化石燃料燃烧和生物质燃烧是污染物多环芳烃（ polycyclic aromatic hydrocarbon， PAHs）的两大来源．放射性碳（14 C）分析近年用于评估这两类源对环境中PAHs的相对贡献．此方法基于化石燃料和生物质的14 C含量差异，即化石燃料不含14C，而生物质的14C浓度有一个较稳定值．14C的自然丰度极低（约10－12），因此检测PAHs这样的痕量污染物的14C含量一度极具挑战．1990年代中期，加速器质谱的技术突破使得对环境样品PAHs的14 C分析具有实用价值．要准确测出PAHs的14 C含量，须先从化学成分复杂的环境样品中分离出高纯度的PAHs．制备气相色谱因其出色的分离能力而成为目前环境样品PAHs14 C分析必备的工具．本文意在简介基于14 C分析的PAHs源解析的基本原理、技术进展，以及评估该方法获得的PAHs源解析结果的准确性．
Combustion of biomass and fossil fuel are two main sources of the pollutants polycyclic aromatic hydrocarbons (PAHs). Radiocarbon (14C) analysis recently has been applied to estimate relative contribution of the two sources. The method is based on the difference of 14 C content in fossil fuel and biomass. Namely, fossil fuel is radiocarbon free, but contemporary biomass has a relatively stable 14 C level. The extremely low natural abundance of 14 C ( about 10-12 ) once made it challenging to measure 14C content of trace pollutants like PAHs. 14C analysis became practical since mid?1990s due to the development of micro?scale accelerator mass spectrometer ( AMS ) . For accurate 14 C analysis, it is a prerequisite to harvest individual PAHs with high purity from the chemically complex environmental samples. Owing to its excellent separation efficiency, preparative capillary gas chromatography is currently an essential tool in PAHs 14C analysis of environmental samples. Fundamental and technical progresses of 14C?based PAHs source apportionment are introduced in this article, and accuracy of the method is also assessed.
参考文献
| [1] | Lima A L C;Farrington J W;Reddy C M .Combustion-derived polycyclic aromatic hydrocarbons in the environment-A review[J].Environmental Forensics,2005,6(2):109-131. |
| [2] | Khaiwal Ravindra;Ranjeet Sokhi;Rene Van Grieken .Atmospheric polycyclic aromatic hydrocarbons: Source attribution, emission factors and regulation[J].Atmospheric environment,2008(13):2895-2921. |
| [3] | Harvey R G.Polycyclic aromatic hydrocarbons:Chemistry and carcinogenicity[M].Cambridge University Press Archive,1991 |
| [4] | Daniel U.Pedersen;John L.Durant;Bruce W.Penman;Charles L.Crespi;Harold F.Hemond;Arthur L.Lafleur;Glen R.Cass .Human-Cell Mutagens in Respirable Airborne Particles in the Northeastern United States.1.Mutagenicity of Fractionated Samples[J].Environmental Science & Technology: ES&T,2004(3):682-689. |
| [5] | ROY M. HARRISON;D. J. T. SMITH;L. LUHANA .Source Apportionment of Atmospheric Polycyclic Aromatic Hydrocarbons Collected from an Urban Location in Birmingham, U.K.[J].Environmental Science & Technology: ES&T,1996(3):825-832. |
| [6] | Randolph K. Larsen III;Joel E. Baker .Source apportionment of polycyclic aromatic hydrocarbons in the urban atmosphere: a comparison of three methods[J].Environmental Science & Technology: ES&T,2003(9):1873-1881. |
| [7] | Yunker MB.;Macdonald RW.;Vingarzan R.;Mitchell RH.;Goyette D. Sylvestre S. .PAHs in the Fraser River basin: a critical appraisal of PAH ratios as indicators of PAH source and composition [Review][J].Organic Geochemistry: A Publication of the International Association of Geochemistry and Cosmochemistry,2002(4):489-515. |
| [8] | X.L.ZHANG;S.TAG;W.X.LIU;Y.YANG;Q.ZUO .Source Diagnostics of Polycyclic Aromatic Hydrocarbons Based on Species Ratios:A Multimedia Approach[J].Environmental Science & Technology: ES&T,2005(23):9109-9114. |
| [9] | O′malley V P;Abrajano Jr T A;Hellou J .Determination of the 13C/12C ratios of individual PAH from environmental samples:Can PAH sources be apportioned[J].Organic Geochemistry,1994,21(6):809-822. |
| [10] | Okuda T.;Kumata H.;Naraoka H.;Takada H. .Origin of atmospheric polycyclic aromatic hydrocarbons (PAHs) in Chinese cities solved by compound-specific stable carbon isotopic analyses[J].Organic Geochemistry: A Publication of the International Association of Geochemistry and Cosmochemistry,2002(12):1737-1745. |
| [11] | Currie L;Eglinton T;Benner Jr B et al.Radiocarbon "dating” of individual chemical compounds in atmospheric aerosol:First results comparing direct isotopic and multivariate statistical apportionment of specific polycyclic aromatic hydrocarbons[J].Nuclear Instruments and Methods in Physics Research Section B:Beam Interactions with Materials and Atoms,1997,123(1):475-486. |
| [12] | Christopher M. Reddy;Ann Pearson;Li Xu;Ann P. Mcnichol;Bruce A. Benner;Jr.;Stephen A. Wise;George A. Klouda;Lloyd A. Currie;Timothy I. Eglinton .Radiocarbon as a tool to apportion the sources of polycyclic aromatic hydrocarbons and black carbon in environmental samples[J].Environmental Science & Technology: ES&T,2002(8):1774-1782. |
| [13] | Mook W G.Introduction to isotope hydrology:Stable and radioactive isotopes of hydrogen,carbon,and oxygen-chapter 5[M].Taylor and Francis,2005:25. |
| [14] | Elisabeth Galarneau .Source Specificity And Atmospheric Processing Of Airborne Pahs: Implications For Source Apportionment[J].Atmospheric environment,2008(35):8139-8149. |
| [15] | Hirohide Kanke;Masao Uchida;Tomoaki Okuda;Minoru Yoneda;Hideshige Takada;Yasuyuki Shibata;Masatoshi Morita .Compound-specific radiocarbon analysis of polycyclic aromatic hydrocarbons (PAHs) in sediments from an urban reservoir[J].Nuclear Instruments and Methods in Physics Research, Section B. Beam Interactions with Materials and Atoms,2004(0):545-554. |
| [16] | Mandalakis M;Gustafsson O;Reddy CM;Li X .Radiocarbon apportionment of fossil versus biofuel combustion sources of polycyclic aromatic hydrocarbons in the Stockholm metropolitan area[J].Environmental Science & Technology: ES&T,2004(20):5344-5349. |
| [17] | MANOLIS MANDALAKIS;ORJAN GUSTAFSSON;TOMAS ALSBERG;ANNA-LENA EGEBACK;CHRISTOPHER;M.REDDY;LI XU;JANA KLANOVA;IVAN HOLOUBEK;EURIPIDES G.STEPHANOU .Contribution of Biomass Burning to Atmospheric Polycyclic Aromatic Hydrocarbons at Three European Background Sites[J].Environmental Science & Technology: ES&T,2005(9):2976-2982. |
| [18] | Kumata H;Uchida M;Sakuma E;Uchida T;Fujiwara K;Tsuzuki M;Yoneda M;Shibata Y .Compound class specific C-14 analysis of polycyclic aromatic hydrocarbons associated with PM10 and PM1.1 aerosols from residential areas of suburban Tokyo[J].Environmental Science & Technology: ES&T,2006(11):3474-3480. |
| [19] | Zencak Z;Klanova J;Holoubek I;Gustafsson O .Source apportionment of atmospheric PAHs in the western balkans by natural abundance radiocarbon analysis[J].Environmental Science & Technology: ES&T,2007(11):3850-3855. |
| [20] | Sheesley, R.J.;Krus?, M.;Krecl, P.;Johansson, C.;Gustafsson, ?. .Source apportionment of elevated wintertime PAHs by compound-specific radiocarbon analysis[J].Atmospheric chemistry and physics,2009(10):3347-3356. |
| [21] | G. F. Slater;A. A. Benson;C. Marvin .PAH Fluxes to Siskiwit Revisted: Trends in Fluxes and Sources of Pyrogenic PAH and Perylene Constrained via Radiocarbon Analysis[J].Environmental Science & Technology: ES&T,2013(10):5066-5073. |
| [22] | Li Xu;Mei Zheng;Xiang Ding .Modern and Fossil Contributions to Polycyclic Aromatic Hydrocarbons in PM_(2.5) from North Birmingham, Alabama in the Southeastern U.S.[J].Environmental Science & Technology: ES&T,2012(3):1422-1429. |
| [23] | Libby W F .Atmospheric helium three and radiocarbon from cosmic radiation[J].Physical Review,1946,69(11-12):671. |
| [24] | Libby W F;Anderson E C;Arnold J R .Age determination by radiocarbon content:World-wide assay of natural radiocarbon[J].SCIENCE,1949,109(2827):227-228. |
| [25] | Quan Hua;Mike Barbetti;Andrzej Z Rakowski .ATMOSPHERIC RADIOCARBON FOR THE PERIOD 1950-2010[J].Radiocarbon: An international journal of cosmogenic isotopic research,2013(4):2059-2072. |
| [26] | Stuiver M;Polach H A .Discussion:Reporting of 14C Data[J].RADIOCARBON,1977,19(3):355-363. |
| [27] | Clayton G D;Arnold J R;Patty F A .Determination of sources of particulate atmospheric carbon[J].SCIENCE,1955,122(3173):751-753. |
| [28] | Currie L A.Environmental radiocarbon measurements[A].,1978:372-390. |
| [29] | Shah S R;Pearson A .Ultra-Microscale (5-25 μg C) Analysis of Individual Lipids by 14C AMS:Assessment and Correction for Sample Processing Blanks[J].RADIOCARBON,2007,49(1):69-82. |
| [30] | Pearson A.;Schneider RJ.;Von Reden KF.;Zheng Y.;McNichol AP. .Microscale AMS C-14 measurement at NOSAMS[J].Radiocarbon: An international journal of cosmogenic isotopic research,1998(1 Pt.1 SpecialIssueS):61-75. |
| [31] | Masao Uchida;Yasuyuki Shibata;Minoru Yoneda;Toshiyuki Kobayashi;Masatoshi Morita .Technical progress in AMS microscale radiocarbon analysis[J].Nuclear Instruments and Methods in Physics Research, Section B. Beam Interactions with Materials and Atoms,2004(0):313-317. |
| [32] | Reddy C M;Xu L;O′connor R .Using radiocarbon to apportion sources of polycyclic aromatic hydrocarbons in household soot[J].Environmental Forensics,2003,4(3):191-197. |
| [33] | Mandalakis M;Zebuhr Y;Gustafsson O .Efficient isolation of polyaromatic fraction from aliphatic compounds in complex extracts using dimethylformamide-pentane partitionings[J].Journal of chromatography, A: Including electrophoresis and other separation methods,2004(1/2):111-117. |
| [34] | Mandalakis M;Gustafsson O .Optimization of a preparative capillary gas chromatography-mass spectrometry system for the isolation and harvesting of individual polycyclic aromatic hydrocarbons[J].Journal of Chromatography A,2003,996(1/2):163-172. |
| [35] | Zhang, X.;Zhao, L.;Wang, Y.;Xu, Y.;Zhou, L. .Optimization of programmed-temperature vaporization injection preparative capillary GC for compound specific radiocarbon analysis[J].Journal of separation science,2013(13):2136-2144. |
| [36] | Ball, G.I.;Xu, L.;McNichol, A.P.;Aluwihare, L.I..A two-dimensional, heart-cutting preparative gas chromatograph facilitates highly resolved single-compound isolations with utility towards compound-specific natural abundance radiocarbon (~(14)C) analyses[J].Journal of chromatography, A: Including electrophoresis and other separation methods,2012:122-131. |
| [37] | Sciarrone D;Panto S;Tranchida P Q et al.Rapid isolation of high solute amounts using an online four-dimensional preparative system:normal phase-liquid chromatography coupled to methyl siloxane-ionic liquid-wax phase gas chromatography[J].,2014,86(9):4295-4301. |
| [38] | Suess H E .Radiocarbon concentration in modern wood[J].SCIENCE,1955,122(3166):415-417. |
| [39] | Hsueh DY;Krakauer NY;Randerson JT;Xu XM;Trumbore SE;Southon JR .Regional patterns of radiocarbon and fossil fuel-derived CO2 in surface air across North America[J].Geophysical Research Letters,2007(2):2816-1-2816-6-0. |
| [40] | Xi, X.T.;Ding, X.F.;Fu, D.P.;Zhou, L.P.;Liu, K.X..Δ~(14)C level of annual plants and fossil fuel derived CO_2 distribution across different regions of China (Conference Paper)[J].Nuclear Instruments and Methods in Physics Research, Section B. Beam Interactions with Materials and Atoms,2013:515-519. |
| [41] | Wang, Wenwen;Pataki, Diane E. .Spatial patterns of plant isotope tracers in the Los Angeles urban region[J].Landscape Ecology,2010(1):35-52. |
| [42] | Park J H;Hong W;Park G et al.Comparison of Distribution Maps of Delta C-14 in 2010 and 2011 in Korea[J].RADIOCARBON,2013,55(2/3):841-847. |
| [43] | Ding P;Shen C D;Yi W X et al.Fossil-fuel-derived CO2 contribution to the urban atmosphere in Guangzhou,South China,estimated by (CO2)-C-14 Observation,2010-2011[J].RADIOCARBON,2013,55(2/3):791-803. |
| [44] | Zhou W J;Wu S G;Huo W W et al.Tracing fossil fuel CO2 using Delta C-14 in Xi′an City,China[J].Atmospheric Environment,2014,94:538-545. |
| [45] | Xi X T;Ding X F;Fu D P et al.Regional Delta C-14 patterns and fossil fuel derived CO2 distribution in the Beijing area using annual plants[J].Chinese Science Bulletin,2011,56(16):1721-1726. |
| [46] | Klinedinst D B;Currie L A .Direct quantification of PM2.5 fossil and biomass carbon within the Northern Front Range Air Quality Study′s domain[J].Environmental Science and Technology,1999,33(23):4146-4154. |
| [47] | Zencak Z;Elmquist M;Gustafsson O .Quantification and radiocarbon source apportionment of black carbon in atmospheric aerosols using the CTO-375 method[J].Atmospheric environment,2007(36):7895-7906. |
| [48] | Southon J .Are the fractionation corrections correct:Are the isotopic shifts for C-14/C-12 ratios in physical processes and chemical reactions really twice those for C-13/C-12[J].RADIOCARBON,2011,53(4):691-704. |
| [49] | Zdenek Zencak;Christopher M. Reddy;Emma L. Teuten;Li Xu;Ann P. McNichol;Orjan Gustafsson .Evaluation of Gas Chromatographic Isotope Fractionation and Process Contamination by Carbon in Compound-Specific Radiocarbon Analysis[J].Analytical chemistry,2007(5):2042-2049. |
| [50] | Eglinton TI;Aluwihare LI;Bauer JE;Druffel ERM;Mcnichol AP .GAS CHROMATOGRAPHIC ISOLATION OF INDIVIDUAL COMPOUNDS FROM COMPLEX MATRICES FOR RADIOCARBON DATING[J].Analytical chemistry,1996(5):904-912. |
| [51] | Slater GF;White HK;Eglinton TI;Reddy CM .Determination of microbial carbon sources in petroleum contaminated sediments using molecular C-14 analysis[J].Environmental Science & Technology: ES&T,2005(8):2552-2558. |
| [52] | Teuten E L;Xu L;Reddy C M .Two abundant bioaccumulated halogenated compounds are natural products[J].SCIENCE,2005,307(5711):917-920. |
| [53] | ANITRA E. INGALLS;ANN PEARSON .Ten; Years of Compound-Specific Radiocarbon Analysis[J].Oceanography,2005(3):18-31. |
| [54] | 赵美训,于蒙,张海龙,陶舒琴.单体分子放射性碳同位素分析在海洋科学及环境科学研究中的应用[J].海洋学报（中文版）,2014(04):1-10. |
| [55] | Synal, H.-A..Developments in accelerator mass spectrometry[J].International journal of mass spectrometry,2013:192-202. |
| [56] | Jimmy Flarakos;Rosa G. Liberman;Steven R. Tannenbaum;Paul L. Skipper .Integration of Continuous-Flow Accelerator Mass Spectrometry with Chromatography and Mass-Selective Detection[J].Analytical chemistry,2008(13):5079-5085. |
| [57] | McIntyre C P;Galutschek E;Roberts M L et al.A continuous-flow gas chromatography C-14 accelerator mass spectrometry system[J].RADIOCARBON,2010,52(2):295-300. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%