[Show abstract][Hide abstract] ABSTRACT: Based on the observation by a Regional Air Quality Monitoring Network including 16 monitoring stations, temporal and spatial variations of ozone (O3), NO2 and total oxidant (Ox) were analyzed by both linear regression and cluster analysis. A fast increase of regional O3 concentrations of 0.86 ppbV/yr was found for the annual averaged values from 2006 to 2011 in Guangdong, China. Such fast O3 increase is accompanied by a correspondingly fast NOx reduction as indicated by a fast NO2 reduction rate of 0.61 ppbV/yr. Based on a cluster analysis, the monitoring stations were classified into two major categories – rural stations (non-urban) and suburban/urban stations. The O3 concentrations at rural stations were relatively conserved while those at suburban/urban stations showed a fast increase rate of 2.0 ppbV/yr accompanied by a NO2 reduction rate of 1.2 ppbV/yr. Moreover, a rapid increase of the averaged O3 concentrations in springtime (13%/yr referred to 2006 level) was observed, which may result from the increase of solar duration, reduction of precipitation in Guangdong and transport from Eastern Central China. Application of smog production algorithm showed that the photochemical O3 production is mainly volatile organic compounds (VOC)-controlled. However, the photochemical O3 production is sensitive to both NOx and VOC for O3 pollution episode. Accordingly, it is expected that a combined NOx and VOC reduction will be helpful for the reduction of the O3 pollution episodes in Pearl River Delta while stringent VOC emission control is in general required for the regional O3 pollution control.
Journal of Environmental Sciences. 01/2014; 26(1):23-36.
[Show abstract][Hide abstract] ABSTRACT: With rapid economic development and the acceleration of urbanization, air pollution has become a serious problem in the mega-city Guangzhou, China. A field campaign to sample and analyze particulate matter (PM) chemical components was performed from July 6, 2006 to July 26, 2006, in Guangzhou. During the campaign, the average mass concentration of PM10 was 89.0 ± 46.6 μg m− 3 (the error represents one standard deviation). The PM10, sulfate, nitrate, ammonium, organic carbon (OC), and elemental carbon (EC) mass frequency distributions were analyzed. The [NO3−]/[SO42 −] mass ratio varied from 0.1 to 0.3, with an average of 0.2. A Pearson correlation analysis between [SO42 −] and [NH4+] and between [NO3−] and [Na+] showed that SO42 − existed as (NH4)2SO4 and NO3− existed as NH4NO3 and NaNO3. Sulfate, nitrate, ammonium, EC and POM (particulate organic matter) accounted for 24.4%, 4.9%, 5.7%, 5.7% and 21.0%, respectively, of the PM10 mass concentration during clean days and 25.7%, 3.9%, 7.9%, 5.4% and 20.8%, respectively, on hazy days. Among these species, SNA (sulfate, nitrate, and ammonium) were the most abundant, accounting for 35.0% and 37.5% of the PM10 during clean and hazy days, respectively. The sum of POM and EC accounted for 26.7% and 26.2% of PM10 in Guangzhou during clean and hazy days, respectively. There was no apparent difference in the chemical composition of PM10 between clean and haze days.
Atmospheric Research 01/2014; 137:25–34. · 2.20 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Size-resolved aerosols were continuously collected by a Nano Sampler for 13 days at an urban site in Beijing during winter 2012 to measure the chemical composition of ambient aerosol particles. Data collected by the Nano Sampler and an ACSM (Aerodyne Aerosol Chemical Speciation Monitor) were compared. Between the data sets, similar trends and strong correlations were observed, demonstrating the validity of the Nano Sampler. PM10 and PM2.5 concentrations during the measurement were 150.5 ± 96.0 μg/m3 (mean ± standard variation) and 106.9 ± 71.6 μg/m3, respectively. The PM2.5/PM10 ratio was 0.70 ± 0.10, indicating that PM2.5 dominated PM10. The aerosol size distributions showed that three size bins of 0.5–1, 1–2.5 and 2.5–10 μm contributed 21.8%, 23.3% and 26.0% to the total mass concentration (TMC), respectively. OM (organic matter) and SIA (secondary ionic aerosol, mainly SO42 −, NO3− and NH4+) were major components of PM2.5. Secondary compounds (SIA and secondary organic carbon) accounted for half of TMC (about 49.8%) in PM2.5, and suggested that secondary aerosols significantly contributed to the serious particulate matter pollution observed in winter. Coal burning, biomass combustion, vehicle emissions and SIA were found to be the main sources of PM2.5. Mass concentrations of water-soluble ions and undetected materials, as well as their fractions in TMC, strikingly increased with deteriorating particle pollution conditions, while OM and EC (elemental carbon) exhibited different variations, with mass concentrations slightly increasing but fractions in TMC decreasing.
[Show abstract][Hide abstract] ABSTRACT: In situ measurements of size-resolved aerosol chemical compositions and its optical properties were concurrently carried out at an urban site in mega-city Beijing from October 24 to November 9, 2007. The main objective was to quantitatively study the relationship between aerosol chemical compositions and its hygroscopic properties, to estimate the influence of relative humidity (RH) on aerosol scattering coefficient and to quantitatively investigate visibility impairment due to particle hygroscopic growth. The hygroscopic factor of aerosol scattering coefficient (f(RH)), which is defined as the ratio of aerosol scattering coefficient at wet condition to that at dry condition (RH ≤ 30%), was calculated with the measured aerosol optical properties at dry and ambient conditions. The relationship between f(RH) and RH was fitted by empirical equation and the fitting parameters were calculated. Meanwhile, f(RH) for externally mixed aerosols or internally mixed aerosols was modeled based on size segregated particulate chemical composition. The modeled f(RH) agreed well with the measured f(RH). Empirical formula for atmospheric visibility based on mass concentration of PM2.5 and f(RH) was proposed. The result of this study is not only proven that RH, in addition to the mass concentration of PM2.5, played an important role on visibility impairment, but also provide practical aid for air quality control to improve the visibility in the megacity region of Beijing.
Atmospheric Research 10/2013; s 132–133:91–101. · 2.20 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: A new instrument for measuring atmospheric nitrous acid (HONO) was developed, consisting of a double-wall glass stripping coil sampler coupled with ion chromatography (SC-IC). SC-IC is featured by small size (50 x 35 x 25 cm) and modular construction, including three independent parts: the sampling unit, the transfer and supporting unit, and the detection unit. High collection efficiency (> 99%) was achieved with 25 micromol/L Na2CO3 as absorption solution even in the presence of highly acidic compounds. This instrument has a detection limit of 8 pptv at 15 min time resolution, with a measurement uncertainty of 7%. Potential interferences from NO(x), NO2+SO2, NO2+VOCs, HONO+O3, HNO3, peroxyacetyl nitrite (PAN) and particle nitrite were quantified in laboratory studies and were found to be insignificant under typical atmospheric conditions. Within the framework of the 3C-STAR project, inter-comparison between the SC-IC and LOPAP (long path liquid absorption photometer) was conducted at a rural site in the Pearl River Delta. Good agreement was achieved between the two instruments over three weeks. Both instruments determined a clear diurnal profile of ambient HONO concentrations from 0.1 to 2.5 ppbv. However, deviations were found for low ambient HONO concentrations (i.e. < 0.3 ppbv), which cannot be explained by previous investigated interference species. To accurately determine the HONO budget under illuminated conditions, more intercomparison of HONO measurement techniques is still needed in future studies, especially at low HONO concentrations.
Journal of Environmental Sciences 05/2013; 25(5):895-907. · 1.77 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: This study was conceived to evaluate the global scientific output of secondary organic aerosol (SOA) research over the past 20 years and to assess the characteristics of the research patterns, tendencies, and methods in the papers. Data were based on the online version of Science Citation Index Expanded from 1992 to 2011. Publications referring to SOAs were assessed by distribution of the number of publications and times cited, source categories, source journals, author keywords, KeyWords Plus, and the most cited publications in these years. By synthetic analysis of author keywords, KeyWords Plus, titles, and abstracts, it was concluded that modeling is currently and will at least over the next decade continue to be the predominant research method to validate state-of-the-art knowledge of SOAs, and that the foci of SOA research will be the key precursors terpenes and isoprene, the mechanisms of oxidation and gas-phase reactions, and emission inventories.
[Show abstract][Hide abstract] ABSTRACT: The objective of this study is to quantify the relation of aerosol chemical compositions and optical properties, and to assess the impact of relative humidity (RH) on atmospheric visibility and aerosol direct radiative forcing (ADRF). Mass concentration and size distribution of aerosol chemical compositions as well as aerosol optical properties were concurrently measured at Guangzhou urban site during the PRD (Pearl River Delta) campaign from 1 to 31 July, 2006. Gaseous pollutant NO2 and meteorological parameter were simultaneously monitored. Compared with its dry condition, atmospheric ambient extinction coefficient σext(RH) averagely increased about 51% and atmospheric visibility deceased about 35%, among which RH played an important role on the optical properties of water soluble inorganic salts. (NH4)2SO4 is the most important component responsible for visibility degradation at Guangzhou. In addition, the asymmetry factor g increased from 0.64 to 0.74 with the up-scatter fraction β decreasing from 0.24 to 0.19 when RH increasing from 40% to 90%. At 80% RH, the ADRF increased about 280% compared to that at dry condition and it averagely increased about 100% during the campaign under ambient conditions. It can be inferred that aerosol water content is a key factor and could not be ignored in assessing the role of aerosols in visibility impairment and radiative forcing, especially in the regions with high RH.
[Show abstract][Hide abstract] ABSTRACT: In response to increasing trends in sulfur deposition in Northeast Asia, three countries in the region (China, Japan, and Korea) agreed to devise abatement strategies. The concepts of critical loads and source-receptor (S-R) relationships provide guidance for formulating such strategies. Based on the Long-range Transboundary Air Pollutants in Northeast Asia (LTP) project, this study analyzes sulfur deposition data in order to optimize acidic loads over the three countries. The three groups involved in this study carried out a full year (2002) of sulfur deposition modeling over the geographic region spanning the three countries, using three air quality models: MM5-CMAQ, MM5-RAQM, and RAMS-CADM, employed by Chinese, Japanese, and Korean modeling groups, respectively. Each model employed its own meteorological numerical model and model parameters. Only the emission rates for SO(2) and NO(x) obtained from the LTP project were the common parameter used in the three models. Three models revealed some bias from dry to wet deposition, particularly the latter because of the bias in annual precipitation. This finding points to the need for further sensitivity tests of the wet removal rates in association with underlying cloud-precipitation physics and parameterizations. Despite this bias, the annual total (dry plus wet) sulfur deposition predicted by the models were surprisingly very similar. The ensemble average annual total deposition was 7,203.6 ± 370 kt S with a minimal mean fractional error (MFE) of 8.95 ± 5.24 % and a pattern correlation (PC) of 0.89-0.93 between the models. This exercise revealed that despite rather poor error scores in comparison with observations, these consistent total deposition values across the three models, based on LTP group's input data assumptions, suggest a plausible S-R relationship that can be applied to the next task of designing cost-effective emission abatement strategies.
Environmental Science and Pollution Research 08/2012; 19(9):4073-89. · 2.76 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: The authors conducted a 2-year follow-up of 40 cardiovascular disease patients (mean age = 65.6 years (standard deviation, 5.8)) who underwent repeated measurements of cardiovascular response before and during the 2008 Beijing Olympics (Beijing, China), when air pollution was strictly controlled. Ambient levels of particulate matter with an aerodynamic diameter less than 2.5 µm (PM(2.5)), black carbon, nitrogen dioxide, sulfur dioxide, ozone, and carbon monoxide were measured continuously, with validation of concurrent real-time measurements of personal exposure to PM(2.5) and carbon monoxide. Linear mixed-effects models were used with adjustment for individual risk factors, time-varying factors, and meteorologic effects. Significant heart rate variability reduction and blood pressure elevation were observed in association with exposure to air pollution. Specifically, interquartile-range increases of 51.8 µg/m(3), 2.02 µg/m(3), and 13.7 ppb in prior 4-hour exposure to PM(2.5), black carbon, and nitrogen dioxide were associated with significant reductions in the standard deviation of the normal-to-normal intervals of 4.2% (95% confidence interval (CI): 1.9, 6.4), 4.2% (95% CI: 1.8, 6.6), and 3.9% (95% CI: 2.2, 5.7), respectively. Greater heart rate variability declines were observed among subjects with C-reactive protein values above the 90th percentile, subjects with a body mass index greater than 25, and females. The authors conclude that autonomic and vascular dysfunction may be one of the mechanisms through which air pollution exposure can increase cardiovascular disease risk, especially among persons with systemic inflammation and overweight.
American journal of epidemiology 07/2012; 176(2):117-26. · 5.59 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Most previous O3 simulations were based only on gaseous phase photochemistry. However, some aerosol-related processes, namely, heterogeneous reactions occurring on the aerosol surface and photolysis rate alternated by aerosol radiative influence, may affect O3 photochemistry under high aerosol loads. A three-dimensional air quality model, Models-3/Community Multi-scale Air Quality-Model of Aerosol Dynamics, Reaction, Ionization, and Dissolution, was employed to simulate the effects of the above-mentioned processes on O3 formation under typical high O3 episodes in Beijing during summer. Five heterogeneous reactions, i.e., NO2, NO3, N2O5, HO2, and O3, were individually investigated to elucidate their effects on 03 formation. The results showed that the heterogeneous reactions significantly affected O3 formation in the urban plume. NO2 heterogeneous reaction increased O3 to 90 ppb, while HO2 heterogeneous reaction decreased O3 to 33 ppb. In addition, O3 heterogeneous loss decreased O3 to 31 ppb. The effects of NO2, NO3, and N2O5 heterogeneous reactions showed opposite O3 concentration changes between the urban and extra-urban areas because of the response of the reactions to the two types of O3 formation regimes. When the aerosol radiative influence was included, the photolysis rate decreased and O3 decreased significantly to 73 ppb O3. The two aerosol-related processes should be considered in the study of O3 formation because high aerosol concentration is a ubiquitous phenomenon that affects the urban- and regional air quality in China.
Journal of Environmental Sciences 01/2012; 24(4):645-56. · 1.77 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: The impact of nitrous acid (HONO) chemistry on regional ozone and particulate matter in Pearl River Delta region was investigated using the community multiscale air quality (CMAQ) modeling system and the CB05 mechanism. Model simulations were conducted for a ten-day period in October 2004. Compared with available observed data, the model performance for NOx, SO2, PM10, and sulfate is reasonably good; however, predictions of HONO are an order of magnitude lower than observed data. The CB05 mechanism contains several homogenous reactions related to HONO. To improve the model performance for HONO, direct emissions, two heterogeneous reactions, and two surface photolysis reactions were incorporated into the model. The inclusion of the additional formation pathways significantly improved simulated HONO compared with observed data. The addition of HONO sources enhances daily maximum 8-hour ozone by up to 6 ppbV (8%) and daily mean PM2.5 by up to 17 ug/m3 (12%). They also affected ozone control strategy in Pearl River Delta region.
Advances in Meteorology 01/2012; 2012. · 1.24 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Epidemiologic studies have attributed adverse health effects to air pollution; however, controversy remains regarding the relationship between ambient oxidants [ozone (O₃) and nitrogen dioxide (NO₂)] and mortality, especially in Asia. We conducted a four-city time-series study to investigate acute effects of O₃ and NO₂ in the Pearl River Delta (PRD) of southern China, using data from 2006 through 2008.
We used generalized linear models with Poisson regression incorporating natural spline functions to analyze acute mortality in association with O₃ and NO₂, with PM₁₀ (particulate matter ≤ 10 μm in diameter) included as a major confounder. Effect estimates were determined for individual cities and for the four cities as a whole. We stratified the analysis according to high- and low- exposure periods for O₃.
We found consistent positive associations between ambient oxidants and daily mortality across the PRD cities. Overall, 10-μg/m³ increases in average O₃ and NO₂ concentrations over the previous 2 days were associated with 0.81% [95% confidence interval (CI): 0.63%, 1.00%] and 1.95% (95% CI: 1.62%, 2.29%) increases in total mortality, respectively, with stronger estimated effects for cardiovascular and respiratory mortality. After adjusting for PM₁₀, estimated effects of O₃ on total and cardiovascular mortality were stronger for exposure during high-exposure months (September through November), whereas respiratory mortality was associated with O₃ exposure during nonpeak exposure months only.
Our findings suggest significant acute mortality effects of O₃ and NO₂ in the PRD and strengthen the rationale for further limiting the ambient pollution levels in the area.
Environmental Health Perspectives 12/2011; 120(3):393-8. · 7.26 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Several studies reported acute mortality and morbidity effects of exposure to carbon monoxide (CO); which, however, has been least studied in Chinese population at regional scale.
We conducted a time-series analysis assessing mortality effects of CO in four cities located in the Pearl River Delta (PRD) of China, a labor and resource intensive city cluster, using daily mortality and air pollution data (2006-2008). Generalized linear model with Poisson regression incorporating natural spline functions was used to analyze the effects of exposure to ambient CO on total (nonaccidental), cardiovascular and respiratory mortality. Effect estimates were determined first for individual cities, and then focused for the mega-city Guangzhou.
We found exposure to CO was significantly associated with increased mortality in the mega-city of Guangzhou and medium-sized industrial city of Foshan. In specific, per 0.5ppm increase in the average lag 1-2 (previous two days) exposure to CO was associated with 3.04% [95% confidence interval (CI), 2.18-3.90%], 3.62% (95% CI, 2.20-5.06%) and 3.72% (95% CI, 1.71-5.76%) increases in excessive risks (ERs) of total, cardiovascular and respiratory mortality, in Guangzhou. Further, we observed significant heterogeneity in mortality effects of exposure to CO among the four PRD cities of different development levels: stronger mortality effects were found in larger, more developed and industrialized cities.
Exposure to ambient CO is associated with significant increases in total, cardiovascular and respiratory mortality in Chinese population. CO is an established biologic toxicant, whereas the effects and possible mechanisms of exposure to ambient level of CO and co-pollutants warrant further investigation.
Science of The Total Environment 12/2011; 410-411:34-40. · 3.16 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Hydroxyl radicals (OH) are a key species in atmospheric photochemistry. In the lower atmosphere, up to ~30% of the primary OH radical production is attributed to the photolysis of nitrous acid (HONO), and field observations suggest a large missing source of HONO. We show that soil nitrite can release HONO and explain the reported strength and diurnal variation of the missing source. Fertilized soils with low pH appear to be particularly strong sources of HONO and OH. Thus, agricultural activities and land-use changes may strongly influence the oxidizing capacity of the atmosphere. Because of the widespread occurrence of nitrite-producing microbes, the release of HONO from soil may also be important in natural environments, including forests and boreal regions.
[Show abstract][Hide abstract] ABSTRACT: Three comprehensive acid deposition models were used to simulate the sulfur concentrations over northeast Asia over the period
covering entire year of 2002, and discussed the aggregated uncertainties and discrepancies of the three models. The participating
models are from the countries participating in the project of Longrange Transboundary Air Pollutants in Northeast Asia (LTP):
China, Japan and Korea. The Eulerian Model-3/CMAQ (by China), Regional Air Quality Model (RAQM, by Japan), and Comprehensive
Acid Deposition Model (CADM, by Korea) were employed by each country with common emissions data established by the administrative
agencies of China, Japan and Korea. The episodic simulation results between 1 to 15, March 2002 are also presented, during
which aircraft measurements were carried out over the Yellow sea. The episodic results show both a wide short-term variability
in simulations against measurements, and maximum concentration differences of 3∼5 times among the three models, requiring
that further attention before confidence among the three models can be claimed for short-term simulations. However, the year-long
cumulative simulations showed almost the same general features, with lower aggregated uncertainties between the three models,
produced by the long term integration over northeast Asia.
Key wordsModel intercomparison–Long-range Transboundary Air Pollutants in Northeast Asia (LTP)–sulfur concentration simulation–Northeast Asia
Asia-Pacific Journal of the Atmospheric Sciences 08/2011; 47(4):399-411. · 0.78 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: PM2.5 samples were collected in a regional sampling network with three sites in Hong Kong and four sites in the adjacent inland Pearl River Delta (PRD) or Guangdong Province during four months/seasons from 2002-2003. Trans-boundary transport between Hong Kong and the inland PRD is inevitable under the influence of Asian monsoon. In summer, Hong Kong serves as the upwind site of the inland PRD while during other seasons it is under the influence of continental emissions. Previous studies have recognized the importance of using chemical signatures to differentiate local vs. regional contributions to air pollutants in Hong Kong such as the CO/NOx ratio, ratios of different VOC species. In this study, detailed chemical speciation by gas chromatography-mass spectrometry was performed with PM2.5 samples to identify new chemical signatures to distinguish aerosols in Hong Kong from those from the inland PRD. Since Hong Kong is not influenced by the continental emissions from the inland PRD during summer, comparison focused on chemical data obtained from this season for chemical signatures. The new ratios developed from the current study include LCPI/HCPI ratio of alkanes (0.39 +/- 0.02 in Hong Kong vs. 0.78 +/- 0.08 in the inland PRD), pyrene to benzo[ghi]perylene ratio (0.97 +/- 0.21 in Hong Kong compared to 0.20 +/- 0.06 in the inland PRD), and the ratio of 1,2-benzenedioic acid to 1,4-benzenedioic acid (1.8 +/- 0.1 in Hong Kong vs. 0.6 +/- 0.05 in the inland PRD). Results from this study also revealed that Hong Kong was impacted by ship emissions as reflected by substantially high V/Ni ratio (9 +/- 2) while this ratio was about 1-2 at all sites in the inland PRD, which is very close to typical ratios from residual oil combustion.
Journal of Environmental Sciences 07/2011; 23(7):1143-9. · 1.77 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Epidemiologic evidence for a causative association between black carbon (BC) and health outcomes is limited.Objectives: We estimated associations and exposure-response relationships between acute respiratory inflammation in schoolchildren and concentrations of BC and particulate matter with an aerodynamic diameter of ≤ 2.5 μm (PM2.5) in ambient air before and during the air pollution intervention for the 2008 Beijing Olympics.
We measured exhaled nitric oxide (eNO) as an acute respiratory inflammation biomarker and hourly mean air pollutant concentrations to estimate BC and PM2.5 exposure. We used 1,581 valid observations of 36 subjects over five visits in 2 years to estimate associations of eNO with BC and PM2.5 according to generalized estimating equations with polynomial distributed-lag models, controlling for body mass index, asthma, temperature, and relative humidity. We also assessed the relative importance of BC and PM2.5 with two-pollutant models.
Air pollution concentrations and eNO were clearly lower during the 2008 Olympics. BC and PM2.5 concentrations averaged over 0-24 hr were strongly associated with eNO, which increased by 16.6% [95% confidence interval (CI), 14.1-19.2%] and 18.7% (95% CI, 15.0-22.5%) per interquartile range (IQR) increase in BC (4.0 μg/m3) and PM2.5 (149 μg/m3), respectively. In the two-pollutant model, estimated effects of BC were robust, but associations between PM2.5 and eNO decreased with adjustment for BC. We found that eNO was associated with IQR increases in hourly BC concentrations up to 10 hr after exposure, consistent with effects primarily in the first hours after exposure.
Recent exposure to BC was associated with acute respiratory inflammation in schoolchildren in Beijing. Lower air pollution levels during the 2008 Olympics also were associated with reduced eNO.
Environmental Health Perspectives 06/2011; 119(10):1507-12. · 7.26 Impact Factor