氯化石蜡产品中短链和中链同系物的指纹分布
|
摘要
使用气相色谱-电子捕获负化学电离质谱(GC-ECNI-MS),对包含CP-42、CP-52和CP-70三种常见氯含量的22个CPs产品进行了测定,分析了不同氯含量的CPs产品中短链氯化石蜡(SCCPs)和中链氯化石蜡(MCCPs)同系物的分布模式.SCCPs同系物呈现5种分布特征,分别是CP-42型、三类CP-52型和CP-70型,MCCPs同系物呈现4种分布特征,分别是CP-42型和三类CP-52型,CP-70产品中MCCPs同系物未呈现出一致的分布规律.CPs生产原料石蜡中烷烃的成分组成和CPs生产工艺的不同,是造成产品同系物分布模式不一致的原因.通过统计学分析,得到CPs产品中SCCPs和MCCPs同系物的指纹分布,这是开展环境中CPs的源解析、迁移转化、归趋和毒性风险评价等研究的有利工具.
Twenty-two CP products with three chlorine contents(CP-42, CP-52, and CP-70) were determined using gas chromatography coupled with electron capture negative ionization mass spectrometry(GC-ECNI-MS), and the distribution patterns of short chain chlorinated paraffin(SCCP) and medium chain chlorinated paraffin(MCCP) homologues were explored. Five classes of distribution patterns, namely, CP-42 type, three CP-52 types, and CP-70 type were found for SCCP homologues. And four classes of distribution patterns, namely, CP-42 type and three CP-52 types were found for MCCP homologues. MCCP homologues in CP-70 products did not show consistent pattern. The reason for distinct homologue patterns in CP products could be attributed to different composition of alkane in paraffin(raw material) and production process. The fingerprint patterns of SCCP and MCCP homologues in CP products were characterized via statistical analysis, which can be useful tools for studies of source identification, migration and transformation, fate, toxicity risk assessment of CPs in the environment.
Twenty-two CP products with three chlorine contents(CP-42, CP-52, and CP-70) were determined using gas chromatography coupled with electron capture negative ionization mass spectrometry(GC-ECNI-MS), and the distribution patterns of short chain chlorinated paraffin(SCCP) and medium chain chlorinated paraffin(MCCP) homologues were explored. Five classes of distribution patterns, namely, CP-42 type, three CP-52 types, and CP-70 type were found for SCCP homologues. And four classes of distribution patterns, namely, CP-42 type and three CP-52 types were found for MCCP homologues. MCCP homologues in CP-70 products did not show consistent pattern. The reason for distinct homologue patterns in CP products could be attributed to different composition of alkane in paraffin(raw material) and production process. The fingerprint patterns of SCCP and MCCP homologues in CP products were characterized via statistical analysis, which can be useful tools for studies of source identification, migration and transformation, fate, toxicity risk assessment of CPs in the environment.
引文
[1]Pellizzato F,Ricci M,Held A,et al.Analysis of short-chain chlorinated paraffins:a discussion paper[J].Journal of Environmental Monitoring,2007,9(9):924-930.
[2]Shojania S.The enumeration of isomeric structures for polychlorinated n-alkanes[J].Chemosphere,1999,38(9):2125-2141.
[3]Bayen S,Obbard J P,Thomas G O.Chlorinated paraffins:A review of analysis and environmental occurrence[J].Environment International,2006,32(7):915-929.
[4]张海军,高媛,马新东等.短链氯化石蜡(SCCPs)的分析方法、环境行为及毒性效应研究进展[J].中国科学:化学,2013,43(3):255-264.Zhang H J,Gao Y,Ma X D,et al.Research advances in analytical methods,environmental behaviors and toxic effects of short chain chlorinated paraffins(SCCPs)[J].SCENTIA SINICA Chinica,2013,43(3):255-264.
[5]UNEP.Eighth meeting of the conference of the parties to the stockholm convention[EB/OL].http://www.pops.int/TheConvention/ConferenceoftheParties/Meetings/COP8/tabid/5309/Default.aspx/2017-07-03.
[6]唐恩涛,姚丽芹.氯化石蜡行业现状及发展趋势[J].中国氯碱,2005,2:1-3.Tang E T,Yao L Q.Industry Status of chlorinated paraffin and its development trends[J].China Chlor-Alkali,2005,2:1-3.
[7]Randegger-Vollrath A.Determination of chlorinated paraffins in cutting fluids and lubricants[J].Fresenius Journal of Analytical Chemistry,1998,360(1):62-68.
[8]Castells P,Santos F J,Galceran M T.Evaluation of three ionisation modes for the analysis of chlorinated paraffins by gas chromatography/ion-trap mass spectrometry[J].Rapid Communications in Mass Spectrometry,2004,18(5):529-536.
[9]Zencak Z,Reth M,Oehme M.Determination of total polychlorinated n-alkane concentration in biota by electron ionization-MS/MS[J].Analytical Chemistry,2004,76(7):1957-1962.
[10]Gj?s N,Gustavsen K O.Determination of chlorinated paraffins by negative ion chemical ionization mass spectrometry[J].Analytical Chemistry,1982,54(8):1316-1318.
[11]Wang Y,Li J,Cheng Z,et al.Short-and medium-chain chlorinated paraffins in air and soil of subtropical terrestrial environment in the Pearl River Delta,South China:Distribution,composition,atmospheric deposition fluxes,and environmental fate[J].Environmental Science&Technology,2013,47(6):2679-2687.
[12]Zeng L,Zhao Z,Li H,et al.Distribution of short chain chlorinated paraffins in marine sediments of the East China Sea:Influencing factors,transport and implications[J].Environmental Science&Technology,2012,46(18):9898-9906.
[13]Gao Y,Zhang H,Su F,et al.Environmental occurrence and distribution of short chain chlorinated paraffins in sediments and soils from the Liaohe River Basin,P.R.China[J].Environmental Science&Technology,2012,46(7):3771-3778.
[14]Tomy G T,Stern G A,Muir D C G,et al.Quantifying C10-C13polychloroalkanes in environmental samples by high-resolution gas chromatography/electron capture negative ion high-resolution mass spectrometry[J].Analytical Chemistry,1997,69(14):2762-2771.
[15]Tomy G T,Stern G A.Analysis of C14-C17polychloro-n-alkanes in environmental matrixes by accelerated solvent extraction-highresolution gas chromatography/electron capture negative ion highresolution mass spectrometry[J].Analytical Chemistry,1999,71(21):4860-4865.
[16]Gao W,Wu J,Wang Y,et al.Quantification of short-and medium-chain chlorinated paraffins in environmental samples by gas chromatography quadrupole time-of-flight mass spectrometry[J].Journal of Chromatography A,2016,1452:98-106.
[17]Korytár P,Parera J,Leonards P E G,et al.Characterization of polychlorinated n-alkanes using comprehensive two-dimensional gas chromatography-electron-capture negative ionisation time-of-flight mass spectrometry[J].Journal of Chromatography A,2005,1086(1):71-82.
[18]Xia D,Gao L,Zheng M,et al.A novel method for profiling and quantifying short-and medium-chain chlorinated paraffins in environmental samples using comprehensive two-dimensional gas chromatography-electron capture negative ionization high-resolution time-of-flight mass spectrometry[J].Environmental Science&Technology,2016,50(14):7601-7609.
[19]Li T,Gao S,Ben Y,et al.Screening of chlorinated paraffins and unsaturated analogues in commercial mixtures:Confirmation of their occurrences in the atmosphere[J].Environmental Science Technology,2018,52(4):1862-1870.
[2]Shojania S.The enumeration of isomeric structures for polychlorinated n-alkanes[J].Chemosphere,1999,38(9):2125-2141.
[3]Bayen S,Obbard J P,Thomas G O.Chlorinated paraffins:A review of analysis and environmental occurrence[J].Environment International,2006,32(7):915-929.
[4]张海军,高媛,马新东等.短链氯化石蜡(SCCPs)的分析方法、环境行为及毒性效应研究进展[J].中国科学:化学,2013,43(3):255-264.Zhang H J,Gao Y,Ma X D,et al.Research advances in analytical methods,environmental behaviors and toxic effects of short chain chlorinated paraffins(SCCPs)[J].SCENTIA SINICA Chinica,2013,43(3):255-264.
[5]UNEP.Eighth meeting of the conference of the parties to the stockholm convention[EB/OL].http://www.pops.int/TheConvention/ConferenceoftheParties/Meetings/COP8/tabid/5309/Default.aspx/2017-07-03.
[6]唐恩涛,姚丽芹.氯化石蜡行业现状及发展趋势[J].中国氯碱,2005,2:1-3.Tang E T,Yao L Q.Industry Status of chlorinated paraffin and its development trends[J].China Chlor-Alkali,2005,2:1-3.
[7]Randegger-Vollrath A.Determination of chlorinated paraffins in cutting fluids and lubricants[J].Fresenius Journal of Analytical Chemistry,1998,360(1):62-68.
[8]Castells P,Santos F J,Galceran M T.Evaluation of three ionisation modes for the analysis of chlorinated paraffins by gas chromatography/ion-trap mass spectrometry[J].Rapid Communications in Mass Spectrometry,2004,18(5):529-536.
[9]Zencak Z,Reth M,Oehme M.Determination of total polychlorinated n-alkane concentration in biota by electron ionization-MS/MS[J].Analytical Chemistry,2004,76(7):1957-1962.
[10]Gj?s N,Gustavsen K O.Determination of chlorinated paraffins by negative ion chemical ionization mass spectrometry[J].Analytical Chemistry,1982,54(8):1316-1318.
[11]Wang Y,Li J,Cheng Z,et al.Short-and medium-chain chlorinated paraffins in air and soil of subtropical terrestrial environment in the Pearl River Delta,South China:Distribution,composition,atmospheric deposition fluxes,and environmental fate[J].Environmental Science&Technology,2013,47(6):2679-2687.
[12]Zeng L,Zhao Z,Li H,et al.Distribution of short chain chlorinated paraffins in marine sediments of the East China Sea:Influencing factors,transport and implications[J].Environmental Science&Technology,2012,46(18):9898-9906.
[13]Gao Y,Zhang H,Su F,et al.Environmental occurrence and distribution of short chain chlorinated paraffins in sediments and soils from the Liaohe River Basin,P.R.China[J].Environmental Science&Technology,2012,46(7):3771-3778.
[14]Tomy G T,Stern G A,Muir D C G,et al.Quantifying C10-C13polychloroalkanes in environmental samples by high-resolution gas chromatography/electron capture negative ion high-resolution mass spectrometry[J].Analytical Chemistry,1997,69(14):2762-2771.
[15]Tomy G T,Stern G A.Analysis of C14-C17polychloro-n-alkanes in environmental matrixes by accelerated solvent extraction-highresolution gas chromatography/electron capture negative ion highresolution mass spectrometry[J].Analytical Chemistry,1999,71(21):4860-4865.
[16]Gao W,Wu J,Wang Y,et al.Quantification of short-and medium-chain chlorinated paraffins in environmental samples by gas chromatography quadrupole time-of-flight mass spectrometry[J].Journal of Chromatography A,2016,1452:98-106.
[17]Korytár P,Parera J,Leonards P E G,et al.Characterization of polychlorinated n-alkanes using comprehensive two-dimensional gas chromatography-electron-capture negative ionisation time-of-flight mass spectrometry[J].Journal of Chromatography A,2005,1086(1):71-82.
[18]Xia D,Gao L,Zheng M,et al.A novel method for profiling and quantifying short-and medium-chain chlorinated paraffins in environmental samples using comprehensive two-dimensional gas chromatography-electron capture negative ionization high-resolution time-of-flight mass spectrometry[J].Environmental Science&Technology,2016,50(14):7601-7609.
[19]Li T,Gao S,Ben Y,et al.Screening of chlorinated paraffins and unsaturated analogues in commercial mixtures:Confirmation of their occurrences in the atmosphere[J].Environmental Science Technology,2018,52(4):1862-1870.