Isotopic signatures and source apportionment of Pb in ambient PM2.5.

Particulate lead (Pb) is a primary air pollutant that affects society because of its health impacts. This study investigates the source sectors of Pb associated with ambient fine particulate matter (PM2.5) over central-western Taiwan (CWT) with new constraints on the Pb-isotopic composition. We demonstrate that the contribution of coal-fired facilities is overwhelming, which is estimated to reach 35 ± 16% in the summertime and is enhanced to 57 ± 24% during the winter monsoon seasons. Moreover, fossil-fuel vehicles remain a major source of atmospheric Pb, which accounts for 12 ± 5%, despite the current absence of a leaded gasoline supply. Significant seasonal and geographical variations in the Pb-isotopic composition are revealed, which suggest that the impact of East Asian (EA) pollution outflows is important in north CWT and drastically declines toward the south. We estimate the average contribution of EA outflows as accounting for 35 ± 15% (3.6 ± 1.5 ng/m3) of the atmospheric Pb loading in CWT during the winter monsoon seasons.

Multiscale Temporal Variations of Atmospheric Mercury Distinguished by the Hilbert-Huang Transform Analysis Reveals Multiple El Niño-Southern Oscillation Links.

Atmospheric mercury (Hg) cycling is sensitive to climate-driven changes, but links with various teleconnections remain unestablished. Here, we revealed the El Niño-Southern Oscillation (ENSO) influence on gaseous elemental mercury (GEM) concentrations recorded at a background station in East Asia using the Hilbert-Huang transform (HHT). The timing and magnitude of GEM intrinsic variations were clearly distinguished by ensemble empirical mode decomposition (EEMD), revealing the amplitude of the GEM concentration interannual variability (IAV) is greater than that for diurnal and seasonal variability. We show that changes in the annual cycle of GEM were modulated by significant IAVs at time scales of 2-7 years, highlighted by a robust GEM IAV-ENSO relationship of the associated intrinsic mode functions. With confirmation that ENSO modulates the GEM annual cycle, we then found that weaker GEM annual cycles may have resulted from El Niño-accelerated Hg evasion from the ocean. Furthermore, the relationship between ENSO and GEM is sensitive to extreme events (i.e., 2015-2016 El Niño), resulting in perturbation of the long-term trend and atmospheric Hg cycling. Future climate change will likely increase the number of extreme El Niño events and, hence, could alter atmospheric Hg cycling and influence the effectiveness evaluation of the Minamata Convention on Mercury.

Long-term (2003-2018) trends in aerosol chemical components at a high-altitude background station in the western North Pacific: Impact of long-range transport from continental Asia.

This study examined the long-term trends in chemical components in PM2.5 (particulate matter with aerodynamic diameter ≤2.5 µm) samples collected at Lulin Atmospheric Background Station (LABS) located on the summit of Mt. Lulin (2862 m above mean sea level) in Taiwan in the western North Pacific during 2003-2018. High ambient concentrations of PM2.5 and its chemical components were observed during March and April every year. This enhancement was primarily associated with the long-range transport of biomass burning (BB) smoke emissions from Indochina, as revealed from cluster analysis of backward air mass trajectories. The decreasing trends in ambient concentrations of organic carbon (-0.67% yr-1; p = 0.01), elemental carbon (-0.48% yr-1; p = 0.18), and non-sea-salt (nss) K+ (-0.71% yr-1; p = 0.04) during 2003-2018 indicated a declining effect of transported BB aerosol over the western North Pacific. These findings were supported by the decreasing trend in levoglucosan (-0.26% yr-1; p = 0.20) during the period affected by the long-range transport of BB aerosol. However, NO3- displayed an increasing trend (0.71% yr-1; p = 0.003) with considerable enhancement resulting from the air masses transported from the Asian continent. Given that the decreasing trends were for the majority of the chemical components, the columnar aerosol optical depth (AOD) also demonstrated a decreasing trend (-1.04% yr-1; p = 0.0001) during 2006-2018. Overall decreasing trends in ambient (carbonaceous aerosol and nss-K+) as well as columnar (e.g., AOD) aerosol loadings at the LABS may influence the regional climate, which warrants further investigations. This study provides an improved understanding of the long-term trends in PM2.5 chemical components over the western North Pacific, and the results would be highly useful in model simulations for evaluating the effects of BB transport on an area.

A New Monitoring Effort for Asia: The Asia Pacific Mercury Monitoring Network (APMMN).

The Asia Pacific Mercury Monitoring Network (APMMN) cooperatively measures mercury in precipitation in a network of sites operating in Asia and the Western Pacific region. The network addresses significant data gaps in a region where mercury emission estimates are the highest globally, and available measurement data are limited. The reduction of mercury emissions under the Minamata Convention on Mercury also justifies the need for continent-wide and consistent observations that can help determine the magnitude of the problem and assess the efficacy of reductions over time. The APMMN's primary objectives are to monitor wet deposition and atmospheric concentrations of mercury and assist partners in developing their own monitoring capabilities. Network planning began in 2012 with wet deposition sampling starting in 2014. Currently, eight network sites measure mercury in precipitation following standardized procedures adapted from the National Atmospheric Deposition Program. The network also has a common regional analytical laboratory (Taiwan), and quality assurance and data flagging procedures, which ensure the network makes scientifically valid and consistent measurements. Results from our ongoing analytical and field quality assurance measurements show minimal contamination in the network and accurate analytical analyses. We are continuing to monitor a potential concentration and precipitation volume bias under certain conditions. The average mercury concentration in precipitation was 11.3 (+9.6) ng L-1 for 139 network samples in 2018. Concentrations for individual sites vary widely. Low averages compare to the low concentrations observed on the U.S. West Coast; while other sites have average concentrations similar to the high values reported from many urban areas in China. Future APMMN goals are to (1) foster new network partnerships, (2) continue to collect, quality assure, and distribute results on the APMMN website, (3) provide training and share best monitoring practices, and (4) establish a gaseous concentration network for estimating dry deposition.

Urban air pollution and meteorological factors affect emergency department visits of elderly patients with chronic obstructive pulmonary disease in Taiwan.

Both air pollution and meteorological factors in metropolitan areas increased emergency department (ED) visits from people with chronic obstructive pulmonary disease (COPD). Few studies investigated the associations between air pollution, meteorological factors, and COPD-related health disorders in Asian countries. This study aimed to investigate the relationship between the environmental factors and COPD-associated ED visits of susceptible elderly population in the largest Taiwanese metropolitan area (Taipei area, including Taipei city and New Taipei city) between 2000 and 2013. Data of air pollutant concentrations (PM10, PM2.5, O3, SO2, NO2 and CO), meteorological factors (daily temperature, relative humidity and air pressure), and daily COPD-associated ED visits were collected from Taiwan Environmental Protection Administration air monitoring stations, Central Weather Bureau stations, and the Taiwan National Health Insurance database in Taipei area. We used a case-crossover study design and conditional logistic regression models with odds ratios (ORs), and 95% confidence intervals (CIs) for evaluating the associations between the environmental factors and COPD-associated ED visits. Analyses showed that PM2.5, O3, and SO2 had significantly greater lag effects (the lag was 4 days for PM2.5, and 5 days for O3 and SO2) on COPD-associated ED visits of the elderly population (65-79 years old). In warmer days, a significantly greater effect on elderly COPD-associated ED visits was estimated for PM2.5 with coexistence of O3. Additionally, either O3 or SO2 combined with other air pollutants increased the risk of elderly COPD-associated ED visits in the days of high relative humidity and air pressure difference, respectively. This study showed that joint effect of urban air pollution and meteorological factors contributed to the COPD-associated ED visits of the susceptible elderly population in the largest metropolitan area in Taiwan. Government authorities should review existing air pollution policies, and strengthen health education propaganda to ensure the health of the susceptible elderly population.

Comparing ozone metrics on associations with outpatient visits for respiratory diseases in Taipei Metropolitan area.

This study reported cumulative 6-day (lag 0-5 days) relative risks (RR) and confidence intervals (CI) of daily outpatient visits for total respiratory disease (RD), asthma, and chronic airway obstruction not otherwise classified (CAO) associated with three ozone metrics (daily 1-h maximum (O3, 1 h max), 8-h average maximum (O3, 8 h max), 24-h average (O3, 24 h avg)), and an alternative oxidant indicator (Ox) in Taipei Metropolitan, using distributed lag non-linear models after controlling for potential confounders. The Ox showed the strongest association with outpatient visits for total RD (RR = 1.10, 95% CI: 1.10, 1.11) and asthma (RR = 1.18, 95% CI: 1.00, 1.39) in the cold season. The O3, 24 h avg appeared to be the optimal ozone metric associating with total RD than O3, 1 h max and O3, 8 h max based on model selection. In conclusion, outpatient visits for total RD associated with ozone vary with ozone metrics, disease and season.

Temperature, nitrogen dioxide, circulating respiratory viruses and acute upper respiratory infections among children in Taipei, Taiwan: a population-based study.

OBJECTIVE: This study investigated whether outpatient visits of acute upper respiratory infections for children aged less than 15 years are associated with temperature, air pollutants and circulating respiratory viruses in Taipei, Taiwan, from 2003 to 2007. METHODS: Outpatient records for acute upper respiratory infections (ICD9 CM codes: 460, 462, 463,464, 465.9 and 487) in a randomly selected sample (n=39,766 children in 2005) was used to estimate the cumulative relative risks (RR) associated with average temperature lasting for 8 days (lag 0-7 days), air pollutants (NO2, O3 and PM(2.5)) lasting for 6 days (lag 0-5 days), and virus-specific positive isolation rate lasting for 11 days (lag 0-10 days) using distributed lag non-linear models after controlling for relative humidity, wind speed, day of week, holiday effects and long-term trend. RESULTS: Average temperature of 33 °C was associated with the lowest risk for outpatient visits of acute upper respiratory infections. Relative to 33 °C, cumulative 8-day RR was highest at 15 °C of ambient average temperature [RR=1.94; 95% confidence interval (CI): 1.78, 2.11]. With the first quartile as reference, cumulative 6-day RRs were 1.25 (95% CI: 1.21, 1.29) for NO2, 1.04 (95% CI: 1.01, 1.06) for O3, and 1.00 (95% CI: 0.98, 1.03) for PM(2.5) at the 95th percentile. Per-standard deviation (SD) increase of virus-specific isolation rate for influenza type A (SD=13.2%), type B (SD=8.76%), and adenoviruses (SD=5.25%) revealed statistical significance for overall 11-day RRs of 1.02 (95% CI: 1.01, 1.03), 1.05 (95% CI: 1.03, 1.06) and 1.04 (95% CI: 1.03, 1.05), respectively. CONCLUSIONS: Current study suggested a positive association between outpatient visits for acute upper respiratory infections and ambient environment factors, including average temperature, air pollutants, and circulating respiratory viruses.

The impact of ground-level fireworks (13 km long) display on the air quality during the traditional Yanshui Lantern Festival in Taiwan.

In this study, the concentrations of CO, non-methane hydrocarbons, NO(X), SO(2), benzene, toluene, ethylbenzene, xylene (BTEX), PM10, and PM2.5 were continuously monitored before and after the fireworks display during the traditional Lantern Festival from March 2-7, 2007 in Yanshui Town, Taiwan. Major roads in Yanshui Town were surrounded by fireworks 13 km in length, with the display lasting for 45 min. More than 200 small firecracker towers popped up randomly in town, resulting in exceedingly inhomogeneous air quality until the end of display at 03:00 the next day, March 5. During the fireworks display, the hourly concentration of PM10 and PM2.5 at Yanshui Primary School reached about 429 and 250 µg m⁻³, respectively, which is 10 times the normal level, and 6 s values even went as high as 1,046 and 842 µg m⁻³, respectively. Similarly, BTEX concentration went up to about five to 10 times its normal value during the fireworks display. As indicated by the distribution of submicron particle sizes, the number of particles with a diameter less than 100 nm increased abruptly during the event period. Metal components with concentrations of more than 10 times higher than the normal value at Yanshui Primary School were Sr, K, Ba, Pb, Al, Mg, and Cu, in sequence. Among water-soluble ions, the content of K( + ), Mg²( + ), and Cl( - ) increased the most, all of which were related to the materials used in the fireworks. The results of this study indicate that fireworks can cause an abrupt increase in the concentration of trace substances in the air within a short period. Although the risks of these trace substances on public health remain to be further assessed, the study results can be utilized in the management of folk events.

The changes in different ozone metrics and their implications following precursor reductions over northern Taiwan from 1994 to 2007.

The changes of different O(3) metrics such as O(3_avg) (daily mean), O(X) (NO(2) + O(3)), O(3_8h) (daily maximum 8-h moving average), O(3_max) (daily maximum 1-h average), and exceedances of O(3_8h) and O(3_max) at 16 air quality monitoring stations over northern Taiwan from 1994 to 2007 are evaluated. The O(3_avg) at the background site displays an increasing trend at 0.54 +/-0.21 ppb (1.28 +/-0.49%) per year. The O(X) at urban sites shows a significant increase, indicating that even with the effect of reduced NO titration increasing photochemical production is evident. The exceedances of O(3_8h) (>80 ppb) are about 14.9% higher than O(3_max) (>120 ppb) with more exceedances at coastal or background sites, where the anthropogenic O(3) precursor emissions are lower. In addition to increasing background O(3) and reductions in NO titration, increasing O(3) production efficiency also plays a key role in the increase of moderate to high O(3) concentrations. The findings help explain the different trends in exceedances and levels of O(3_8h) and O(3_max) and are likewise important in the formation of O(3) control strategies.

On-road emission factors from light-duty vehicles measured in Hsuehshan Tunnel (12.9 km), the longest tunnel in Asia.

This study is based on 82 days of continuous air-quality monitoring using two mobile monitoring vans provided by the Taiwan Environmental Protection Administration (TEPA). The purpose of the study is to reveal variations of air quality without forced ventilation from on-road emissions of light-duty vehicles (LDV) inside the Hsuehshan Tunnel. Since it was opened to traffic in June 2006, only LDV have been allowed to pass the Hsuehshan Tunnel, the longest tunnel in Taiwan and in Asia. The hourly concentrations of air pollutants at four monitoring sites inside the tunnel (pollutant: downslope entrance, downslope exit, upslope entrance, upslope exit) are as follows: (CO: 6.9 +/- 5.4, 13.6 +/- 8.7, 4.6 +/- 3.2, 14.6 +/- 8.0 ppm), (NO(X): 534 +/- 311, 1198 +/- 640, 460 +/- 242, 1704 +/- 692 ppb), (SO2: 7 +/- 5, 18 +/- 10, 9 +/- 4, 26 +/- 10 ppb), (NMHC: 1.9 +/- 2.5, 3.5 +/- 3.0, 0.8 +/- 0.9, 2.7 +/- 1.9 ppm), (PM10: 50 +/- 28, 62 +/- 29, 59 +/- 25, 85 +/- 30 microg m(-3)), and (PM(2.5): 31 +/- 18, 45 +/- 22, 35 +/- 18, 62 +/- 23 microg m(-3)). The emission factors (EFs) from LDV in this study (pollutant: downslope EF, upslope EF in mg veh(-1) km(-1)) is estimated respectively as follows: (CO: 909 +/- 469, 1468 +/- 631), (NO(X): 145 +/- 67, 331 +/- 166), (SO2: 3 +/- 2, 6 +/- 3), (NMHC: 96 +/- 65, 121 +/- 63), (PM10: 2 +/- 2, 5 +/- 4), and (PM(2.5): 2 +/- 2, 4 +/- 3). It shows that the upslope pollutant EFs are twice as big as those of the downslope. However, among these EFs, the NMHC EF is less affected by the road gradient. Likewise, its upslope EF is only 1.3 times as big as that of the downslope. In summary, the results are useful for examining the emissions from the local fleet of vehicles under the driving conditions present during the study and for observing the changes in fleet emission rates upon future replication of the study.

Evaluation of the temporal variations of air quality in Taipei City, Taiwan, from 1994 to 2003.

Data collected from the five air-quality monitoring stations established by the Taiwan Environmental Protection Administration in Taipei City from 1994 to 2003 are analyzed to assess the temporal variations of air quality. Principal component analysis (PCA) is adopted to convert the original measuring pollutants into fewer independent components through linear combinations while still retaining the majority of the variance of the original data set. Two principal components (PCs) are retained together explaining 82.73% of the total variance. PC1, which represents primary pollutants such as CO, NO(x), and SO(2), shows an obvious decrease over the last 10 years. PC2, which represents secondary pollutants such as ozone, displays a yearly increase over the time period when a reduction of primary pollutants is obvious. In order to track down the control measures put forth by the authorities, 47 days of high PM(10) concentrations caused by transboundary transport have been eliminated in analyzing the long-term trend of PM(10) in Taipei City. The temporal variations over the past 10 years show that the moderate peak in O(3) demonstrates a significant upward trend even when the local primary pollutants have been well under control. Monthly variations of PC scores demonstrate that primary pollution is significant from January to April, while ozone increases from April to August. The results of the yearly variations of PC scores show that PM(10) has gradually shifted from a strong correlation with PC1 during the early years to become more related to PC2 in recent years. This implies that after a reduction of primary pollutants, the proportion of secondary aerosols in PM(10) may increase. Thus, reducing the precursor concentrations of secondary aerosols will be an effective way to lower PM(10) concentrations.

Evaluation of the trend of air quality in Taipei, Taiwan from 1994 to 2003.

The data collected from the five air quality monitoring stations established by the Taiwan Environmental Protection Administration (TEPA) in Taipei City were analyzed to assess the changes in air quality. The analyses reveal that the air quality in Taipei City improved over the last decade from 1994 to 2003, as evidenced by the significant downward trends of the various primary air pollutant concentrations, such as CO, NO(X), SO(2), and PM(10). An air pollution fee was collected by TEPA in 1995, and several air pollution control measures were likewise taken to improve the air quality in Taiwan. However, although the extreme daily maximum O(3) concentrations occurred more frequently in earlier years and showed a downward trend, its moderately high concentrations increased annually in recent years. It implied that after the reduction of various primary pollutant concentrations, the effective reduction of O(3) pollution still remains an important issue.

Assessment of PM10 enhancement by yellow sand on the air quality of Taipei, Taiwan in 2001.

The impact of long-range transport of yellow sand from Asian Continent to the Taipei Metropolitan Area (Taipei) not only deteriorates air quality but also poses health risks to all, especially the children and the elderly. As such, it is important to assess the enhancement of PM(10) during yellow sand periods. In order to estimate PM(10) enhancement, we adopted factor analysis to distinguish the yellow-sand (YS) periods from non-yellow-sand (NYS) periods based on air quality monitoring records. Eight YS events were identified using factor analysis coupling with an independent validation procedure by checking background site values, examining meteorological conditions, and modeling air mass trajectory from January 2001 to May 2001. The duration of each event varied from 11 to 132 h, which was identified from the time when the PM(10) level was high, and the CO and NOx levels were low. Subsequently, we used the artificial neural network (ANN) to simulate local PM(10) levels from related parameters including local gas pollutants and meteorological factors during the NYS periods. The PM(10) enhancement during the YS periods is then calculated by subtracting the simulated PM(10) from the observed PM(10) levels. Based on our calculations, the PM(10) enhancement in the maximum hour of each event ranged from 51 to 82%. Moreover, in the eight events identified in 2001, it was estimated that a total amount of 7,210 tons of PM(10) were transported by yellow sand to Taipei. Thus, in this study, we demonstrate that an integration of factor analysis with ANN model could provide a very useful method in identifying YS periods and in determining PM(10) enhancement caused by yellow sand.