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1.
Results of our aerosol study, performed during 1983–1984 in Beijing, demonstrate that ambient carbonaceous aerosols are derived principally from coal combustion. Different SO2 oxidation processes have been observed in summer and winter. The winter sulfate appears to be produced locally and associated with products of incomplete combustion.  相似文献   

2.
One-week integrated fine particulate matter (i.e., particles <2.5 microm in diameter; PM2.5) samples were collected continuously with a low-flow rate sampler at a downtown site (Chegongzhuang) and a residential site (Tsinghua University) in Beijing between July 1999 and June 2000. The annual average concentrations of organic carbon (OC) and elemental carbon (EC) at the urban site were 23.9 and 8.8 microg m(-3), much higher than those in some cities with serious air pollution. Similar weekly variations of OC and EC concentrations were found for the two sampling sites with higher concentrations in the winter and autumn. The highest weekly variations of OC and EC occurred in the winter, suggesting that combustion sources for space heating were important contributors to carbonaceous particles, along with a significant impact from variable meteorological conditions. High emissions coupled with unfavorable meteorological conditions led to the max weekly carbonaceous concentration the week of November 18-25, 1999. The weekly mass ratios of OC:EC ranged between 2 and 4 for most samples and averaged 2.9, probably suggesting that secondary OC (SOC) is present most weeks. The range of contemporary carbon fraction, based on the C14 analyses of eight samples collected in 2001, is 0.330-0.479. Estimated SOC accounted for approximately 38% of the total OC at the two sites. Average OC and EC concentrations at Tsinghua University were 25% and 18%, respectively, higher than those at Chegongzhuang, which could be attributed to different local emissions of primary carbonaceous particles and gaseous precursors of SOC, as well as different summer photochemical intensities between the two locations.  相似文献   

3.
4.
We have used Raman spectroscopy to characterize a variety of carbon-containing particulate matter, including samples collected in ambient urban atmospheres. Based on the Raman spectra of known, commercial particles, we derive a simple empirical model that reflects their microchemistry and microphysics. This model gives information on the crystal size and morphology of the graphitic component, which correlates with the known characteristics of the commercial samples. We derive similar information about the graphitic component of the ambient particles, and suggest that this method might be used to characterize ambient particles systematically in the future.  相似文献   

5.
Carbonaceous aerosol concentrations were determined for total suspended particle samples collected from Muztagh Ata Mountain in western China from December 2003 to February 2006. Elemental carbon (EC) varied from 0.004 to 0.174 μg m?3 (average = 0.055 μg m?3) while organic carbon (OC) ranged from 0.12 to 2.17 μg m?3 and carbonate carbon (CC) from below detection to 3.57 μg m?3. Overall, EC was the least abundant fraction of carbonaceous species, and the EC concentrations approached those in some remote polar areas, possibly representing a regional background. Low EC and OC concentrations occurred in winter and spring while high CC in spring and summer was presumably due to dust from the Taklimakan desert, China. OC/EC ratios averaged 10.0, and strong correlations between OC and EC in spring–winter suggest their cycles are coupled, but lower correlations in summer–autumn suggest influences from biogenic OC emissions and secondary OC formation. Trajectory analyses indicate that air transported from outside of China brings ~0.05 μg m?3 EC, ~0.42 μg m?3 OC, and ~0.10 μg m?3 CC to the site, with higher levels coming from inside China. The observed EC was within the range of loadings estimated from a glacial ice core, and implications of EC-induced warming for regional climate and glacial ice dynamics are discussed.  相似文献   

6.
In order to better understand the characteristics of atmospheric carbonaceous aerosol at a background site in Northeast Asia, semicontinuous organic carbon (OC) and elemental carbon (EC), and time-resolved water-soluble organic carbon (WSOC) were measured by a Sunset OC/ EC and a PILS-TOC (particle-into-liquid sampler coupled with an online total organic carbon) analyzer, respectively, at the Gosan supersite on Jeju Island, Korea, in the summer (May 28-June 17) and fall (August 24-September 30) of 2009. Hourly average OC concentration varied in the range of approximately 0.87-28.38 microgC m-3, with a mean of 4.07+/- 2.60 microgC m-3, while the hourly average EC concentration ranged approximately from 0.04 to 8.19 .microgC m-3, with a mean of 1.35 +/- 0.71 microgC m-3, from May 28 to June 17, 2009. During the fall season, OC varied in the approximate range 0.9-9.6 microgC m-3, with a mean of 2.30 +/-0.80 microgC m-3, whereas EC ranged approximately from 0.01 to 5.40 microgC m-3, with a mean of 0.66 +/- 0.38 microgC m-3. Average contributions of EC to TC and WSOC to OC were 26.0% +/- 9.7% and 20.6% +/-7.4%, and 37.6% +/- 23.5% and 57.2% +/- 22.2% during summer and fall seasons, respectively. As expected, clear diurnal variation of WSOC/OC was found in summer, varying from 0.22 during the nighttime up to 0.72 during the daytime, mainly due to the photo-oxidation process. In order to investigate the effect of air mass pathway on the characteristics of carbonaceous aerosol, 5-day back-trajectory analysis was conducted using the HYSPLIT model. The air mass pathways were classified into four types: Continental (CC), Marine (M), East Sea (ES) and Korean Peninsula (KP). The highest OC/EC ratio of 3.63 was observed when air mass originated from the Continental area (CC). The lowest OC/EC ratio of 0.79 was measured when air mass originated from the Marine area (M). A high OC concentration was occasionally observed at Gosan due to local biomass burning activities. The contribution of secondary OC to total OC varied approximately between 8.4% and 32.2% and depended on air mass type.  相似文献   

7.
Carbonaceous aerosols were studied at three background sites in south and southwest China. Hok Tsui in Hong Kong had the highest concentrations of carbonaceous aerosols (OC = 8.7 ± 4.5 μg/m3, EC = 2.5 ± 1.9 μg/m3) among the three sites, and Jianfeng Mountains in Hainan Island (OC = 5.8 ± 2.6 μg/m3, EC = 0.8 ± 0.4 μg/m3) and Tengchong mountain over the east edge of the Tibetan Plateau (OC = 4.8 ± 4.0 μg/m3, EC = 0.5 ± 0.4 μg/m3) showed similar concentration levels. Distinct seasonal patterns with higher concentrations during the winter, and lower concentrations during the summertime were observed, which may be caused by the changes of the regional emissions, and monsoon effects. The industrial and vehicular emissions in East, Southeast and South China, and the regional open biomass burning in the Indo-Myanmar region of Asia were probably the two major potential sources for carbonaceous matters in this region.  相似文献   

8.
In August 2003 during the anticipated month of the 2008 Beijing Summer Olympic Games, we simultaneously collected PM10 and PM2.5 samples at 8, 100, 200 and 325 m heights up a meteorological tower and in an urban and a suburban site in Beijing. The samples were analysed for organic carbon (OC) and elemental carbon (EC) contents. Particulate matter (PM) and carbonaceous species pollution in the Beijing region were serious and widespread with 86% of PM2.5 samples exceeding the daily National Ambient Air Quality Standard of the USA (65 μg m−3) and the overall daily average PM10 concentrations of the three surface sites exceeding the Class II National Air Quality Standard of China (150 μg m−3). The maximum daily PM2.5 and PM10 concentrations reached 178.7 and 368.1 μg m−3, respectively, while those of OC and EC reached 22.2 and 9.1 μg m−3 in PM2.5 and 30.0 and 13.0 μg m−3 in PM10, respectively. PM, especially PM2.5, OC and EC showed complex vertical distributions and distinct layered structures up the meteorological tower with elevated levels extending to the 100, 200 and 300 m heights. Meteorological evidence suggested that there exist fine atmospheric layers over urban Beijing. These layers were featured by strong temperature inversions close to the surface (<50 m) and more stable conditions aloft. They enhanced the accumulation of pollutants and probably caused the complex vertical distributions of PM and carbonaceous species over urban Beijing. The built-up of PM was accompanied by transport of industrial emissions from the southwest direction of the city. Emissions from road traffic and construction activities as well as secondary organic carbon (SOC) are important sources of PM. High OC/EC ratios (range of 1.8–5.1 for PM2.5 and 2.0–4.3 for PM10) were found, especially in the higher levels of the meteorological tower suggesting there were substantial productions of SOC in summer Beijing. SOC is estimated to account for at least 33.8% and 28.1% of OC in PM2.5 and PM10, respectively, with higher percentages at the higher levels of the tower.  相似文献   

9.
Sources of carbonaceous aerosols collected from three sites of Chattanooga, TN (CH), Muscle Shoals, AL (MS), and Look Rock, TN (LR) in the Tennessee Valley Region (TVR) were apportioned using both organic tracer-based chemical mass balance (CMB) modeling and radiocarbon (14C) measurement and the results were compared. Eight sources were resolved by CMB, among which wood combustion (averaging 0.92 μg m−3) was the largest contributor to primary organic carbon (OC) concentrations, followed by gasoline exhaust (0.35 μg m−3), and diesel exhaust (0.18 μg m−3). The identified primary sources accounted for 43%, 71%, and 14% of measured OC at CH, MS, and LR, respectively. Contributions from the eight primary sources resolved by CMB could explain 107±10% of ambient elemental carbon (EC) concentrations, with diesel exhaust (66±32%) and wood combustion (37±33%) as the most important contributors. The fossil fractions in total carbon determined by 14C measurements were in reasonably good agreement with that in primary (OC+EC) carbon apportioned by CMB in the MS winter samples. The comparison between the 14C and CMB results revealed that contemporary sources dominated other OC in the TVR, especially in summertime (84% contemporary).  相似文献   

10.
Aerosol samples were collected from 2002 to 2003 in Terceira, one of the islands of the Azores archipelago in the north-eastern Atlantic. The atmospheric samples have been analysed for its carbonaceous content and for lipid class compounds. The major constituents that comprise plant wax are n-alkanes (C23–C33, with and odd-to-even carbon predominance and carbon maxima at 29 or 31), n-alkanols (C22–C30, even-to-odd) and n-alkanoic acids (C22–C30, even-to-odd), with minor amounts of n-alkanals and polycyclic biomarkers, such as phytosterols. Some alkanedioic acids and phthalates were also detected. The occurrence of short-chain homologues may indicate an additional marine source, probably introduced into the atmosphere via sea spray. Changes in the composition of the homologous series derived from terrestrial plants throughout the observation period may be related to alterations in the regional sources and transport pathways. These terrestrial lipids contributed up to 47% of the total compound mass, while the marine input was estimated to be inferior to 19%, both of them being more representative in summer. Biomass burning sources represented approximately 1% of the total inputs to the organic aerosol for the most part of the year, excepting during the spring, when it contributed to 10%. Petroleum products and plasticizers presented higher contributions (up to 19%) during the winter months. Secondary constituents resulting from oxidation during transport varied from 14% to 37% of the apportioned organic mass. The fraction derived from soil resuspension accounted for 2–16%.  相似文献   

11.
12.
Continuous observation of PM2.5 was conducted in Taiyuan, a heavily polluted city in China, during high pollution season from December 2005 to February 2006. The results of this study showed that PM2.5 and carbonaceous species pollution were serious during winter in Taiyuan. The organic carbon (OC) and element carbon (EC) were accounted for 18.6±11.2% and 2.9±1.6% of PM2.5, respectively, which indicated that carbonaceous aerosols were key components for control fine particles pollution in Taiyuan. Coal combustion was a dominant source of OC and EC of PM2.5 in the urban area of Taiyuan during winter. The impact of local and remote particle sources on urban air quality was assessed using PM2.5 concentration rose and 3-day back trajectories of air masses arriving at Taiyuan. The meteorological conditions were found to affect the ambient concentrations of PM2.5, OC, EC and OC/EC ratio.  相似文献   

13.
Okuda T  Katsuno M  Naoi D  Nakao S  Tanaka S  He K  Ma Y  Lei Y  Jia Y 《Chemosphere》2008,72(6):917-924
Daily observations of hazardous trace metal concentrations in aerosols in Beijing, China were made in the period from 2001 to 2006. We considered coal combustion as a major source of some anthropogenic metals by achieving a correlation analysis and by investigating enrichment factors and relative composition of metals. A possible extra source of some specific metals, such as Cu and Sb, was brake abrasion particles, however, we did not think the transport-related particle was a major source for the hazardous anthropogenic metals even though they could originate from vehicle exhaust and brake/tire abrasion particles. A time-trend model was used to describe temporal variations of chemical constituent concentrations during the five-year period. Several crustal elements, such as Al, Ti, V, Cr, Mn, Fe, and Co, did not show clear increases, with annual rates of change of -15.2% to 3.6%. On the other hand, serious increasing trends were noted from several hazardous trace metals. Cu, Zn, As, Cd, and Pb, which are derived mainly from anthropogenic sources, such as coal combustion, showed higher annual rate of change (4.9-19.8%, p<0.001) according to the regression model. In particular, the Cd and Pb concentrations increased remarkably. We hypothesize that the trend towards increasing concentrations of metals in the air reflects a change that has occurred in the process of burning coal, whereby the use of higher temperatures for coal combustion has resulted in increased emissions of these metals. The increasing use of low-rank coal may also explain the observed trends. In addition, nonferrous metal smelters are considered as a potential, albeit minor, reason for the increasing atmospheric concentrations of anthropogenic hazardous metals in Beijing city.  相似文献   

14.
The study addresses the characteristics of elemental carbon (EC) and organic carbon (OC) distributions in the Netherlands by using Black Smoke (BS) data in combination with dedicated measurements and modelling. The BS levels indicate a large-scale background concentration over the Netherlands with low spatial variability and a gradient with highest levels (∼9 μg m−3) in the south gradually decreasing to the north-west (∼5.5 μg m−3). The BS concentrations at rural sites in the Netherlands are highly correlated due to common (diffuse) sources and large-scale meteorology. Superimposed on the regional background are the contributions of local/urban sources. Urban and rural BS levels show a distinct variation over the week with minimum levels on Sundays.BS levels do not reflect a real concentration as they are obtained via an optical measurement in combination with an outdated calibration curve to arrive at total suspended particles (TSP). We have found that the relation between BS and EC in the Netherlands is linear and highly correlated but dependent on station type. Application of these relations to the BS time series yields a gradient in the rural background EC concentration from 0.5 μg m−3 in the north to 0.7 μg m−3 in the south of the Netherlands. The relationship between OC and BS appears to be location specific and is determined by the BS–EC relation in combination with a characteristic OC/EC ratio. OC/EC ratios are ∼5 at regional background sites and ∼2 at traffic locations. Minimum OC/EC ratios at the traffic sites reflect the primary OC/EC ratio of traffic. We argue that estimation of secondary organic aerosol by assuming the minimum OC/EC ratio to be a proxy for the primary OC/EC is not allowed since this approach does not account for sources with high OC/EC ratios. Based on European scale modelling and the measured data, we estimate that national sources contribute ∼40–60% to Dutch EC levels.The rather costly and laborious EC measurements provide a better indicator of the carbonaceous fraction in ambient particulate matter (PM) but the cheap BS method may provide valuable information on spatial distribution of EC when used in combination with validation sites to characterise the EC–BS relationship.  相似文献   

15.
In this study, aerosol vertical distributions of 17 in-situ aircraft measurements during 2005 and 2006 springs are analyzed. The 17 flights are carefully selected to exclude dust events, and the analyses are focused on the vertical distributions of aerosol particles associated with anthropogenic activities. The results show that the vertical distributions of aerosol particles are strongly affected by weather and meteorological conditions, and 3 different types of aerosol vertical distributions corresponding to different weather systems are defined in this study. The measurement with a flat vertical gradient and low surface aerosol concentrations is defined as type-1; a gradual decrease of aerosols with altitudes and modest surface aerosol concentrations is defined as type-2; a sharp vertical gradient (aerosols being strongly depressed in the PBL) with high surface aerosol concentrations is defined as type-3. The weather conditions corresponding to the 3 different aerosol types are high pressure, between two high pressures, and low pressure systems (frontal inversions), respectively. The vertical mixing and horizontal transport for the 3 different vertical distributions are analyzed. Under the type-1 condition, the vertical mixing and horizontal transport were rapid, leading to strong dilution of aerosols in both vertical and horizontal directions. As a result, the aerosol concentrations in PBL (planetary boundary layer) were very low, and the vertical distribution was flat. Under the type-2 condition, the vertical mixing was strong and there was no strong barrier at the PBL height. The horizontal transport (wind flux) was modest. As a result, the aerosol concentrations were gradually reduced with altitude, with modest surface aerosol concentrations. Under the type-3 condition, there was a cold front near the region. As a result, a frontal inversion associated with weak vertical mixing appeared at the top of the inversion layer, forming a very strong barrier to prevent aerosol particles being exchanged from the PBL height to the free troposphere. As a result, the aerosol particles were strongly depressed in the PBL height, producing high surface aerosol concentrations. The measured vertical aerosol distributions have important implications for studying the effects of aerosols on photochemistry. The J[O3] values are reduced by 11%, 48%, and 50%, under the type-1, type-2, and type-3 conditions, respectively. This result reveals that atmospheric oxidant capacity (OH concentrations) is modestly reduced under the type-1 condition, but is significantly reduced under the type-2 and type-3 conditions. This result also suggests that the effect of aerosol particles on surface solar flux is an integrated column effect, and detailed vertical distributions of aerosol particles are very important for assessing the impacts of aerosol on photochemistry.  相似文献   

16.
Rural and background sites provide valuable information on the concentration and optical properties of organic, elemental, and water-soluble organic carbon (OC, EC, and WSOC), which are relevant for understanding the climate forcing potential of regional atmospheric aerosols. To quantify climate- and air quality-relevant characteristics of carbonaceous aerosol in the central United States, a regional background site in central Texas was chosen for long-term measurement. Back trajectory (BT) analysis, ambient OC, EC, and WSOC concentrations and absorption parameters are reported for the first 15 months of a long-term campaign (May 2011–August 2012). BT analysis indicates consistent north–south airflow connecting central Texas to the Central Plains. Central Texas aerosols exhibited seasonal trends with increased fine particulate matter (<2.5 μm aerodynamic diameter, PM2.5) and OC during the summer (PM2.5 = 10.9 μg m?3 and OC = 3.0 μg m?3) and elevated EC during the winter (0.22 μg m?3). When compared to measurements in Dallas and Houston, TX, central Texas OC appears to have mixed urban and rural sources. However, central Texas EC appears to be dominated by transport of urban emissions. WSOC averaged 63% of the annual OC, with little seasonal variability in this ratio. To monitor brown carbon (BrC), absorption was measured for the aqueous WSOC extracts. Light absorption coefficients for EC and BrC were highest during summer (EC MAC = 11 m2 g?1 and BRC MAE365 = 0.15 m2 g?1). Results from optical analysis indicate that regional aerosol absorption is mostly due to EC with summertime peaks in BrC attenuation. This study represents the first reported values of WSOC absorption, MAE365, for the central United States.
Implications:Background concentration and absorption measurements are essential in determining regional potential radiative forcing due to atmospheric aerosols. Back trajectory, chemical, and optical analysis of PM2.5 was used to determine climatic and air quality implications of urban outflow to a regional receptor site, representative of the central United States. Results indicate that central Texas organic carbon has mixed urban and rural sources, while elemental carbon is controlled by the transport of urban emissions. Analysis of aerosol absorption showed black carbon as the dominant absorber, with less brown carbon absorption than regional studies in California and the southeastern United States.  相似文献   

17.
Alves C  Pio C  Carvalho A  Santos C 《Chemosphere》2006,63(1):153-164
A labour-intensive analytical technique was applied to atmospheric particulate matter samples collected in a German urban/industrial influenced grassland location (Melpitz) and in a Finnish forest area (Hyyti?l?) in order to achieve a detailed chemical speciation of the organic content. The representative nature of the solvent and water-extractable fractions was determined. The organic compounds identified in the solvent extracts are represented by primary compounds with both anthropogenic and biogenic origin, which mainly derive from the vegetation waxes and from petrogenic sources. Secondary products resulting from the oxidation of volatile organic compounds were also detected. The German meadow presented the highest levels of sugars and acidic compounds in the water extracts, whilst polyols were the most abundant class in the Finnish forest. The major compounds of these classes were malic acid, mannitol, arabitol, glucose and sucrose. Levoglucosan was also found in the water extract.  相似文献   

18.
Sampling and analysis of carbonaceous compounds in particulate matter presents a number of difficulties related to artefacts during sampling and to the distinction between organic (OC) and elemental carbon (EC) during analysis. Our study reports on a comparative analysis of OC, EC and WSOC (water-soluble organic carbon) concentrations, as well as sampling artefacts, for PM2.5 aerosol in three European cities (Amsterdam, Barcelona and Ghent) representing Southern and Western European urban environments. Comparability of results was ensured by using a single system for sample analysis from the different sites. OC and EC concentrations were higher in the vicinity of roads, thus having higher levels in Amsterdam (3.9–6.7 and 1.7–1.9 μg m−3, respectively) and Barcelona (3.6–6.9 and 1.5–2.6 μg m−3) than in Ghent (2.7–5.4 and 0.8–1.2 μg m−3). A relatively larger influence of secondary organic aerosols (SOA), as deduced from a larger OC/EC ratio, was observed in Ghent. In absolute sense, WSOC concentrations were similar at the three sites (1.0–2.3 μg m−3). Positive artefacts were higher in Southern (11–16% of the OC concentration in Barcelona) than in Western Europe (5–12% in Amsterdam, 5–7% in Ghent). During special episodes, the contribution of carbonaceous aerosols from non-local sources accounted for 67–69% of the OC concentration in Western Europe, and for 44% in Southern Europe.  相似文献   

19.
Carbonaceous components (organic carbon [OC] and elemental carbon [EC]) and optical properties (light absorption and scattering) of fine particulate matter (aerodynamic diameter <2.5 μm; PM2.5) were simultaneously measured at an urban site in Gwangju, Korea, during the winter of 2011. OC was further classified into OC1, OC2, OC3, and OC4, based on a temperature protocol using a Sunset OC/EC analyzer. The average OC and EC concentrations were 5.0 ± 2.5 and 1.7 ± 0.9 μg C m?3, respectively. The average single-scattering albedo (SSA) at a wavelength of 550 nm was 0.58 ± 0.11, suggesting that the aerosols observed in the winter of 2011 had a local warming effect in this area. During the whole sampling period, “stagnant PM” and “long-range transport PM” events were identified. The light absorption coefficient (babs) was higher during the stagnant PM event than during the long-range transport PM event due to the existence of abundant light-absorbing OC during the stagnant PM event. In particular, the OC2 and OC3 concentrations were higher during the stagnant PM event than those during the long-range transport event, suggesting that OC2 and OC3 might be more related to the light-absorbing OC. The light scattering coefficient (bscat) was similar between the events. On average, the mass absorption efficiency attributed to EC (σEC) was 9.6 m2 g?1, whereas the efficiency attributed to OC (σOC) was 1.8 m2 g?1 at λ = 550 nm. Furthermore, the σEC is comparable among the PM event days, but the σOC for the stagnant PM event was significantly higher than that for the long-range transport PM event (1.7 vs. 0.5).

Implications: Optical and thermal properties of carbonaceous aerosol were measured at Gwangju, and carbonaceous aerosol concentration and optical property varied between “stagnant PM” and “long-range transport PM” events. More abundant light absorbing OC was observed during the stagnant PM event.  相似文献   

20.
The mass concentration of carbonaceous species, organic carbon (OC), and elemental carbon (EC) using a semicontinuous thermo-optical EC-OC analyzer, and black carbon (BC) using an Aethalometer were measured simultaneously at an urban mega city Delhi in Ganga basin from January 2011 to May 2012. The concentrations of OC, EC, and BC exhibit seasonal variability, and their concentrations were ~2 times higher during winter (OC 38.1?±?17.9 μg m?3, EC 15.8?±?7.3 μg m?3, and BC 10.1?±?5.3 μg m?3) compared to those in summer (OC 14.1?±?4.3 μg m?3, EC 7.5?±?1.5 μg m?3, and BC 4.9?±?1.5 μg m?3). A significant correlation between OC and EC (R?=?0.95, n?=?232) indicate their common emission sources with relatively lower OC/EC ratio (range 1.0–3.6, mean 2.2?±?0.5) suggests fossil fuel emission as a major source of carbonaceous aerosols over the station. On average, mass concentration of EC was found to be ~38 % higher than BC during the study period. The measured absorption coefficient (babs) was significantly correlated with EC, suggesting EC as a major absorbing species in ambient aerosols at Delhi. Furthermore, the estimated mass absorption efficiency (σabs) values are similar during winter (5.0?±?1.5 m2 g?1) and summer (4.8?±?2.8 m2 g?1). Significantly high aerosol loading of carbonaceous species emphasize an urgent need to focus on air quality management and proper impact assessment on health perspective in these regions.  相似文献   

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