西安地区PM_(2.5)中环境持久性自由基(EPFRs)性质及来源研究
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摘要
环境持久性自由基(environmental persistent free radicals, EPFRs)是一种近年来备受关注的环境风险物质,可能会危害人体健康.本研究利用溶剂萃取方法从西安市大气PM_(2.5)样品中分离出物质,运用电子顺磁共振波谱(EPR)技术分析了不同大气污染状况下大气PM_(2.5)样品及类黑碳成分中EPFRs的种类和含量,并分别测定PM_(2.5)和类黑碳成分催化H_2O_2产生羟基自由基的能力.结果表明:PM_(2.5)中的EPFRs约有85%～90%是由类黑碳成分产生的.可见光照(400～700 nm)前后,PM_(2.5)样品中EPFRs的含量增加10%～20%.此外,实验结果亦表明PM_(2.5)中能催化H_2O_2产生羟基自由基的物质主要是PM_(2.5)中水溶性物质而不是类黑碳.大气PM_(2.5)中的EPFRs没有显著催化H_2O_2产生羟基自由基的能力,也不能将O_2分子转化为活性氧物质.
Environmental persistent free radicals(EPFRs) are environmental risk substances that have received much attention in recent years, which may have serious effects on human health. In this study, a solvent-extraction method was used to separate the BC-like(black carbon like) substance from the atmospheric PM_(2.5) samples in Xi′an. The types and concentrations of EPFRs in PM_(2.5) and BC-like substance were analyzed under different atmospheric pollution conditions with electron paramagnetic resonance(EPR) spectroscopy, respectively as well as the ability of catalyzing H_2O_2 to generate hydroxyl radicals. The results showed that about 85%～90% of the EPFRs in PM_(2.5) were produced by the BC-like substance. Before and after the visible light(400～700 nm), the content of EPFRs in PM_(2.5) increased by 10%～20%. In addition, it was found that the substances who could catalyze H_2O_2 to generate hydroxyl radicals in PM_(2.5) were mainly water-soluble substances rather than BC-like substance. And this experiment also found that EPFRs in atmospheric PM_(2.5) neither had significant ability to catalyze H_2O_2 to generate hydroxyl radicals nor converted O_2 molecules to generate reactive oxygen species.
Environmental persistent free radicals(EPFRs) are environmental risk substances that have received much attention in recent years, which may have serious effects on human health. In this study, a solvent-extraction method was used to separate the BC-like(black carbon like) substance from the atmospheric PM_(2.5) samples in Xi′an. The types and concentrations of EPFRs in PM_(2.5) and BC-like substance were analyzed under different atmospheric pollution conditions with electron paramagnetic resonance(EPR) spectroscopy, respectively as well as the ability of catalyzing H_2O_2 to generate hydroxyl radicals. The results showed that about 85%～90% of the EPFRs in PM_(2.5) were produced by the BC-like substance. Before and after the visible light(400～700 nm), the content of EPFRs in PM_(2.5) increased by 10%～20%. In addition, it was found that the substances who could catalyze H_2O_2 to generate hydroxyl radicals in PM_(2.5) were mainly water-soluble substances rather than BC-like substance. And this experiment also found that EPFRs in atmospheric PM_(2.5) neither had significant ability to catalyze H_2O_2 to generate hydroxyl radicals nor converted O_2 molecules to generate reactive oxygen species.
引文
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Gehling W, Dellinger B. 2013. Environmentally persistent free radicals and their lifetimes in PM2.5[J]. Environmental Science & Technology, 47(15): 8172-8178
Khachatryan L, Dellinger B. 2011. Environmentally persistent free radicals (EPFRs)-2. Are free hydroxyl radicals generated in aqueous solutions?[J]. Environmental Science & Technology, 45(21): 9232-9239
Künzli N, Mudway I S, G?tschi T, et al. 2006. Comparison of oxidative properties, light absorbance, and total and elemental mass concentration of ambient PM2.5 collected at 20 European sites[J]. Environmental Health Perspectives, 114(5):684-690
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Myhre G. 2009. Consistency between satellite-derived and modeled estimates of the direct aerosol effect[J]. Science, 325(5937):187-190
Nawrot T S, Kuenzli N, Sunyer J, et al. 2009. Oxidative properties of ambient PM2.5 and elemental composition Heterogeneous associations in 19 European cities[J]. Atmospheric Environment, 43(30):4595-4602
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Shaltout A A, Boman J, Shehadeh Z F, et al. 2015. Spectroscopic investigation of PM2.5 collected at industrial, residential and traffic sites in Taif, Saudi Arabia[J]. Journal of Aerosol Science, 79: 97-108
Thevenot P T, Saravia J, Jin N, et al. 2013. Radical-containing ultrafine particulate matter initiates epithelial-to-mesenchymal transitions in airway epithelial cells[J]. American Journal of Respiratory Cell & Molecular Biology, 48(2): 188-197
Truong H, Lomnicki S, Dellinger B. 2010. Potential for misidentification of environmentally persistent free radicals as molecular pollutants in particulate matter[J]. Environmental Science & Technology, 44(6): 1933-1939
Vejerano E, Rao G, Khachatryan L, et al. 2018. Environmentally persistent free radicals: Insights on a New Class of Pollutants[J]. Environmental Science & Technology, 52(5):2468-2481
Vejerano E, Lomnicki S, Dellinger B. 2010. Formation and stabilization of combustion-generated environmentally persistent free radicals on an Fe(III)2O3/silica surface[J]. Environmental Science & Technology, 45(2): 589-594
Wang P, Pan B, Li H, et al. 2018. The overlooked occurrence of environmentally persistent free radicals in an area with low-rank coal burning, Xuanwei, China[J]. Environmental Science & Technology, 52(3):1054-1061
Yang L L, Liu G, Zheng M, et al. 2017. Highly elevated levels and particle-size distributions of environmentally persistent free radicals in haze-associated atmosphere[J]. Environmental Science & Technology, 51(14): 7936-7944
Yeh T F, Syu J M, Cheng C, et al. 2010. Graphite oxide as a photocatalyst for hydrogen production from water[J]. Advanced Functional Materials, 20(14): 2255-2262
Zhou L, Tang J, Ernst M, et al. 2001. Continuous measurement of baseline atmospheric carbon monoxide in western China[J]. Chinese Journal of Enviromental Science, 22(3):1-5
Arangio A M, Tong H, Socorro J, et al. 2016. Quantification of environmentally persistent free radicals and reactive oxygen species in atmospheric aerosol particles[J]. Atmospheric Chemistry & Physics, 16(20): 13105-13119
Blakley R L, Henry D D, Smith C J. 2001. Lack of correlation between cigarette mainstream smoke particulate phase radicals and hydroquinone yield[J]. Food & Chemical Toxicology, 39(4): 401-406
Chen Q, Sun H, Wang M, et al. 2018. Dominant fraction of EPFRs from Nonsolvent-Extractable organic matter in fine particulates over Xi′an, China[J]. Environmental Science & Technology, 52(17): 9646-9655
Chen Q, Wang M, Wang Y, et al. 2018. Rapid determination of environmentally persistent free radicals (EPFRs) in atmospheric particles with a quartz sheet-based approach using electron paramagnetic resonance (EPR) spectroscopy[J]. Atmospheric Environment, 184: 140-145
Cormier S A, Lomnicki S, Backes W, et al. 2006. Origin and health impacts of emissions of toxic by-products and fine particles from combustion and thermal treatment of hazardous wastes and materials[J]. Environ Health Perspect, 114(6):810-817
Cruz A L, Cook R L, Lomnicki S M, et al. 2012. Effect of low temperature thermal treatment on soils contaminated with pentachlorophenol and environmentally persistent free radicals[J]. Environmental Science & Technology, 46(11):5971-5978
D′Arienzo M, Gamba L, Morazzoni F, et al. 2017. Experimental and theoretical investigation on the catalytic generation of environmentally persistent free radicals from benzene[J]. The Journal of Physical Chemistry C, 121(17): 9381-9393
Dellinger B, Lomnicki S, Khachatryan L, et al. 2007. Formation and stabilization of persistent free radicals[J]. Proceedings of the Combustion Institute International Symposium on Combustion, 31(1):521-528
Dellinger B, Pryor W A, Cueto R, et al. 2001. Role of free radicals in the toxicity of airborne fine particulate matter[J]. Chemical Research in Toxicology, 14(10):1371-1377
Fan J, Zhang R, Tao W K, et al. 2008. Effects of aerosol optical properties on deep convective clouds and radiative forcing[J]. Journal of Geophysical Research Atmospheres, 113(D8):1-16
Fuertes A B, Arbestain M C, Sevilla M, et al. 2010. Chemical and structural properties of carbonaceous products obtained by pyrolysis and hydrothermal carbonisation of corn stover[J]. Soil Research, 48(7): 618-626
Ingram D J E, Tapley J G, Jackson R, et al. 1954. Paramagnetic resonance in carbonaceous solids[J]. Nature, 174(4434):797-798
Gehling W, Dellinger B. 2013. Environmentally persistent free radicals and their lifetimes in PM2.5[J]. Environmental Science & Technology, 47(15): 8172-8178
Khachatryan L, Dellinger B. 2011. Environmentally persistent free radicals (EPFRs)-2. Are free hydroxyl radicals generated in aqueous solutions?[J]. Environmental Science & Technology, 45(21): 9232-9239
Künzli N, Mudway I S, G?tschi T, et al. 2006. Comparison of oxidative properties, light absorbance, and total and elemental mass concentration of ambient PM2.5 collected at 20 European sites[J]. Environmental Health Perspectives, 114(5):684-690
Li Y, Henze D K, Jack D, et al. 2016. Assessing public health burden associated with exposure to ambient black carbon in the United States[J]. Science of the Total Environment, 539:515-525
Lomnicki S, Truong H, Vejerano E, et al. 2008. Copper oxide-based model of persistent free radical formation on combustion-derived particulate matter[J]. Environmental Science & Technology, 42(13):4982-4988
Lyons M J, Spence J B. 1960. Environmental free radicals[J]. British Journal of Cancer, 14(4):703-708
Myhre G. 2009. Consistency between satellite-derived and modeled estimates of the direct aerosol effect[J]. Science, 325(5937):187-190
Nawrot T S, Kuenzli N, Sunyer J, et al. 2009. Oxidative properties of ambient PM2.5 and elemental composition Heterogeneous associations in 19 European cities[J]. Atmospheric Environment, 43(30):4595-4602
秦莎莎, 侯斌, 赵国栋,等. 2017. 西安市2015年恶性肿瘤发病分析[J]. 中国卫生统计, 34(4):616-617
任信荣,王会祥, 邵可声,等. 2002. 北京市大气OH自由基测量结果及其特征[J]. 环境科学, 23(4):24-27
Shaltout A A, Boman J, Shehadeh Z F, et al. 2015. Spectroscopic investigation of PM2.5 collected at industrial, residential and traffic sites in Taif, Saudi Arabia[J]. Journal of Aerosol Science, 79: 97-108
Thevenot P T, Saravia J, Jin N, et al. 2013. Radical-containing ultrafine particulate matter initiates epithelial-to-mesenchymal transitions in airway epithelial cells[J]. American Journal of Respiratory Cell & Molecular Biology, 48(2): 188-197
Truong H, Lomnicki S, Dellinger B. 2010. Potential for misidentification of environmentally persistent free radicals as molecular pollutants in particulate matter[J]. Environmental Science & Technology, 44(6): 1933-1939
Vejerano E, Rao G, Khachatryan L, et al. 2018. Environmentally persistent free radicals: Insights on a New Class of Pollutants[J]. Environmental Science & Technology, 52(5):2468-2481
Vejerano E, Lomnicki S, Dellinger B. 2010. Formation and stabilization of combustion-generated environmentally persistent free radicals on an Fe(III)2O3/silica surface[J]. Environmental Science & Technology, 45(2): 589-594
Wang P, Pan B, Li H, et al. 2018. The overlooked occurrence of environmentally persistent free radicals in an area with low-rank coal burning, Xuanwei, China[J]. Environmental Science & Technology, 52(3):1054-1061
Yang L L, Liu G, Zheng M, et al. 2017. Highly elevated levels and particle-size distributions of environmentally persistent free radicals in haze-associated atmosphere[J]. Environmental Science & Technology, 51(14): 7936-7944
Yeh T F, Syu J M, Cheng C, et al. 2010. Graphite oxide as a photocatalyst for hydrogen production from water[J]. Advanced Functional Materials, 20(14): 2255-2262
Zhou L, Tang J, Ernst M, et al. 2001. Continuous measurement of baseline atmospheric carbon monoxide in western China[J]. Chinese Journal of Enviromental Science, 22(3):1-5
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