车内挥发性有机物污染的分析评价及吸附光催化研究
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摘要
车内空气环境中挥发性有机物(VOC)是影响车内空气品质的主要污染物之一,毒性高、危害大,是引起“驾车综合症、新车味道”的主要因素。如何改善车内空气质量,如何控制车内VOC污染已迫在眉睫。本研究从长沙市车内空气污染调查入手,采样分析了125辆汽车内VOC的污染浓度。
抽样调查发现车内苯、甲苯、乙苯、二甲苯、对/间二甲苯、邻二甲苯、苯乙烯、乙酸正丁酯、十一烷与TVOC浓度均值各是83.6、215.9、75.6、184.3、117.6、66.7.25.0.29.1.62.9与1459.6μg/m3,车内苯、甲苯、二甲苯与TVOC浓度超过国家室内空气质量标准限值的比例依次是14.4%、65.6%、37.6%与92.0%。研究还表明车内游离VOC浓度与车内温度、车内湿度或者汽车排量成正比,与车内体积、车龄或者总里程成反比,随通风方式、运行速度、车内气流、采样地点或者车辆档次的不同而变化。就车内VOC污染程度而言,汽油车>柴油车,真皮内饰车>非真皮内饰车,空调车>非空调车,小轿车>出租车>公交车,车内吸烟远远大于非吸烟。
通过逐步回归法得出车内VOC质量浓度与13个影响因子之间的最优回归方程,其中Y苯=16.8+1.8X温度+0.46X湿度-1.29X车龄+6.46X内饰；通过因素分析发现车内VOC浓度的13个影响因子可由三个主成分反映出75.3%,使用聚类分析表明车龄与温度聚类最紧密,最后综合得出车内VOC浓度的最大影响因子是车龄,其次是车内温度。通过曲线拟合表明车内VOC浓度与车龄成一元三次方程函数关系,其中Y甲苯=332.87-13.27X年龄+0.41(X车龄)2-0.01(X车龄)3;与车内温度成自然对数函数关系,其中Y=甲苯=-695.81+262.27ln(X温度)。
进一步还发现车内游离VOC污染对车内空气品质的损失率随车内温度的升高而变大,随车龄的增加而变小,随同—VOC浓度的增大而升高,随不同VOC浓度超标倍数的增多而变大,小轿车>出租车>公交车。车内空气中VOC污染的平均等级为轻污染,清洁、末污染、轻污染、中污染与重污染车的数量比例依次占1.6%、16.0%、66.4%、16.0%与0.0%。通过计算得出车内VOC污染损失率评价公式中的mi与ai为常数,分别是5.89与32.45。
基于健康风险评价公式,反推导得出车内空气中苯的危险致癌浓度(CD)与暴露者的寿命(AL)、体重(BE)、暴露频率(EF)、暴露时间(ET)、呼吸速率(IR)、暴露年限(LT)的函数方程为CD=1.40×AL×BE÷EF÷ET÷IR÷LT。当车内游离苯污染的致癌风险为1×10-4时,车内男性乘客、女性乘客、男性司机与女性司机的CD分别是450、470、67.5与70.4μg/m3。车内VOC污染的非致癌危险指数都低于基准值1,对车内驾乘人员都不构成非致癌风险；苯对司机的致癌风险较高,平均值为1.21×104,需采取控制措施。车内VOC的非致癌危险与苯的致癌风险程度都是男性司机>女性司机>男性乘客>女性乘客,原因是由于男性呼吸率高于女性而平均寿命低于女性,司机每天的暴露时间比乘客的长。
采用振荡浸渍法合成了Pt/TiO2/ACF复合材料,净化试验结果表明：载铂量为1.0%时,效果最佳；延长反应时间或者增加净化材料用量,可提高降解率；阳光照射导致复合材料对车内苯、甲苯、乙苯、二甲苯、苯乙烯与TVOC浓度的平均去除率分别是76.1%、75.5%、74.7%、75.9%、76.2%与76.3%；车内游离VOC在Pt/TiO2/ACF材料上的净化,形成了吸附-催化-吸附-催化的良性循环；Pt的沉积提高了TiO2光催化性,也增强了Pt/TiO2/ACF材料对车内空气中VOC污染的吸附光催化净化效率。
Volatile Organic Compounds (VOC) are one of the most important pollutants of Automotive Indoor Air Quality (AIAQ) and the primary factor on "Automobile Driving Syndrome, New Car Smell" because of their high toxicity and harm. So, how to improve the AIAQ and to control the in-car VOC pollution is to be imminent. In this research, the investigation of in-car air pollution in Changsha and the VOC mass concentrations in interior air of125vehicles were obtained.
The mean levels of airborne benzene, toluene, ethylbenzene, xylenes, p/m-xylene, o-xylene, styrene, butyl acetate, undecane and TVOC in cars were83.6,215.9,75.6,184.3,117.6,66.7,25.0,29.1,62.9and1459.6μg/m3, respectively, through the sample investigation. The rates of cars tested where the interior concentrations exceeded the limit levels of Chinese Indoor Air Quality Standard were14.4%for benzene,65.6%for toluene,37.6%for xylenes and92.0%for TVOC. The VOC levels increased when in-car temperature, exhaust volume or relative humidity increased, and decreased when car age, interior volume or travel distance rose. The VOC pollution was higher in leather trims cars than in non-leather trims ones, in air-conditioned cars than in non-air-conditioned ones, in gas cars than in diesel oil ones, in saloon cars than in taxis or buses, and changed with the differences of ventilation modes, vehicular grades, driving speed, sampling space or interior airflow speed. Smoking caused in-car VOC mass concentrations to increase greatly.
Through stepwise of multiple linear regression analysis, the optimal regression equations between VOC levels and13influencing factors were drawn, for example, Ybenzene=16.8+1.8X3+0.46X4-1.29X6+6.46X7; with principal component analysis, the13factors had three principal components and the percentage of total variance achieved75.3%; through cluster analysis, the strongest subcluster included the car age and interior temperature. In conclusion, car age (X6) is the most important factors influencing the in-car VOC concentrations, followed by interior temperature (X3). With the curve estimation, the cubic equation of a variable is between in-car VOC levels and car age such as Ytoluene=332.87-13.27X6+0.41(X6)2-0.01(X6)3, and the nature logarithm function is between in-car VOC concentrations and temperature such as Yxylenes=-695.81+262.27ln(X3).
The pollution loss rate of AIAQ increased when the interior temperature, the same VOC level or the exceeding standard times of different VOC levels increased, and decreased when the car age rose. As for the average rank of AIAQ, the sampled cars were the light pollution; the heavy, middling, light, clean and no pollution car was0.0%,16.0%,66.4%,16.0%and1.6%, respectively. The mi and bi are constant, and is5.89and32.45in turn in the equation of pollution loss rate.
With the health risk assessment, the non-carcinogenic danger coefficient (HI) of in-car VOC pollution by far is lower than the datum value (1), and does not harm the personnel; the benzene carcinogenic risk (Rz) to drivers is dangerous and the mean value is1.21×10-4. To the man driver, the Rz or HI of VOC is biggest, followed by that of woman driver, man passenger and woman passenger because the feminine mean lifetime excels in the male, but the breathing rate is lower than the masculine result and the exposure time of driver is longer than that of passenger. Through calculating, CD=1-40×AL×BE÷EF÷ET÷IR÷LT and in the equation, the CD, AL, BE, EF, ET, IR and LT is the dangerous levels, lifetime, body weights, exposure frequency, exposure time, inhalation rate and exposure duration, respectively. When the Rz is1×10-4, the Co for man passengers, woman passengers, man drivers and woman drivers is450,470,67.5and70.4μg/m3in turn.
Through the vibration and impregnation method, the compound material of Pt/TiO2/ACF was synthesized. When the platinum quantity is1.0%, the effect is best; to lengthen the reaction time or increase used amount, the purification efficiency is higher. The elimination rate of in-car benzene, toluene, ethylbenzene, xylenes, styrene and TVOC density respectively is76.1%,75.5%,74.7%,75.9%,76.2%and76.3%with sunlight illumination; the purification efficiency of the material to in-car VOC has formed the positive cycle of adsorption-catalysis-adsorption-catalysis. The Pt deposition enhanced the TiO2photochemical catalysis and strengthened the purification efficiency of the compound materials to in-car VOC pollution.
抽样调查发现车内苯、甲苯、乙苯、二甲苯、对/间二甲苯、邻二甲苯、苯乙烯、乙酸正丁酯、十一烷与TVOC浓度均值各是83.6、215.9、75.6、184.3、117.6、66.7.25.0.29.1.62.9与1459.6μg/m3,车内苯、甲苯、二甲苯与TVOC浓度超过国家室内空气质量标准限值的比例依次是14.4%、65.6%、37.6%与92.0%。研究还表明车内游离VOC浓度与车内温度、车内湿度或者汽车排量成正比,与车内体积、车龄或者总里程成反比,随通风方式、运行速度、车内气流、采样地点或者车辆档次的不同而变化。就车内VOC污染程度而言,汽油车>柴油车,真皮内饰车>非真皮内饰车,空调车>非空调车,小轿车>出租车>公交车,车内吸烟远远大于非吸烟。
通过逐步回归法得出车内VOC质量浓度与13个影响因子之间的最优回归方程,其中Y苯=16.8+1.8X温度+0.46X湿度-1.29X车龄+6.46X内饰；通过因素分析发现车内VOC浓度的13个影响因子可由三个主成分反映出75.3%,使用聚类分析表明车龄与温度聚类最紧密,最后综合得出车内VOC浓度的最大影响因子是车龄,其次是车内温度。通过曲线拟合表明车内VOC浓度与车龄成一元三次方程函数关系,其中Y甲苯=332.87-13.27X年龄+0.41(X车龄)2-0.01(X车龄)3;与车内温度成自然对数函数关系,其中Y=甲苯=-695.81+262.27ln(X温度)。
进一步还发现车内游离VOC污染对车内空气品质的损失率随车内温度的升高而变大,随车龄的增加而变小,随同—VOC浓度的增大而升高,随不同VOC浓度超标倍数的增多而变大,小轿车>出租车>公交车。车内空气中VOC污染的平均等级为轻污染,清洁、末污染、轻污染、中污染与重污染车的数量比例依次占1.6%、16.0%、66.4%、16.0%与0.0%。通过计算得出车内VOC污染损失率评价公式中的mi与ai为常数,分别是5.89与32.45。
基于健康风险评价公式,反推导得出车内空气中苯的危险致癌浓度(CD)与暴露者的寿命(AL)、体重(BE)、暴露频率(EF)、暴露时间(ET)、呼吸速率(IR)、暴露年限(LT)的函数方程为CD=1.40×AL×BE÷EF÷ET÷IR÷LT。当车内游离苯污染的致癌风险为1×10-4时,车内男性乘客、女性乘客、男性司机与女性司机的CD分别是450、470、67.5与70.4μg/m3。车内VOC污染的非致癌危险指数都低于基准值1,对车内驾乘人员都不构成非致癌风险；苯对司机的致癌风险较高,平均值为1.21×104,需采取控制措施。车内VOC的非致癌危险与苯的致癌风险程度都是男性司机>女性司机>男性乘客>女性乘客,原因是由于男性呼吸率高于女性而平均寿命低于女性,司机每天的暴露时间比乘客的长。
采用振荡浸渍法合成了Pt/TiO2/ACF复合材料,净化试验结果表明：载铂量为1.0%时,效果最佳；延长反应时间或者增加净化材料用量,可提高降解率；阳光照射导致复合材料对车内苯、甲苯、乙苯、二甲苯、苯乙烯与TVOC浓度的平均去除率分别是76.1%、75.5%、74.7%、75.9%、76.2%与76.3%；车内游离VOC在Pt/TiO2/ACF材料上的净化,形成了吸附-催化-吸附-催化的良性循环；Pt的沉积提高了TiO2光催化性,也增强了Pt/TiO2/ACF材料对车内空气中VOC污染的吸附光催化净化效率。
Volatile Organic Compounds (VOC) are one of the most important pollutants of Automotive Indoor Air Quality (AIAQ) and the primary factor on "Automobile Driving Syndrome, New Car Smell" because of their high toxicity and harm. So, how to improve the AIAQ and to control the in-car VOC pollution is to be imminent. In this research, the investigation of in-car air pollution in Changsha and the VOC mass concentrations in interior air of125vehicles were obtained.
The mean levels of airborne benzene, toluene, ethylbenzene, xylenes, p/m-xylene, o-xylene, styrene, butyl acetate, undecane and TVOC in cars were83.6,215.9,75.6,184.3,117.6,66.7,25.0,29.1,62.9and1459.6μg/m3, respectively, through the sample investigation. The rates of cars tested where the interior concentrations exceeded the limit levels of Chinese Indoor Air Quality Standard were14.4%for benzene,65.6%for toluene,37.6%for xylenes and92.0%for TVOC. The VOC levels increased when in-car temperature, exhaust volume or relative humidity increased, and decreased when car age, interior volume or travel distance rose. The VOC pollution was higher in leather trims cars than in non-leather trims ones, in air-conditioned cars than in non-air-conditioned ones, in gas cars than in diesel oil ones, in saloon cars than in taxis or buses, and changed with the differences of ventilation modes, vehicular grades, driving speed, sampling space or interior airflow speed. Smoking caused in-car VOC mass concentrations to increase greatly.
Through stepwise of multiple linear regression analysis, the optimal regression equations between VOC levels and13influencing factors were drawn, for example, Ybenzene=16.8+1.8X3+0.46X4-1.29X6+6.46X7; with principal component analysis, the13factors had three principal components and the percentage of total variance achieved75.3%; through cluster analysis, the strongest subcluster included the car age and interior temperature. In conclusion, car age (X6) is the most important factors influencing the in-car VOC concentrations, followed by interior temperature (X3). With the curve estimation, the cubic equation of a variable is between in-car VOC levels and car age such as Ytoluene=332.87-13.27X6+0.41(X6)2-0.01(X6)3, and the nature logarithm function is between in-car VOC concentrations and temperature such as Yxylenes=-695.81+262.27ln(X3).
The pollution loss rate of AIAQ increased when the interior temperature, the same VOC level or the exceeding standard times of different VOC levels increased, and decreased when the car age rose. As for the average rank of AIAQ, the sampled cars were the light pollution; the heavy, middling, light, clean and no pollution car was0.0%,16.0%,66.4%,16.0%and1.6%, respectively. The mi and bi are constant, and is5.89and32.45in turn in the equation of pollution loss rate.
With the health risk assessment, the non-carcinogenic danger coefficient (HI) of in-car VOC pollution by far is lower than the datum value (1), and does not harm the personnel; the benzene carcinogenic risk (Rz) to drivers is dangerous and the mean value is1.21×10-4. To the man driver, the Rz or HI of VOC is biggest, followed by that of woman driver, man passenger and woman passenger because the feminine mean lifetime excels in the male, but the breathing rate is lower than the masculine result and the exposure time of driver is longer than that of passenger. Through calculating, CD=1-40×AL×BE÷EF÷ET÷IR÷LT and in the equation, the CD, AL, BE, EF, ET, IR and LT is the dangerous levels, lifetime, body weights, exposure frequency, exposure time, inhalation rate and exposure duration, respectively. When the Rz is1×10-4, the Co for man passengers, woman passengers, man drivers and woman drivers is450,470,67.5and70.4μg/m3in turn.
Through the vibration and impregnation method, the compound material of Pt/TiO2/ACF was synthesized. When the platinum quantity is1.0%, the effect is best; to lengthen the reaction time or increase used amount, the purification efficiency is higher. The elimination rate of in-car benzene, toluene, ethylbenzene, xylenes, styrene and TVOC density respectively is76.1%,75.5%,74.7%,75.9%,76.2%and76.3%with sunlight illumination; the purification efficiency of the material to in-car VOC has formed the positive cycle of adsorption-catalysis-adsorption-catalysis. The Pt deposition enhanced the TiO2photochemical catalysis and strengthened the purification efficiency of the compound materials to in-car VOC pollution.
引文
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