激光共振电离质谱用钚源的制备及探测效率测定
|
摘要
为提高激光共振电离质谱(LRIMS)中钚的原子化效率,设计制备了金属包覆钚源,以期提高LRIMS测量痕量钚的灵敏度。本工作设计加工了适用于痕量钚制源的电沉积装置,研究了水相中痕量钚的电沉积条件,实现了痕量钚的定量电沉积;对比研究了金属铂和钛的电镀条件及性能,确定了以钛为包覆层的真空蒸镀条件,实现了镀层厚度为1μm、金属钛包覆的高效钚源中钚的总沉积率达95%。研究表明,制备的高效钚源经过LRIMS测试,仪器对钚样品的总探测效率为2.5×10-4,原子化效率提高至7.7%,较直接滴加源提高3个数量级,为LRIMS法高灵敏测量环境中痕量钚奠定了基础。
To get higher atomization efficiency of Pu used for laser resonance ionization mass spectrometer(LRIMS)which can improve the sensitivity of trace Pu measured by mass spectrometry,Pu source covered with metal was made by electrodeposition.The quantitative electrodeposition of Pu was achieved by designing an electrodepositor and optimizing electrodeposition conditions.Compared with Pt coating,a Ti coating was prepared by vacuum evaporation,and the thickness of which is 1μm.The whole deposition rate of Pu is above 95%.The total detection efficiency of LRMIS for Pu is 2.5×10-4,and the atomization efficiency of Pu source coated by Ti is 7.7%,which are three orders of magnititude higher than direct drop source.This lays the foundation for analy-sis of trace amounts of Pu in the environment by LRIMS with high sensitivity.
To get higher atomization efficiency of Pu used for laser resonance ionization mass spectrometer(LRIMS)which can improve the sensitivity of trace Pu measured by mass spectrometry,Pu source covered with metal was made by electrodeposition.The quantitative electrodeposition of Pu was achieved by designing an electrodepositor and optimizing electrodeposition conditions.Compared with Pt coating,a Ti coating was prepared by vacuum evaporation,and the thickness of which is 1μm.The whole deposition rate of Pu is above 95%.The total detection efficiency of LRMIS for Pu is 2.5×10-4,and the atomization efficiency of Pu source coated by Ti is 7.7%,which are three orders of magnititude higher than direct drop source.This lays the foundation for analy-sis of trace amounts of Pu in the environment by LRIMS with high sensitivity.
引文
[1]PIBIDA L,NRTERSHUSER W,HUTCHINSON J M R,et al.Evaluation of resonance ionization mass spectrometry for the determination of135 Cs/137 Cs isotope ratios in low-level samples[J].Radiochim Acta,2001,89:161-168.
[2]M LLER P,BLAUM K,BUSHAW B A,et al.Trace detection of 41 Ca in nuclear reactor concrete by diode-laser-based resonance ionization mass spectrometry[J].Radiochim Acta,2000,88:487-493.
[3]WATANABE K,IGUCHI T,OGITA T,et al.Development of failed fuel detection and location technique using resonance ionization mass spectrometry[J].Journal of Nuclear Science and Technology,2001,38(10):844-849.
[4]邓中国,魏子章.提高热电离质谱灵敏度和防止放射性污染技术研究[J].质谱学报,1999,33(6):553-557.DENG Zhongguo,WEI Zizhang.Improvement sensibility and protection radioactivity contamination technique for TIMS[J].Journal of Chinese Mass Spectrometry Society,1999,33(6):553-557(in Chinese).
[5]KUNZ D,HUBER G,PASSLER G,et al.Resonance ionization mass spectrometry(RIMS)with pulsed and CW-lasers on plutonium[J].Hyperfine Interactions,2006,162:159-166.
[6]李志明,邓虎,朱凤蓉,等.三光子逐步激光共振电离质谱测定镥同位素比值[J].质谱学报,2002,23(3):156-159.LI Zhiming,DENG Hu,ZHU Fengrong,et al.Determination of lutetium isotopic ratio using three-photon stepwise resonance ionization mass spectrometry[J].Journal of Chinese Mass Spectrometry Society,2002,23(3):156-159(in Chinese).
[7]KARAM L R,PIBIDA L,MCMAHON C A.Use of resonance ionization mass spectrometry for determination of Cs ratios in solid samples[J].Applied Radiation and Isotopes,2002,56:369-374.
[8]RIEGEL J,DEIBENBERGER R,HERRMANN G,et al.Resonance ionization mass spectrometry for trace analysis of neptunium[J].Appl Phys B,1993,56:275-280.
[9]WENDELER H,DEISSENBERGER R,URBAN F J,et al.Electrolytic preparation of actinide filaments for laser resonance ionization spectroscopy[J].Nuclear Instruments and methods in Physics Research A,1993,334:93-95.
[10]邓中国.扩散型表面电离源及其在铀、钚和镎等元素质谱分析中的应用[J].原子能科学技术,1989,23(4):70-75.DENG Zhongguo.A surface ionization-diffusiontype ionization source and mass spectrometric measuring U,Pu,Np and other actinide elements by using IT[J].Atomic Energy Science and Technology,1989,23(4):70-75(in Chinese).
[11]张皓东,谢刚,李荣兴,等.钛、钽及铬熔融盐电镀的研究进展[J].科学技术与工程,2004,6(4):504-507.ZHANG Haodong,XIE Gang,LI Rongxing,et al.Research development of melt salt electroplate of rare metal[J].Science Technology and Engineering,2004,6(4):504-507(in Chinese).
[12]孙志华,刘佑厚,张晓云,等.钛及钛合金的电镀工艺评述[J].腐蚀与防护,2005,26(11):493-496.SUN Zhihua,LIU Youhou,ZHANG Xiaoyun,et al.A review of electroplating technology on titanium and titanium alloys[J].Corrosion&Protection,2005,26(11):493-496(in Chinese).
[13]陈泽民,张巧云,王艳霞,等.低碳钢表面铝-钛复合层的制备及其性能[J].材料保护,2011,44(9):71-75.CHEN Zemin,ZHANG Qiaoyun,WANG Yanxia,et al.Preparation of Al-Ti composite coating on the surface of low carbon steel and evaluation of performance of the coating[J].Journal of Materials Protection,2011,44(9):71-75(in Chinese).
[14]蔡积庆.电镀铂工艺[J].电镀与环保,1998,18(1):12-14.CAI Jiqing.Platinum plating process[J].Electroplating&Finishing,1998,18(1):12-14(in Chinese).
[15]李树棠,伍光浦.草酸-硝酸体系中铀、镎、钚、镅、锔的同时电沉积[J].辐射防护,1983,8(1):53-58.LI Shutang,WU Guangpu.Simultaneous electrodeposition of uranium,neptunium,plutonium,americium and curium in oxalic acid-nitric acid system[J].Radiation Protection,1983,8(1):53-58(in Chinese).
[16]贾瑞和,刘秉仁,梁俊福,等.电沉积法制备镅、钚和镎的α源[J].同位素,2000,13(3):135-141.JIA Ruihe,LIU Bingren,LIANG Junfu,et al.The preparation of alpha sources for plutonium,neptunium and americium by electrodeposition[J].Journal of Isotopes,2000,13(3):135-141(in Chinese).
[2]M LLER P,BLAUM K,BUSHAW B A,et al.Trace detection of 41 Ca in nuclear reactor concrete by diode-laser-based resonance ionization mass spectrometry[J].Radiochim Acta,2000,88:487-493.
[3]WATANABE K,IGUCHI T,OGITA T,et al.Development of failed fuel detection and location technique using resonance ionization mass spectrometry[J].Journal of Nuclear Science and Technology,2001,38(10):844-849.
[4]邓中国,魏子章.提高热电离质谱灵敏度和防止放射性污染技术研究[J].质谱学报,1999,33(6):553-557.DENG Zhongguo,WEI Zizhang.Improvement sensibility and protection radioactivity contamination technique for TIMS[J].Journal of Chinese Mass Spectrometry Society,1999,33(6):553-557(in Chinese).
[5]KUNZ D,HUBER G,PASSLER G,et al.Resonance ionization mass spectrometry(RIMS)with pulsed and CW-lasers on plutonium[J].Hyperfine Interactions,2006,162:159-166.
[6]李志明,邓虎,朱凤蓉,等.三光子逐步激光共振电离质谱测定镥同位素比值[J].质谱学报,2002,23(3):156-159.LI Zhiming,DENG Hu,ZHU Fengrong,et al.Determination of lutetium isotopic ratio using three-photon stepwise resonance ionization mass spectrometry[J].Journal of Chinese Mass Spectrometry Society,2002,23(3):156-159(in Chinese).
[7]KARAM L R,PIBIDA L,MCMAHON C A.Use of resonance ionization mass spectrometry for determination of Cs ratios in solid samples[J].Applied Radiation and Isotopes,2002,56:369-374.
[8]RIEGEL J,DEIBENBERGER R,HERRMANN G,et al.Resonance ionization mass spectrometry for trace analysis of neptunium[J].Appl Phys B,1993,56:275-280.
[9]WENDELER H,DEISSENBERGER R,URBAN F J,et al.Electrolytic preparation of actinide filaments for laser resonance ionization spectroscopy[J].Nuclear Instruments and methods in Physics Research A,1993,334:93-95.
[10]邓中国.扩散型表面电离源及其在铀、钚和镎等元素质谱分析中的应用[J].原子能科学技术,1989,23(4):70-75.DENG Zhongguo.A surface ionization-diffusiontype ionization source and mass spectrometric measuring U,Pu,Np and other actinide elements by using IT[J].Atomic Energy Science and Technology,1989,23(4):70-75(in Chinese).
[11]张皓东,谢刚,李荣兴,等.钛、钽及铬熔融盐电镀的研究进展[J].科学技术与工程,2004,6(4):504-507.ZHANG Haodong,XIE Gang,LI Rongxing,et al.Research development of melt salt electroplate of rare metal[J].Science Technology and Engineering,2004,6(4):504-507(in Chinese).
[12]孙志华,刘佑厚,张晓云,等.钛及钛合金的电镀工艺评述[J].腐蚀与防护,2005,26(11):493-496.SUN Zhihua,LIU Youhou,ZHANG Xiaoyun,et al.A review of electroplating technology on titanium and titanium alloys[J].Corrosion&Protection,2005,26(11):493-496(in Chinese).
[13]陈泽民,张巧云,王艳霞,等.低碳钢表面铝-钛复合层的制备及其性能[J].材料保护,2011,44(9):71-75.CHEN Zemin,ZHANG Qiaoyun,WANG Yanxia,et al.Preparation of Al-Ti composite coating on the surface of low carbon steel and evaluation of performance of the coating[J].Journal of Materials Protection,2011,44(9):71-75(in Chinese).
[14]蔡积庆.电镀铂工艺[J].电镀与环保,1998,18(1):12-14.CAI Jiqing.Platinum plating process[J].Electroplating&Finishing,1998,18(1):12-14(in Chinese).
[15]李树棠,伍光浦.草酸-硝酸体系中铀、镎、钚、镅、锔的同时电沉积[J].辐射防护,1983,8(1):53-58.LI Shutang,WU Guangpu.Simultaneous electrodeposition of uranium,neptunium,plutonium,americium and curium in oxalic acid-nitric acid system[J].Radiation Protection,1983,8(1):53-58(in Chinese).
[16]贾瑞和,刘秉仁,梁俊福,等.电沉积法制备镅、钚和镎的α源[J].同位素,2000,13(3):135-141.JIA Ruihe,LIU Bingren,LIANG Junfu,et al.The preparation of alpha sources for plutonium,neptunium and americium by electrodeposition[J].Journal of Isotopes,2000,13(3):135-141(in Chinese).