Washout effect and diurnal variation for chlorinated hydrocarbons in ambient air

Chloroderivatives such as, 1,1,1-trichloroethane (C₂H₃Cl₃) carbontetrachloride (CCl₄), trichloroethylene (C₂HCl₃) and tetrachloroethylene (C₂Cl₄) in air were analyzed intermittently every half hour by ECD-gas chromatography with a programmed automatic gas inlet system for about seven weeks. The results showed a washout effect by rain related to the solubility in water. Decreases in daytime on clear days was demonstrated in the diurnal variation of C₂H₃Cl₃ from the statistical analysis, while distinct reduction of CCl₄ in daytime on clear days was not observed. On clear days, C₂HCl₃ showed the largest reduction while CCl₄ showed the least among C₂H₃Cl₃, CCl₄ and C₂HCl₃. This is compatible with conjectures from the reactivity with air pollutants such as NO,NO₂ and OH radicals in simulated photochemical chambers.     

An intercomparison of formaldehyde measurement techniques at ambient concentration

A study was conducted to evaluate five techniques for determining ambient formaldehyde concentrations. One technique used a spectroscopic determination, and the other four techniques used derivatization followed by fluorometric analysis or high-performance liquid chromatography with detection by u.v. absorption. Formaldehyde was generated by two techniques. In the first technique, zero air was bubbled through a solution of aqueous formaldehyde to produce gas-phase formaldehyde. Various compounds serving as possible interferences were added singly or in combination to these air mixtures. In the second technique, formaldehyde was generated as a product from controlled irradiations of hydrocarbons and nitrogen oxides in a smog chamber operated in a dynamic mode. The study was conducted as a blind intercomparison with no knowledge by the participants of the HCHO concentrations or the interferences added.The data from each of the techniques were compared against mean values in each sampling period. For formaldehyde in zero air, average deviations for each of the techniques ranged between 15 and 30%. At a formaldehyde concentration of 10 ppb, each technique showed no evidence for interferences by O₃ (190 ppbv), NO₂ (300 ppbv), SO₂ (20 ppbv), and H₂O₂ (7 ppbv). The agreement for formaldehyde concentrations measured for the photochemical mixtures was similar to that of the mixtures in zero air.Ambient measurements were also performed on three evenings and for one 36-h period. Ambient formaldehyde concentrations ranged from 1 to 10 ppbv. Ambient H₂O₂ measurements were also performed. A strong correlation in the diurnal concentration profile for formaldehyde and H₂O₂ was observed over the 36-h period.     

Seasonal and diurnal variations of ambient PM2.5 concentration in urban and rural environments in Beijing

Three years of measurement of PM_2.5 with 5-min time resolution was conducted from 2005 to 2007 in urban and rural environments in Beijing to study the seasonal and diurnal variations in PM_2.5 concentration. Pronounced seasonal variation was observed in the urban area, with the highest concentrations typically observed in the winter and the lowest concentrations generally found in the summer. In the rural area, the maximum in PM_2.5 concentration usually appeared during the spring, followed by a second maximum in the summer, while the minimum generally occurred in the winter. Significant diurnal variations in PM_2.5 concentration were observed in both urban and rural areas. In the urban area, the PM_2.5 concentration displays a bimodal pattern, with peaks between 7:00 and 8:00 a.m. and between 7:00 and 11:00 p.m. The minimum generally appears around noon. The morning peak is attributed to enhanced anthropogenic activity during rush hours. The decreases of boundary layer height and wind speed in the afternoon companying with increased source activity during the afternoon rush hour result in the highest PM_2.5 concentration during evening hours. In the rural area, the PM_2.5 concentration shows a unimodal pattern with a significant peak between 5:00 and 11:00 p.m.The seasonal and diurnal variations in PM_2.5 concentration in the urban area are mostly dominated by the seasonal and diurnal variability of boundary layer and source emissions. The year-to-year variability of rainfall also has an important influence on the seasonal variation of PM_2.5 in the urban area. The seasonal and diurnal wind patterns are more important factors for PM_2.5 variation in the rural area. Southerly winds carry pollutants emitted in southern urban areas northward and significantly enhance the PM_2.5 concentration level in the rural area.     

Origin of low-molecular-weight dicarboxylic acids and their concentration and size distribution variation in suburban aerosol

The concentrations and size distributions of low molecular weight dicarboxylic acids in suburban particulate matter collected in early and mid-autumn 2002 and early and mid-summer 2003 in Tainan, Taiwan, were analyzed. PM_2.5 contained, on average, 449.3 ng m⁻³ oxalic acid, 53.0 ng m⁻³ malic acid, 45.5 ng m⁻³ maleic acid, 29.6 ng m⁻³ succinic acid, 20.8 ng m⁻³ malonic acid, and 11.6 ng m⁻³ tartaric acid. Bar tartaric acid, concentrations were higher during the day, indicating that these acids are photochemical products. Furthermore, the malonic acid–succinic acid ratio of 0.79 during daytime and 0.60 during nighttime demonstrates that more succinic acid is converted to malonic acid during daytime, and that aerosol dicarboxylic acids predominantly originate from photochemical oxidation during daytime. The concentration peak of oxalic acid occurred in the condensation and droplet modes (0.32–1.0 μm), as did that of sulfate. In early summer, succinic acid, malonic acid, and oxalic acid major concentration peaks occurred at 0.32–0.54 μm, indicative of the relationship created by photochemical decomposition of succinc acid into malonic acid into oxalic acid. This photochemical decomposition accelerated in mid-summer such that most concentration peaks for succinic and malonic acids also occurred at 0.32–1.0 μm. Mid-summer is also the wettest period of the four in Tainan, with 85% RH. As a result of hygroscopic reactions in mid-summer, malonic acid and oxalic acid major concentration peaks shifted from 0.32–0.54 μm or 0.54–1.0 μm to 1.0–1.8 μm, thus extending the range in which these species were found to larger particle sizes, and this shift was highly correlated with a shift in succinic acid size distribution. This latter observation offers additional evidence that succinic acid is photochemically decomposed into malonic acid and oxalic acid and that the presence of malonic and oxalic acids in the wet mid-summer atmosphere is made more obvious via hygroscopic growth. Close correlation between succinic acid and Na⁺ and succinic acid and NO₃⁻ in the coarse mode is related to sea spray.     

Modeling in-stream attenuation of N-nitrosodimethylamine and formaldehyde during urban river transportation based on seasonal and diurnal variation

Environmental Science and Pollution Research - Disinfection by-products (DBPs) discharged from sewage treatment plants (STPs) could harm downstream receiving waters and drinking water resources....     

Sources and photodecomposition of formaldehyde and acetaldehyde in Rome ambient air

Atmospheric levels of formaldehyde and acetaldehyde as well as their diurnal and seasonal variations were investigated from 1994 to 1997 in downtown Rome during sunny and wind calm days. Hourly concentrations of formaldehyde ranged from 8 to 28 ppbV in summer and 7 to 17 ppbv in winter; acetaldehyde concentrations varied correspondingly within the 3–18 and 2–7 ppbv intervals. Percentages of both aldehydes photochemically produced were estimated through a simple relationship based upon the comparison of individual ratios of formaldehyde and acetaldehyde to toluene in ambient air and automobile emission. Photochemical production was found to weigh upon atmospheric levels for 80–90% in summer days. It dropped below 35% in the winter period, when direct emission from traffic largely predominated. Photochemical summer source was more efficient for acetaldehyde than for formaldehyde, especially in the early morning. The importance of formaldehyde as the major source of hydroxyl radicals in Rome was also assessed.     

Derivation of ambient water quality criteria for formaldehyde.

This paper describes the derivation of aquatic life water quality criteria for formaldehyde, developed in accordance with United States Environmental Protection Agency's (USEPA's) Guidelines for Deriving Numerical National Water Quality Criteria for the Protection of Aquatic Organisms and Their Uses. The initial step in deriving water quality criteria was to conduct an extensive literature search to assemble available acute and chronic toxicity data for formaldehyde. The literature search identified a large amount of information on acute toxicity of formaldehyde to fish and aquatic invertebrates. These acute data were evaluated with respect to data quality, and poor quality or uncertain data were excluded from the data base. The resulting data base met the USEPA requirements for criteria derivation by having data for at least one species in at least eight different taxonomic families. One shortcoming of the literature-derived data base, however, was that few studies involved analytical confirmation of nominal formaldehyde concentrations and reported toxicity endpoints. Also, there were relatively few data on chronic toxicity. The acute toxicity data set consisted of data for 12 species of fish, 3 species of amphibians, and 11 species of invertebrates. These data were sufficient, according to USEPA guidelines, to calculate a final acute value (FAV) of 9.15 mg/l, and an acute aquatic life water quality criterion (one-half the FAV) of 4.58 mg/l. A final acute-chronic ratio (ACR) was calculated using available chronic toxicity data and USEPA-recommended conservative default assumptions to account for missing data. Using the FAV and the final ACR (5.69), the final chronic aquatic life water quality criterion was determined to be 1.61 mg/l.     

Polycyclic aromatic hydrocarbons in the ambient air of suburban and industrial regions of central Taiwan

The concentrations of gas-phase and particle-bound polycyclic aromatic hydrocarbons (PAHs) were measured simultaneously at an industrial area (Taichung Industrial Park) and a suburban area (Tunghai University Campus) in Taichung, Taiwan. Twenty-four hours samplings for two consecutive days were performed between August and December 2002 at both sampling sites. Ambient air particle-bound PAHs were collected on quartz filters and gas-phase PAHs were collected on glass cartridges using a PUF Sampler, respectively. Both types of samples were extracted with a DCM/n-hexane mixture (50/50, v/v) for 24 h, then the extracts were subjected to gas chromatography-mass spectrometric (GC-MS) analysis. Total PAHs concentrations at the Taichung Industrial Park (TIP) sampling site and the Tunghai University Campus (THUC) sampling site were found to be 1232.3+/-963.6 and 609.8+/-356.3 ng/m(3), respectively. Stationary combustion processes were mainly responsible for PAHs sources at the TIP sampling site, while traffic vehicle exhaust was the largest contributor for PAHs sources at the THUC sampling site.     

Vertical and diurnal characterization of volatile organic compounds in ambient air in urban areas

More than half of the world's population lives in cities, and their populations are rapidly increasing. Information on vertical and diurnal characterizations of volatile organic compounds (VOCs) in urban areas with heavy ambient air pollution can help further understand the impact of ambient VOCs on the local urban environment. This study characterized vertical and diurnal variations in VOCs at 2, 13, 32, 58, and 111 m during four daily time periods (7:00 to 9:00 a.m., 12:00 to 2:00 p.m., 5:00 to 7:00 p.m., and 11:00 p.m. to 1:00 a.m.) at the upwind of a high-rise building in downtown, Kaohsiung City, Taiwan. The study used gas chromatography-mass spectrometry to analyze air samples collected by silica-coated canisters. The vertical distributions of ambient VOC profiles showed that VOCs tended to decrease at greater heights. However, VOC levels were found to be higher at 13 m than at ground level at midnight from 11:00 p.m. to 1:00 a.m. and higher at 32 than 13 m between 7:00 and 9:00 a.m. These observations suggest that vertical dispersion and dilution of airborne pollutants could be jointly affected by local meteorological conditions and the proximity of pollution sources. The maximum concentration of VOCs was recorded during the morning rush hours from 7:00 to 9:00 a.m., followed by rush hours from 5:00 to 7:00 p.m., hours from 12:00 to 2:00 p.m., and hours from 11:00 p.m. to 1:00 a.m., indicating that the most VOC compounds in urban air originate from traffic and transportation emissions. The benzene-toluene-ethyl benzene-xylene (BTEX) source analysis shows that BTEX at all heights were mostly associated with vehicle transportation activities on the ground.     

Variations and sources of ambient formaldehyde for the 2008 Beijing Olympic games

As the host city of the 2008 Olympic games, Beijing implemented a series of air pollution control measures before and during the Olympic games. Ambient formaldehyde (HCHO) concentrations were measured using a fluorometric instrument based on a diffusion scrubber and the Hantzsch reaction; hydrocarbons were simultaneously measured using gas chromatography–mass spectrometry (GC–MS). Meteorological parameters, CO, O₃, and NO₂ concentrations were measured by standard commercial instrumentation. In four separate periods: (a) before the vehicle plate number control (3–19 July); (b) during the Olympic Games (8–24 August); (c) during the Paralympic Games (6–17 September) and (d) after the vehicle control was ceased (21–28 September), the average HCHO mixing ratios were 7.31 ± 2.67 ppbv, 5.54 ± 2.41 ppbv, 8.72 ± 2.48 ppbv, and 6.42 ± 2.79 ppbv, while the total non-methane hydrocarbons (NMHCs) measured were 30.41 ± 18.08 ppbv, 18.12 ± 9.38 ppbv, 30.50 ± 13.37 ppbv, and 33.33 ± 15.85 ppbv, respectively. Both HCHO and NMHC levels were the lowest during the Olympic games, and increased again during the Paralympic games even with the same vehicle control measures operative. Similar diurnal HCHO and O₃ patterns indicated that photo-oxidation of NMHCs may be the major source of HCHO. The diurnal profile of total NMHCs was very similar to that of NO₂ and CO: morning and evening peaks appeared in rush hours, indicating even after strict vehicle control, automobile emission may still be the dominant source of the HCHO precursors. The contributions of HCHO, alkanes, alkenes, and aromatics to OH loss rates were also calculated. HCHO contributed 22 ± 3% to the total VOCs and 24 ± 1% to the total OH loss rate. HCHO was not only important in term of abundance, but also important in chemical reactivity in the air.     

Rainwater formaldehyde: concentration,deposition and photochemical formation

Formaldehyde (HCHO) concentrations were measured in 116 rain samples in Wilmington, NC from June 1996 to February 1998. Concentrations ranged from below the detection limit of 10 nM, to 13 μM, in the range of HCHO levels reported at other locations worldwide. The volume-weighted annual average rainwater formaldehyde concentration was 3.3±0.3 μM and comprised approximately 3% of the measured dissolved organic carbon. Using the volume weighted average HCHO concentration and annual precipitation of 1.4 m, an annual formaldehyde deposition of 4.6 mmol m⁻² yr⁻¹ was determined. Rainwater is a significant source of formaldehyde to surface waters and may contribute as much as 30 times the resident amount found in natural waters of southeastern North Carolina during the summer. Formaldehyde concentrations did not correlate with precipitation volume suggesting continuous supply during rain events. Evidence is presented which indicates part of this supply may be from direct photochemical production in the aqueous phase. Formaldehyde levels exhibited a distinct seasonal oscillation, with higher concentrations during the summer. This pattern is similar to that observed with other rainwater parameters at this site including pH, nitrate, and ammonium, and is most likely the result of increased photochemical production, as well as biogenic and anthropogenic emissions during summer months. The concentration of formaldehyde in both winter El Nino rains and summer tropical rains was less than half its concentration in non-El Nino or non-tropical events, suggesting significant terrestrial input. Formaldehyde was correlated with hydrogen peroxide and non-sea-salt sulfate deposition suggesting a relationship between HCHO, H₂O₂, S(VI) within the troposphere.     

福州市东郊大气气溶胶物理特性及其来源分析

利用GRIMM180环境颗粒物监测仪观测了2012年12月至2013年11月福州市东郊气溶胶数浓度和质量浓度,分析了该地区气溶胶粒子的主要物理特征。结果表明,福州市东郊气溶胶数浓度和质量浓度都有着明显的季节变化特征,冬季最高,夏季最低;与京津冀、长三角和西部大城市相比,福州市东郊气溶胶质量浓度较低,空气质量较好。从PM_(2.5)在PM10中所占比例来看,PM_(2.5)是影响福州市东郊空气质量最主要的因子。在冬季气溶胶数浓度日变化基本呈双峰分布,早晨和傍晚分别出现峰值;夏季呈单峰分布,峰值出现在午后。利用后向轨迹HYSPLIT-4模式,经过聚类分析得到,在春季、秋季和冬季福州市气团输送来源主要是北方内陆和福州本地及邻近地区;而在夏季海洋是气团的主要输送来源。     

高表面氧MnOx/类水滑石催化剂常温催化低浓度甲醛的性能

常温催化氧化技术是去除室内低浓度甲醛(HCHO)的一种有效方法,其中过渡金属氧化物锰基催化剂在催化降解方面性能优异,相较于贵金属催化剂,具有成本低、活性高、稳定性良好、应用前景广等优点。采用共沉淀法制备了类水滑石载体和锰基/类水滑石催化剂,将类水滑石与锰基氧化物相结合用于常温催化氧化,克服了锰基氧化物常温条件下因大量吸附水蒸气而导致稳定性降低的缺点,同时研究考察了载体组成、煅烧温度、氧化锰负载量等对催化剂常温催化氧化性能的影响,并通过XRD、SEM、BET、EPR、XPS等技术对催化剂进行了微观表征。结果表明,当类水滑石中n(Mg)∶n(Al)=4∶1,氧化锰负载量 (质量分数) 为40%,煅烧温度为200 ℃时,所述MnO_x/Mg₄Al₁催化剂性能最佳,其48 h甲醛去除率高达98.5%,甲醛质量浓度由1.000 mg·m^-3降至0.015 mg·m⁻³。类水滑石载体表面存有大量羟基基团,有利于吸附低浓度甲醛及中间产物进而利于催化剂催化氧化性能提升。通过XPS分析可知,相较于MnO_x催化剂,MnO_x/Mg₄Al₁催化剂中O_β/(O_α+O_β)相对含量比例由35.7%提升至88.0%,表面氧含量(O_β)大幅提升,其在甲醛常温催化氧化过程中发挥着极其重要作用。本研究结果可为常温催化氧化甲醛提供参考。     

Impact of ambient temperature on hospital admissions for respiratory diseases in suburban rural villages in northwest China

Environmental Science and Pollution Research - Extreme temperature is strongly associated with human health, but few studies are available for the effects of extreme temperatures on respiratory...     

Prediction of ozone concentration in ambient air using multivariate methods

Multivariate statistical methods including pattern recognition (Principal Component Analysis--PCA) and modeling (Multiple Linear Regression--MLR, Partial Least Squares--PLS, as well as Principal Component Regression--PCR) methods were carried out to evaluate the state of ambient air in Miskolc (second largest city in Hungary). Samples were taken from near the ground at a place with an extremely heavy traffic. Although PCA is not able to determine the significance of variables, it can uncover their similarities and classify the cases. PCA revealed that it is worth to separate day and night data because different factors influence the ozone concentrations during all day. Ozone concentration was modeled by MLR and PCR with the same efficiency if the conditions of meteorological parameters were not changed (i.e. morning and afternoon). Without night data, PCR and PLS suggest that the main process is not a photochemical but a chemical one.     

Spatio-temporal covariation of urban particle number concentration and ambient noise

Mobile measurements of ambient noise and particle number concentrations were carried out within an urban residential area in Essen, Germany, during summer 2008. A busy major road with a traffic intensity of about 44,000 vehicles per day was situated within the study area. The spatio-temporal distribution of noise and particles was closely coupled to road traffic on the major road. Total particle number concentrations in proximity to the main road were on average between 25,000 cm^?3 and 35,000 cm^?3 while sound levels reached 70–78 dB(A). These estimates were more than double-fold (factor 2.4) in comparison to the urban residential background. At a 50 m distance off the road particle number concentrations were decaying to about 50% of the initial value. The measurements were characterised by close spatial correlation between total particle number concentration and ambient noise with correlation coefficients of up to r = 0.74. However, during one measurement day coupling between both quantities was weak due to higher turbulent mixing within the canopy layer and a change in ambient wind directions. Enhanced dilution of particle emission from road traffic by turbulent mixing and ‘decoupling’ from the influence of road traffic are believed to be responsible.     

Climatology and forecast modeling of ambient carbon monoxide in Phoenix, Arizona

We perform a climatology of factors influencing ambient carbon monoxide (CO), in which we examine the relationships between meteorology, traffic patterns, and CO at seasonal, weekly, and diurnal time scales in Phoenix, Arizona. From this analysis we identify a range of potentially important variables for statistical CO modeling. Using stepwise multivariate regression, we create a suite of models for hourly and 8-h ambient CO designed for daily operational forecasting purposes. The resulting models include variables and interaction terms related to anticipated nocturnal atmospheric stability as well as antecedent and climatological CO behavior. The models are evaluated using a range of error statistics and skill measures. The most successful approach employs a two-stage modeling strategy in which an initial prediction is made that may, depending on the forecast value, be followed by a second prediction that improves upon the first. The best models provide accurate daily forecasts of CO, with explained variances approaching 0.9 and errors under 1 ppm.     

Nonlinear analysis and prediction of coarse particulate matter concentration in ambient air

This study attempts to characterize and predict coarse particulate matter (PM10) concentration in ambient air using the concepts of nonlinear dynamical theory. PM10 data observed daily from 1999 to 2002 at a site in Mumbai, India, was used to study the applicability of the chaos theory. First, the autocorrelation function and Fourier power spectrum were used to analyze the behavior of the time-series. The dynamics of the time-series was additionally studied through correlation integral analysis and phase space reconstruction. The nonlinear predictions were then obtained using local polynomial approximation based on the reconstructed phase space. The results were then compared with the autoregressive model. The results of nonlinear analysis indicated the presence of chaotic character in the PM10 time-series. It was also observed that the nonlinear local approximation outperforms the autoregressive model, because the observed relative error of prediction for the autoregressive model was greater than the local approximation model. The invariant measures of nonlinear dynamics computed for the predicted time-series using the two models also supported the same findings.