天然含放矿物的水热蚀变研究进展
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摘要
矿物固化体作为第二代高放废物固化体,具有良好的热稳定性、化学稳定性以及辐照稳定性。然而,目前用于化学稳定性研究的矿物固化体,很少含有放射性核素,或者没有积累足够的辐照损伤缺陷,所以很难反应固化体在真实地质处置库中的行为,并且在实验室研究中,也难以长期(1×10~4～10×10~4年)模拟HLW处置库中的物理化学条件。而自然界中的一些含放射性核素的矿物,经过百万年甚至上亿年的地质作用后,仍然保持着稳定的成分和形态。这些天然矿物因自辐照作用而在结构上与含放矿物固化体具有相似性,本文比较了天然矿物与HLW固化体水热蚀变的异同,并通过大量文献调研总结了天然矿物水热蚀变的现状,以为矿物固化体长期化学稳定性的研究提供科学依据和评估数据。
As the second-generation candidate materials for immobilizing high level radioactive-wastes(HLW), mineral hosts have good thermal stability, chemical stability and irradiation stability. However, as most mineral hosts which were currently used to study their chemical stabilities contain little radionuclides, or inadequately accumulated irradiation damage defects, they can hardly to reflect the real behavior of radioactive-waste hosts in geological disposal facilities(GDF). In addition, it is very difficult to simulate the long-term(10 000-100 000 years) physical and chemical conditions of the GDF for dealing with the HLW in the laboratory. Some natural radionuclide-bearing minerals still maintain stable compositions and crystal forms after millions even billions of years of geological processes. Their structures due to the self-irradiation are similar to those of the radionuclide-bearing mineral hosts. In this paper, a comparative study has been carried out on the similarities and differences of hydrothermal alteration between the natural minerals and HLW hosts, on the basis of reviews of the research status of the hydrothermal alteration of natural minerals through a large number of literature investigation, in order to provide scientific basis and evaluation data for researches on the long-term chemical stability of the HLW mineral hosts.
As the second-generation candidate materials for immobilizing high level radioactive-wastes(HLW), mineral hosts have good thermal stability, chemical stability and irradiation stability. However, as most mineral hosts which were currently used to study their chemical stabilities contain little radionuclides, or inadequately accumulated irradiation damage defects, they can hardly to reflect the real behavior of radioactive-waste hosts in geological disposal facilities(GDF). In addition, it is very difficult to simulate the long-term(10 000-100 000 years) physical and chemical conditions of the GDF for dealing with the HLW in the laboratory. Some natural radionuclide-bearing minerals still maintain stable compositions and crystal forms after millions even billions of years of geological processes. Their structures due to the self-irradiation are similar to those of the radionuclide-bearing mineral hosts. In this paper, a comparative study has been carried out on the similarities and differences of hydrothermal alteration between the natural minerals and HLW hosts, on the basis of reviews of the research status of the hydrothermal alteration of natural minerals through a large number of literature investigation, in order to provide scientific basis and evaluation data for researches on the long-term chemical stability of the HLW mineral hosts.
引文
[1]罗上庚.放射性废物处理与处置[M].环境科学出版社,2007.
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[3]盛嘉伟,罗上庚,汤宝龙.高放废液的玻璃固化及固化体的浸出行为与发展情况[J].硅酸盐学报,1997(1):83-88.
[4]梁栋,刘伟,杨仲田,等.γ辐照对改性钠基膨润土影响的初步研究[J].矿物学报,2015,35(1):103-106.
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[6]ICENHOWER JP,STRACHAN DM,LINDBERG MJ,et al.Dissolution Kinetics of Titanate-Based Ceramic Waste Forms:Results from Single-Pass Flow Tests on Radiation Damaged Specimens[R].2003.
[7]MITAMURA H,MATSUMOTO S,STEWART M W A,et al.α-Decay Damage Effects in Curium‐Doped Titanate Ceramic Containing Sodium‐Free High‐Level Nuclear Waste[J].J Am Ceram Soc,1994,77(9):2255-2264.
[8]董发勤,张宝述,卢喜瑞,等.含An(3+),(4+)放射性废物的矿物固化研究[J].矿物学报,2012,32(S1):11-12.
[9]RINGWOOD AE,KESSON SE,WARE NG,et al.Immobilisation of high level nuclear reactor wastes in synroc[J].Nature,1979,278(5701):219-223.
[10]惠小朝,李子颖,冯张生,等.陕西华阳川铀多金属矿床铀赋存状态研究[J].矿物学报,2014,34(4):573-580.
[11]谭盛恒,叶瑛.微波合成掺铝羟基磷灰石及其对Co 2+的吸附作用[J].矿物学报,2010,30(S1):185-186.
[12]李国武,杨光明,熊明.烧绿石超族矿物分类新方案及烧绿石超族矿物[J].矿物学报,2014,34(2):153-158.
[13]EWING RC.Nuclear waste forms for actinides.[J].Proc Natl Acad Sci U S A,1999,96(7):3432-3439.
[14]MURAKAMI T,CHAKOUMAKOS BC,EWING RC,et al.Alpha-Decay Event Damage in Zircon[J].Am.Mineral.,1991,76:9-10(9):1510-1532.
[15]陈宣华,董树文,史静.地质年代学发展历史的简要回顾及前景[J].世界地质,2009,28(3):384-396.
[16]章荣清,孙卫东,Bernd,等.锡石LA-ICP-MSU-Pb定年在稀有金属矿床研究中的应用[J].矿物学报,2015,35(s1):368.
[17]范晨子,胡明月,赵令浩,等.锆石铀-铅定年激光剥蚀-电感耦合等离子体质谱原位微区分析进展[J].岩矿测试,2012,31(1):29-46.
[18]GREENWOOD HJ.An Introduction to the Rock Forming Minerals by W.A.Deer[M].Longman Scientific&Technical,1992:509-517.
[19]RIZVANOVA NG,LEVCHENKOV OA,BELOUS AE,et al.Zircon reaction and stability of the u-pb isotope system during interaction with carbonate fluid:experimental hydrothermal study[J].Contributions to Mineralogy and Petrology,2000,139(1):101-114.
[20]RIZVANOVA NG,LEVCHENKOV OA,BELOUS AE,et al.The dynamics of the interaction of zircon with hydrothermal carbonate fluid[J].Geochemistry International,1996,34(3):226-235.
[21]RIZVANOVA NG,GAIDAMAKO IM,LEVCHENKOV OA,et al.Interaction of metamict zircon with fluids of various composition[J].Geochemistry International,2007,45(5):465-477.
[22]PIDGEON RT,O'NEIL JR,SILVER LT.Uranium and lead isotopic stability in a metamict zircon under experimental hydrothermal conditions[J].Science,1966,154(3756):1538-1540.
[23]TOLE MP.The kinetics of dissolution of zircon(ZrSiO4)[J].Geochim.Cosmochim.Acta,1985,49(2):453-458.
[24]SINHA AK,WAYNE DM,HEWITT DA.The hydrothermal stability of zircon:preliminary experimental and isotopic studies[J].Geochim.Cosmochim.Acta,1992,56(9):3551-3560.
[25]TROCELLIER P,DELMAS R.Chemical durability of zircon[J].Nuclear Inst.and Methods in Physics Research,B,2001,181(1):408-412.
[26]中华人民共和国核行业标准.放射性废物体和废物包的特性鉴定.2005.
[27]GEISLER T,ZHANG M,SALJE EKH.Recrystallization of almost fully amorphous zircon under hydrothermal conditions:an infrared spectroscopic study[J].J Nucl Mater,2003,320(3):280-291.
[28]HAYWARD PJ,CECCHETTO EV.Development of sphene-based glass ceramics tailored for canadian waste disposal conditions[J].Mrs Proceedings,1981,6.
[29]BANCROFT GM,METSON JB,KRESOVIC RA,et al.Leaching studies of natural and synthetic titanites using secondary ion mass spectrometry[J].Geochim Cosmochim Acta,1987,51(4):911-918.
[30]AUDUBERT F,CARPENA J,LACOUT JL,et al.Elaboration of an iodine-bearing apatite iodine diffusion into a Pb3(VO4)2 matrix[J].Solid State Ionics,1997,95(1):113-119.
[31]K?HLER SJ,HAROUIYA N,CHA?RAT C,et al.Experimental studies of REE fractionation during water-mineral interactions:REE release rates during apatite dissolution from pH 2.8 to 9.2[J].Chem Geol,2005,222(3/4):168-182.
[32]ZHANG M,MADDRELL ER,ABRAITIS PK,et al.Impact of leach on lead vanado-iodoapatite[Pb5(VO4)3I]:an infrared and raman spectroscopic study[J].Materials Science and Engineering B,2007,137(1-3):149-155.
[33]OELKERS EH,POITRASSON F.An experimental study of the dissolution stoichiometry and rates of a natural monazite as a function of temperature from 50 to 230°C and pH from 1.5 to 10[J].Chem Geol,2002,191(1/2/3):73-87.
[34]POITRASSON F,CHENERY S,SHEPHERD T J.Electron microprobe and LA-ICP-MS study of monazite hydrothermal alteration::Implications for U-Th-Pb geochronology and nuclear ceramics[J].Geochimica Et Cosmochimica Acta,2000,64(19):3283-3297.
[35]LUMPKIN GR.Alpha-decay damage and aqueous durability of actinide host phases in natural systems[J].J Nucl Mater,2001,289(1/2):136-166.
[36]GEISLER T,P?ML P,STEPHAN T,et al.Letter:experimental observation of an interface-controlled pseudomorphic replacement reaction in a natural crystalline pyrochlore[J].American Mineralogist,2005,90(10):1683-1687.
[37]RYZHENKO BN,KOVALENKO NI,PRISYAGINA NI,et al.Experimental determination of zirconium speciation in hydrothermal solutions[J].Geochemistry International,2008,46(4):328-339.
[38]KORZHINSKAYA VS,NEKRASOV IY.Stability of the association ZrSiO4-SiO2-ZrO2 in alkali solutions at temperature 500 degrees C and pressure 1 kbar[J].Doklady Akademii nauk/[Rossi?skaia akademii nauk],1998,359(2):205-207.
[39]KOVALENKO NI,RYZHENKO BN.Comparative study of the solubility of zircon and baddeleyite[J].Geochemistry International,2009,47(4):405-413.
[40]KORZHINSKAYA V S.Effect of physico-chemical conditions on pyrochlore solubility in fluoride solutions at t=300-550℃and p=500-1000bar[J].Vestnik Otdelenia nauk o Zemle RAN,2012,4.
[41]RINGWOOD AE,OVERSBY VM,KESSON SE,et al.Immobilization of high-level nuclear reactor wastes in synroc:a current appraisal[J].MRSOnline Proceedings Library,1981,6:16-19.
[42]GUY C,AUDUBERT F,LARTIGUE JE,et al.New conditionings for separated long-lived radionuclides[J].Comptes Rendus Physique,2002,3(7):827-837.
[43]TSVETKOV VI,IVANOV IA,NECHAEV AF.Diffusion of some critical radionuclides in mineral-like ceramic materials[J].Radiochemistry,2016,58(5):532-537.
[44]GEISLER T,SCHALTEGGER U,TOMASCHEK F.Re-equilibration of zircon in aqueous fluids and melts[J].Elements,2007,3(1):43-50.
[45]EWING RC,HAAKER RF,LUTZE W.Leachability of zircon as a function of alpha dose[J].MRS Online Proceedings Library,1981,11.
[46]WEBER WJ,WALD JW,MATZKE H.Effects of self-radiation damage in cm-doped gd2ti2o7 and cazrti2o7[J].Journal of Nuclear Materials,1986,138(2-3):196-209.
[47]P?ML P,GEISLER T,COBOS-SABATéJ,et al.The mechanism of the hydrothermal alteration of cerium-and plutonium-doped zirconolite[J].Journal of Nuclear Materials,2011,410(1-3):10-23.
[48]STRACHAN DM,SCHEELE RD,BUCK EC,et al.Radiation damage effects in candidate titanates for pu disposition:pyrochlore[J].Journal of Nuclear Materials,2005,345(2-3):109-135.
[49]FENG X,BATES JK,BUCK EC,et al.Long-term comparison of dissolution behavior between fully radioactive and simulated nuclear waste glasses[J].Nucl Technol,1993,104(104):193-206.
[50]FENG Xiangdong,BATES J K,BUCK E C,et al.Long-term comparison of dissolution behavior between fully radioactive and simulated nuclear waste glasses[J].Nuclear Technology,1993,104(2):193-206.
[51]CHêNE J,TROCELLIER P.Investigation of alkali borosilicate glass durability using tritium tracing,β-autoradiography,scanning electron microscopy and ion beam analysis[J].J Non-Cryst Solids,2004,337(1):86-96.
[52]XU XS,ZHANG M,ZHU KY,et al.Reverse age zonation of zircon formed by metamictisation and hydrothermal fluid leaching[J].Lithos,2012,150(10):256-267.
[53]GEISLER,RASHWAN T,RAHN AA,et al.Low-temperature hydrothermal alteration of natural metamict zircons from the Eastern Desert,Egypt[J].Mineralogical Magazine,2003,67(3):485-508.
[2]陈璋如.类似物研究和矿物学问题[J].矿物学报,2001,21(3):71-74.
[3]盛嘉伟,罗上庚,汤宝龙.高放废液的玻璃固化及固化体的浸出行为与发展情况[J].硅酸盐学报,1997(1):83-88.
[4]梁栋,刘伟,杨仲田,等.γ辐照对改性钠基膨润土影响的初步研究[J].矿物学报,2015,35(1):103-106.
[5]BATES JK,BRADLEY JP,TEETSOV A,et al.Colloid formation during waste form reaction:implications for nuclear waste disposal[J].Science,1992,256(5057):649-51.
[6]ICENHOWER JP,STRACHAN DM,LINDBERG MJ,et al.Dissolution Kinetics of Titanate-Based Ceramic Waste Forms:Results from Single-Pass Flow Tests on Radiation Damaged Specimens[R].2003.
[7]MITAMURA H,MATSUMOTO S,STEWART M W A,et al.α-Decay Damage Effects in Curium‐Doped Titanate Ceramic Containing Sodium‐Free High‐Level Nuclear Waste[J].J Am Ceram Soc,1994,77(9):2255-2264.
[8]董发勤,张宝述,卢喜瑞,等.含An(3+),(4+)放射性废物的矿物固化研究[J].矿物学报,2012,32(S1):11-12.
[9]RINGWOOD AE,KESSON SE,WARE NG,et al.Immobilisation of high level nuclear reactor wastes in synroc[J].Nature,1979,278(5701):219-223.
[10]惠小朝,李子颖,冯张生,等.陕西华阳川铀多金属矿床铀赋存状态研究[J].矿物学报,2014,34(4):573-580.
[11]谭盛恒,叶瑛.微波合成掺铝羟基磷灰石及其对Co 2+的吸附作用[J].矿物学报,2010,30(S1):185-186.
[12]李国武,杨光明,熊明.烧绿石超族矿物分类新方案及烧绿石超族矿物[J].矿物学报,2014,34(2):153-158.
[13]EWING RC.Nuclear waste forms for actinides.[J].Proc Natl Acad Sci U S A,1999,96(7):3432-3439.
[14]MURAKAMI T,CHAKOUMAKOS BC,EWING RC,et al.Alpha-Decay Event Damage in Zircon[J].Am.Mineral.,1991,76:9-10(9):1510-1532.
[15]陈宣华,董树文,史静.地质年代学发展历史的简要回顾及前景[J].世界地质,2009,28(3):384-396.
[16]章荣清,孙卫东,Bernd,等.锡石LA-ICP-MSU-Pb定年在稀有金属矿床研究中的应用[J].矿物学报,2015,35(s1):368.
[17]范晨子,胡明月,赵令浩,等.锆石铀-铅定年激光剥蚀-电感耦合等离子体质谱原位微区分析进展[J].岩矿测试,2012,31(1):29-46.
[18]GREENWOOD HJ.An Introduction to the Rock Forming Minerals by W.A.Deer[M].Longman Scientific&Technical,1992:509-517.
[19]RIZVANOVA NG,LEVCHENKOV OA,BELOUS AE,et al.Zircon reaction and stability of the u-pb isotope system during interaction with carbonate fluid:experimental hydrothermal study[J].Contributions to Mineralogy and Petrology,2000,139(1):101-114.
[20]RIZVANOVA NG,LEVCHENKOV OA,BELOUS AE,et al.The dynamics of the interaction of zircon with hydrothermal carbonate fluid[J].Geochemistry International,1996,34(3):226-235.
[21]RIZVANOVA NG,GAIDAMAKO IM,LEVCHENKOV OA,et al.Interaction of metamict zircon with fluids of various composition[J].Geochemistry International,2007,45(5):465-477.
[22]PIDGEON RT,O'NEIL JR,SILVER LT.Uranium and lead isotopic stability in a metamict zircon under experimental hydrothermal conditions[J].Science,1966,154(3756):1538-1540.
[23]TOLE MP.The kinetics of dissolution of zircon(ZrSiO4)[J].Geochim.Cosmochim.Acta,1985,49(2):453-458.
[24]SINHA AK,WAYNE DM,HEWITT DA.The hydrothermal stability of zircon:preliminary experimental and isotopic studies[J].Geochim.Cosmochim.Acta,1992,56(9):3551-3560.
[25]TROCELLIER P,DELMAS R.Chemical durability of zircon[J].Nuclear Inst.and Methods in Physics Research,B,2001,181(1):408-412.
[26]中华人民共和国核行业标准.放射性废物体和废物包的特性鉴定.2005.
[27]GEISLER T,ZHANG M,SALJE EKH.Recrystallization of almost fully amorphous zircon under hydrothermal conditions:an infrared spectroscopic study[J].J Nucl Mater,2003,320(3):280-291.
[28]HAYWARD PJ,CECCHETTO EV.Development of sphene-based glass ceramics tailored for canadian waste disposal conditions[J].Mrs Proceedings,1981,6.
[29]BANCROFT GM,METSON JB,KRESOVIC RA,et al.Leaching studies of natural and synthetic titanites using secondary ion mass spectrometry[J].Geochim Cosmochim Acta,1987,51(4):911-918.
[30]AUDUBERT F,CARPENA J,LACOUT JL,et al.Elaboration of an iodine-bearing apatite iodine diffusion into a Pb3(VO4)2 matrix[J].Solid State Ionics,1997,95(1):113-119.
[31]K?HLER SJ,HAROUIYA N,CHA?RAT C,et al.Experimental studies of REE fractionation during water-mineral interactions:REE release rates during apatite dissolution from pH 2.8 to 9.2[J].Chem Geol,2005,222(3/4):168-182.
[32]ZHANG M,MADDRELL ER,ABRAITIS PK,et al.Impact of leach on lead vanado-iodoapatite[Pb5(VO4)3I]:an infrared and raman spectroscopic study[J].Materials Science and Engineering B,2007,137(1-3):149-155.
[33]OELKERS EH,POITRASSON F.An experimental study of the dissolution stoichiometry and rates of a natural monazite as a function of temperature from 50 to 230°C and pH from 1.5 to 10[J].Chem Geol,2002,191(1/2/3):73-87.
[34]POITRASSON F,CHENERY S,SHEPHERD T J.Electron microprobe and LA-ICP-MS study of monazite hydrothermal alteration::Implications for U-Th-Pb geochronology and nuclear ceramics[J].Geochimica Et Cosmochimica Acta,2000,64(19):3283-3297.
[35]LUMPKIN GR.Alpha-decay damage and aqueous durability of actinide host phases in natural systems[J].J Nucl Mater,2001,289(1/2):136-166.
[36]GEISLER T,P?ML P,STEPHAN T,et al.Letter:experimental observation of an interface-controlled pseudomorphic replacement reaction in a natural crystalline pyrochlore[J].American Mineralogist,2005,90(10):1683-1687.
[37]RYZHENKO BN,KOVALENKO NI,PRISYAGINA NI,et al.Experimental determination of zirconium speciation in hydrothermal solutions[J].Geochemistry International,2008,46(4):328-339.
[38]KORZHINSKAYA VS,NEKRASOV IY.Stability of the association ZrSiO4-SiO2-ZrO2 in alkali solutions at temperature 500 degrees C and pressure 1 kbar[J].Doklady Akademii nauk/[Rossi?skaia akademii nauk],1998,359(2):205-207.
[39]KOVALENKO NI,RYZHENKO BN.Comparative study of the solubility of zircon and baddeleyite[J].Geochemistry International,2009,47(4):405-413.
[40]KORZHINSKAYA V S.Effect of physico-chemical conditions on pyrochlore solubility in fluoride solutions at t=300-550℃and p=500-1000bar[J].Vestnik Otdelenia nauk o Zemle RAN,2012,4.
[41]RINGWOOD AE,OVERSBY VM,KESSON SE,et al.Immobilization of high-level nuclear reactor wastes in synroc:a current appraisal[J].MRSOnline Proceedings Library,1981,6:16-19.
[42]GUY C,AUDUBERT F,LARTIGUE JE,et al.New conditionings for separated long-lived radionuclides[J].Comptes Rendus Physique,2002,3(7):827-837.
[43]TSVETKOV VI,IVANOV IA,NECHAEV AF.Diffusion of some critical radionuclides in mineral-like ceramic materials[J].Radiochemistry,2016,58(5):532-537.
[44]GEISLER T,SCHALTEGGER U,TOMASCHEK F.Re-equilibration of zircon in aqueous fluids and melts[J].Elements,2007,3(1):43-50.
[45]EWING RC,HAAKER RF,LUTZE W.Leachability of zircon as a function of alpha dose[J].MRS Online Proceedings Library,1981,11.
[46]WEBER WJ,WALD JW,MATZKE H.Effects of self-radiation damage in cm-doped gd2ti2o7 and cazrti2o7[J].Journal of Nuclear Materials,1986,138(2-3):196-209.
[47]P?ML P,GEISLER T,COBOS-SABATéJ,et al.The mechanism of the hydrothermal alteration of cerium-and plutonium-doped zirconolite[J].Journal of Nuclear Materials,2011,410(1-3):10-23.
[48]STRACHAN DM,SCHEELE RD,BUCK EC,et al.Radiation damage effects in candidate titanates for pu disposition:pyrochlore[J].Journal of Nuclear Materials,2005,345(2-3):109-135.
[49]FENG X,BATES JK,BUCK EC,et al.Long-term comparison of dissolution behavior between fully radioactive and simulated nuclear waste glasses[J].Nucl Technol,1993,104(104):193-206.
[50]FENG Xiangdong,BATES J K,BUCK E C,et al.Long-term comparison of dissolution behavior between fully radioactive and simulated nuclear waste glasses[J].Nuclear Technology,1993,104(2):193-206.
[51]CHêNE J,TROCELLIER P.Investigation of alkali borosilicate glass durability using tritium tracing,β-autoradiography,scanning electron microscopy and ion beam analysis[J].J Non-Cryst Solids,2004,337(1):86-96.
[52]XU XS,ZHANG M,ZHU KY,et al.Reverse age zonation of zircon formed by metamictisation and hydrothermal fluid leaching[J].Lithos,2012,150(10):256-267.
[53]GEISLER,RASHWAN T,RAHN AA,et al.Low-temperature hydrothermal alteration of natural metamict zircons from the Eastern Desert,Egypt[J].Mineralogical Magazine,2003,67(3):485-508.