PARTICULATE MATTER < 10 #m (PM10) AND TOTAL
SUSPENDED PARTICULATES (TSP) IN URBAN, RURAL AND
ALPINE AIR IN SWITZERLAND
CH. MONN, i" O. BRAENDLI,:~ G. SCHAEPPI,t CH. SCHINDLER,§
U. ACKERMANN-LIEBRICH,§ PH. LEUENBERGER¶ and SAPALDIA TEAM
i" Federal Institute of Technology, Institute for Hygiene and Applied Physiology, Clausiusstr. 25, CH-8092
Ziirich, Switzerland; :~ Ziircher H6henklink Wald, CH-8636 Faltigberg, Switzerland; § Institute for Social
and Preventive Medicine, Steinengraben 49, CH-4051 Basle, Switzerland; ¶ Centre Hospitalier
Universitaire Vaudois, Rue de Bugnon, CH-1011 Lausanne, Switzerland
Abstract—
Ambient concentrations of particulate matter of less than 10 μm aerodynamic diameter were measured in Switzerland for a 1 year period in 1993 at a dozen urban, rural and alpine sites. PM10 concentrations ranged between 10 μgm -a (alpine) and 33 μgm -3 (urban). Highest concentrations were found at Lugano, in the south of the Alps, and in urban sites of the Swiss Plateau (350-670 m.s.l.). Rural levels were one-third lower than the urban levels and relatively homogeneously distributed. Alpine sites showed considerably lower levels. The ratios between PM1o and TSP were found to be between 0.6 and 0.75, and the highest ratios were found in the most polluted urban sites. Seasonal variation of particulate pollution showed peak levels during winter and autumn, mainly during cold temperature-inversions.
Statistical analyses have shown a good correlation between PM10 and NO z and SO 2, and TSP in urban areas.
1. INTRODUCTION
Recent epidemiological studies have shown that suspended particulate matter considerably influences respiratory health. Associations between suspended particulate matter and lung function parameters, respiratory symptoms and mortality have been found (Braun et al., 1992; Pope and Dockery, 1992; Dockery et al., 1993). Sino," 1991, a study in Switzerland (SAPALDIA: Swiss Study on Air Pollution and Lung Diseases in Adults) has investigated the relationships between prevalence of chronic lung diseases and longterm exposure to ambient air pollution.
In epidemiological studies, respiratory healthrelated effects were found for TSP and distinct finer fractions (e.g. PMlo, PM2.s). Respiratory health effects are biologically expected to be associated with particles smaller than 10#m passing the nose and entering lung alveoli. In addition to the particle size, the number of inhaled particles can be of great importance: a change of the median particle diameter from 1 to 0.1 #m increases the number of particles by more than a factor of a thousand for a constant mass fraction. This can cause problems in the macrophage clearing mechanism. Macrophage clearing is more efficient for a smaller number of larger particles than for very high numbers of fine particles (Kreyling,1994).
Total suspended particle mass fraction does not seem to be the best parameter for the explanation of respiratory diseases; it can, however, be a good indicator if the particle size distribution does not vary greatly between regions.
In the U.S.A., an air quality standard for PMto (annual mean: less than 50 #g m-3) was introduced in the late eighties because of its known adverse effect on the human respiratory system. It is assumed that PMto represents anthropogenic pollution, whilst the origin of larger particles is mainly natural. As well as the size distribution, chemical composition (e.g. acidity, sulphates, nitrates, PAHs) of particles can induce health-related effects (Spengler et al., 1990). The greatest proportion of these chemicals is found within the PM10 fraction.
Within SAPALDIA, air pollutants and meteorological factors were measured routinely at continuously operated monitoring sites. Some sites have a long tradition of monitoring TSP and sulphur dioxide dating back to the mid-seventies. In 1987, after introducing new air quality standards for Switzerland, more than two dozen continuous monitoring sites, mainly for gaseous pollutants, were installed. The air quality standard for TSP was set at 70/zg m-3 (annual mean) which was not exceeded in the last few years. Whilst for gaseous pollutants the measuring techniques were standardised, the measuring methods for total suspended particulates varied greatly between different sites. Therefore, interpretations on regional differences in TSP levels have to be made carefully.
In 1993, a PM10 measuring programme was initiated in order to quantify pollution levels at sites reflecting differences in climate and gaseous pollution.
As we used identical sampling devices in all places,uncertainties in particulate pollution derived from the use of different techniques were removed. As fine particles undergo long-range transport, a similarity in PM10 levels at rural sites was expected.
The major objectives of the PM10 measuring programme during 1993 were as follows:
• to quantify PM10 levels in urban, rural and alpine air and their seasonal variation;
• to assess the fraction of PM10 within TSP and its variation over sites and time;
• to analyse correlations between other air pollutants and meteorological factors.
2. EXPERIMENTAL
Study sites: Figure 1 gives the map of the PM10 measuring sites. Eight of the regions are SAPALDIA study sites (underlined). In addition, PM10 data from three sites of an additional study (SCARPOL: Swiss Study on Childhood Allergy and Respiratory Symptoms with Respect to Pollution, Climate and Pollen) are presented (Langnan, Ziirich, Berne).
Monitors for PMlo were installed at fixed site monitoring stations in SAPALDIA. Measuring sites can be grouped into three major categories: urban and suburban regions (Lugano, Geneva, Basle, Berne, Ziirich, Aarau), rural regions (Binningen, Wald, Payerne, Langnau) and alpine regions (Davos, Montana).
Detailed description of monitoring sites--Aarau: town centre (383 m.s.l, rooftop, 25 m above ground), Basle (St. Johann): town centre, local road (3 m above ground, 260 m.s.l.); Binningen (dose to Basle: rural/suburban, hill, 3 m.a.g.,
300m.s.l.); Davos: outside town on flat valley plateau (3 m.a.g., 1580 m.s.l.); Berne: University of Berne, Terrace (2 m.a.g., 533 m.s.l.); Geneva: town centre, residential/office area, local road (3 m, 380 m.s.l.); Lugano: town centre, local road (3 m.a.g., 280 m.s.1.); Montana: remote on slope near forest (3 m.a.g., 1350 m.s.1.); Wald: outside village, hill slope, no road (3 m.a.g., 630 m.s.l.); Ziirich: close to town centre, local road (5 m.a.g., 460 m.s.l.); Payerne: outside village, no road (2.5 m.a.g., 460 m.s.l.); Langnau: rural, no road (2 m.a.g., 700 m.s.l.) PMt o measurements: PM10 was determined using sharpcut, low-volume cascade impactors (MEM: micro environmental monitors) which were developed at the Harvard School of Public Health. This method has been used in other U.S. studies (Marple et al., 1987; Lioy et al., 1988). Air is drawn through a two-stage impaction inlet, where particles greater than 10 #m are collected. Smaller particles pass the impaction stages and are collected on Teflon filters (Type Gelman Sciences PTFE R2PJ041, pore size 2 #m, diameter 41 mm). The air flow was 4 ~' min- 1. The sampling period was one week. Teflon filters were stored in an environmental chamber with constant air humidity (50% relative humidity) and at temperatures between 20 and 23°C. Filters were weighed before exposure (Mettler: limit of detection 0.01 mg, precision _+ 5%). After exposure, the filters were dried in a dry chamber (silica gel) for a minimum of 24 h and then stored in the environmental chamber for a minimum of 24 h before final weighing. Measurements took place between the 4th of January 1993 and the 4th of January 1994. At Basle, the monitoring period was between Febuary 1993 and February 1994.
PM10 concentrations were calculated for a standard atmosphere on the Swiss Plateau for 950 mbar and 283 K.
TSP measurements and gaseous measurement: Different techniques were used for measuring TSP. We will present TSP data only for SAPALDIA sites, where known technology, such as "High-Vol sampling" (Digitel, for 24 hourly means on glass fibre filters), beta attenuation (FAG, continuous monitor) and a tapered element oscillating microbalance (TEOM) were used. High volume samplers were run at a volume of 40 m a h- 1, the other monitors with a flow of 1-3 m 3 h- 1. The treatment of glass fibre filters was similar to the treatment of PM10 Teflon filters. From these data, daily means were calculated.
In order to compare data with PM10 levels, weekly averages were computed. When more than three days of any week was missing, the week was excluded.
(Instruments used in the SAPALDIA study during 1993-- "Digitel": Binnlngen, Geneva, Ziirich, Payerne, Lugano; High-Vol. self construction: Aarau. "FAG": Davos, "TEOM': Wald. "Elecos": Montana.) Analyses from technical field comparison studies between these monitors showed that data from Digitel and FAG monitor corresponded within a range of _+ 15%. Data from TEOM were always lower than for the other monitors. This monitor is actually designed for PM10 measurements. It can be run with an inlet for TSP but field experiments showed readings much lower.
The instrument readings were similar to monitors determining PM10 mass fraction. Readings were about 30% lower
than for the other TSP monitors. As these observations were consistent, we reassessed the Wald TSP data by multiplying
TEOM readings with a factor of 1.4.
Gaseous pollutant~; were measured using standard techniques: SO2 (fluorescence: "Monitor Labs", "Horiba"), NOx (chemiluminescence: "Monitor Labs", "Horiba"), O 3 (UV absorption: "Monitor Labs").
Meteorological parameters for air temperature, relative humidity, global radiation and wind speed were obtained from the Swiss Network of Meteorology (Swiss Institute for Meteorology) which uses standard technology. At Wald, air temperature and relative humidity were measured at the local air pollution monitor.
Statistical analysis: Statist
顆粒物 < 10 #m (PM10) 和總懸浮顆粒物 (TSP) 在城市、 農村和高山空氣在瑞士通道 MONN 我"O.BRAENDLI: ~ G.SCHAEPPI,t 叢集辛德勒,§美國阿克曼-利布裡希,§ 博士 LEUENBERGER¶ 和 SAPALDIA 的團隊我"聯邦研究所的技術、 衛生和研究所應用的生理學,Clausiusstr。25,CH-8092Ziirich,瑞士;: ~ Ziircher H6henklink 沃爾德,CH 8636 Faltigberg,瑞士;§ 社會研究所和預防醫學,49,Steinengraben CH 4051 巴塞爾,瑞士;¶ 中心醫院十三區 Vaudois,Rue de Bugnon,CH-1011年洛桑,瑞士抽象 — —1993 年 1 年期在十幾個城市、 農村和高山地盤測量在瑞士空氣中小於 10 微米空氣動力學直徑的顆粒物的濃度。PM10 濃度介於 10 μgm-a (高山) 和 33 μgm-3 (城市)。在阿爾卑斯山,南部和瑞士高原 (350-670 m.s.l.) 城市地點在 Lugano,發現最高的濃度。農村水準低於城市水準的三分之一,並分佈相對均勻。高山的網站顯示顯著較低水準。PM1o 和 TSP 之間的比率被發現 0.6 至 0.75,和最高的比率在污染最嚴重的城市遺址被發現。顆粒物污染的季節變化在冬季和秋季,主要發生在冷的溫度反轉顯示峰值水準。統計分析表明在城市地區 PM10 和沒有 z 和如此 2,TSP 之間的良好關係。1.介紹最近的流行病學研究表明懸浮顆粒物有較大影響呼吸系統的健康。之間的關聯懸浮微粒物質和肺功能參數、 呼吸道症狀和死亡率已被發現 (布勞恩等人,1992 年;教皇和海豹,1992 年;多克裡 et al.,1993年)。中,"1991 年,瑞士的一項研究 (SAPALDIA: 瑞士研究空氣污染和肺部疾病成人) 慢性肺疾病患病率和長期暴露于環境空氣污染之間的關係進行了調查。在流行病學研究中,呼吸 healthrelated 效應被發現 TSP 和不同細分數 (如 PMlo、 PM2.s)。呼吸系統健康的影響生物預計將與顆粒小於 10 #m 通過鼻子和進入肺泡。除了顆粒尺寸,吸入粒子數目可以具有重要意義: 從 1 到 0.1 #m 的中位數粒徑變化增加粒子數目由一個多因素的恒定的品質分數為一千。這可以導致巨噬細胞清除機制問題。巨噬細胞清除是更有效的數量較少的較大的顆粒比為非常高數量的細顆粒 (克,1994年)。總懸浮顆粒物品質分數似乎不是呼吸系統疾病; 解釋的最佳參數然而,可以很好的指標如果粒子大小分佈卻變化不大區域之間。在美國,空氣品質標準為年初 (年平均: 小於 50 #g m-3) 介紹了八十年代末期由於其已知對人體呼吸系統的不利影響。它被假設年初表示匯的人為污染,而較大粒子的起源是主要自然。細微性分佈,以及微粒的化學成分 (如酸度、 硫酸鹽、 硝酸鹽、 多環芳烴) 能誘導健康相關效應 (斯賓格勒 et al.,1990年)。這些化學物質的最大比例是 PM10 分數內發現的。在 SAPALDIA 內, 空氣污染物和氣象因素測定經常在不斷經營監測網站。有些網站擁有悠久的監測 TSP 和空氣中的二氧化硫追溯到七十年代中期。1987 年後引入新的空氣品質標準,瑞士,, 連續 20 多個監測點,主要為氣態污染物,安裝了。空氣品質標準的求解 tsp 問題被設定在 70/zg m-3 (年平均) 不超過在過去的幾年。雖然為氣態污染物測量技術進行標準化,總懸浮粒子的測量方法差別很大不同網站之間。因此,對 TSP 水準區域差異的解釋必須時應謹慎。1993 年,為了量化污染程度反映了不同的氣候和氣態污染地點發起 PM10 測量方案。我們在所有的地方使用相同的採樣設備,顆粒物污染來自使用不同技術的不確定性被去除了。細顆粒進行遠距離遷移,預期會 PM10 水準在農村地區的相似性。PM10 1993 年測量方案的主要目標如下:• 如果要定量 PM10 水準在城市、 農村和高山空氣和季節消長規律;• 如果要評估的分數 PM10 TSP 和其變化內地點和時間;• 分析其他空氣污染物和氣象因素之間的相關性。2.實驗研究網站: 圖 1 給出了匹配的 PM10 測量網站的電子地圖。8 個地區是 SAPALDIA 研究地點 (帶底線)。此外,PM10 資料從三個地點,另一項研究 (SCARPOL: 瑞士研究兒童過敏和呼吸道症狀污染、 氣候和花粉) 介紹 (龍,Ziirich,伯恩)。PMlo 顯示器安裝在固定監測站在 SAPALDIA 的網站。測量網站可以分為三個主要方面: 城市和城郊地區 (Lugano、 日內瓦、 巴塞爾、 伯恩、 Ziirich、 Aarau)、 比寧根、 沃爾德、 佩耶納 (Langnau) 的農村地區和高山地區 (達沃斯,蒙大拿州)。詳細說明監測網站 — — Aarau: 市中心 (383 m.s.l,屋頂,地面 25 米)、 巴塞爾 (聖約翰): 市中心,當地的道路 (3 米以上地面,260 m.s.l.);比寧根 (巴塞爾劑量: 農村或郊區,山,3 m.a.g.,300m.s.l.); Davos: outside town on flat valley plateau (3 m.a.g., 1580 m.s.l.); Berne: University of Berne, Terrace (2 m.a.g., 533 m.s.l.); Geneva: town centre, residential/office area, local road (3 m, 380 m.s.l.); Lugano: town centre, local road (3 m.a.g., 280 m.s.1.); Montana: remote on slope near forest (3 m.a.g., 1350 m.s.1.); Wald: outside village, hill slope, no road (3 m.a.g., 630 m.s.l.); Ziirich: close to town centre, local road (5 m.a.g., 460 m.s.l.); Payerne: outside village, no road (2.5 m.a.g., 460 m.s.l.); Langnau: rural, no road (2 m.a.g., 700 m.s.l.) PMt o measurements: PM10 was determined using sharpcut, low-volume cascade impactors (MEM: micro environmental monitors) which were developed at the Harvard School of Public Health. This method has been used in other U.S. studies (Marple et al., 1987; Lioy et al., 1988). Air is drawn through a two-stage impaction inlet, where particles greater than 10 #m are collected. Smaller particles pass the impaction stages and are collected on Teflon filters (Type Gelman Sciences PTFE R2PJ041, pore size 2 #m, diameter 41 mm). The air flow was 4 ~' min- 1. The sampling period was one week. Teflon filters were stored in an environmental chamber with constant air humidity (50% relative humidity) and at temperatures between 20 and 23°C. Filters were weighed before exposure (Mettler: limit of detection 0.01 mg, precision _+ 5%). After exposure, the filters were dried in a dry chamber (silica gel) for a minimum of 24 h and then stored in the environmental chamber for a minimum of 24 h before final weighing. Measurements took place between the 4th of January 1993 and the 4th of January 1994. At Basle, the monitoring period was between Febuary 1993 and February 1994.PM10 concentrations were calculated for a standard atmosphere on the Swiss Plateau for 950 mbar and 283 K.TSP measurements and gaseous measurement: Different techniques were used for measuring TSP. We will present TSP data only for SAPALDIA sites, where known technology, such as "High-Vol sampling" (Digitel, for 24 hourly means on glass fibre filters), beta attenuation (FAG, continuous monitor) and a tapered element oscillating microbalance (TEOM) were used. High volume samplers were run at a volume of 40 m a h- 1, the other monitors with a flow of 1-3 m 3 h- 1. The treatment of glass fibre filters was similar to the treatment of PM10 Teflon filters. From these data, daily means were calculated.In order to compare data with PM10 levels, weekly averages were computed. When more than three days of any week was missing, the week was excluded.(Instruments used in the SAPALDIA study during 1993-- "Digitel": Binnlngen, Geneva, Ziirich, Payerne, Lugano; High-Vol. self construction: Aarau. "FAG": Davos, "TEOM': Wald. "Elecos": Montana.) Analyses from technical field comparison studies between these monitors showed that data from Digitel and FAG monitor corresponded within a range of _+ 15%. Data from TEOM were always lower than for the other monitors. This monitor is actually designed for PM10 measurements. It can be run with an inlet for TSP but field experiments showed readings much lower.The instrument readings were similar to monitors determining PM10 mass fraction. Readings were about 30% lowerthan for the other TSP monitors. As these observations were consistent, we reassessed the Wald TSP data by multiplyingTEOM readings with a factor of 1.4.Gaseous pollutant~; were measured using standard techniques: SO2 (fluorescence: "Monitor Labs", "Horiba"), NOx (chemiluminescence: "Monitor Labs", "Horiba"), O 3 (UV absorption: "Monitor Labs").Meteorological parameters for air temperature, relative humidity, global radiation and wind speed were obtained from the Swiss Network of Meteorology (Swiss Institute for Meteorology) which uses standard technology. At Wald, air temperature and relative humidity were measured at the local air pollution monitor. Statistical analysis: Statist
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