海水中~(131)I的快速检测技术
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摘要
日本福岛核事故发生以后,对海洋环境中关键放射性核素的快速检测技术提出了更高的要求。人工放射性核素~(131)I在核反应裂变产物中活度相对较高且半衰期短,是用来快速评价核污染的关键性核素之一。本工作从亚铁氰化钾、硝酸铜及硝酸银为原料出发,制备出亚铁氰化铜和亚铁氰化银混合(CuFC/AgFC)吸附材料并分散于聚丙烯纤维富集柱上,来实现水环境中~(131)I现场快速富集。通过室内模拟实验发现:在流速为6.25L/min,~(131)I在海水中I~-初始浓度为24μmol/L时,单次吸附效率即可达到50%以上;而当海水中I~-初始浓度为4μmol/L时,一定体积的海水在连续循环8次后(CuFC/AgFC)聚丙烯纤维富集柱吸附效率达到100%。本方法制源时间约40min,测样时间约12~24h,故最快可在30h内完成海水中~(131)I的分析。本方法的检测限与分析周期均低于目前GB/T 13272-1991水中~(131)I的分析标准,极大地提高了~(131)I的分析时间。除此之外,该法可以同时分析海水中的~(137) Cs(~(134) Cs),有望作为淡水和近岸环境中常规监测和应急时对关键核素~(131)I和~(137) Cs(~(134) Cs)进行快速测定的备选方法之一。
After the Fukushima nuclear accident,the rapid detection of critical radionuclides in the marine environment has been required.~(131)I,an artificial radionuclide released from nuclear reaction with high activity but very short half-life,is one of the critical nuclides for rapid assessment of nuclear contamination.In the present study,the compound of CuFC/AgFC were embedded on the polypropylene fiber column to study the enrichment of ~(131)I.The CuFC/AgFC enrichment column can adsorb iodine isotopes efficiently.These results show that within the flow rate of 6.25L/min,the sorption efficiency of ~(131)I by one cycle time of seawater can reach 50%when the initial concentration of I(as I~-form)is 24μmol/L.However,the sorption efficiency by eight cycles times of seawater can reach 100%even when the initial concentration of I(as I~-form)is 4μmol/L.It usually takes 40minutes to prepare the targets after the enrichment experient,and then 12-24hours for the ~(131)I analysis by HPGegamma spectrometry.Therefore,the method of ~(131)I in seawater in the present work can be completed in 30h,which significantly improves the analysis for ~(131)I.Both the detection limit and analysis time of this method in the present work are much lower than the current GB/T 13272-1991standard.Moreover,this method can detect ~(137)Cs(~(134)Cs)in seawater simultaneously,which is expected to be one of the alternative methods to rapidly detect ~(131)I and~(137)Cs(~(134)Cs)in freshwater/seawater nearshores for routine monitoring and also emergency cases.
After the Fukushima nuclear accident,the rapid detection of critical radionuclides in the marine environment has been required.~(131)I,an artificial radionuclide released from nuclear reaction with high activity but very short half-life,is one of the critical nuclides for rapid assessment of nuclear contamination.In the present study,the compound of CuFC/AgFC were embedded on the polypropylene fiber column to study the enrichment of ~(131)I.The CuFC/AgFC enrichment column can adsorb iodine isotopes efficiently.These results show that within the flow rate of 6.25L/min,the sorption efficiency of ~(131)I by one cycle time of seawater can reach 50%when the initial concentration of I(as I~-form)is 24μmol/L.However,the sorption efficiency by eight cycles times of seawater can reach 100%even when the initial concentration of I(as I~-form)is 4μmol/L.It usually takes 40minutes to prepare the targets after the enrichment experient,and then 12-24hours for the ~(131)I analysis by HPGegamma spectrometry.Therefore,the method of ~(131)I in seawater in the present work can be completed in 30h,which significantly improves the analysis for ~(131)I.Both the detection limit and analysis time of this method in the present work are much lower than the current GB/T 13272-1991standard.Moreover,this method can detect ~(137)Cs(~(134)Cs)in seawater simultaneously,which is expected to be one of the alternative methods to rapidly detect ~(131)I and~(137)Cs(~(134)Cs)in freshwater/seawater nearshores for routine monitoring and also emergency cases.
引文
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[4] Wang J L,Jiang Y F,Huang D K,et al.Promotion of the lower limit of detection of gamma emitting nuclides in radioaerosol samples after Fukushima accident[J].J Radioanal Nucl Chem,2012,292:1297-1301
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[10]Hou X L,Yan X J.Study on the concentration and seasonal variation of inorganic elements in 35species of marine algae[J].Science of the Total Environment,1998,222(3):141-156.
[11]Flynn W W.A rapid solvent extraction method for the determination of radio-iodine in sea water[J].Anal Chim Acta,1975,76(1):113-119.
[12]Couture R A,Seitz M G.Sorption of anions of iodine by iron oxides and kaolinite[J].Nucl Chem Waste Manag,1983,4(4):301-306.
[13]Fairman W D,Sediet J.A rapid and sensitive method for the determination of iodine-131in milk by ion exchange on silver chloride[J].Anal Chem,1966,38(9):1171-1175.
[14]GB/T 13272-1991水中碘-131的分析方法[S].北京:国家环境保护局,1991.
[15]Buesseler K,Casso S,Hartman M,et al.Determination of fission-products and actinides in the Black Sea following the Cherynobyl accident[J].J Radioanal Nucl Chem,1990,138(1):33-47.
[16]Zheleznov V V,Vysotskii V L.Application of fibrous carbon ferrocyanide sorbents for removing cesium and cobalt from large volumes of sea water[J].Atomic Energy,2002,92(6):493-500.
[17]Sharygin L M,Muromskii A Y.Inorganic sorbent for selective treatment of liquid radioactive wastes[J].Radiochem,2004,46(2):185-189.
[18]Baskaran M,Hong G H,Santschi P H.Radionuclide analysis in seawater[M]∥Practical Guidelines for the Analysis of Seawater.US:CRC Press,2009:259-304.
[19]何建华,陈立奇,门武,等.海水中137 Cs的快速富集与分析[J].台湾海峡,2011,30(4):280-285.
[20]Wang J L,Baskaran M,Niedermiller J.Mobility of137 Cs in freshwater lakes:a mass balance and diffusion study of Lake St.Clair,Southeast Michigan,USA[J].Geochim Cosmochim Acta,2017,218:323-342.
[21]张慧芳,高晓雷,郭探,等.单质碘、碘酸根和碘离子的吸附研究进展[J].核化学与放射化学,2011,33(3):129-135.
[22]刘国峰,郝存兴,肖思胤,等.放射性核素碘-131的吸附技术综述[C]∥公共安全中的化学问题研究进展.北京:中国化学会,2013.
[23]党爱翠,龙爱民,陈绍勇.海洋生态系统中碘的分布及形态转化[J].海洋湖沼通报,2012(4):146-154.
[24]李发美.分析化学[M].第六版.北京:人民卫生出版社,2007.
[25]Currie L A.Limits for qualitative detection and quantitative determination:application to radiochemistry[J].Anal Chem,1968,40(3):586-593.
[26]邓芳芳,林武辉,于涛,等.海洋沉积物中90Sr的分析方法[J].核化学与放射化学,2015,37(4):231-237.
[2] Oikawa S,Takata H,Watabe T,et al.Distribution of the Fukushima-derived radionuclides in seawater in the Pacific off the coast of Miyagi,Fukushima,and Ibaraki Prefectures,Japan[J].Biogeosciences,2013,10(7):5031-5047.
[3] Kryshev I I,Kryshev A I,Sazykina T G.Dynamics of radiation exposure to marine biota in the area of the Fukushima NPP in March-May 2011[J].J Environ Radioact,2012,114:157-161.
[4] Wang J L,Jiang Y F,Huang D K,et al.Promotion of the lower limit of detection of gamma emitting nuclides in radioaerosol samples after Fukushima accident[J].J Radioanal Nucl Chem,2012,292:1297-1301
[5]刘丹彤,王锦龙,毕倩倩,等.福岛核事故后上海气溶胶中131I、134 Cs和137 Cs的来源途径分析[J].核化学与放射化学,2017,39(1):103-112.
[6]陈彬,胡晓燕,邵亮,等.福岛核事故期间杭州地区雨水中131I监测[J].辐射防护通讯,2012,32(2):45-46.
[7] Scott R.Observations on the iodo-amino-acids of marine algae using iodine-131[J].Nature,1954,173(4414):1098-1099.
[8] Birks J L.Medical radionuclides in marine environment[J].Nature,1975,255(5510):621-622.
[9] Druehl L D,Cackette M,D′Auria J M.Geographical and temporal distribution of iodine-131in the brown seaweed Fucus subsequent to the Chernobyl incident[J].Marine Biology,1988,98(1):129-131.
[10]Hou X L,Yan X J.Study on the concentration and seasonal variation of inorganic elements in 35species of marine algae[J].Science of the Total Environment,1998,222(3):141-156.
[11]Flynn W W.A rapid solvent extraction method for the determination of radio-iodine in sea water[J].Anal Chim Acta,1975,76(1):113-119.
[12]Couture R A,Seitz M G.Sorption of anions of iodine by iron oxides and kaolinite[J].Nucl Chem Waste Manag,1983,4(4):301-306.
[13]Fairman W D,Sediet J.A rapid and sensitive method for the determination of iodine-131in milk by ion exchange on silver chloride[J].Anal Chem,1966,38(9):1171-1175.
[14]GB/T 13272-1991水中碘-131的分析方法[S].北京:国家环境保护局,1991.
[15]Buesseler K,Casso S,Hartman M,et al.Determination of fission-products and actinides in the Black Sea following the Cherynobyl accident[J].J Radioanal Nucl Chem,1990,138(1):33-47.
[16]Zheleznov V V,Vysotskii V L.Application of fibrous carbon ferrocyanide sorbents for removing cesium and cobalt from large volumes of sea water[J].Atomic Energy,2002,92(6):493-500.
[17]Sharygin L M,Muromskii A Y.Inorganic sorbent for selective treatment of liquid radioactive wastes[J].Radiochem,2004,46(2):185-189.
[18]Baskaran M,Hong G H,Santschi P H.Radionuclide analysis in seawater[M]∥Practical Guidelines for the Analysis of Seawater.US:CRC Press,2009:259-304.
[19]何建华,陈立奇,门武,等.海水中137 Cs的快速富集与分析[J].台湾海峡,2011,30(4):280-285.
[20]Wang J L,Baskaran M,Niedermiller J.Mobility of137 Cs in freshwater lakes:a mass balance and diffusion study of Lake St.Clair,Southeast Michigan,USA[J].Geochim Cosmochim Acta,2017,218:323-342.
[21]张慧芳,高晓雷,郭探,等.单质碘、碘酸根和碘离子的吸附研究进展[J].核化学与放射化学,2011,33(3):129-135.
[22]刘国峰,郝存兴,肖思胤,等.放射性核素碘-131的吸附技术综述[C]∥公共安全中的化学问题研究进展.北京:中国化学会,2013.
[23]党爱翠,龙爱民,陈绍勇.海洋生态系统中碘的分布及形态转化[J].海洋湖沼通报,2012(4):146-154.
[24]李发美.分析化学[M].第六版.北京:人民卫生出版社,2007.
[25]Currie L A.Limits for qualitative detection and quantitative determination:application to radiochemistry[J].Anal Chem,1968,40(3):586-593.
[26]邓芳芳,林武辉,于涛,等.海洋沉积物中90Sr的分析方法[J].核化学与放射化学,2015,37(4):231-237.