湿式氧化法处理放射性废离子交换树脂研究进展
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摘要
随着世界核电事业的发展,核设施产生的废离子交换树脂的安全处理已成为困扰各国的难题。湿式氧化法具有反应条件温和、工序简单、经济有效等优点,近年来在放射性废物处理领域受到广泛关注。本文概述了国内外废树脂湿式氧化处理技术,包括酸煮解、超临界水氧化分解法、间接电化学氧化分解法和湿式过氧化氢氧化法;重点分析了废树脂湿式过氧化氢氧化法的发展现状、影响因素、反应机理、反应动力学以及放射性核素的去向;并进一步探讨了湿式氧化法在废树脂处理领域的发展方向及应用前景。
With the development of nuclear industry, the treatment and disposal of spent radioactive ion exchange resins has become a problem that needs to be solved at present. Because of the moderate reaction conditions, simple equipment, and low operational cost, wet air oxidation has recently received considerable attention from the research field of radioactive wastes treatment. In this paper, various advanced wet air oxidation processes for treatment of spent resins are summarized, including acid boiling degradation, supercritical water oxidation, electrochemical oxidation, and wet catalytic oxidation with hydrogen peroxide. The development status, influencing factors,reaction mechanism and kinetics of wet catalytic oxidation, as well as the distribution of radioactive nuclides in the off-gas, decomposition solution and solid residue, are briefly introduced. The future research directions and applications are also discussed.
With the development of nuclear industry, the treatment and disposal of spent radioactive ion exchange resins has become a problem that needs to be solved at present. Because of the moderate reaction conditions, simple equipment, and low operational cost, wet air oxidation has recently received considerable attention from the research field of radioactive wastes treatment. In this paper, various advanced wet air oxidation processes for treatment of spent resins are summarized, including acid boiling degradation, supercritical water oxidation, electrochemical oxidation, and wet catalytic oxidation with hydrogen peroxide. The development status, influencing factors,reaction mechanism and kinetics of wet catalytic oxidation, as well as the distribution of radioactive nuclides in the off-gas, decomposition solution and solid residue, are briefly introduced. The future research directions and applications are also discussed.
引文
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[2]孙奇娜,李俊峰,王建龙.水胶比对水泥固化放射性废树脂的影响[J].原子能科学技术,2012,46(11):1301-1306.Sun Qina,Li Junfeng,Wang Jianlong.Effect of water/binder ratio on cementation of radioactive spent resin[J].Atomic Energy Science and Technology,2012,46(11):1301-1306.
[3]罗上庚.废离子交换树脂的优化处理[J].核科学与工程,2003,23(2):165-172.Luo Shanggeng.Optimizing the management of spent ion exchange Resin[J].Chinese Journal of Nuclear Science and Engineering,2003,23(2):165-172.
[4]Wang J L,Wan Z.Treatment and disposal of spent radioactive ionexchange resins produced in the nuclear industry[J].Progress in Nuclear Energy,2015,78:47-55.
[5]Jārnstrōm R.Microbiological treatment of radioactive waste ion exchange resins[M]//Ion Exchange Advances.Springer Netherlands,1992:245-249.
[6]邱亮,丰俊东.微生物对放射性核素吸附行为的研究进展[J].环境工程,2015(6):30-34.Qiu Liang,Feng Jundong.Researchprogress on biosorption of radionuclides[J].Environmental Engineering,2015(6):30-34.
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[14]Akai Y,Yamada K,Sako T.Ion-exchange resin decomposition in supercritical water[J].High Pressure Research,2001,20:515-524.
[15]Leybros A,Roubaud A,Guichardon P,et al.Ion exchange resins destruction in a stirred supercritical water oxidation reactor[J].The Journal of Supercritical Fluids,2010,51:369-375.
[16]Leybros A,Roubaud A,Guichardon P,et al.Supercritical water oxidation of ion exchange resins:Degradation mechanisms[J].Process Safety and Environmental Protection,2010,88:213-222.
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[18]Kim K,Choi M,Son S H,et al.Treatment of ion exchange resins used in nuclear power plants by super-and sub-critical water oxidation-Aroad to commercial plant from bench-scale facility[J].Chemical Engineering Journal,2012,189-190:213-221.
[19]程娟,李全伟.放射性废树脂氧化分解处理技术[J].同位素,2012,25(2):124-128.Cheng Juan,Li Quanwei.New research progress on the oxidative decomposition technology for spent radioactive ion exchange resin[J].Journal of Isotopes,2012,25(2):124-128.
[20]Kritzer P,Dinjus E.An assessment of supercritical water oxidation(SCWO):Existing problems,possible solutions and new reactor concepts[J].Chemical Engineering Journal,2001,83(3):207-214.
[21]邢海青,马辉,张振涛,等.Ag(II)间接电化学氧化处理TBP技术研究[J].中国原子能科学研究院年报,2009,2010:396-396.Xing Haiqing,Ma Hui,Zhang Zhentao,et al.Study on the treatment of TBP by indirect electrochemical oxidation using Ag(II)[J].Annual Report For China Institute of Atomic Energy,2009,2010:396-396.
[22]成章,王京刚,文明芬,等.间接电化学氧化体系处理废有机溶剂[J].北京化工大学学报(自然科学版),2008,35(2):14-17.Cheng Zhang,Wang Jinggang,Wen Mingfen,et al.Treatment of spent solvent by mediated electrochemical oxidation[J].Journal of Beijing University of Chemical Technology,2008,35(2):14-17.
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[25]Todo F,Sasaki T,Suzuki K.Decomposition of organic wastes by wetoxidation with hydrogen peroxide oxidant[C]//Proceedings of the Fifth International Conference on Radioactive Waste Management and Environmental Remediation,ICEM'95,1995,1099-1101.
[26]Taylor P A.Destruction of ion-exchange resin in waste from the HFIR,T1 and T2 Tanks using Fenton's reagent[R].Ornl/tm,2002.
[27]Zahorodna M,Bogoczek R,Oliveros E,et al.Application of the Fenton process to the dissolution and mineralization of ion exchange resins[J].Catalysis Today,2007,129(1-2):200-206.
[28]Zahorodna M,Oliveros E,W?rner M,et al.Dissolution and mineralization of ion exchange resins:differentiation between heterogeneous and homogeneous(photo-)Fenton processes[J].Photochemical&Photobiological Sciences,2008,7(12):1480-1492.
[29]Gunale T L,Mahajani V V,Wattal P K,et al.Liquid phase mineralization of gel-type anion exchange resin by a hybrid process of Fenton dissolution followed by sonication and wet air oxidation[J].AsiaPacific Journal of Chemical Engineering,2009,4(1):90-98.
[30]Gunale T L,Mahajani V V,Wattal P K,et al.Studies in liquid phase mineralization of cation exchange resin by a hybrid process of Fenton dissolution followed by wet oxidation[J].Chemical Engineering Journal,2009,148(2):371-377.
[31]黃庆村.放射性废离子子交换树脂減容与安定化技术之建立[C]//第五届两岸核能学术交流研讨会论文集,中国台湾台北,2005,18:269-286.Huang Qingcun.The establishment of volume reduction and immobilization technology for radioactive spent ion exchange resins[C].Proceedings of The Fifth Cross-strait Workshop for Nuclear Energy Academic Exchange,China Taiwan Taibei,2005,18:269-286.
[32]耿作红.放射性废离子交换树脂的湿法化学氧化技术研究[D].北京:清华大学核能技术设计研究院,1993.Geng Zuohong.A study on wet chemical oxidation of radioactive spent ion-exchange resin[D].Beijing:Institute of Nuclear Energy Technology of Tsinghua University,1993.
[33]张晔.放射性废离子交换树脂稳定化技术研究[D].北京:清华大学核能技术设计研究院,1994.Zhang Ye.A study on the immobilization technology of radioactive spent ion-exchange resin[D].Beijing:Institute of Nuclear Energy Technology of Tsinghua University,1994.
[34]蹇兴超,云桂春.放射性废离子交换树脂过氧化氢湿法催化氧化技术研究[J].辐射防护,1995,15(3):203-209.Jian Xingchao,Yun Guichun.A Study on wet catalysis oxidation of spent radioactive ion-exchange resin by hydrogen peroxide[J].Radiation Protection,1995,15(3):203-209.
[35]Jian X,Wu T,Yun G.A study of wet catalytic oxidation of radioactive spent ion exchange resin by hydrogen peroxide[J].Nuclear Safety,1996,37(2):149-157.
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