W4-6981/88 13.00+0.

00
Amospkric Enuiromnl Vol. 22, NO. 2. pp. 349-358. 1988
Peqamon Journals Ltd.
Pm&d in Great Britam.

ACID RAIN IN SOUTHWESTERN CHINA

DIANWU ZHAO,* JILING XIom,t Yu Xu$ and WALTER H. CHAN$[(

*Research Center for Eco-environmental Sciences, Academia Sink, P. 0. Box 934, Beijing, China; tGuizhou
Institute of Environmental Sciences, Xinhua Street, Guiyang, China; fchongqing Municipal Institute of
Environmental Research and Monitoring, Guanyinqiao, Chongqing, China; and SOOntarioMinistry of the
Environment, Air Resourazs Branch, 880 Bay Street, Toronto, Ontario, Canada, MSS 1Z8

(First received 23 Jonunry 1987 and in~~a~~or~ 7 July 1987)

Abstmct-Acid rain and acidification of the environment have been environmental issues of concern in
China in recent years. Approximately 90/, of the monitoring stations with a mean pH of less than 5.6 are
located south of the Yangtze River. In this account, new research data have been combined with those
published originally in Chinese to give an overview of the acid rain picture in SW China, a region with the
most serious acid rain problem in China. Results of SW China have been presented in comparison with data
in northern parts of China to not only demonstrate the spatial variability, but also to reflect the impact of
NH,, airborne particles and soil types on rain acidity. Based on pr~ipi~tion and aerosol chemistry
m~su~ments. the source and origin of acid rain in SW China are discussed.

Key word index: Acid rain, chemical composition, source, origin, SW China.

1. INTRODUCTION between the Academia Sinicas Research Centre for

Acid rain and a~difi~tion of the environment have
emerged as environmental issues of increasing concern
in China. Surveys in regions with heavy acid rain
demonstrate that acid rain, either alone or most likely
in consort with other gaseous pollutants, may have
brought about damage to the environment. There are
vast forest areas in the south of China. Reports (Yu et
al., 1985; Chen, 1985, personal communication) re-
vealed evidence of forest damage in Chongqing City,
Sichuan Province and suggested that long-term ex-
posure to acid rain might be responsible for, to some
extent, though very likely indirectly, the injury and
damage of forests there.
Metal structures and concrete works have suffered
severe corrosion in regions in China with severe air
pollution and acid rain (Chen et al., 1986). Compared
with Nanjing (a city with similar meteorological
conditions but light air pollution and low precipitation
acidity), Chongqing and Guiyang both have a very
serious material corrosion problem which is
accelerating.
Since the late 197Os,precipitation samples have been
collected and analyzed for acidity and chemical com-
position in some Chinese cities. In November 1981, the
First National Symposium on Acid Rain was convened
in Beijing. In 1982, the National Environmental
Protection Office (EPO) organized and sponsored two
projects: Nationwide Survey of Acid Rain and
Research on the Formation and Effects of Acid Rain in
the Southwestern Region of China. The Southwestern
Regional Acid Rain Study is a collaborative effort
) To whom correspondence should be addressed.
349
Eco-Environmental Sciences, and local Environmental
Institutes of the Guizhou Province, Sichuan Province
and Chongqing City. Acid rain monitoring studies
have also been carried out in other provinces and cities
by their respective municipal institutes of environ-
mental protection.
Coal combustion is a major source of air pollution
in China; the most common air pollutants being
particulates and SO,,. Energy consumption in China
has increased more than IO-fold over about 30 years
(Table l}. In 1982, the total energy consumption
amounted to 620 Mt of coal equivalent; coal and oil
accounted for 74 :/,and 19%, respectively of the total.
Even though urban cities correspond to only about 7 yf;
of Chinas total surface area, the corresponding usage
of coal was estimated to be above 200 Mt. Coal is
burned generally in medium- and small-sized boilers
and household stoves. These have a small holding
capacity. The former are only equipped with dust
removers while the latter have no emission abatement
equipment at all. The emissions are released through
short chimneys. Under unfavorable meteorological
and/or topographical conditions, severe air pollution
episodes result. Therefore, air pollution is an import-
ant issue in the urban areas of China (Zhao, 1984).
The level of airborne particulates is high throughout
the year. Aside from fly ash resulting from coal
combustion, wind-blown dust is also a major contribu-
tor to airborne particulates. In northern China, the
relative contributions to airborne particulates by coal
burning and wind-blown dust are 2: 3 in the summer
and 3 : 2 in the winter (Wang et al., 1981), whereas in the
southern region, they are estimated to be approxi-
mately 2: 1.
 Table 1. Energy consumption in China*

Total
Total - ^-~~~-.-..__._ ...l_,___.__.
_~
Year (1V ton Coal Eq.) Coal Oil Gas Hydro

t953 54.11 94.33 3.8 1 0.02 1.84

1962 165.40 89.23 6.61 0.93 3.23
1970 292.9i 80.89 14.67 0.92 3.52
I975 454.25 71.85 21.07 2.5f 4.57
1982 619.37 73.92 18.67 2.56 4.85

*Clrinese Statistics Handbook, Statistic Press, 1983, p. 250.

In 1985, SO2 emissions arising from coal burning other authors to give an overview of the acid rain picture in
were about 13 Mt (Wang, 1986). In cities such as southwestern China. The new precipitation results are based
on samples collected in polyethylene containers manually.
Chongqing and Guiyang in southwestern China,
Chemical analyses were carried out using the following
where high S content coals are burned, during periods methods: pH :pH meter, model PHS-2 made in China; SO: .
of stagnation, SOz pollution is more serious (Table 2). NO;, CI-, K+, Na*, NH:: Ton Chromatography, model
In northern cities during winter when coal is used for Dionex-I 6; and Ca2 *, Mg : Inductively Coupled Plasma.
space heating, the SO, levef is elevated. In most Ambient air NH3 concentration wascollected by bubbling
air through a solution of 10 N H,SU, downstream of au
southern cities, rural areas and northern cities during organic filter at a flow rate of 1Ipm. The converted NH; in
non-space heating periods, SO1 levels are low. the dilute H,S04 solution was determined by oxidation with
Airborne particulate concentrations are also higher in Na3rO.
winter months than in summer months.
In general, the atmospheric NO, level is low across
3. RESULTS AND DISCUSSION
the country, commonly not exceeding 50 pgrn. 3
(Zhao, 1984). It appears that NO, in air mainly 3.1. Distribution and chemical composition ojacid rain
originates from coal combustion too. However, the in China
NO, Ievel might be three times higher along main environments monitoring data gathered so far
streets, especially at crossroads in big cities such as demonstrate that acid precipitation does occur in some
Beijing, due to heavy trafk. parts ofChina. A map showing major cities in China is
given in Fig. 1. Approximately 90% of the sampling
2. EXPERIMENTAL
sites with mean precipitation pH lower than 5.6 are
On this accotmt, new research data are presented together located to the south of the Yangtze River (Ji and
with those which have been published originally in Chinese by Cheng, 1982); especially so in Sichuan, Guizhou and

Table 2. Levels of TSP and SO, in selected cities in China (1982)

Mean concentration (llg m-3)

July December Annual
Area City TSP SO, TSP SO, TSP SO,

Northern Shenyang, residential 324 9 769 69i 470 232

clean? 107 6 370 209 221 45

Beijing. residential 165 53 585 388 403 I58

clean 115 6 362 58 263 15

Xian, residential 363 25 836 291 477 124

Chl 245 10 634 86 355 24

Southern Shanghai, residentha) 161 53 322 12t 244 65

Guangzhou. residential I33 48 194 53 174 52

clean IO4 12 fOb 10 119 13

Chongqing*. residential 480 170 870 380 610 260

clean 20 130 40 60 20

Guiyang, residential 863 403 840 419 898 393

clean 160 64 147 la9 159 88
----.
Source: Globat Environmental Monitoring Systemdata of 1982,atmospherkpollution in fivecities
of China.
*Environmental Quality Reports of Chongqmg and Guiyang, 1981.
i Measured at a mountain or a rural site far away from the urban area.
 Acid rain in Southwestern China 351

1 Beijing 2 Tianjin 3 Shenyang 4 Xikn 5 Shanghai 6 Guangzhou 7 ChGngqing 9 Guiyang

9 Lanzhou 10 Nanjing 11 Hangzhou 12 Wuhan 13 Fuzhou 14 Naming 19 Yibin 19 Chengdu

PACIFIC

OCEAN

Fig. 1. Map of the administrative division of the Peoples Republic of China. (Insert map shows South China Sea
Islands.)

Jiangxi Provinces (Table 3) (Yu, 1985). Areas with the
most serious acid rain problem are in the southwestern
region, e.g. Chongqing and Guiyang have annual
volume-weighted mean pH 4.14 and 4.07, respectively.
Figure 2 summarizes the results of a survey carried
out in 1982-1984 in the central part of Guizhou and
eastern parts of Sichuan. Most of the areas have
precipitation pH values < 5.6.
Table 4 shows the precipitation chemistry in some
cities in China. Depending on whether these cities are
located south or north of the Yangtze River, they can
be distinctly classified into two categories: cities with
and without acid rain. The equivalent concentration of
Cl - in the coastal sites (Guiyang, Beijing and Tianjin)
is similar to that of Na+, suggesting an oceanic origin
which contributes little to precipitation acidity. Ca2 +

Table 3. Precipitation pH in Chinese cities

Area City Year PH References

Northern Beijing 2-7. 1982 6.74 This work

Tianjin 1981 6.26 Zhao et al., 1985a
Lanzhou 1. 1981-8. 1982 6.85 Wang et al., 1983
Xian 1. 1982-4. 1983 6.12 Li and Wang, 1984

Southern Nanjing 1982 5.47 MO et ol., 1985

Han&row 9-12. 1981 5.10 Wang and L.i, 1984
Wuhan 8. 1981-3. 1983 5.96 Li and Wang, 1984
Fuzhou 5. 1982 4.49 MO et al., 1984
Nanning 5. 1981-3. 1983 5.33 Li and Wang, 1984
Yibin 1982 4.87 Zhao et al., 1985a
Chongqing 1982-1984 4.14 This work
Guiyang 1982-1984 4.07 This work
352 DIANWU ZHAO et al.

I
.,f \ SHANXI
PUOVINCL i
v-.
\ \
d-- \
--_I ,
\ I

, \

. _ _. i PUOViNCt

GUIZHOU
PROVINCE
I
5.0 (

i
i

0 WKm
,sBo,,

Y
\
.\
WNNAN PROVINCE ; l

Fig. 2. Geographical distribution of precipitation pH for 1982-1984 in southwestern China. Source: Study
Report on Acid Precipitation in Southwestern China. unpublished results by Research Group of Acid
Precipitation in Southwestern China (1986).

and NH; are the major cations. Anion concentrations
are dominated by SO:-, ranging from as low as 70 /b
in Beijing to as high as 90 /, in Guiyang. This is rather
different from Hartes measurements from the Tibetan
Plateau in Qinghai Province (Harte, 1983) where very
high ratios of NO; to SO:- were observed. Pre-
cipitation acidity is heavily governed by the relative
contributionsof SO:-, Ca* and NH:. While thesum
of SO:- and NO; may be comparable in both areas of
high and low acidities, the sum of the cations (NH:
+ Ca2 + + K ) varies significantly from the acid rain
areas to the non-acid rain areas.
Table 5 gives acidity results of precipitation samples
collected and measured at the top of some mountains
far away from cities or industrial areas which have a
minimal impact from pollution sources. The data show
that the precipitation acidities in the study arcas are
low (i.e. with pH higher than 5.6) or at least lower than
those of samples from nearby cities. This is consistent
with the observations made by Harte (1983) in that
Acid rain in Southwestern China 353

high pH values were measured in precipitation samples

at Amne Machin Mountains. However, exceptions do
exist. It has been reported that acid rain is very often
observed at Lushan Mountain of Jiangxi Province and
Emei Mountain of Sichuan Province (Chen, 1985,
personal communication), two famous recreation
mountain areas. It is not yet clear whether anthropo-
genie activities related to tourism are responsible for
the situation.

3.2. The sources of acid rain

For some of the northern cities where there are high
SO2 emissions, there is serious air pollution, but no
acid rain. Beijing and Tianjin are two typical examples.
There are also cases where acid rain is observed in areas
with low SO1 pollution, as in Guangzhou (Ji and
Cheng, 1982) and Fuzhou (MO and Xie, 1982).
Therefore it is clear that the existence of acid rain
depends not only on the very presence of SO2 in the
atmosphere, but also upon other factors such as, to a
great extent, the amount of alkaline material available
as a neutralizing agent (Zhou et a[., 1985a). This point
is also supported by studies in China which show that
the precipitation concentration of H+ does not gener-
ally correlate well with the SO:- concentration.
Airborne particles play an important role in acid
rain formation. Concentrations of total suspended
particulates are high in China (see Table 2). Wind-
blown dust accounts for one-half of the total sus-
pended particulate in the north and one-third in the
south. Aerosol buffering capacity has been determined
for samples obtained in various locations in China by
dissolving air samples in deionized water. The average
pH (n = 12) of the Beijing samples is 8.2 and that of the
Guiyang samples (n = 26) is 5.8 (Zhao et al., 1985b).
The chemical composition of the collected particulate
samples indicates that aerosol buffering capacity in-
creases with increasing Ca+ content, or more pre-
cisely, Ca2 + to SOi- ratio. Size-fractionated samples
have also been collected using a five-stage cascade
impactor in Beijing, Guiyang and Chongqing. In
general, buffering capacity decreases when particle size
decreases from > 7 pm to < 1.1 pm (Table 6). This
observation is consistent with the fact that Ca2+ and
SOi- are primarily associated with coarse and fine
particles, respectively. However, the changes observed
in Beijing are far less than those in Guiyang and
Chongqing (Zhao et al., 1986). Figures 3 and 4, for
instance, show buffering curves for aerosol samples
from Guiyang and Beijing.
Precipitation acidity is affected by particulates
which have a large soil-related contribution. H+
originates primarily from below-cloud scavenging of
SO2 (see also section 3.3). Samples of below-cloud
scavenging of SO2 collected at Guiyang and
Chongqing indicate S(IV) accounts for less than 30 /,
of the total S (Zhao et al., 1985a). The majority of the
SO:- (not originated from washout of S02) may have
its origins from airborne particulates. The origins of
Ca2 + and NH: are not as clear, and may be both
354 DIANWU ZHAO et al

Table 5. Acidity of precipitation at remote areas

Location Mountain, province Year Mean pH No. of samples Reterences

North Altay Mountains, Xinjiang 7-8. 1980 6.4 7 Wang et al., 1983
Huangshan Mountain. Anhui Y-12. 1980 6.84 Not reported MO and Xie, 1982
South Hengshan Mountain, Hunan 1982 6.4 Not reported Yuan, 1984, personal
communication
Shita Mountain, Fujian 5. 1982 6.Y5 24 MO et al., 1984
Jinfo Mourttain, Sichuan 1984 5.89 3 This work
Lushan Mountain, Jiangxi 1981-1983 5.41 Not reported LI and Wang. 1984
Fanjin Mountain, Guizhou 1985 6.1 2 This work

Table 6. pH of sample solution of particulates in various size ranges

Size range (pm)

Area Year Location >I 7-3.3 3.3-2 2-1.1 < 1.1

Acid rain 3. 1985 Guiyang, urban 6.37 5.59 5.31 4.86 4.32
area rural 6.40 5.80 5.15 4.92 4.58

9. 1985 Guiyang, urban 6.62 5.66 5.12 4.82 4.33

rural 7.36 6.08 5.36 5.04 4.90

Non-acid 3. 1985 Beijing, suburban 8.24 7.75 7.48 6.64 7.20

rain area 9. 1985 Beijing, suburban 8.64 7.62 6.16 5.16 4.96

Note: High Volume Andersen Sampler, Whatman- Filter, flow rate 566 /min.- I, sampling time
48 h (Guiyang), 24 h (Beijing), solution volume for each filter 200 ml (Guiyang), 100 ml (Beijing).
blank pH 5.14.

Fig. 3. Buffering curves of particles of different size ranges at a Guiyang

urban site.

natural and anthropogenic, with the former source
being the major contributor.
Atmospheric NHs plays an important role in de-
termining precipitation acidity. Table 7 gives results of
NH, measurements made in Chongqing, Guiyang and
Chengdu, areas with acid rain, as well as measurements
made in Beijing, Langfang and Tianjin, areas with no
acid rain. The NHs concentrations in the acid rain
areas are an order of magnitude lower than those in the
non-acid rain areas. The presence of NHs is intimately
 Acid rain in Southwestern China 355

Added Ii+, PM

Fig. 4. Buffering curves of particles of different size ranges at a Beijing site.

Table 7. Atmospheric ammonia concentration (ppb) in rain in China is obviously not enough to fully address
Chinese cities this problem. However, some comments could be
made based on the facts presented above.
Area Location Year n N%(ppb)
The distribution of acid rain in southwestern China
Acid rain Chongqing 9. 1984 12 5.17 displays strong local influences. The spatial distri-
area bution of acid rain is, in most cases, similar to that of
SO2 concentrations, i.e. in general, high acidity is
Guiyang 9. 1984 16 1.7
Chengdu 9. 1985 2 4.8 observed in urban areas with high SO2 pollution
7. 1984 10 44
whereas in suburban and rural areas where SO2
Non-acid Beijing
rain area pollution is not serious, low acidity is seen in
Langfang 7. 1984 8 64 precipitation.
Tianjin 7. 1984 4 22.8 The source of acid in rain has been studied by means
of measuring gaseous acid pollutant index (GAPI)
Source: Reference (Zhao et al., 1986).
(National Environmental Protection Agency, 1983)
and below-cloud scavenging of S02.
related to the soil nature in the area of study. GAPI is expressed as SO2 derived from the in-
Volatilization of NH3 increases as the soil pH increases crement of acidity (H+) in a pH 5.5 deionized water
(Lau and Charlson, 1977). Soils in the Beijing-Tianjin solution saturated with H202 after pumping air into it
region have pH values around 7-8 whereas those in the through a filter. If there are other acidic gases than SO2
Chongqing-Guiyang region are around 5-6, as shown in the air, GAPI should be higher than the actual SO2
in Fig. 5. This accounts for the decreasing gradient of concentration in air. If alkaline gases are present in the
NH, concentration from north to south. The nature of air, GAP1 should be lower than the air SO2 concen-
soil has a large effect on precipitation acidity and tration. Atmospheric concentrations of SO2 and NH,
therefore the distribution of acid rain in China reflects can be deduced from the concentrations of SOi- and
soil pH. NH: in the absorbing solution. Table 8 shows that
GAPIs are about the same as the atmospheric SO2
3.3. Local source us long-range transport contribution concentrations with negligible contribution of NO, in
It is ofcrucial importance to know whether the acids both Guiyang and Beijing. It appears that the dif-
in precipitation and their precursors originate locally ference between GAP1 and SO2 can be roughly
or are transported from long distances when formulat- attributed to NH3 in the air.
ing control strategy. The current knowledge about acid Figure 6 is an example of results obtained from
356 DIANWU ZHAO ef al.

m 5-6

m 6-7

m >7

Fig. 5. Map ofsoil pH in Peoples Republic ofChina. Source: Soil @China by Institute
of Soil Science, Academia Sin&, Science Press, 1980, p. 342.

Table 8. Gaseous acid pollution index for Guiyang and Beijing

Area Location Year n

Acid rain Guiyang 1984 30 458 467 3.1

area (urban)

Non-acid Beijing 1985 6 34 31.7 10.8

rain area (urban)

Source: Reference (Zhao et al., 1986).

Month

Fig. 6. Volume-weighted monthly average precipitation concentrations of S(W) and

H+ at a Guiyang urban site in 1983.

measurements of below-cloud scavenging of SO1 concentration at the ground level are both high in the
conducted in Guiyang urban area in 1983. There exists winter and low in the summer although it is not
a statistically significant correlation between S(1V)and feasible to establish firmly a correlation between the
H + in precipitation. S(W) in precipitation and SO2 air two species due to the lack of SO2 data. These
 Acid rain in Southwestern China
measurements suggest that the observed rain pH can
be accounted for by the H released from the dissolu-
tion and subsequent oxidation of SO2 in raindrops on
their way from the cloud to ground level. Rain samples
have been collected at an altitude of 3-5 km above
ground using an aircraft in the Guiyang area in 1983.
pH values of these samples are in the range of 6.0-6.54
(n = 5) with a median of 6.24. This fact suggests that
cloud water may not be an important contributor to
precipitation acidity. Therefore, it seems reasonable to
think that acid rain in urban areas in China is mainly
formed through the scavenging of SOz in air below
clouds, particuiarly near the ground.
Three points are important to note. Firstly, in
Chongqing, Guiyang and many other cities, heavy SOz
pollution and strong acid rain occur in the urban areas
and the situation is quite the contrary in the suburbs.
Secondly, precipitation acidity mainly comes from
below-cloud scavenging of SO, in urban areas.
Thirdly, cluster analysis based on the ionic content of
precipitation separates sampling sites of Chongqing
and Guiyang into two categories and then further
divides urban and suburban sites into different sub-
groups (Zhao et al., 1986). These results imply that
there exist clear differences in precipi~tion chemistry
between two cities a few hundred km apart and even
between the urban and suburban areas of the same city.
A tentative conclusion to be drawn from all the above
three results is that acid rain in urban areas of China is
caused mainly by local emissions of S02.
Long distance transport of air pollutants, however,
is by no means altogether absent. Some evidence can
still be found in this respect, by examining the situation
in areas far away from human activities. For example,
levels of SO2 in air, SO:- in rain water and particulates
measured at the top of Fanjin Mountain, a natural
reserve in northeastern Guizhou (260 km to the north-
east of Guiyang) reach 13pgme3, 18peqi- and
8 pgm3, respectively. It is clear that these are higher
than the global background values, suggesting that the
air quality of Fanjin Mountain is markedly influenced
by dense emission areas several hundred kilometers
away, although the amount of transported acidifying
pollutants is not large enough to cause acid rain at this
mountain.
4. CONCLUDING REMARKS
Acid rain and acidifi~tion of the environment have
been environmental issues of concern in China in
recent years. From a national survey (Ji and Cheng,
1982) it was found that approximately 900/, of the
stations with a mean pH < 5.6 were located south of
the Yang&e River which coincides with the areas
where the soil is probably sensitive to acid deposition.
Areas with the most serious acid rain problem are in
the southwestern region, with annual volume-
weighted precipitation pH values of 4.14 and 4.07 at
Chongqing and Guiyang, respectively. The distri-
357
bution of acid rain in southwestern China suggests a
local influence of SO2 emissions.
Acid rain originates from air pollution and in-
evitably bears some signature of air pollution. At
present, air pollution in China has two outstanding
features. One is that the SO2 in air is mainly from low
emission sources, the other is that airborne particulate
levels (half of which can be accounted for by
windblown dust which contains Ca) are often very
high. As far as acid rain formation is concerned, the
first feature means that rain acidity in urban areas
originates primarily from below-cloud scavenging of
SO1 emitted from local sources. The second feature
means that particulates together with the ammonia in
air, make up the atmospheric buffering capacity. At
present, the geographical distribution of rain acidity in
China can roughly be explained by the geographical
distribution of soil pH, despite the serious contri-
bution of SO2 in air. Even though long-distant
transport of acidifying substances does not play a
substantial role in acid rain in southwestern China,
there is evidence of its presence in remote areas.
Ack~ow~edgemenr-me authors would like to thank Dr M,
A. Lusis and Dr J. P. Lodge, Jr for their reading of the
manuscript and valuable suggestions.
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