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1.
Simultaneous measurements of rain acidity and dimethyl sulfide (DMS) at the ocean surface and in the atmosphere were performed at Amsterdam Island over a 4 year period. During the last 2 years, measurements of sulfur dioxide (SO2) in the atmosphere and of methane sulfonic acid (MSA) and non-sea-salt-sulfate (nss-SO4 2-) in rainwater were also performed. Covariations are observed between the oceanic and atmospheric DMS concentrations, atmospheric SO2 concentrations, wet deposition of MSA, nss-SO4 2-, and rain acidity. A comparable summer to winter ratio of DMS and SO2 in the atmosphere and MSA in precipitation were also observed. From the chemical composition of precipitation we estimate that DMS oxidation products contribute approximately 40% of the rain acidity. If we consider the acidity in excess, then DMS oxidation products contribute about 55%.  相似文献   

2.
Aerosols consist of organic and inorganic species, and the composition and concentration of these species depends on their sources, chemical transformation and sinks. In this study an assessment of major inorganic ions determined in three aerosol particle size ranges collected for 1 year at Welgegund in South Africa was conducted. SO42? and ammonium (NH4+) dominated the PM1 size fraction, while SO42? and nitrate (NO3) dominated the PM1–2.5 and PM2.5–10 size fractions. SO42? had the highest contribution in the two smaller size fractions, while NO3? had the highest contribution in the PM2.5–10 size fraction. SO42? and NO3? levels were attributed to the impacts of aged air masses passing over major anthropogenic source regions. Comparison of inorganic ion concentrations to levels thereof within a source region influencing Welgegund, indicated higher levels of most species within the source region. However, the comparative ratio of SO42? was significantly lower due to SO42? being formed distant from SO2 emissions and submicron SO42? having longer atmospheric residencies. The PM at Welgegund was determined to be acidic, mainly due to high concentrations of SO42?. PM1 and PM1–2.5 fractions revealed a seasonal pattern, with higher inorganic ion concentrations measured from May to September. Higher concentrations were attributed to decreased wet removal, more pronounced inversion layers trapping pollutants, and increases in household combustion and wild fires during winter. Back trajectory analysis also revealed higher concentrations of inorganic ionic species corresponding to air mass movements over anthropogenic source regions.  相似文献   

3.
An in-cloud scavenging case study of the major ions (NH4 +, SO4 2- and NO3 -) determining the cloudwater composition at a mountain site (1620 m.a.s.l.) is presented. A comparison between in-cloud measurements of the cloudwater composition, liquid water content, gas concentrations and aerosol concentrations and pre-cloud gas and aerosol concentrations yields the following results. Cloudwater concentrations resulted from scavenging of about half of the available NH3, aerosol NH4 +, aerosol NO3 -, and aerosol SO4 2-. Approximately a third of the SO2 was scavenged by the cloudwater and oxidized to SO4 2-. Cloud acidity during the first two hours of cloud interception (pH 3.24) was determined mostly by the scavenged gases (NH3, SO2, and HNO3); aerosol contributions to the acidity were found to be small. Observations of gas and aerosol concentrations at three elevations prior to several winter precipitation events indicated that NH3 concentrations are typically half (12–80 %) of the total (gas and aerosol) N (-III) concentrations. HNO3 typically is present at much lower concentrations (1–55 %) than aerosol NO3 -. Concentrations of SO2 are a substantial component of total sulfur, with concentrations averaging 60 % (14–76 %) of the total S (IV and VI).  相似文献   

4.
Rainwater samples were collected at five locations in the Pune region, an urban area in the south-west part of India, during 2006–2009. These locations; viz., Swargate (Traffic), Bhosari (Industrial), Pashan, Sangvi (Urban) and Sinhagad (Rural and High Altitude), represent different environments in this region. The study based on chemical analyses of these samples reveals that, on average, rainwater was alkaline at all the locations with pH values of 6.7, 6.16, 5.94, 6.04 and 5.92, respectively. Higher pH value of rainwater at the traffic location than those at the other locations is due mainly to the abundance of Ca2+ caused by vehicle-driven road-side dust. The maximum SO42? and NO3? concentrations were found at Bhosari and Swargate respectively caused by local industrial and vehicular emissions. The average Fractional acidity over Pune area is 0.024, indicating about 98% acidity is neutralized by alkaline constituents. Factor analysis of the results indicated the influence of various sources, such as anthropogenic, soil dust, sea salt and biomass burning.  相似文献   

5.
The temporal variation in concentrations of major water soluble ionic species has been studied from several rain events occurred over Gadanki (13.5 °N, 79.2 °E), located in tropical semi arid region in southern India. The contribution from rain-out (in cloud) and wash-out (below cloud) processes to the total removal of ionic species by rain events is also estimated using the pattern of variations of ionic species within an individual event. A number of rain samples were collected from each rain event during June–November in 2006, 2007 and 2008. On average, nearly 20% of the total NH 4 + and non-sea SO 4 2? is removed by in-cloud scavenging, suggesting that their removal by “below cloud” washout is relatively dominant. In contrast Na+, Ca2+, Mg2+, NO 3 ? and sea-SO 4 2? are mainly removed by below-cloud scavenging or wash-out process. A significant variation in the acidity was observed within rain events with successive precipitation showing higher acidity at the final stage of the precipitation due to partial neutralization of non-sea SO 4 2? . Overall, greater influence of both terrestrial and anthropogenic sources is recorded in the rain events compared to that from marine sources.  相似文献   

6.
The deposition fluxes of inorganic compounds dissolved in fog and rain were quantified for two different ecosystems in Europe. The fogwater deposition fluxes were measured by employing the eddy covariance method. The site in Switzerland that lies within an agricultural area surrounded by the Jura mountains and the Alps is often exposed to radiation fog. At the German mountain forest ecosystem, on the other hand, advection fog occurs most frequently. At the Swiss site, fogwater deposition fluxes of the dominant components SO42− (0.027 mg S m−2 day−1), NO3− (0.030 mg N m−2 day−1) and NH4+ (0.060 mg N m−2 day−1) were estimated to be <5% of the measured wet deposition (0.85, 0.70 and 1.34 mg m−2 day−1, respectively). The corresponding fluxes at the forest site (0.62, 0.82 and 1.16 mg m−2 day−1, respectively) were of the same order of magnitude as wet deposition (1.04, 1.01 and 1.36 mg m−2 day−1), illustrating the importance of fog (or occult) deposition. Trajectory analyses at the forest site indicate significantly higher fogwater concentrations of all major ions if air originated from the east (i.e. the Czech Republic), which is in close agreement with earlier studies.  相似文献   

7.
合肥市降水化学组成成分分析   总被引：5，自引：1，他引：4  
为研究合肥市降水的化学组成成分,于2010年4—9月在合肥市国家基本气象站设立了采样点,进行降水的采集,对降水化学组成成分进行了测定,并系统分析了化学组成成分的特点。结果表明:合肥降水中阴离子主要为SO24-,阳离子主要为NH4+和Ca2+,[SO24-]/[NO3-]当量浓度比值范围为1.23～6.33,大部分样本的比值<3,说明酸雨类型以硝硫混合型为主。降水的酸度与单一离子当量浓度的相关性并不明显,应该是受多种离子综合影响的结果,SO24-与NO3-,Ca2+与Mg2+,NH4+与SO24-,NH4+与NO3-均表现出较好的相关性。  相似文献   

8.
In Northeast Asia, the effect of long-range transport of air pollutants is generally pronounced in spring and winter, but can be important even in summer. This study analyzed summer-time atmospheric transport of elemental carbon (EC) and sulfate (SO4 2?) with the Community Multiscale Air Quality (CMAQ) model driven by the Weather Research and Forecasting (WRF) model. The WRF/CMAQ modeling system was applied to regions ranging from Northeast Asia to the Greater Tokyo Area in Japan in summer 2007. In terms of EC, while the model simulated well the effect of long-range transport, the simulation results indicated that domestic emissions in Japan dominantly contributed (85%) to EC concentrations in the Greater Tokyo. In terms of SO4 2?, the simulation results indicated that both domestic emissions (62%) and long-range transport from the other countries (38%) substantially contributed to SO4 2? concentrations in the Greater Tokyo. Distinctive transport processes of SO4 2? were associated with typical summer-time meteorological conditions in the study region. When a Pacific high-pressure system covered the main island of Japan, domestic emissions, including volcanic emission, dominantly contributed to SO4 2? concentrations in the Greater Tokyo. When a high-pressure system prevailed over the East China Sea and low-pressure systems passed north of Japan, synoptic westerly winds associated with this pressure pattern transported a large amount of SO4 2? from the continent to Japan. In addition, although heavy precipitation and strong wind decreased SO4 2? concentrations near the center of a typhoon, peripheral typhoon winds occasionally played an important role in long-range transport of SO4 2?.  相似文献   

9.
The second Arctic Gas and Aerosol Sampling Program (AGASP-II) was conducted across the Alaskan and Canadian Arctic in April 1986, to study the in situ aerosol, and the chemical and optical properties of Arctic haze. The NOAA WP-3D aircraft, with special instrumentation added, made six flights during AGASP-II. Measurements of wind, pressure, temperature, ozone, water vapor, condensation nuclei (CN) concentration, and aerosol scattering extinction (bsp) were used to determine the location of significant haze layers. The measurements made on the first three flights, over the Arctic Ocean north of Barrow and over the Beaufort Sea north of Barter Island, Alaska are discussed in detail in this report of the first phase of AGASP II. In the Alaskan Arctic the WP-3D detected a large and persistent region of haze between 960 and 750 mb, in a thermally stable layer, on 2, 8, and 9 April 1986. At its most dense, the haze contained CN concentrations >10,000 cm–3 and bsp of 80×10–6 m–1 suggesting active SO2 to H2SO4 gas-to-particle conversion. Calculations based upon observed SO2 concentrations and ambient relative humidities suggest that 104–105 small H2SO4 droplets could have been produced in the haze layers. High concentrations of sub-micron H2SO4 droplets were collected in haze. Ozone concentrations were 5–10 ppb higher in the haze layers than in the surrounding troposphere. Outside the regions of haze, CN concentrations ranged from 100 to 400 cm–3 and bsp values were about (20–40)×10–6 m–1. Air mass trajectories were computed to depict the air flow upwind of regions in which haze was observed. In two cases the back trajectories and ground measurements suggested the source to be in central Europe.  相似文献   

10.
The chemical composition, as well as the sources contributing to rainwater chemistry have been determined at Skukuza, in the Kruger National Park, South Africa. Major inorganic and organic ions were determined in 93 rainwater samples collected using an automated wet-only sampler from July 1999 to June 2002. The results indicate that the rain is acidic and the averaged precipitation pH was 4.72. This acidity results from a mixture of mineral acids (82%, of which 50% is H2SO4) and organic acids (18%). Most of the H2SO4 component can be attributed to the emissions of sulphur dioxide from the industrial region on the Highveld. The wet deposition of S and N is 5.9 kgS⋅ha−1⋅yr−1 and 2.8 kgN⋅ha−1⋅yr−1, respectively. The N deposition was mainly in the form of NH4 +. Terrigenous, sea salt component, nitrogenous and anthropogenic pollutants have been identified as potential sources of chemical components in rainwater. The results are compared to observations from other African regions.  相似文献   

11.
The pH and the concentrations of sulfate, nitrate, ammonia, and calcium in rainwater were measured for two periods of a single midwest rainstorm which occurred over a mesometeorological network in central Illinois on 24–25 July 1979. Regression analysis was used to compare ion concentrations with rainfall amount, and ion balance was used to compare cation and anion concentrations at individual sites. Only the ions SO4 2- and NO3 - show any significant relationship to rainfall amount, decreasing as rainwater amounts increase (r=–0.57 and –0.60, respectively). During the first period of the rainstorm, a sequential sampler measurements allowed the calculation of detailed temporal variations in SO4 2-, pH, and rain rate. SO4 2- decreased, and pH increased as the rate increased and the opposite temporal pattern occurred as the rain decreased at the end of the period. Reasons for these variations are discussed.Research done while a visiting scientist at the Illinois State Water Survey, Champaign, Illinois, U.S.A.  相似文献   

12.
We investigated the acidity and concentrations of water-soluble ions in PM2.5 aerosol samples collected from an urban site in Beijing and a rural site in Gucheng, Hebei Province from November 2016 to January 2017 to gain an insight into the formation of secondary inorganic species. The average SO42–, NO3–, and NH4+ concentrations were 8.3, 12.5, and 14.1 μg m–3, respectively, at the urban site and 14.0, 14.2, and 24.2 μg m–3, respectively, at the rural site. The nitrogen and sulfur oxidation ratios in urban Beijing were correlated with relative humidity (with correlation coefficient r = 0.79 and 0.67, respectively) and the aerosol loadings. Based on a parameterization model, we found that the rate constant of the heterogeneous reactions for SO2 on polluted days was about 10 times higher than that on clear days, suggesting that the heterogeneous reactions in the aerosol water played an essential role in haze events. The ISORROPIA II model was used to predict the aerosol pH, which had a mean (range) of 5.0 (4.9–5.2) and 5.3 (4.6–6.3) at the urban and rural site, respectively. Under the conditions with this predicted pH value, oxidation by dissolved NO2 and the hydrolysis of N2O5 may be the major heterogeneous reactions forming SO42– and NO3– in haze. We also analyzed the sensitivity of the aerosol pH to changes in the concentrations of SO42–, NO3–, and NH4+ under haze conditions. The aerosol pH was more sensitive to the SO42– and NH4+ concentrations with opposing trends, than to the NO3– concentrations. The sensitivity of the pH was relatively weak overall, which was attributed to the buffering effect of NH3 partitioning.  相似文献   

13.
Rainwater samples were collected for the monsoon period of 1988 and 1991–1996 at Dayalbagh (Agra), a suburban site situated in semiaridregion. The mean pH was 7.01 ±1.03 well above 5.6, which is the reference pH. Concentration of Ca2+ was observed to be highest followed by Mg2+, NH4 +,SO4 2–, Cl–,NO3 –, Na+, F– and K+. The ratios of SO4 2– + NO3 – andCa2+ + Mg2+ (TA/TC) have been considered as indicatorfor acidity. In the Agra region ratio of TA/TC is quite below 1.0 indicating alkaline nature of rainwater. The lowest value of 0.24 was observed in 1991 likely due to the lowest rain depth of the decade. The highest value of 0.54 was observed in 1996, a year with a large rain depth and increase in line (vehicular traffic) and area sources (population growth). Good correlation between Ca2+ and NO3 –,Ca2+ and SO4 2– andSO4 2– and NO3 –,indicates that wind carried dust and soil play a significant role in neutralization of precipitation acidity.  相似文献   

14.
Selected applications of baseline aerosol, SO2 and deposition chemistry observations in Canada are reviewed to illustrate how new insight can be gained into features of the atmospheric pathway of trace substances such as sources, transformation and removal. A strong annual variation in Arctic aerosol concentration is a manifestation of particle residence times that are much longer in winter than in summer. Differences in the variation of SO4 = and V concentrations in the Arctic winter are due to SO2 oxidation. The mean rate of oxidation between November and April ranges from 0.04 to 0.25%/h and is a minimum in December, January and February. Br measured on filters in the Arctic peaks in concentration later (March and April) than anthropogenic particulate matter suggesting photochemical production. Acidity in Arctic aerosol and in glacial ice are correlated. The relationship yields a best estimate of acidity in the absence of anthropogenic influences of 5.8 mole/l. Coincident air and precipitation measurements of sulphur oxides indicate that on average in eastern Canada 60% of SO4 = in rain originates from SO2 oxidation in the storm. Trends in Arctic ice core acidity and SO2 emissions in Europe are similar, that is, little variation in the first half of the century and a marked increase since the mid 1950's. This is consistent with meteorological and chemical evidence linking Arctic air pollution with Eurasian sources.  相似文献   

15.
Concentrations of sulfur gases H2S and SO2 have been measured in the marine atmosphere over the Atlantic Ocean at various sites. Mean values of 40 ng H2S m-3 STP and 209 ng SO2 m-3 STP are the results of the measurements. A diurnal variation of H2S concentration was detected on the west coast of Ireland with nighttime concentrations of up to 200 ng H2S m-3 STP and values below detection limit (15 ng H2S m-3 STP) during daytime.  相似文献   

16.
Six years of observations (1980 to 1986) of the composition of lower tropospheric aerosols at Alert on northern Ellesmere Island in the Canadian high Arctic yield insight into the seasonal variation of Arctic air pollutants as well as of substances of natural origin. A principal component analysis of 138 observations of 21 aerosol constituents (major ions, metals, nonmetallic trace elements) for the most polluted period of December to April identified not only a soil, sea salt and anthropogenic aerosol component, but also one associated with photochemical reactions in the atmosphere that occur at polar sunrise. Depending on the source of their gaseous precursors, elements in the photochemical component can be natural or anthropogenic in origin. For instance, SO4 2-, existing mostly as H2SO4, originates probably from both anthropogenic and natural sources while Br– is likely of marine origin. In contrast, SO4 2- in the anthropogenic component has the stoichiometry of NH4HSO4. In the winter months, over 90% of Arctic SO4 2- is in the anthropogenic and photochemical components.In winter, a substantial portion (11 to 35%) of Na+ is associated with the anthropogenic aerosol component suggesting either that marine aerosols have been physically or chemically modified by interactions with air pollution or that there are anthropogenic sources of Na+.The aerosol soil component is controlled by both local and distant dust sources. During a year, it has two peaks at Alert, one in April/May coinciding with the Asian dust storm season and one in September.There is a marked difference in the seasonal variation of particulate Br– and iodine concentrations in the air. Both have a peak in April/May associated with polar sunrise and, hence, photochemical reactions in the atmosphere. However, iodine also peaks in early fall. This may be a product of biogenic iodine emissions to the atmosphere during secondary blooms in northern oceans in late summer.Presented at the Second Conference on Baseline Observations in Atmospheric Chemistry (SABOAC II) in Melbourne, Australia, November 1988  相似文献   

17.
A comprehensive study on the chemical compositions of rainwater was carried out from Jan. to Dec. in 2008 in Chengdu, a city located on the acid rain control zone of southwest China. All samples were analyzed for pH and major ions (F–, Cl?, NO3?, SO42?, K+, Na+, Ca2+, Mg2+, and NH4+). The pH increased due to the result of neutralization caused by the base ions. It was observed that Ca2+ was the most abundant cation with a VWM value of 196.6 μeq/L (17.3–1568.7 μeq/L), accounting for 49.7% (9.4%–79.2%) of the total cations. SO42? was the most abundant anion with VWM value of 212.8 μeq/L (41.8–1227.6 μeq/L). SO42? and NO3? were dominant among the anions, accounting for 90.4%–99.1% of the total measured anions.The concentrations of NO3? were higher than the most polluted cities abroad, which indicated Chengdu has been a severe polluted city over the world. The high fuel consumption from urbanization and the rapid increase of vehicles resulted in the high emission of SO2 and NOx, which were the precursor of the high concentration of acidic ions NO3? and SO42?. It was the main reason of the severe acid rain in Chengdu.The high concentrations of alkaline ions (mainly Ca2+, NH4+) in Chengdu city atmosphere have played an important role to neutralize the acidity of rainwater and the pH value has increased by 0.7 units since 1989. It is worth noting that the emission of NOx from the automobile exhaust is increased and is becoming the important precursor of acid rain now.  相似文献   

18.
In this study, 24-h PM2.5 samples were collected using Harvard Honeycomb denuder/filter-pack system during different seasons in 2006 and 2007 at an urban site in Guangzhou, China. The particles collected in this study were generally acidic (average strong acidity ([H+]) ~ 70 nmol m? 3). Interestingly, aerosol sulfate was not fully neutralized in the ammonia-rich atmosphere (NH3 ~ 30 ppb) and even when NH4+]/[SO42?] was larger than 2. Consequently, strong acidity ([H+]) as high as 170 nmol m? 3 was observed in these samples. The kinetic rate of neutralization of acidity (acidic sulfate) by ambient ammonia was significantly higher than the rate of formation of ammonium nitrate involving HNO3 and NH3 for [NH4+]/[SO42?] ≤ 1.5 and much lower for NH4+]/[SO42?] > 1.5. Therefore, higher nitrate principally formed via homogeneous gas phase reactions involving ammonia and nitric acid were observed for [NH4+]/[SO42?] > 1.5. However, little nitrate, probably formed via heterogeneous processes e.g. reaction of HNO3 with sea salt or crustal species, was observed for [NH4+]/[SO42?] ≤ 1.5. These demonstrate a clear transition in the pathways of ambient ammonia to form aerosol ammonium at [NH4+]/[SO42?] = 1.5 and evidently explain the observed high acidity due to the unneutralized sulfate in the ammonium-rich aerosol (NH4+]/[SO42?] > 1.5). In fact, the measured acidity was almost similar to the excess acid defined as the acid that remains at [NH4+]/[SO42?] = 1.5 due to the un-neutralized fraction of sulfate ([H+] = 0.5[SO42?]). The presence of high excess acid and ammonium nitrate significantly lowered the deliquescence relative humidity of ammonium sulfate (from 80% to 40%) in the ammonium-rich samples.  相似文献   

19.
High volume aerosol samples were collected continuously at Mawson, Antarctica (67°36'S, 62°30'E), from February 1987 through October 1989. All samples were analyzed for Na+, Cl-, SO4 =, NO3 -, methanesulfonate (MSA), NH4 +,7Be, and210Pb. The annual mean concentrations of many of the species are very low, substantially lower than even those over the relatively pristine regions of the tropical and subtropical South Pacific. The concentrations at Mawson are comparable both in magnitude and in seasonality to those which have been measured in long term studies at the South Pole and at the coastal German Antarctic research station, Georg von Neumayer (GvN). This comparability suggests that the aerosol composition may be relatively uniform over a broad sector of the Antarctic. The concentrations of most of the species exhibit very strong and sharply-defined seasonal cycles. MSA, non-sea-salt (nss) SO4 = and NH4 + all exhibit similar cycles, with maxima during the austral summer (December through February) being more than an order of magnitude higher than the winter minima. The limited7Be data appears to exhibit a similar cycle. Although nitrate and210Pb also exhibit relatively high concentrations during the austral summer, their cycles are far more complex than those of the previous species with indications of multiple peaks. As expected, the concentration of sea-salt (as indicated by Na+ and Cl-) peaks during the winter. The results from multiple variable regression analyses indicate that the dominant source of nss SO4 = is the oxidation of dimethylsulfide (DMS) which produces MSA and nss SO4 = in a ratio of about 0.31 (about five times higher than that over the tropical and subtropical oceans). However, a very significant fraction (about 25%) of the nss SO4 = is associated with NO3 -, The seasonal cycle of NO3 - is similar to that of210Pb and distinctly different from that of7Be and MSA. These results indicate that the major source of NO3 - over Antarctica is probably continental as opposed to stratospheric or marine biogenic.  相似文献   

20.
Beijing is one of the largest and most densely populated cities in China. PM2.5 (fine particulates with aerodynamic diameters less than 2.5 μm) pollution has been a serious problem in Beijing in recent years. To study the temporal and spatial variations in the chemical components of PM2.5 and to discuss the formation mechanisms of secondary particles, SO2, NO2, PM2.5, and chemical components of PM2.5 were measured at four sites in Beijing, Dingling (DL), Chegongzhuang (CG), Fangshan (FS), and Yufa (YF), over four seasons from 2012 to 2013. Fifteen chemical components, including organic carbon (OC), elemental carbon (EC), K+, NH4 +, NO3 ?, SO4 2?, Cl?, Al, Ca, Fe, Mg, Na, Pb, Si, and Zn, were selected for analysis. Overall, OC, SO4 2?, NO3 ?, and NH4 + were dominant among 15 components, the annual average concentrations of which were 22.62 ± 21.86, 19.39 ± 21.06, 18.89 ± 19.82, and 13.20 ± 12.80 μg·m?3, respectively. Compared with previous studies, the concentrations of NH4 + were significantly higher in this study. In winter, the average concentrations of OC and EC were, respectively, 3 and 2.5 times higher than in summer, a result of coal combustion during winter. The average OC/EC ratios over the four sites were 4.9, 7.0, 8.1, and 8.4 in spring, summer, autumn, and winter, respectively. The annual average [NO3 ?]/[SO4 2?] ratios in DL, CG, FS, and YF were 1.01, 1.25, 1.08, and 1.12, respectively, which were significantly higher than previous studies in Beijing, indicating that the contribution ratio of mobile source increased in recent years in Beijing. Analysis of correlations between temperature and relative humidity and between SOR ([SO4 2?]/([SO4 2?] + [SO2])) and NOR ([NO3 ?]/([NO3 ?] + [NO2])) indicated that gas-phase oxidation reactions were the major formation mechanism of SO4 2? in spring and summer in urban Beijing, whereas slow gas-phase oxidation reactions and heterogeneous reactions both occurred in autumn and winter. NO3 ? was mainly formed through year-round heterogeneous reactions in urban Beijing.  相似文献   

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