矿物固化核废物的研究进展
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摘要
进入21世纪以来,核废物的处置成为核能利用的一大难题。人造岩石和铁氧化物矿石因在高放废物固化研究中具有良好的性能,近年来被广泛研究。对常见的人造岩石和铁氧化物矿石固化体在含高放核素和模拟核素固化处理方面的进展进行了综述,主要包括其组分、固溶量、化学稳定性和理论计算等方面。与常见的玻璃、水泥固化体相比,人造岩石和铁氧化物矿石固化体在高放核素固化处置中具有明显的优势,是高放废物地质深埋处置的理想固化体。然而,人造岩石和铁氧化物矿石固化体仍处于研究开发阶段,尚未实际应用到放射性核环境中。
In the twenty-first Century,the nuclear waste has aroused a big problem despite of the advantage of nuclear energy. In recent years,artificial rock and iron oxide minerals have been widely studied for the disposal of nuclear waste due to their good performance for the solidification of high radioactive waste. In this work,the progressfocusing on the solidification of common artificial rocks,iron oxide minerals solidified in high radioactive nuclides,and analog nuclides,were presented in detail. The corresponding components,solid-soluted content,chemical stability and theoretical calculation were discussed. Comparing with the glass and cement solidified bodies,the artificial rocks and iron oxide minerals solidified bodies could show noticeable advantages for the high radioisotope solidification treatment. The ideal solidified bodies for deep disposal of high level radioactive waste were suggested. However,two kinds of solidified substrates were still at the stage of research and development and have not yet been applied to the radioactive nuclear environment. High efficient and convenient disposal of high level radioactive waste still face great challenges.
In the twenty-first Century,the nuclear waste has aroused a big problem despite of the advantage of nuclear energy. In recent years,artificial rock and iron oxide minerals have been widely studied for the disposal of nuclear waste due to their good performance for the solidification of high radioactive waste. In this work,the progressfocusing on the solidification of common artificial rocks,iron oxide minerals solidified in high radioactive nuclides,and analog nuclides,were presented in detail. The corresponding components,solid-soluted content,chemical stability and theoretical calculation were discussed. Comparing with the glass and cement solidified bodies,the artificial rocks and iron oxide minerals solidified bodies could show noticeable advantages for the high radioisotope solidification treatment. The ideal solidified bodies for deep disposal of high level radioactive waste were suggested. However,two kinds of solidified substrates were still at the stage of research and development and have not yet been applied to the radioactive nuclear environment. High efficient and convenient disposal of high level radioactive waste still face great challenges.
引文
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[24]王烈林,谢华,文清云,等.锕系核素烧绿石模拟固化体化学稳定性研究[J].西南科技大学学报,2015,30(3):25-30.
[25]谢华,唐敬友.Gd_(1.6)Nd_(0.4)Zr_2O_7烧绿石的快速合成及其组织结构研究[J].原子能科学技术,2012,46(4):390-395.
[26]Zhao P Z,LI,XU.Synthesis and Structural Transformations of(Gd(1–x)Cex)2Zr2O(7+x):An Analogue for Pu Immobilization[J].Acta Physico Chimica Sinica,2013,29(6):1168-1172.
[27]Smith F N,Um W,Taylor C D,et al.Computational I-nvestigation of Technetium(IV)Incorporation into Inverse Spin-els:Magnetite(Fe3O4)and Trevorite(Ni Fe2O4)[J].Environmental Science&Technology,2016,50(10):5216.
[28]Marshall T A,Morris K,Law G T,et al.Incorporation and retention of 99-Tc(IV)in magnetite under high p H conditi-ons.[J].Environmental Science&Technology,2014,48(20):11853-11862.
[29]Qi Z,Joshi T P,Liu R,et al.Synthesis of Ce(III)-dop-ed Fe3O4magnetic particles for efficient removal of antimony-from aqueoussolution[J].Journal of Hazardous Materials,2017(329):193-204.
[30]Huan W,Cheng C,Yang Y,et al.A study on the mag-netic and photoluminescence properties of Eun+and Sm3+doped Fe3O4nanoparticles[J].Journal of Nanoscience&Nanotechnolo-gy,2012,12(6):4621.
[31]Lastovina T A,Budnyk A P,Kudryavtsev E A,et al.S-olvothermal synthesis of Sm3+-doped Fe3O4nanoparticles[J].Ma-terials Science&Engineering,2017(C):110-116.
[32]Kumbhar A G,Kishorek,Venkateswaran G,et al.Dissol-ution of Ce,Zr and La containing magnetites and nickel ferrite in citric acid-EDTA-gallic acid formulation[J].Hydrometallurgy,2003,68(1):171-181.
[33]Kerisit S,Felmy A R,Ilton E S.Atomistic simulations of uranium incorporation into iron(hydr)oxides[J].Environment-al Science&Technology,2011,45(7):2770-2776.
[34]Frances N.Smith,Christopher D.Taylor,Wooyong Um,et al.Technetium Incorporation into Goethite(α-Fe OOH):An Atomic-Scale Investigation[J].Environmental Science&Technology,2015,49(22).
[35]Um W,Chang H,Icenhower J P,et al.Iron oxide wast-e form for stabilizing 99Tc[J].Journal of Nuclear Materials,2012,429(1-3):201-209.
[36]Um W,Chang H S,Icenhower J P,et al.Immobilizatio-n of 99-technetium(VII)by Fe(II)-goethite and limited reoxidation[J].Environmental Science&Technology,2011,45(11):4904-4913.
[37]Frances N.Skomurski,Kevin M.Rosso,Kenneth M.K-rupka,et al.Technetium Incorporation into Hematite(α-Fe2O3)[J].Environmental Science&Technology,2010,44(15):5855.
[38]Liu J,Pearce C I,Qafoku O,et al.Tc(VII)reduction-kinetics by titanomagnetite(Fe3-xTixO4)nanoparticles[J].Geochi-mica Et Cosmochimica Acta,2012,92(9):67-81.
[2]Navrotsky A,Mazeina L,Majzlan J.Size-driven structu-ral and thermodynamic complexity in iron oxides[J].Science,2008,319(5870):1635.
[3]Mc Beth,Lloyd J M,Law J R,et al.Redox interactionsof technetium with iron-bearing minerals[J].Mineralogical Mag-azine,2011,75(4):2419-2430.
[4]Duff M C,Coughlin J U,Hunter D B.Uranium co-pre-cipitation with iron oxide minerals[J].Geochimica Et Cosmochi-mica Acta,2002,66(20):3533-3547.
[5]Dodge C J,Francis A J,Gillow J B,et al.Association of uranium with iron oxides typically formed on corroding steelsurfaces[J].Environmental Science&Technology,2002,36(1-6):3504-3511.
[6]Frances N,Skomurski,Kevin M,Rosso,Kenneth M,K-rupka,et al.Technetium Incorporation into Hematite(α-Fe2O3)[J].Environmental Science&Technology,2010,44(15):5855.
[7]Skomurski F N,Ilton E S,Engelhard M H,et al.Hete-rogeneous reduction of U6+,by structural Fe2+,from theory andexperiment[J].Geochimica Et Cosmochimica Acta,2011,75(22):7277
[8]Luksic S A,Riley B J,Schweiger M,et al.Incorporati-ng technetium in minerals and other solids:A review[J].Journ-al of Nuclear Materials,2015(466):526-538.
[9]Hrma P,Crum J V,Bredt P R,et al.Vitrification and testing of a Hanford high-level waste sample.Part 2:Phase id-entification andwa-ste form leachability[J].Journal of Nuclear Materials,2005,345(1):31-40.
[10]Akatov A A,Nikonov B S,Omel’Yanenko B I,et al.Structure of borosilicate glassy materials with high concentratio-ns of sodium,iron,and aluminum oxides[J].Glass Physics&Chemistry,2009,35(3):245-259.
[11]Akatov A A,Nikonov B S,Omel Yanenko B I,et al.I-nfluence of the content of a surrogate of iron aluminate high l-evel wastes on the phase composition and structure of glassy-materials for their immobilization[J].Glass Physics&Chemistry,2010,36(1):45-52.
[12]罗上庚,杨建文.人造岩石固化包容锕系核素废物[J].化学学报,2000,58(12):1608-1614.
[13]Teng Y,Wu L,Ren X,et al.Synthesis and chemical d-urability of U-doped sphene ceramics[J].Journal of Nuclear M-aterials,2014,444(1-3):270-273.
[14]Zhang Y,Kong L,Aughterson R D,et al.Phase evolut-ion from Ln2Ti2O7(Ln=Y and Gd)pyrochlores to brannerites inglass withuranium incorporation[J].Journal of the American Ceramic Society,2017(100).
[15]张瑞珠,郭志猛,李燕.钛酸盐陶瓷固化放射性废物[J].硅酸盐通报,2005,24(4):16-19.
[16]Kutty K V G,Asuvathraman R,Madhavan R R,et al.Actinide immobilization in crystalline matrix:a study of uraniu-m incorporation in gadolinium zirconate[J].Journal of Physics&Chemistry of Solids,2005,66(2-4):596-601.
[17]赵发香.钛基陶瓷固化模拟核素铀的研究[D].绵阳:西南科技大学,2011.
[18]文冠军.自蔓延高温合成富钙钛锆石型人造岩石及其对模拟锕系核素固化性能研究[D].绵阳:西南科技大学,2016.
[19]段涛,卢喜瑞,刘小楠,等.Gd(2-x)NdxZr2O7(Nd=An(Ⅲ),0≤x≤2.0)模拟固化体固溶量与其物相、密度、硬度之间的关系[J].物理学报,2012,61(21):212801-212801.
[20]苏思瑾.模拟双核素放射性废物的钆锆烧绿石固化及稳定性研究[D].绵阳:西南科技大学,2015.
[21]Patwe S J,Tyagi A K.Solubility of Ce and Sr in the pyrochlore lattice of Gd Zr O for simulation of Pu and alkaline-earth metal[J].Ceramics International,2006,32(5):545-548.
[22]Shu X,Fan L,Lu X,et al.Structure and performance evolution of the system(Gd1–xNdx)2(Zr1–yCey)2O7(0≤x,y≤1.0)[J].Journal of the European Ceramic Society,2015,35(11):3095-3102.
[23]Xirui Lu,Dong F,Song G,et al.Phase and rietveld re-finement of pyrochlore Gd2Zr2O7,used for immobilization of Pu(IV)[J].Journal of Wuhan University of Technology-Mater,2014,29(2):233-236.
[24]王烈林,谢华,文清云,等.锕系核素烧绿石模拟固化体化学稳定性研究[J].西南科技大学学报,2015,30(3):25-30.
[25]谢华,唐敬友.Gd_(1.6)Nd_(0.4)Zr_2O_7烧绿石的快速合成及其组织结构研究[J].原子能科学技术,2012,46(4):390-395.
[26]Zhao P Z,LI,XU.Synthesis and Structural Transformations of(Gd(1–x)Cex)2Zr2O(7+x):An Analogue for Pu Immobilization[J].Acta Physico Chimica Sinica,2013,29(6):1168-1172.
[27]Smith F N,Um W,Taylor C D,et al.Computational I-nvestigation of Technetium(IV)Incorporation into Inverse Spin-els:Magnetite(Fe3O4)and Trevorite(Ni Fe2O4)[J].Environmental Science&Technology,2016,50(10):5216.
[28]Marshall T A,Morris K,Law G T,et al.Incorporation and retention of 99-Tc(IV)in magnetite under high p H conditi-ons.[J].Environmental Science&Technology,2014,48(20):11853-11862.
[29]Qi Z,Joshi T P,Liu R,et al.Synthesis of Ce(III)-dop-ed Fe3O4magnetic particles for efficient removal of antimony-from aqueoussolution[J].Journal of Hazardous Materials,2017(329):193-204.
[30]Huan W,Cheng C,Yang Y,et al.A study on the mag-netic and photoluminescence properties of Eun+and Sm3+doped Fe3O4nanoparticles[J].Journal of Nanoscience&Nanotechnolo-gy,2012,12(6):4621.
[31]Lastovina T A,Budnyk A P,Kudryavtsev E A,et al.S-olvothermal synthesis of Sm3+-doped Fe3O4nanoparticles[J].Ma-terials Science&Engineering,2017(C):110-116.
[32]Kumbhar A G,Kishorek,Venkateswaran G,et al.Dissol-ution of Ce,Zr and La containing magnetites and nickel ferrite in citric acid-EDTA-gallic acid formulation[J].Hydrometallurgy,2003,68(1):171-181.
[33]Kerisit S,Felmy A R,Ilton E S.Atomistic simulations of uranium incorporation into iron(hydr)oxides[J].Environment-al Science&Technology,2011,45(7):2770-2776.
[34]Frances N.Smith,Christopher D.Taylor,Wooyong Um,et al.Technetium Incorporation into Goethite(α-Fe OOH):An Atomic-Scale Investigation[J].Environmental Science&Technology,2015,49(22).
[35]Um W,Chang H,Icenhower J P,et al.Iron oxide wast-e form for stabilizing 99Tc[J].Journal of Nuclear Materials,2012,429(1-3):201-209.
[36]Um W,Chang H S,Icenhower J P,et al.Immobilizatio-n of 99-technetium(VII)by Fe(II)-goethite and limited reoxidation[J].Environmental Science&Technology,2011,45(11):4904-4913.
[37]Frances N.Skomurski,Kevin M.Rosso,Kenneth M.K-rupka,et al.Technetium Incorporation into Hematite(α-Fe2O3)[J].Environmental Science&Technology,2010,44(15):5855.
[38]Liu J,Pearce C I,Qafoku O,et al.Tc(VII)reduction-kinetics by titanomagnetite(Fe3-xTixO4)nanoparticles[J].Geochi-mica Et Cosmochimica Acta,2012,92(9):67-81.