concentration
(g m3)
15.7156.64 (34.5)
6.7672.90 (39.4)
6.7672.90 (37.3)
20.770.2 (30.8)
20.770.2 (38.8)
12.726.7 (18.0)
78.1 29.7
27.72116.89 (57.4)
180
89.9
28.8
82
17.8217.9 (94.6)
58150 (89.2)
125 29.0
138 57.8
References
This study
This study
This study
Li et al.[23]
Li et al.[23]
Li et al.[23]
Cao et al.[25]
Ho et al.[38]
Chen et al.[39]
Dong et al.[40]
Dong et al.[40]
Cheng et al.[41]
Wang et al.[12]
Li et al.[23]
Song et al.[18]
Song et al.[18]
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Beijing
Beijing
Sampling time
Metals in PM2.5
The concentrations of Al, Cd, Mn, Ni, Pb, and Zn in PM2.5
sampled from February 2010 to September 2011 are
presented in Table 3. The average concentrations of these
metals in PM2.5 throughout the sampling period were in
the following order: Al > Zn > Pb > Mn > Ni > Cd.
Similar to the seasonal patterns of the PM2.5 mass
concentration, the concentrations of the studied metals in
PM2.5 did not show any signicant variations between the
dry and wet seasons. However, the air mass from mainland
China carried signicantly higher Cd and Pb concentrations
than that from the South China Sea (Table 2), as was the
case for the mass concentrations.
The seasonal variation in heavy metals in aerosols could be
affected by the sources, the transportation, and the
meteorological conditions.[37] In this study, the metal concentrations in PM2.5 did not show any signicant difference
between the dry and wet seasons, which was similar to
the seasonal patterns of metals in total suspended
particles at Guangzhou and Foshan, where the dominant
sources of metals in aerosols were local emissions around
the cities.[27,28] During a haze period (October 2004) in
Zhaoqing, where DHS is located, the air pollutants
including particulate matters had mainly diffused from
the central PRD.[42] Anthropogenic emissions within the
PRD are potentially releasing metals into PM2.5, which
could be transported into DHS. To identify the sources
and evaluate the inuence of the anthropogenic emissions
Table 2. Heavy metal concentrations (Cd and Pb), mass concentrations, and Pb isotopic ratios in PM2.5 from different air
mass categories. Data are shown as mean SD. Signicant differences were found for the Cd, Pb, and PM2.5 mass
concentrations between categories
Cd
Categories
Mainland China
South China Sea
East China Sea
Pb
ng m3
5.06 2.3a*
0.82 0.21b
2.48 0.74ab
Mass concentration
g m3
149.26 41.34a
44.55 21.43b
97.97 31.66ab
48.67 16.2 a
18.90 10.5b
25.35 13.65ab
206
Pb/207Pb
1.1620 0.0019
1.1837 0.0455
1.1566 0.0043
208
Pb/207Pb
2.0318 0.0428
2.0489 0.0502
2.0494 0.0666
208
Pb/206Pb
2.3610 0.0491
2.4236 0.0325
2.3782 0.0519
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*For certain metals or mass concentrations, data marked with the same letter indicate no signicant differences between
categories according to ANOVA analysis at P level of 0.05.
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Overall
Dry season
Wet season
CX =CR aerosol
CX =CR crust
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CONCLUSIONS
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Acknowledgements
This project has been jointly supported by the National
Natural Science Foundation of China (Nos. 30972365,
31170427) and the Knowledge Innovation Program of the
Chinese Academy of Sciences (No. KSCX2-EW-J-28). The
authors wish to thank Dr Q. Q. Chi and Dr H. B. Li for their
great assistance with isotope measurements at the Institute of
Urban Environment, Chinese Academy of Sciences. The
authors also thank the National Ecosystem Research Network
of China-DHS Forest Ecosystem for offering the meteorological
data for DHS. The authors gratefully acknowledge the NOAA
Air Resources Laboratory (ARL) for providing the HYSPLIT
transport and dispersion model and/or READY website
(http://www.ready.noaa.gov) used in this publication.
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