Science of the Total Environment 382 (2007) 324 – 341 www.elsevier.com/locate/scitotenv Long-term visibility trends in one highly urbanized, one highly industrialized, and two Rural areas of Taiwan Ying I. Tsai a,b,⁎, Su-Ching Kuo c , Wen-Jhy Lee b,d , Chien-Lung Chen e , Pei-Ti Chen f a c Department of Environmental Engineering and Science, Chia Nan University of Pharmacy and Science, 60, Sec. 1, Erh-Jen Rd., Jen-Te, Tainan, Taiwan 717, ROC b Sustainable Environment Research Center, National Cheng Kung University, 1, University Rd., Tainan, Taiwan 701, ROC Department of Applied Chemistry, Chia Nan University of Pharmacy and Science, 60, Sec. 1, Erh-Jen Rd., Jen-Te, Tainan, Taiwan 717, ROC d Department of Environmental Engineering, National Cheng Kung University, 1, University Rd., Tainan, Taiwan 701, ROC e Department of Finance, Fortune Institute of Technology, 1-10, Nwongchang Rd., Daliao, Kaohsiung, Taiwan 831, ROC f Department of Hospitality Management, Chung Hua University, 707, Sec. 2, Wu-Fu Rd., Hsinchu, Taiwan 300, ROC Received 4 August 2006; received in revised form 24 April 2007; accepted 26 April 2007 Available online 4 June 2007 Abstract Visibility trends on the island of Taiwan were investigated employing visibility and meteorological (1961–2003), and air pollutant (1994–2003) data from one highly urbanized center (Taipei), one highly industrialized center (Kaohsiung), and two rural centers (Hualien and Taitung). Average annual visibility (1961–2003) was significantly higher at the rural centers. Unlike at the other centers, visibility in Taipei improved between 1992 (6.6 km) and 2003 (9.9 km), and this can be linked to the construction and expansion of a mass transit rail system in Taipei, the use of which has helped reduce emissions of traffic related air pollutants, particles, and NO2. This has left Kaohsiung with the lowest annual visibility since 1994, despite its 1961–2003 average being superior to that of Taipei. Precipitation lowers visibility, as demonstrated by the all-centers correlation coefficient for visibility and precipitation of − 0.92. Hence, frequency of precipitation is one of the factors contributing to the average annual visibility number. The poorest air quality category (‘episode’), most commonly experienced in Taipei and Kaohsiung, was characterized by relatively high concentrations of PM10 and NOx at those centers, with comparatively high atmospheric pressure and comparatively low visibility and wind speed. Excepting O3, pollutant concentrations were slightly higher during weekdays, although there was no consistent, significant difference in weekday–weekend visibility. Principal component analysis demonstrated that visibility was markedly reduced in Taipei, Kaohsiung, and Hualien by increased vehicular emissions, road traffic dust, and industrial activity, but not in Taitung, where visibility was as a result superior to that at the other centers and degradation in visibility was likely a response to long-range transport of pollutants rather than local sources. Optimal empirical regression models indicated a negative impact on visibility for each of PM10, SO2 and NO2, particularly so for PM10, and validity of these models for Taipei, Kaohsiung, and Hualien was confirmed by correlation coefficients of simulated and observed average visibility of 0.63–0.72 for daily visibility and 0.85–0.88 for monthly visibility. For Taitung these figures were only 0.46 and 0.50, respectively, indicating that simulations for Taitung should include long-range transport as a pollutant source. © 2007 Elsevier B.V. All rights reserved. Keywords: Visibility deterioration; Air quality; Weekend effect; Principal component analysis; Empirical model ⁎ Corresponding author. Department of Environmental Engineering and Science, Chia Nan University of Pharmacy and Science, 60, Sec. 1, ErhJen Rd., Jen-Te, Tainan, Taiwan 717, ROC. Tel.: +886 6 266 0208; fax: +886 6 266 9090. E-mail address: [email protected] (Y.I. Tsai). 0048-9697/$ - see front matter © 2007 Elsevier B.V. All rights reserved. doi:10.1016/j.scitotenv.2007.04.048 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 1. Introduction Visibility is related to the reduction in brightness as photons are absorbed or scattered by particles in the atmosphere between the viewer and the object; atmospheric extinction. Atmospheric species can therefore be assigned an extinction coefficient, the sum of their scattering and absorption coefficients. The scattering coefficient of atmospheric pollutants and hence their effect on visibility has been shown to differ according to pollutant characteristics (Cohen, 1975; Horvath, 1995, 1996; Seinfeld and Pandis, 1998; Tsai, 2005). Visibility is therefore a highly relevant factor in studies of atmospheric pollution, is used as a referent for differentiating good and poor air quality (Tsai and Cheng, 1999), and forms part of comprehensive meteorological and climatological analyses. Appel et al. (1985) found that the main culprits in atmospheric visibility degradation are PM2.5 and NO2. The specific content of PM2.5 is a most important factor in its effect on visibility because the size and chemical composition of each component particle affects its ability to refract, scatter, and absorb light. Sulfates were found to be responsible for about 60–70% of atmospheric extinction in the eastern US, while in the inner mountain west sulfates were responsible for 30%, carbon aerosols for 35%, and coarse mass for between 15– 25% (Malm and Day, 2000). There is a strong association between presence of PM2.5 and presence of PM10, to the extent that a targeted reduction of PM10 is likely to lead to an increase in atmospheric visibility (Malm and Day, 2000; Tsai et al., 2003). Indeed, Kim et al. (2001) reported that during Asian dust storm periods, when hourly averaged concentration of PM10 rose from 33 to 602 μg m− 3, hourly averaged visibility decreased from 62 km to just 2 km. Chan et al. (1999) found that poor visibility in Brisbane, Australia, was mainly caused by emissions of pollutants from traffic sources, followed by secondary sulfates and biomass burning, while Lee and Sequeira (2002) indicated that fine ammoniated sulfate aerosol is probably the predominant water-soluble inorganic visibility-reducing component in Hong Kong. Stuart and Hoff (1994) took long-term visibility data from 140 observation stations and developed a novel statistical technique by which the frequency distributions of the unbiased data and median visibilities were consistent with expectations about the geographic behavior of visibility. Their results showed that the average summer visibility at the Inuvik and Dawson Creeks within the Canadian Arctic Circle was up to 109 km and 222 km, respectively, reducing to 23 km and 76 km, 325 respectively, in winter, possibly due to the ‘arctic haze’ effect. In the Visibility Impairment Due to Sulfur Transport and Transformation in the Atmosphere (VISTTA) project (Blumenthal et al., 1981), it was found that NO2 in the emissions from Arizona Navajo coal-fired power plant led to brown clouds and the disappearance of blue light. However, the secondary photochemical particles did not affect air quality in the region beyond 100 km from the plant at low relative humidity. The observed aerosol in the study region was partially from wildfires in southern California, to the southwest. Using data from 36 monitoring stations across the US, the Interagency Monitoring of Protected Visual Environments (IMPROVE) project (Sisler and Malm, 1994) discovered from the seasonal visibility variations that watersoluble aerosols cause the visibility to deteriorate and that humidity is a major factor influencing light scattering of atmospheric aerosols. The scattering coefficient of atmospheric particles was implicated in the results of the Region Visibility Experimental Assessment in the Lower Fraser Valley (REVEAL) project (Pryor et al., 1997), which showed that although atmospheric PM2.5 was b 20 μg m− 3, visibility was reduced to b 10 km. It was calculated that sulfate and nitrate particles contributed between 55–67% of the light scattering effect of the fine particulate. Lowenthal et al. (1997) also indicated in the REVEAL project that, for towns in a basin about 50–80 km east of Vancouver, 40% of PM2.5 was from traffic emissions while secondary sulfate contributed about 26% of the total pollution. The contribution from nitrate varied dramatically from 9–20%. Day et al. (1997) used the IMPROVE project results to analyze the atmospheric aerosol compositions from 1988 to 1994 for the Great Smoky Mountains National Park and discovered that summer SO42− and organic carbon concentrations were higher than in other seasons; the aerosol was mostly acidic. Winter saw higher concentrations of SO2 and NO3− than other seasons, indicating that SO2 was not converted into SO42− during winter. The winter aerosol was mostly neutral. Finally, in the Measurement of Haze Visual Effects (MOHAVE) project, Gebhart and Malm (1997) discovered that the sulfur-containing material, organic carbon, light-absorbing elemental carbon and some trace elements in emissions from southern California during summer may be transported to Southern Nevada/ Southwestern Arizona. During winter, however, these contaminants did not disperse easily from their source, instead lingering in regions to the north or the Grand Canyon region to the east, and causing higher concentrations of pollutants in the Grand Canyon region. 326 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 Malm and Gebhart (1997) additionally showed, based on the relationship between sulfur-containing substances and Se, that about 50% of sulfur-containing particles originated from a local coal-fired power plant. In winter, about 50% of sulfur-containing substances were from wood burning while in summer various sources from cities became more important. Of relevance to visibility and air quality studies is a phenomenon known as the weekend effect, in which O3 concentration is higher on weekends than on weekdays in spite of the fact that ozone pollutant precursors such as NO and volatile organic compounds are lower on weekends. The weekend effect has been reported in America since the 1970s (Cleveland et al., 1974; Elkus and Wilson, 1977; Qin et al., 2004) and was reported in Tainan, Taiwan, in 2005 by Tsai, associated with higher weekend visibility. Situated off the south-east coast of China, Taiwan has a warm and humid climate. The hottest month is July, with average temperatures near 30 °C, and the coldest month is January, with average temperatures near 20 °C. As elsewhere in the region, chronic and acute episodes of visibility degradation in Taiwan are readily evident to the resident and visitor alike. However, there has been no extensive cross-Taiwan study of long term visibility degradation to date, perhaps in part because monitoring of critical air pollutants and atmospheric chemical data was not detailed until about 15 years ago. In this research therefore, four geographically distant centers across Taiwan; Taipei, Kaohsiung, Hualien, and Taitung, representing three identifiably different local pollutant mixes, were chosen for analysis of visibility and air quality over time. Taipei, in the north of Taiwan, is the largest metropolitan area and the capital of Taiwan, with a population of approximately 2.7 million and a population density of 9676 km− 2. It is surrounded by hills or mountains and suffers significant emissions of pollutants from automobiles and factories. Kaohsiung, on a flat plain on the south-west coast, is the biggest port and most heavily industrialized city in Taiwan, with a population of approximately 1.5 million and a population density of 9333 km− 2. It suffers significant emissions of pollutants from both automobiles and fuel combustion from numerous petrochemical and metal processing industrial areas. Taipei and Kaohsiung will henceforth be referred to as ‘metropolitan areas’. Both occasionally suffer 24-h PM10 levels of N150 μg m− 3, leading to an ‘episode’ air quality classification under the Taiwan National Ambient Air Quality Standards (NAAQS) classification system. Such events are also generally associated with visibility deterioration linked to chemical smog (Tsai et al., 2003; Tsai, 2005). Hualien, in the east of Taiwan, is a typical rural area, with a population of approximately 360,000 and a population density of 77 km− 2. Taitung, in the southeast of Taiwan, is also typical rural, with a population of approximately 240,000 and a population density of 69 km− 2. Both of these ‘non-metropolitan’ centers are surrounded by hills or mountains and neither has any significant emissions of industrial pollutants, only low-density traffic emissions. Two data sets, one covering the period 1961–2003 and one 1994–2003, were utilized to determine changes in visibility over time and the specific factors affecting visibility in the study area, aided by a Varimax-rotated principal component analysis employed to establish the relationships between major air pollutants, meteorological parameters, and visibility. 2. Materials and methods 2.1. Visibility observations Visibility observations came from the N400,000 sets of meteorological data and visibility observations made between 1961 and 2003 by Weather Service Office (WSO) staff at the Taipei, Kaohsiung, Hualien, and Tawu (for Taitung) WSOs, shown in Fig. 1. Visibility observations are made at a height of 20–36 m, on the roof of the building, and require that an operator scans the horizon of at least 180° for predetermined sets of objects made up of easily identifiable structures and objects such as tall buildings, towers, and mountain ridges. The furthest distance at which it is possible to see more than half the set of objects at that distance is recorded as the prevailing visibility. Between 1961 and 2003, visibility observations were made five times a day (0800, 0900, 1100, 1400 and 1700 h). The daily visibility has been continually observed for more than 40 years by different observers. Over this time, selection of targets has at times changed as the horizon itself has changed due to municipal or regional development. Following World Meteorological Organization (WMO) rules, observations were always made by two operators, both specially trained, who arrived at a consensus for each observation, so guarding against individual observer differences. Also, procedures remained constant throughout the period, reducing the risk of variation from non-operator factors to a minimum. 2.2. Air quality data The air quality data in this study came from approximately one million sets recorded between 1994 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 327 Fig. 1. Position of weather observation and air quality monitoring stations, major industrial areas, major emission sources and highways in four centers in Taiwan. and 2003 at seventeen monitoring stations that form part of the Taiwan Air Quality Monitoring Network (TAQMN). Nine of the monitoring stations (henceforth referred to as ‘sites’) were in Taipei: Hsintien (HT), Tucheng (TC), Panchiao (PC), Hsinchuang (HC), Tsailiao (TL), Shinlin (SL), Chungshan (CS), Wanhua (WH), and Kuting (KT). Six were in Kaohsiung: Jenwu (JW), Nanzi (NZ), Tsoying (TY), Chiankin (CK), Chiancheng (CC), and Hsiaokang (HK). One was in Hualien (HL) and one was in Taitung (TT), and the locations of all can be seen in Fig. 1. The TAQMN stations monitor air pollutants according to reference or equivalent United States Environmental Protection Agency (US EPA) methods. PM10 is monitored at the sites using a β-gauge automated particle sampler from Kimoto Electric Co., Ltd., Japan, while sulfur dioxide (SO2), carbon monoxide (CO), ozone (O3), and oxides of nitrogen (NO and NO2) are monitored using instruments from Thermo Environmental Instruments, Inc., USA. Continuous 24 h trace gas measurements of SO2, CO, O3 and nitrogen oxides (NOx) were made using pulsed fluorescence, infrared absorption, absorption of ultraviolet light and chemiluminescence, respectively. Each site is equipped with an automated calibration system identical to those used for the regulatory monitoring of air quality in Taiwan (Tsai et al., 2003; Tsai, 2005). Minimum detectable limits provided by the aforementioned companies and confirmed in the 328 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 field are 1 ppbv for SO2, 0.1 ppmv for CO, 2 ppbv for O3, 10 μg m− 3 for PM10, and 1 ppbv for NOx. Unfortunately, there was no data available for PM2.5 or for the chemical composition of PM10. 2.3. Treatment and categorization of data The Pollutant Standard Index (PSI) in Taiwan is based on daily observations of the five criteria pollutants. For each pollutant, a sub-index is calculated from a segmented linear function that transforms ambient concentrations onto a scale extending from 0 to 500. A 24 h PSI value of b 50 is categorized as a ‘clear’ air quality day, one of 50–100 as ‘moderate,’ and one of ≥ 100 as ‘hazy and unhealthy’ or ‘episode’ air quality. As discussed, PM10 is mostly a reliable surrogate for PM2.5, and of the five criteria air pollutants monitored by the TAQMN it is the one most closely correlated with air quality. A 24 h PM10 concentration of b 50 μg m− 3 leads to a ‘clear’ categorization, and corresponds to a PSI b50, while one of N 150 μg m− 3 leads to a ‘hazy and unhealthy’ or ‘PM10 episode’ categorization. 2.4. Mixing layer height Mixing layer height (Mix), the height at which aerosol dispersion occurs in the atmospheric boundary layer, is an important parameter in the assessment of pollutant concentration and dispersal and a crucial input parameter in local visibility models. Its calculation, using relative humidity, pressure, wind vector, cloud fraction, zenith angle, and rain duration data obtained by interpolation of the surface weather station data, is based on a Lagrangian model (Tu, 1999), which parameterizes the mixing layer height (Holzworth, 1972), where the land parameters are determined according to Tsuang and Tu (2002). The input lapse rate above a mixing layer height was either set at a default value of the wet lapse rate (− 6.5 °K km − 1 ) or calculated according to rawinsonde data. 2.5. Statistical methods Variation in visibility can be described using a Weibull distribution, a standardized exponential distribution that uses a cumulative frequency, F, of a parameter V to simulate the visibility: F ¼ 1 e ð C Þ V k ð1Þ where k is defined as the form factor and C is defined as the scale factor. Both k and C can be either normal or log-normal distributions. Stuart and Hoff (1994) applied the Weibull distribution to fit the frequency of occurrence of visibility between 0.8–24.1 km. At the confidence level of 95%, the correlation coefficient of the fit, r, can be as high as 0.997, indicating that the Weibull distribution offers an excellent estimation of the actual mean visibility. In contrast to the Wiebull distribution, the principal component analysis (PCA) eigenvector model is a relatively simple and effective tool for the identification of relationships in voluminous environmental data containing multiple factors using the eigenvector decomposition of a matrix of pairwise correlations among many variables (Miller et al., 2002). It was first applied to estimate sources of urban ambient inhalable particulate in Boston (Thurston and Spengler, 1985). PCA has since then been successfully applied in numerous source apportionment studies of air pollutants and environmental issues (Statheropoulos et al., 1998; Tsai et al., 2003; Tsai, 2005). Pryor et al. (1994) identified the sources of visibilitydegrading aerosol for the impaired visibility observed in the Lower Fraser Valley (LFV) of British Columbia, Canada. They discovered that five significant principal components accounted for over 70% of the explainable variance in the fine particle speciation dataset. The loading correlation coefficients of these components were used in evaluating the sources contributing to particulate light scattering and it was found that traffic emissions and wood burning contributed most of the light scattering. The PCA technique is, in principle, a data reduction exercise and simplifies possible models describing the data set. Data reduction is achieved by finding linear combinations (principal components, PCs) of the original variables, which account for as much of the original total variance as possible. It was used in this study to identify which pollutants and meteorological factors influenced visibility and to rank their importance, in so doing identifying relationships and trends. To determine the major factors correlated with visibility, a Varimax-rotated PCA, solved by eigenvector decomposition and used to redistribute the variance as well as to provide a more interpretable structure to the factors, was performed on dimensionless standardized data sets from the air quality monitoring stations and the weather service office data collected between 1994 and 2003. Air quality and meteorological data were calculated with PCs from a correlation matrix of visibility observations, meteorological parameters, and air pollutant concentrations. Only principal components with eigen values N1.0 were considered to be meaningful in the analysis Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 and interpretation of visibility and causative factors. Loading correlation coefficients of larger than or equal to 0.6 between the PCs and the original variables were considered as influential source identity to each PC. Further details of the statistical technique, including theory and procedure, have been presented by Thurston and Spengler (1985), Richman (1986) and by us in earlier publications (Tsai et al., 2003; Tsai, 2005). 3. Results and discussion 3.1. Annual and monthly visibilities It can be seen from Fig. 2 that the general trend in visibility for Kaohsiung, Hualien, and Taitung for the entire period 1961 to 2003 is one of decline. The exception is Taipei, which has seen an improving trend in visibility from 1994. Between 1961 and 2003 the metropolitan centers (Taipei and Kaohsiung) experienced the poorest annual average visibility (8.8 ± 1.5 km and 13.9 ± 5.9 km, respectively). In Taipei, visibility was 11.1 km in 1960 and had dropped to 6.6 km in 1992. Since then the trend has apparently reversed, with visibility in 2003 averaging 9.9 km. This reversal can be linked to the construction and expansion of a mass transit rail system in Taipei, the use of which has helped reduce emissions of traffic related air pollutants, particles, and NO2. In Kaohsiung, meanwhile, visibility worsened from 25.7 km in 1960 to an annual low of 4.9 km in 2000, subsequent to which the annual averages suggest a relatively unchanging picture going forward. In the non-metropolitan centers average annual visibility between 1961 and 2003 was 22.8 ± 6.9 km (Hualien) and 25.7 ± 5.0 km (Taitung). Both centers experienced a continued worsening of visibility from the 329 start to the end of the period, although in 2003 visibility still remained significantly better than for Taipei and Kaohsiung. In Hualien visibility dropped from 33.7 km in 1960 to a low of 13.1 in 2003 while in Taitung it dropped from 35.3 km in 1960 to a low of 16.2 km in 2003. This unabated worsening reflects increasing local traffic density and industrial emissions (albeit still at a much lower level than in the metropolitan centers) and long range transport pollutants, mostly from industrial and urban centers to the west. The best month for visibility (highest monthly average) was June or July for all centers. The worst month for visibility showed more variability: for Taipei it was March, for Kaohsiung December, for Hualien March using the 1961–2003 data set and February using the 1994–2003 data set, and for Taitung February using 1961–2003 and May using 1994–2003. 3.2. Precipitation and visibility Visibility was reduced by precipitation. This can be seen from Table 1, which shows that when precipitation days are included in the data set the average annual visibility for the period 1961–2003 suffers a higher percentage reduction for the centers with higher precipitation frequency (i.e. more days with precipitation). Average annual visibility for 1961–2003 for Taipei, the center with the highest precipitation frequency of 13.2%, is reduced by 0.58 km or 6.63% of the ‘all observations’ visibility with precipitation days included, whereas for Kaohsiung, the center with the lowest precipitation frequency of 5.58%, visibility is reduced by only 0.25 km or 1.79% of the ‘all observations’ visibility. These results are similar to those obtained by Stuart and Hoff (1994) at Sault Ste. Marie, Canada. During rain, the median visibility in Sault Ste. Marie dropped from 33.5 km for all hours to 8.5 km. Median visibility fell further to 7.3 km during smoky or hazy days and to 3.5 km in foggy conditions. 3.3. Air quality and visibility Fig. 2. Time series of mean annual visibilities in Taiwan, 1961–2003. Table 2 shows air quality data from nine monitoring stations in Taipei, six in Kaohsiung, and one in Hualien and Taitung in the period 1994–2003, classified using 24-h PM10 into the three PSI categories of ‘clear,’ ‘moderate,’ and ‘episode.’ Visibility was highly correlated with air quality categories at the metropolitan centers of Taipei and Kaohsiung whereas visibility associated with ‘moderate’ air quality was slightly worse than that associated with ‘episode’ air quality at Hualien and Taitung. 330 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 Table 1 Degradation in visibility attributable to precipitation, 1961–2003 Area Visibility during all observations (km) Change in visibility due to inclusion of days with precipitation (km) Change in visibility (%) a, y Precipitation frequencies (%), x Correlation coefficient (r) b and relationship Taipei Kaohsiung Hualien Taitung 8.78 13.95 22.81 25.75 − 0.58 − 0.25 − 1.33 − 0.89 −6.63 −1.79 −5.82 −3.47 13.20 5.58 10.23 9.83 −0.922 y = −0.650x + 1.884 a ðvisibility for all observationsvisbility for not rainingÞ b 100k. visibility for all observations Relationship between precipitation frequency and percentage change in visibility. The data for Taipei show that visibility was lowest (5.7 to 6.6 km) in ‘episode’ air quality, characterized by relatively high concentrations of PM10 and NOx, a relatively high atmospheric pressure, and a relatively low wind speed. Taipei has a higher average concentration of NOx than the other centers and concentrations of PM10 and NOx in Taipei during ‘clear’ air quality are lower than during ‘moderate’ or ‘episode’ air quality. Indeed, the PM10 concentration associated with ‘episode’ air quality is approximately five to six times that associated with ‘clear’ air quality (169.0–189.6 μg m− 3 compared with 29.4–34.9 μg m− 3), while the NOx concentration is about three times greater. ‘Clear’ air quality in Taipei (visibility 11.4 to 12.0 km) is also characterized by a relatively low atmospheric pressure and relatively high wind speed. Site TL experienced the most ‘episode’ air quality hours (698), while HT experienced the least (43). Site TL also experienced the highest NOx concentration and HT the lowest, demonstrating good correlation between NOx and ‘episode’ air quality. Conversely, no correlation is demonstrated between PM10 concentration and air quality within the Taipei ‘episode’ data as site HT experienced the highest PM10 concentration but the best visibility, although it is worth noting that wind speed was extraordinarily high (3.7) at this site. Kaohsiung ‘episode’ visibility was the worst visibility experienced at any of the four centers, at a mere 3.2 to 3.4 km. Like Taipei, the concomitant air quality was characterized by relatively high concentrations of PM10 and NOx, a relatively high atmospheric pressure, and a relatively low wind speed. PM10 concentration associated with ‘episode’ air quality is approximately five to six times that associated with ‘clear’ air quality, while the NOx concentration is about 3.6 times greater. ‘Clear’ air quality is characterized by a relatively low atmospheric pressure and relatively high wind speed as well as relatively lower concentrations of PM10 and NOx. Visibility in Kaohsiung, which almost exactly matched visibility in Taipei in 1994, has deteriorated in the period since then at the same time as visibility in Taipei has improved (Fig. 2). Air quality in the period 1994–2003 was also worse in Kaohsiung: ‘episode’ air quality accounted for between 3.8 and 9.1% of observations, depending on site, compared with just 0.1– 1.7% of observations in Taipei. Furthermore, ‘moderate’ air quality accounted for another 59.9–66.4% of observations in Kaohsiung and ‘clear’ air quality for only 25.8–35.5%, whereas in Taipei ‘moderate’ air quality accounted for 21.1–50.5% of observations and ‘clear’ air quality for a very significant 47.8–78.8% of observations. In ‘clear’ air quality, visibility in Taipei was on average just 1.4 times visibility in Kaohsiung. The deterioration in visibility in Kaohsiung from ‘clear’ to ‘episode’ air quality was, however, more severe than the equivalent deterioration in Taipei, such that ‘episode’ visibility in Taipei was 1.87 times that in Kaohsiung. This effect occurred in spite of overall higher average PM10 and NOx concentrations in Taipei during ‘episode’ air quality, indicating that the pollutant mix from industrial sources (in Kaohsiung) has a much stronger extinction effect than the pollutant mix from traffic sources (in Taipei). Air quality in the non-metropolitan centers was significantly better than in Kaohsiung or Taipei: ‘episode’ air quality accounted for only 0.13% of observations in Hualien and 0.03% in Taitung, while ‘clear’ air quality accounted for 86.1% and 91.3% of observations. Only PM10 concentrations and air pressure (highest in ‘episode’ air quality) showed unidirectional change through the air quality categories in Hualien and Taitung. Visibility was significantly better in all air quality categories, but it did not increase from ‘episode’ to ‘moderate’ to ‘clear’ air quality categories, as it had done for Kaohsiung and Taipei. It was 14.4, 13.0, and 15.0 km in Hualien for ‘episode,’ ‘moderate,’ and ‘clear’ air quality, respectively, and 18.8, 18.3, and 20.6 km in Taitung. There was a further absence of unidirectional change through air quality categories in the NOx and wind speed data, bringing into question the Table 2 Summary of average visibility (km), 24 h PM10 (μg m-3), 1 h NOx (ppbv), wind speed (m s-1) and atmospheric pressure (hPa) within three air quality categories between 1994 and 2003 at 17 sites in two metropolitan areas and two rural areas Air quality Taipei HT TC HC TL SL CS WH KT 264 672 463 698 120 343 220 179 6.2 169.0 53.1 2.6 1012.5 6.0 180.9 71.4 2.2 1013.2 6.4 174.2 60.3 2.2 1013.4 6.1 178.2 72.2 2.2 1013.6 6.4 181.7 36.0 2.7 1013.1 6.3 180.9 70.5 2.4 1013.7 5.7 181.7 59.1 2.4 1014.4 5.8 185.2 62.9 3.1 1014.2 (b) Moderate days (PSI 100–50) Occurrence 8689 14346 Number (h) a Visibility 7.7 8.6 24 h PM10 69.1 73.5 29.4 40.1 1 h NOx Wind speed 2.8 2.6 Pressure 1012.9 1011.8 (c) Clear days (PSI b 50) Occurrence 32467 26226 Number (h) a Visibility 11.4 11.7 24 h PM10 29.4 31.4 1 h NOx 23.8 30.6 Wind speed 3.1 3.2 Pressure 1012.1 1012.6 a PC 18368 9.2 76.5 45.6 2.7 1012.2 20567 12.0 34.1 40.4 3.3 1012.6 16165 9.1 75.2 36.9 2.6 1011.8 24009 11.7 32.0 31.1 3.3 1012.5 20576 9.4 75.6 46.3 2.7 1012.0 19454 12.0 34.9 38.6 3.3 1012.6 11420 8.0 70.8 35.1 2.7 1012.6 29204 11.6 30.8 27.5 3.1 1012.1 17660 8.8 74.7 54.6 2.7 1012.5 22222 12.0 34.2 49.1 3.2 1012.4 13180 8.2 72.6 40.4 2.7 1012.5 27223 11.7 31.8 35.5 3.1 1012.2 12919 8.1 72.0 55.4 2.8 1012.6 26830 11.9 32.4 47.7 3.1 1011.9 JW NZ TY CK CC HK 3009 1528 1835 3224 2659 3653 3.4 171.2 58.1 2.5 1015.1 3.4 167.3 45.9 2.5 1015.4 3.3 170.9 41.5 2.4 1015.2 3.3 172.3 44.2 2.4 1015.7 3.2 170.2 64.2 2.4 1015.6 3.2 170.5 74.6 2.4 1015.7 25485 4.9 96.5 45.9 2.6 1013.5 12240 10.2 33.0 24.5 2.8 1008.1 Occurrence number is defined as the hours those PSI values are greater than 100, the range of 50–100 or less than 50. The priority pollutants are PM 26328 4.9 91.1 34.1 2.6 1013.5 12715 10.0 35.3 25.4 2.8 1008.2 24411 4.5 92.4 32.3 2.5 1013.9 14476 9.9 31.6 20.4 2.8 1008.1 26034 4.9 95.7 31.9 2.6 1013.2 10703 10.8 36.6 21.4 2.8 1008.1 26711 5.1 93.6 45.6 2.6 1013.2 10837 10.5 36.8 30.3 2.8 1008.0 25606 5.1 95.7 51.6 2.6 1013.2 10951 10.3 37.2 31.1 2.7 1007.9 Hualien Taitung HL TT 53 13 14.4 178.3 13.4 3.3 1017.0 18.8 184.9 15.9 2.7 1014.5 5578 3313 13.0 64.7 22.8 2.7 1013.8 18.3 63.8 13.1 2.9 1013.8 34991 15.0 29.6 19.4 2.8 1010.9 34954 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 (a) Episode (PSI ≥ 100) 43 Occurrence Number (h) a Visibility 6.6 24 h PM10 189.6 1 h NOx 35.8 Wind speed 3.7 Pressure 1013.7 Kaohsiung 20.6 28.6 12.1 2.4 1011.3 . 10 331 332 Table 3 T-test and the mean (± standard deviation) levels of air pollutants and visibility during weekend and weekday periods at nine air quality monitoring stations in Taipei, 1994–2003 Taipei Hsintien 2.8 ± 3.8 b (n = 5714) CO (ppmv) 0.58 ± 0.30 (n = 5843) 33 ± 22 O3 (ppbv) (n = 5614) PM10 (μg m– 3) 36 ± 25 (n = 5828) NOx (ppbv) 20 ± 13 (n = 5672) SO2 (ppbv) Tucheng Panchiao Hsinchuang Tsailiao Shinlin Weekday t-test a Weekend Weekday t-test Weekend Weekday t-test Weekend Weekday t-test Weekend Weekday t-test Weekend Weekday t-test 3.4 ± 4.6 (n = 28,445) 0.68 ± 0.40 (n = 28,543) 30 ± 24 (n = 27,422) 41 ± 29 (n = 28,303) 26 ± 19 (n = 27,554) 10.5 6.3 ± 7.4 (n = 28,514) 0.79 ± 0.47 (n = 28,579) 28 ± 24 (n = 26,742) 50 ± 36 (n = 27,828) 36 ± 31 (n = 27,148) 16.9 7.7 ± 8.4 (n = 27,561) 1.00 ± 0.59 (n = 27,372) 25 ± 23 (n = 26,178) 58 ± 40 (n = 26,832) 45 ± 29 (n = 26,275) 17.6 8.0 ± 9.1 (n = 28,668) 0.78 ± 0.52 (n = 28,601) 30 ± 23 (n = 27,305) 51 ± 37 (n = 27,650) 36 ± 28 (n = 27,016) 24.4 5.7 ± 5.9 (n = 28,268) 1.10 ± 0.70 (n = 28,190) 23 ± 19 (n = 27,915) 59 ± 42 (n = 27,390) 45 ± 33 (n = 27,002) 15.4 3.6 ± 4.3 (n = 27,403) 0.72 ± 0.49 (n = 28,412) 27 ± 19 (n = 26,865) 45 ± 33 (n = 27,759) 31 ± 28 (n = 26,472) 10.5 17.6 5.9 10.5 25.8 4.5 ± 5.7 (n = 5820) 0.68 ± 0.36 (n = 5854) 30 ± 22 (n = 5528) 43 ± 31 (n = 5751) 27 ± 23 (n = 5634) 17.1 7.2 13.4 20.9 5.6 ± 6.5 (n = 5694) 0.80 ± 0.43 (n = 5678) 28 ± 21 (n = 5449) 49 ± 35 (n = 5597) 34 ± 21 (n = 5486) 24.7 7.3 15.0 27.5 5.0 ± 6.4 (n = 5904) 0.61 ± 0.37 (n = 5911) 33 ± 22 (n = 5632) 44 ± 33 (n = 5762) 25 ± 21 (n = 5608) 22.8 11.3 14.1 28.1 4.4 ± 5.1 (n = 5824) 0.88 ± 0.51 (n = 5834) 25 ± 19 (n = 5798) 52 ± 36 (n = 5686) 34 ± 25 (n = 5616) 22.4 9.8 12.2 23.5 2.9 ± 3.7 (n = 5571) 0.62 ± 0.37 (n = 5876) 29 ± 18 (n = 5508) 40 ± 28 (n = 5716) 24 ± 22 (n = 5567) 15.1 7.0 10.1 16.8 Taipei Chungshan SO2 (ppbv) CO (ppmv) O3 (ppbv) −3 PM10 (μg m ) NOx (ppbv) a b Wanhua Kuting Visibility (km) Weekend Weekday t-test Weekend Weekday t-test Weekend Weekday t-test Weekend Weekday t-test 4.4 ± 5.2 (n = 5883) 0.85 ± 0.46 (n = 5849) 25 ± 19 (n = 5600) 48 ± 33 (n = 5681) 40 ± 26 (n = 5643) 5.5 ± 5. 8 (n = 28,569) 1.13 ± 0.68 (n = 28,522) 22 ± 20 (n = 27,151) 55 ± 38 (n = 27,124) 54 ± 34 (n = 27,080) 13.2 3.8 ± 4.6 (n = 5843) 0.80 ± 0.38 (n = 5793) 29 ± 21 (n = 5824) 42 ± 30 (n = 5709) 29 ± 17 (n = 5620) 4.9 ± 5.5 (n = 28,240) 1.03 ± 0.57 (n = 28,189) 26 ± 23 (n = 28,431) 49 ± 35 (n = 27,630) 39 ± 24 (n = 26,771) 15.2 3.6 ± 4. 6 (n = 5811) 0.81 ± 0.44 (n = 5890) 26 ± 20 (n = 5591) 42 ± 29 (n = 5657) 39 ± 23 (n = 5689) 4.5 ± 5.0 (n = 28,348) 1.10 ± 0.68 (n = 28,673) 23 ± 22 (n = 27,254) 50 ± 35 (n = 27,100) 53 ± 32 (n = 27,199) 12.9 10.7 ± 6.2 (n = 2541) 10.6 ± 6.1 (n = 12,753) 1.1 30.0 11.4 12.9 28.6 For a level of significance of 0.05, tcritical (0.975; ∞) = 1.96. Associated standard deviation. 29.3 8.6 14.0 29.1 31.1 7.8 16.5 31.9 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 Weekend Table 4 T-test and the mean (± standard deviation) levels of air pollutants and visibility during weekend and weekday periods at eight air quality monitoring stations in Kaohsiung, Hualien and Taitung, 1994–2003 Kaohsiung Weekend SO2 (ppbv) 13 ± 16 (n = 5591) CO (ppmv) 0.61 ± 0.28 (n = 5797) O3 (ppbv) 37 ± 27 (n = 5558) PM10 (μg m− 3) 77 ± 50 (n = 5774) 33 ± 25 NOx (ppbv) (n = 5550) Nanzi Weekday t-test 16 ± 18 9.7 (n = 27,654) 0.65 ± 0.31 9.8 (n = 28,272) 35 ± 26 6.2 (n = 26,906) 84 ± 53 9.4 (n = 27,840) 42 ± 30 19.5 (n = 26,640) a Weekend Weekday 6.0 ± 7.4 (n = 5660) 0.54 ± 0.23 (n = 5729) 38 ± 28 (n = 5367) 73 ± 44 (n = 5554) 26 ± 19 (n = 5347) 7.1 ± 7.5 9.6 (n = 28,243) 0.57 ± 0.25 9.1 (n = 28,608) 37 ± 29 3.3 (n = 26,619) 80 ± 48 10.7 (n = 27,801) 33 ± 23 20.1 (n = 26,634) Hualien CO (ppmv) O3 (ppbv) PM10 (μg m− 3) NOx (ppbv) a b Chiankin t-test Weekend 7.7 ± 7.6 (n = 5835) 0.74 ± 0.56 (n = 5675) 43 ± 29 (n = 5433) 71 ± 49 (n = 5754) 25 ± 21 (n = 5600) Taitung Hualien SO2 (ppbv) Tsoying Taitung t-test Weekend Weekday 0.72 ± 0.93 (n = 5728) 0.58 ± 0.27 (n = 5859) 23 ± 14 (n = 5441) 32 ± 23 (n = 5744) 17 ± 12 (n = 5503) 0.92 ± 0.96 (n = 28,125) 0.67 ± 0.36 (n = 28,466) 21 ± 13 (n = 26,290) 35 ± 23 (n = 27,730) 21 ± 14 (n = 26,560) 14.0 0.44 ± 0.50 (n = 5227) 0.49 ± 0.24 (n = 5505) 27 ± 13 (n = 5504) 31 ± 22 (n = 5392) 9.9 ± 5.2 (n = 5338) 0.6 ± 1.5 (n = 26,239) 0.59 ± 0.29 (n = 26,724) 26 ± 13 (n = 26,767) 33 ± 23 (n = 26,307) 12.7 ± 7.0 (n = 25,720) 9.5 19.1 8.7 ± 8.9 (n = 5669) 0.74 ± 0.37 (n = 5595) 41 ± 28 (n = 5387) 73 ± 49 (n = 5511) 27 ± 22 (n = 5439) Weekday t-test 9. 5 ± 9.3 5.8 (n = 27,712) 0.83 ± 0.50 12.0 (n = 27,559) 40 ± 29 0.89 (n = 26,224) 79 ± 52 8.1 (n = 27,462) 31 ± 25 11.0 (n = 26,265) Weekend Hsiaokang Weekday t-test Weekend 14 ± 12 15 ± 13 6.2 (n = 5180) (n = 25,508) – – –b – – – 80 ± 47 (n = 5626) 38 ± 28 (n = 5462) 87 ± 51 10.5 (n = 27,581) 44 ± 33 32.1 (26544) Hualien Visibility (km) Weekday 9.1 t-test Weekend 8.7 ± 8.1 8.1 (n = 28,356) 0.76 ± 0.52 3.4 (n = 27,783) 42 ± 32 2.4 (n = 26,418) 75 ± 51 4.5 (n = 27,939) 29 ± 25 12.6 (n = 26,887) Kaohsiung Weekend 18.1 Weekday Chiancheng Weekday 15 ± 14 (n = 5702) 0.78 ± 0.53 (n = 5550) 37 ± 30 (n = 5424) 81 ± 47 (n = 5624) 40 ± 33 (n = 5502) t-test 16 ± 15 4.9 (n = 28,109) 0.87 ± 0.59 10.2 (n = 27,326) 35 ± 29 6.2 (n = 26,535) 89 ± 51 10.5 (n = 27,736) 50 ± 39 17.8 (n = 26,734) Taitung Visibility (km) Visibility (km) t-test Weekend Weekday t-test Weekend Weekday t-test Weekend Weekday t-test 8.1 6.5 ± 4.6 (n = 2482) 6.3 ± 4.8 (n = 12,393) 1.7 14.5 ± 4.7 (n = 2481) 14.8 ± 4.6 (n = 12,386) 2.2 20.5 ± 5.2 (n = 2518) 20.3 ± 5.0 (n = 12,712) 1.3 25.3 5.3 5.6 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 Jenwu 27.9 For a level of significance of 0.05, tcritical (0.975; ∞) = 1.96. Incomplete data for analysis. 333 334 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 relationships of these factors with air quality apparently identified in the Kaohsiung and Taipei data. Moreover, contrary to observations for Kaohsiung and Taipei, the average wind speed during ‘episode’ air quality was higher than in ‘clear’ air quality for both Hualien and Taitung, meaning either that wind speed is not a causative factor in ‘clear’ air quality or that it was overridden by another factor or factors in Hualien and Taitung. It is proposed that there is ‘another factor’ that explains the association of higher wind speeds with ‘episode’ air quality in Hualien and Taitung: long range transport of PM2.5–10 within Asian dust storm winds (Mori et al., 2002; Chen et al., 2004; Nakamura et al., 2005; Tsai and Chen, 2006a). PM2.5–10 contributes significantly to the local PM10 mass, leading to an ‘episode’ air quality categorization, but does not interfere with visibility as fine particles (PM2.5) do (Cheng and Tsai, 2000), and hence ‘episode’ air quality is not associated with a deterioration in visibility in Hualien and Taitung. Hualien, and for the most part unsupported by statistical significance. A statistically significant weekend effect, with ozone concentrations higher during weekends than during weekdays, was observed at all sites other than Chiankin in Kaohsiung. This result is similar to that obtained by Pryor and Steyn (1995) at LFV, Canada, where ozone concentrations varied by days of the week and were uniformly higher on weekends. Additionally, typical NOx concentrations were higher, though not uniformly, during weekdays, while concentrations of both ozone and NOx increased notably between 1984 and 1991. Their hebdomadal cycles exhibited a negative correlation. Pryor (1998) also noted that although both NOx and volatile organic compounds (VOCs) are precursors to the formation of O3, the ozone concentrations in the LFV area was VOC-sensitive but not NOxsensitive. 3.4. Weekend versus weekday visibility and air quality Tables 5 and 6 show correlation coefficients of mixing layer height (Mix) with air quality/meteorological factors at the moment when Mix changes, one hour after a change, and two hours after a change. Correlation coefficients of Mix with visibility show that at all centers a change in visibility is most correlated with Mix one hour after a change in Mix, that is, that the greatest change in visibility has occurred at this time. Of the pollutants, O3 has a correlation coefficient at a change in Mix of between 0.31 and 0.47, and continues to show positive correlation at one and two hours after a change, indicating that changes in O3 concentration are synchronized with changes in the Mix. This outcome is indicative of a higher Mix leading to higher solar radiation leading to stronger photochemical reactions and more O3. The concentration patterns of CO, PM10 and NOx, meanwhile, show a negative correlation with change in Mix, indicative of falling levels of these pollutants as Mix rises. In Taipei, Hualien, and Taitung, except for NOx at site Hsintien and PM10 at site Shinlin, the negative correlation between these pollutants and Mix weakens with time from the change in Mix, indicating that these pollutants are easily dispersed into the atmosphere as Mix rises. In contrast to all other sites (except Shinlin, as already noted), all sites in Kaohsiung bar Nanzi experienced a negative correlation between PM10 and Mix that was stronger at one hour than it was at the time of a change in Mix, indicative of a lag in the diffusion of PM10 on a rise in Mix. This is because the stronger photochemical reactions that result from a higher Mix lead in Kaohsiung Average weekend and weekday visibilities and air pollutant levels for the period 1994 to 2003 were calculated and subjected to a t-test (Tables 3 and 4). Standard deviations for SO2 were slightly greater than ± 100% of the arithmetic mean, whereas those of all other parameters fell within ± 100% of the arithmetic mean. This indicates that when using SO2 as a visibility parameter in further investigation of empirical models for visibility studies (Section 3.7), the log-normal distribution of SO2 must be considered while the other parameters may be regarded as normal distributions when carrying out regression analyses of these models. Hence, the quantile–quantile plots and Mann–Whitney tests were not used in discussing visibility in relation to SO2 (Pryor and Steyn, 1995; Pryor, 1998). Average weekend and weekday visibilities showed slight differences at all four centers. At Taipei, Kaohsiung, and Taitung visibility was slightly higher at weekends, but not statistically significant, whereas at Hualien visibility was slightly lower at weekends, and this difference was statistically significant, with a t-test value of 2.2. Levels of SO2, CO, PM10, and NOx were slightly lower at weekends at all centers, indicating that all centers experienced less anthropogenic pollution from automobile, industrial and other sources at this time, and differences were statistically significant. No definitive conclusion can be drawn from these data regarding any difference in weekend visibility because the differences noted are slight, contrary in the case of 3.5. Mixing layer height and air quality/visibility Taipei Hsintien Tucheng Panchiao Hsinchuang Tsailiao Shinlin Mixing layer height Mixing layer height Mixing layer height Mixing layer height Mixing layer height Mixing layer height Realtime CO −0.01 O3 0.41 PM10 −0.34 NOx −0.02 After 1h After 2h Realtime After 1h After 2h Realtime After 1h After 2h Realtime After 1h After 2h Realtime After 1h After 2h Realtime After 1h After 2h − 0.09 0.31 − 0.33 − 0.09 − 0.09 0.22 − 0.32 − 0.10 − 0.15 0.46 − 0.28 − 0.12 − 0.01 0.36 − 0.25 − 0.02 −0.01 0.27 −0.19 −0.01 − 0.20 0.47 − 0.23 − 0.24 −0.07 0.37 −0.21 −0.19 − 0.07 0.26 − 0.16 − 0.18 − 0.19 0.42 − 0.20 − 0.17 − 0.09 0.31 − 0.18 − 0.10 − 0.11 0.21 − 0.09 − 0.12 − 0.11 0.39 − 0.25 − 0.09 − 0.04 0.26 − 0.23 − 0.03 − 0.02 0.16 − 0.18 − 0.02 −0.12 0.32 −0.25 −0.12 − 0.02 0.20 − 0.26 − 0.01 −0.01 0.10 −0.19 −0.05 Taipei CO O3 PM10 NOx a Chungshan Wanhua Kuting Mixing layer height Mixing layer height Mixing layer height Mixing layer height Real-time After 1 h After 2 h Real-time After 1 h After 2 h Real-time After 1 h After 2 h − 0.13 0.41 − 0.23 − 0.18 − 0.01 0.28 − 0.22 − 0.07 − 0.02 0.17 − 0.16 − 0.08 − 0.17 0.45 − 0.28 − 0.16 − 0.03 0.32 − 0.24 − 0.09 − 0.03 0.21 − 0.20 − 0.09 −0.13 0.44 −0.26 −0.19 − 0.03 0.33 − 0.22 − 0.11 −0.02 0.21 −0.18 −0.12 Ventilation index: multiply by mixing layer height and wind speed. Visibility Pressure Wind speed Ventilation index Real-time After 1 h After 2 h 0.08 0.35 0.10 0.68 0.09 0.32 0.18 0.62 0.07 0.31 0.12 0.59 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 Table 5 Correlation coefficients of visibility, air qualities and meteorological parameters affected by mixing layer height real-time, and 1 and 2 h lagged in Taipei, 1994–2003 335 336 Kaohsiung Hualien Jenwu Nanzi Tsoying Chiankin Hsiaokang Hualien Mixing layer height Mixing layer height Mixing layer height Mixing layer height Mixing layer height Mixing layer height Realtime CO − 0.12 O3 0.39 PM10 − 0.22 NOx − 0.06 After 1h After 2h Realtime After 1h After 2h Realtime After 1h After 2h Realtime After 1h After 2h Realtime After 1h After 2h Realtime After 1h After 2h − 0.02 0.24 − 0.23 − 0.04 −0.06 0.21 −0.13 −0.07 − 0.06 0.46 − 0.27 − 0.15 − 0.06 0.30 − 0.27 − 0.04 − 0.01 0.29 − 0.17 − 0.12 −0.19 0.44 −0.21 −0.20 − 0.01 0.30 − 0.25 − 0.05 − 0.08 0.28 − 0.13 − 0.17 − 0.18 0.44 − 0.22 − 0.17 − 0.01 0.31 − 0.26 − 0.04 −0.08 0.27 −0.13 −0.15 − 0.16 0.43 − 0.21 − 0.17 − 0.01 0.28 − 0.22 − 0.06 − 0.07 0.25 − 0.11 − 0.15 − 0.21 0.33 − 0.06 − 0.22 −0.17 0.24 −0.01 −0.20 − 0.11 0.23 − 0.01 − 0.16 Taitung Kaohsiung Hualien Taitung Mixing layer height Mixing layer height Mixing layer height Taitung Mixing layer height CO O3 PM10 NOx a Real-time After 1 h After 2 h − 0.13 0.31 − 0.12 − 0.13 − 0.10 0.24 − 0.08 − 0.08 −0.12 0.21 −0.09 −0.11 Visibility Pressure Wind speed Ventilation index Ventilation index: multiply by mixing layer height and wind speed. Real-time After 1 h After 2 h Real-time After 1 h After 2 h Real-time After 1 h After 2 h 0.12 0.25 0.19 0.78 0.17 0.35 0.04 0.71 0.12 0.24 0.09 0.66 0.11 0.02 0.02 0.65 0.15 0.01 0.11 0.57 0.02 0.02 0.07 0.53 0.04 0.09 0.02 0.63 0.04 0.17 0.03 0.51 0.01 0.09 0.05 0.41 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 Table 6 Correlation coefficients of visibility, air qualities and meteorological parameters affected by mixing layer height real-time, and 1 and 2 h lagged in Kaohsiung, Hualien and Taitung, 1994–2003 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 to the formation of photochemical particulates such as sulfate and nitrate that are not as rapidly or evenly diffused as aerosol (Tsai and Chen, 2006b) and, as a result, PM10 has its greatest impact on visibility (i.e. improving visibility by its absence) in Kaohsiung one hour after a rise in Mix. A high correlation coefficient of 0.63–0.78 for the ventilation index indicates that changes in this index are synchronized with the change of the mixing layer height and also indicates that changes in ventilation index are associated with different rates of vertical and horizontal dispersion of pollutants (Seibert et al., 2000). 3.6. Principal component analysis for visibility The major factors determining visibility in each center were identified via PCA, using the data obtained between 1994 and 2003. In Taipei, there were nine PCs with eigen values N1.0, representing a total 88.5% of the variance, while in Kaohsiung there were four, representing a total 89.0% of the variance. There were three in Hualien and Taitung, representing a total of 60.3% and 52.7% of the variance, respectively. In Taipei and Kaohsiung the first PC (PC1) with loading correction coefficients ≥ 0.6 consisted of SO2, CO, NO2 and PM10. It accounts for 33.9% of the explainable variance in Taipei, where variation in these four species was consistent at all nine sites, indicating that they originate from the same sources. CO and NO2 both come from transportation emissions. CO represents emissions of black carbon and is thus related to the absorption coefficient. Its concentration at site Chungshan in Taipei was closely related with visibility as observed at the nearby Taipei weather service office. SO2, from the burning of heavy fuels, is converted into sulfate via photochemical reaction and, as sulfate can influence visibility, SO2 and visibility exhibited a moderate correlation. PC1 accounts for 62.0% of the explainable variance in Kaohsiung, where variation in PM10 concentration was the main factor affecting visibility, a relationship that was stronger than in Taipei. In Hualien and Taitung PC1 consisted of only CO and NO2, and accounts for 33.5% of the explainable variance in Hualien and 20.4% in Taitung, indicative of the impact on visibility from transportation emissions. In addition to the low percentage figure for PC1 in Taitung, PC3 (13.5% of the variance) contains none of the pollutants, SO2, CO, NO2, PM10 and O3, indicating that these pollutants do not affect visibility significantly in Taitung. Hence, visibility in Hualien is affected to some extent by traffic pollution, while visibility in Taitung is the least affected by air pollution in general. 337 O3 was highly correlated between centers and was the primary component of PC2 at all four centers, indicating that it is evenly distributed and that all four centers were equally influenced by photochemical reactions. In Taitung, once again worthy of special comment, both O3 and PM10 are predominantly PC2-related species, revealing that PM10 is not likely sourced locally but rather from long-range transport. It is concluded that visibility in Taipei and Kaohsiung in the period was determined mostly by fugitive dust, transportation emissions, the products of photochemical reactions, and industrial emissions as there are clear correlations between relevant air pollutants and visibility. In Kaohsiung, especially, visibility has high correlation (N0.90) with PC1, PM10, and NO2. Furthermore, as the explainable variance for Hualien and Taitung is low (PCs with eigen values N1.0 account for just 60.3% and 52.7% of the variance, respectively), it is concluded that undefined parameters representing pollutants from sources outside the study area are important determining factors in visibility at these centers. 3.7. Empirical models for visibility The optimal empirical model for each center, using data from the period 1994 to June 2002 (one year prior to the end of the available data set), is shown in Table 7. Because the light scattering cross section of particles is significantly increased at relative humidity (RH) N90% (e.g. that of an ammonium sulfate particle by a factor of five or more above that of the dry particle at 35–40% RH) (Malm and Day, 2001; Tsai and Kuo, 2005), causing a degradation in visibility (Tang et al., 1981), data collected at RH N 90% was excluded from the PCA in developing empirical models in this study capable of relating visibility to meteorological factors and pollutant concentrations, as was data collected during precipitation. With only visibility and the meteorological factors of temperature, relative humidity and wind speed included in the analysis, regression coefficients were 0.44 for Taipei, 0.53 for Kaohsiung, 0.44 for Hualien, and 0.37 for Taitung, indicating a low or moderate correlation. Correlation rose with the average airborne pollutant concentrations included in the analysis, and with the PCs for each center included it rose further, represented by a coefficient of 0.69 for Taipei, 0.77 for Kaohsiung, 0.63 for Hualien, and 0.47 for Taitung. The regression coefficients of the individual contributors to each empirical model are also listed in Table 7. All have p values b0.0001 and, moreover, within the 95% confidence level the parameters 338 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 fluencing the photochemical effect on visibility. Moreover, although the extent of the influence varies, correlation of temperature and wind speed with visibility is positive while correlation of RH with visibility is negative. The models developed for rural Hualien and Taitung are inferior, and this is especially true of the model for Taitung, in which only 22.4% of the variance (r2) is explained by air pollutants and meteorological parameters. More suitable models are likely to include estimated using the model are not equal to 0, demonstrating that each meets the requirements for multivariate regression analyses. PM10, O3, SO2 and NO2 are the most influential air pollutants, all having a negative correlation with visibility. Whereas variations of ozone concentration will not change the visibility, they represent the potential yield of photochemicals, e.g. carbon, sulfate and nitrate, that cause light extinction. Thus, ozone is carefully considered as a parameter in- Table 7 Regression results for the optimal empirical models of visibility in Taipei, Kaohsiung, Hualien and Taitung, 1994–June 2002 Region Empirical model Taipei Vis = 0.195 × Temp − 0.274 × RH + 0.419 × Ws − 0.126 × [O3]e − 4.07 × ln[PM10]f − 0.845 × ln[SO2]g + 45.03h Vis = 0.486 × Temp − 0.159 × RH + 0.310 × Ws − 0.064 × [O3] − 0.025 × [NO2]i − 3.117 × ln[PM10] + 20.84 Vis = 0.195 × Temp − 0.146 × RH − 0.123 × [O3] − 0.149 × [NO2] − 0.791 × ln[PM10] + 28.32 Vis = 0.303 × Temp − 0.106 × RH − 0.075 × [O3] − 0.128 × [NO2] − 0.787 × ln[PM10] + 26.31 Kaohsiung Hualien Taitung a Regression coefficient (r) b c d 0.69 0.77 0.63 0.47 Regression coefficient Estimated regression coefficient Estimated standard deviation t testj p value Taipei β1 [Temp] β2 [RH] β3 [Ws] β4 [O3] β5 ln[PM10] β6 ln[SO2] β7 0.195 − 0.274 0.419 − 0.126 − 4.07 − 0.845 45.03 0.008 0.004 0.025 0.003 0.10 0.069 0.66 24.3 − 61.0 16.5 − 43.4 − 39.4 − 12.3 68.6 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 Kaohsiung β1 [Temp] β2 [RH] β3 [Ws] β4 [O3] β5 [NO2] β6 ln[PM10] β7 0.486 − 0.159 0.310 − 0.064 − 0.025 − 3.117 20.84 0.009 0.004 0.028 0.002 0.003 0.079 0.56 54.3 − 38.1 11.2 − 39.0 − 7.3 − 39.3 37.4 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 Hualien β1 [Temp] β2 [RH] β3 [O3] β4 [NO2] β5 ln[PM10] β6 0.195 − 0.146 − 0.123 − 0.149 − 0.791 28.32 0.007 0.004 0.003 0.004 0.047 0.42 26.1 − 39.2 − 46.7 − 34.5 − 16.7 67.5 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 Taitung β1 [Temp] β2 [RH] β3 [O3] β4 [NO2] β5 ln[PM10] β6 0.303 − 0.106 − 0.075 − 0.128 − 0.787 26.31 0.010 0.004 0.003 0.009 0.049 0.46 31.2 − 27.6 − 25.5 − 13.7 − 16.2 57.4 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 b0.0001 Visibility (km). bAtmospheric temperature (°C). cRelative humidity (%). dWind speed (m s− 1). eO3 in ppbv. fPM10 in μg m− 3. gSO2 in ppbv. empirical constant (km). iNO2 in ppbv. jFor a level of significance of 0.05, tcritical (0.975; ∞) = 1.96. a h Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 Table 8 Rise in visibility due to a 50% drop in concentration of PM10, O3 and NO2, based on the optimal empirical model Region Taipei Kaohsiung Taitung Hualien Increase of visibility (km) A 50% drop in PM10 value A 50% drop in O3 value A 50% drop in NO2 value 2.8 2.2 0.6 0.5 0.13 0.06 0.09 0.12 – 0.03 0.12 0.15 the impact of long-range transport pollutants extant in these centers, and additional studies on these pollutants are necessary in order to develop such models. Using the optimal empirical model, the improvement in visibility resulting from a 50% fall in PM10, O3, and NO2 concentration was estimated (Table 8). This 339 revealed that visibility is most sensitive to changes in PM10 concentration, especially in Taipei and Kaohsiung, where a 50% drop in PM10 would improve visibility by 2.8 km and 2.2 km, respectively. Comparatively, the effect of a 50% drop in O3 or NO2 on visibility would be almost inconsequential: an additional 0.06–0.13 km for O3 and 0.03–0.15 km for NO2. Moreover, the regression data in Table 7 show that visibility is not significantly sensitive to NO2 concentration and that O3 has the least influence on visibility. 3.8. Verification of the optimal empirical models for local visibilities To verify the validity of the empirical models, they were applied to the period July 2002 to June 2003, being the data period excluded from the input into the models, Fig. 3. Simulated and observed monthly mean hourly visibility in Taiwan using the optimal empirical model of visibility in this study, July 2002–June 2003. (a) Taipei, (b) Kaohsiung, (c) Hualien, (d) Taitung. 340 Y.I. Tsai et al. / Science of the Total Environment 382 (2007) 324–341 and the simulated results compared with the observed data for that period. The correlation coefficient of the simulated and observed average daily visibility was 0.71 for Taipei, 0.72 for Kaohsiung, 0.63 for Hualien, and 0.46 for Taitung, whilst that of the average monthly visibility (Fig. 3) was as high as 0.88 for Taipei, 0.87 for Kaohsiung, 0.85 for Hualien, but a still low 0.50 for Taitung. These data show that the models for Taipei, Kaohsiung, and Hualien were highly effective in simulating visibility observations at those centers between July 2002 and June 2003, but that the model for Taitung was not, and a potential solution for this has already been posited here, indicating that simulations for Taitung should include long-range transport as a pollutant source. 4. Conclusions For the period 1961–2003 the average annual visibility in a highly urbanized center in Taiwan (Taipei) was worse than that in a highly industrialized center (Kaohsiung), which in turn was worse than that in two rural centers (Hualien and Taitung). Unlike at the other centers, however, visibility in Taipei showed a rising trend from 1992 to the end of the study period, such that average annual visibility since 1994 has been superior to that in Kaohsiung. This improvement in Taipei can be linked to the construction and expansion of a mass transit rail system in the city, the use of which has helped reduce emissions of traffic related air pollutants, particles, and NO2. At all centers, visibility deteriorated in the rain. Hence, frequency of precipitation is one of the factors contributing to the average annual visibility number. High atmospheric pressure and low wind speed are unfavorable to dispersion and transportation of pollutants. Under these conditions, visibility was adversely affected by high concentrations of pollutants (PM10 and NOx), resulting in ‘episode’ visibility as low as 5.7– 6.6 km in Taipei and 3.2–3.4 km in Kaohsiung. Conversely, ‘clear’ air quality was characterized by low atmospheric pressure, high wind speeds, low PM10, and visibility as high as 11.4–12.0 km in Taipei and 9.9– 10.8 km in Kaohsiung. Excepting O3, which showed the ‘weekend effect’ concentration pattern, air pollutant concentrations were slightly higher on weekdays than on weekends. This did not, however, translate into statistically significant weekday–weekend visibility trends. A change in Mix had in the main a negative correlation with pollutant concentrations that weakened at one hour from the change, indicative of immediate dispersal of pollutants. In Kaohsiung, however, the negative correlation with PM10 strengthened at one hour after the change, indicative of a delay in dispersal, and as a result PM10 had its greatest impact on visibility (i.e. improving visibility by its absence) in Kaohsiung one hour after a rise in Mix. In general, the greatest change in visibility was noted one hour after Mix changed. Visibility in both Taipei and Kaohsiung is affected by fugitive dust, mobile emissions, and industrial emissions, the latter especially in Kaohsiung where the visibility is seriously affected by PM10 and NO2. In Taitung, air pollutants influence visibility the least. Optimum empirical models demonstrated that of PM10, O3, SO2 and NO2, PM10 has the most significant influence on visibility. A 50% drop in PM10 was shown to raise the visibility by between 0.5 km (for Hualien) and 2.8 km (for Taipei). The models were shown to be highly effective in simulating visibility observations for Taipei, Kaohsiung, and Hualien, but not for Taitung. A model for this latter center is likely to benefit from the inclusion of long-range transport sources of pollution. Acknowledgements This work was financially supported by the National Science Council of the ROC under Contract Nos. NSC 89-2211-E-041-012, NSC 89-2211-E-041-020 and NSC 93-2211-E-041-003. 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