放射性废有机相(TBP/OK)处理技术综述
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摘要
放射性废有机相主要成分包括TBP、煤油以及少量降解产物和放射性核素,属易燃易爆物质。这类废物虽然年产生量小,但经过核设施多年的运行和累积存放,贮量逐年增多,对社会和自然环境造成安全隐患,亟需进行处理。对目前世界范围内放射性废有机相(TBP/OK)的各种处理方法进行了介绍,包括焚烧法、湿法氧化法、加合物形成相分离-焚烧处理法、碱性水解法、吸收法、水泥固化法和蒸馏法,分析了各种处理方法的优缺点。此外,对放射性废有机相处理方法的工程应用进行了考虑。结合各核设施产生的放射性废有机相的实际源项,可优先考虑使用碱性水解法、Fenton法和吸收法等技术对其进行处理。
The main components of radioactive waste organic phase include TBP,kerosene,a small amount of degradation products and radionuclides,which are flammable and explosive substances. Although radioactive waste organic phase is produced in a small amount per year,after long-term operation and cumulative storage by nuclear facilities,its amount increases year by year,and there are potential hazard to the society and environment,which are in urgent need of treatment.Various treatment methods for radioactive waste organic phase( TBP/OK) at preset in the world were introduced in this paper,including incineration, wet oxidation, adduct formation phase separation-incineration treatment, alkaline hydrolysis,absorption,cement solidification and distillation method,and the advantages and disadvantages of various treatment methods were analyzed. In addition,the engineering application of the TBP/OK treatment methods was considered. Combined with the actual source of TBP/OK produced by each nuclear facility,it can be preferentially treated by techniques such as alkaline hydrolysis,Fenton method and absorption method,etc.
The main components of radioactive waste organic phase include TBP,kerosene,a small amount of degradation products and radionuclides,which are flammable and explosive substances. Although radioactive waste organic phase is produced in a small amount per year,after long-term operation and cumulative storage by nuclear facilities,its amount increases year by year,and there are potential hazard to the society and environment,which are in urgent need of treatment.Various treatment methods for radioactive waste organic phase( TBP/OK) at preset in the world were introduced in this paper,including incineration, wet oxidation, adduct formation phase separation-incineration treatment, alkaline hydrolysis,absorption,cement solidification and distillation method,and the advantages and disadvantages of various treatment methods were analyzed. In addition,the engineering application of the TBP/OK treatment methods was considered. Combined with the actual source of TBP/OK produced by each nuclear facility,it can be preferentially treated by techniques such as alkaline hydrolysis,Fenton method and absorption method,etc.
引文
[1]汪家鼎,陈家镛.溶剂萃取手册[M].北京:化学工业出版社,2001.
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[3] International Atomic Energy Agency. Treatment and Conditioning of Radioactive Organic Liquids[R]. IAEA-TECDOC-656. Vienna:IAEA,1992.
[4] International Atomic Energy Agency. Advances in Technologies for the Treatment of Low and Intermediate Level Radioactive Liquid Wastes[R]. Technical Reports Series No. 370. Vienna:IAEA,1994.
[5] International Atomic Energy Agency. Predisposal Management of Organic Radioactive Waste[R]. Technical Reports Series No. 427.Vienna:IAEA,2004.
[6] Dussossoy J L. Incineration of Radioactive Organic Liquids[R].Report CEC-EUR-9621. London:Graham&Trotman,1985:97-103.
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[10] Lewandowski K E. Savannah River Plant Incineration Demonstration[R]. Report DP-MS-83-90. Aiken,SC:Savannah River Lab,1983.Dussossoy J L.
[11] Rwe Nukem Gmbh. Pyrolysis of Radioactive Organic Waste[R].Products Descriptions of NUKEM. 2000.
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[13] Mabrouk M,Lemont F,Baronnet J M. Incineration of radioactive organic liquid wastes by underwater thermal plasma[J]. Journal of physics,2012,406(1):1-8.
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[15]程昌明,童洪辉,兰伟.模拟放射性废树脂热等离子体处理系统设计及试验分析[J].高压电技术,2013,39(7):1584-1589.
[16]徐文兵,吕永红,陈明周,等.热等离子体处理模拟放射性废物试验研究[J].核动力工程,2015,36(6):175-179.
[17]江贻满,倪国华,宋晔,等.热等离子体对模拟有机低放射性废物固化处理试验分析[J].2013,高电压技术,2013,13(9):1750-1756.
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[19] Balaji S, Chung SJ, Matheswaran M. Destruction of organic pollutants by cerium(Ⅳ)MEO process:a study on the influence of process conditions for EDTA mineralization[J]. Journal of Hazardous Materials,2008,150(3):596-603.
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[21]成章.废有机溶剂磷酸三丁酯(TBP)的处理研究[D].北京:北京化工大学,2008.
[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,2008,35(2):14-17.
[23] Christophe J, Gerard D, Turc H A. Method and device for oxidizing materials in supercritical water[P]. PCT Patent,WO200230836-A1. 2002-04-18.
[24] Laura A W,Steven J B. Hydrothermal processing of radioactive combustible waste[R]. AICHE Spring Meeting,New Orleans,LA,1998.
[25]杨林月,张振涛.超临界水氧化技术处理磷酸三丁酯的实验研究[J].原子能科学技术,2016,50(12):2138-2144.
[26] Cooper J F. Destruction of organic wastes by ammonium peroxydisulfate with electrolytic regeneration of oxidant[R].Prepared for submittal to the Sixth International Conference on Radioactive Waste Management and Environmental Remediation October 12-16,1997,Singapore,Republic of Singapoxe.
[27] Wilks J P, Holt N S. Wet Oxidation of Mixed Organic and Inorganic Radioactive Sludge Wastes from a Water Reactor[J].Wastes Management,1990,10(3):197-203.
[28] Evans D W. Treatment of Steam Generator Chemical Cleaning Wastes:development and Operation of the Bruce Spent Solvent Treatment Facility[C]//Proc. 5thInt. Symp. of Chemical Oxidation. Nashville,TN,USA. 1995.
[29] Wattal P K,Deshingkar D S,Srinivas C,et al. Combined Processes and Techniques for Processing of Organic Radioactive Waste[R].IAEA-TECDOC-1336. Vienna:IAEA,2003:121-136.
[30] Miyamoto T,Motoyama M,Shibuya M. Development of Wetoxidation Treatment System for Filter Backwash Sludge and Ion Exchange Resins[J]. WM’03 Conference,2003,Tucson,AZ.
[31]冀小元,云桂春. H2O2-Fe2+/Ti O2-H2SO4处理废有机溶剂的研究[J].污染防治技术,1996,9(1&2):15-20.
[32]刘祖发,丁波,刘珍珍,等. Fenton试剂氧化降解水体有机磷酸酯的动力学研究[J].亚热带资源与环境学报,2016,11(1):1-8.
[33] Claire-emilie vaudey SRJPDKCC. 2013. Nochar Polymers:an aqueous and organic liquid solidification process for Cadarache Lor(liquides Organiques Radioactifs)[C]//Wm2013 Conference,1-16.
[34]方祥洪.模拟放射性有机废液的吸收法处理与作用机制研究[D].成都:成都理工大学,2017.
[35]花榕,张志宾,刘淑娟,等.碱矿渣胶凝材料固化废TBP的配方初步研究[J].原子能科学技术,2013,47(11):1956-1960.
[36]罗上庚,S Drobnik.废TBP-溶剂的固化研究[J].核科学与工程,1985,5(4):332-337.
[37]顾忠茂.核废物处理技术[M].北京:原子能出版社,2009.
[38]陈宝生,王维国,周秀珠,等.磷酸加合水解法分离TBP和煤油的研究[J].
[39]丁欢,李军,金央,等.磷酸三丁酯在碱中的降解研究[J].化学工程师,2015(11):51-53.
[40]严沧生,梁永丰,战仕全.放射性废树脂处理技术工程应用的选择[J].辐射防护,2016,36(4):232-239.
[2] International Atomic Energy Agency. Options for the Treatment and Solidification of Organic Radioactive Wastes[R]. Technical Reprots Series No.294. Vienna:IAEA,1989.
[3] International Atomic Energy Agency. Treatment and Conditioning of Radioactive Organic Liquids[R]. IAEA-TECDOC-656. Vienna:IAEA,1992.
[4] International Atomic Energy Agency. Advances in Technologies for the Treatment of Low and Intermediate Level Radioactive Liquid Wastes[R]. Technical Reports Series No. 370. Vienna:IAEA,1994.
[5] International Atomic Energy Agency. Predisposal Management of Organic Radioactive Waste[R]. Technical Reports Series No. 427.Vienna:IAEA,2004.
[6] Dussossoy J L. Incineration of Radioactive Organic Liquids[R].Report CEC-EUR-9621. London:Graham&Trotman,1985:97-103.
[7] Klingler L M. Defense Waste Cyclone Incineration Demonstration Program[R]. Report MLM-2716. Miamisburg,OH:Mound Lab.1980.
[8] Baehr W,Hempelmann W,Krause H. Incineration Plant for Radioactive Waste at the Nuclear Research Centre[R]. Report KFK-2418. Karlsruhe:Kernforschungszentrum,1977.
[9] Dirks F,Hempelmann W. The Incineration Plant of the Karlsruhe Nuclear Research Centre:regional Solution[R]. Report CECEUR-9621. London:Graham&Trotman,1985:34-47.
[10] Lewandowski K E. Savannah River Plant Incineration Demonstration[R]. Report DP-MS-83-90. Aiken,SC:Savannah River Lab,1983.Dussossoy J L.
[11] Rwe Nukem Gmbh. Pyrolysis of Radioactive Organic Waste[R].Products Descriptions of NUKEM. 2000.
[12]张存平,甘学英,林美琼.热解焚烧废TBP/OK料液配制[J].原子能科学技术,2004,38(2):181-184.
[13] Mabrouk M,Lemont F,Baronnet J M. Incineration of radioactive organic liquid wastes by underwater thermal plasma[J]. Journal of physics,2012,406(1):1-8.
[14] Mabrouk M,Marchand M,Russello A,et al. Development of a submerged thermal plasma process for combustion of organic liquid waste[J]. Plasma Chemistry and Plasma Processing,2015,35(1):45-60.
[15]程昌明,童洪辉,兰伟.模拟放射性废树脂热等离子体处理系统设计及试验分析[J].高压电技术,2013,39(7):1584-1589.
[16]徐文兵,吕永红,陈明周,等.热等离子体处理模拟放射性废物试验研究[J].核动力工程,2015,36(6):175-179.
[17]江贻满,倪国华,宋晔,等.热等离子体对模拟有机低放射性废物固化处理试验分析[J].2013,高电压技术,2013,13(9):1750-1756.
[18] Wieczorek H,Oser B. Development and Active Demonstration of Acid Digestion of Plutonium-Bearing Waste[C] ANS Conf.Niagara Falls,Hinsdale,IL:American Nuclear Society,1986.
[19] Balaji S, Chung SJ, Matheswaran M. Destruction of organic pollutants by cerium(Ⅳ)MEO process:a study on the influence of process conditions for EDTA mineralization[J]. Journal of Hazardous Materials,2008,150(3):596-603.
[20] Zoher Chiba. Mediated electrochemical oxidation as an alternative to incineration for mixed wastes[R]. WM 96 Symposia,Tucson,AZ,March 1,1995.
[21]成章.废有机溶剂磷酸三丁酯(TBP)的处理研究[D].北京:北京化工大学,2008.
[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,2008,35(2):14-17.
[23] Christophe J, Gerard D, Turc H A. Method and device for oxidizing materials in supercritical water[P]. PCT Patent,WO200230836-A1. 2002-04-18.
[24] Laura A W,Steven J B. Hydrothermal processing of radioactive combustible waste[R]. AICHE Spring Meeting,New Orleans,LA,1998.
[25]杨林月,张振涛.超临界水氧化技术处理磷酸三丁酯的实验研究[J].原子能科学技术,2016,50(12):2138-2144.
[26] Cooper J F. Destruction of organic wastes by ammonium peroxydisulfate with electrolytic regeneration of oxidant[R].Prepared for submittal to the Sixth International Conference on Radioactive Waste Management and Environmental Remediation October 12-16,1997,Singapore,Republic of Singapoxe.
[27] Wilks J P, Holt N S. Wet Oxidation of Mixed Organic and Inorganic Radioactive Sludge Wastes from a Water Reactor[J].Wastes Management,1990,10(3):197-203.
[28] Evans D W. Treatment of Steam Generator Chemical Cleaning Wastes:development and Operation of the Bruce Spent Solvent Treatment Facility[C]//Proc. 5thInt. Symp. of Chemical Oxidation. Nashville,TN,USA. 1995.
[29] Wattal P K,Deshingkar D S,Srinivas C,et al. Combined Processes and Techniques for Processing of Organic Radioactive Waste[R].IAEA-TECDOC-1336. Vienna:IAEA,2003:121-136.
[30] Miyamoto T,Motoyama M,Shibuya M. Development of Wetoxidation Treatment System for Filter Backwash Sludge and Ion Exchange Resins[J]. WM’03 Conference,2003,Tucson,AZ.
[31]冀小元,云桂春. H2O2-Fe2+/Ti O2-H2SO4处理废有机溶剂的研究[J].污染防治技术,1996,9(1&2):15-20.
[32]刘祖发,丁波,刘珍珍,等. Fenton试剂氧化降解水体有机磷酸酯的动力学研究[J].亚热带资源与环境学报,2016,11(1):1-8.
[33] Claire-emilie vaudey SRJPDKCC. 2013. Nochar Polymers:an aqueous and organic liquid solidification process for Cadarache Lor(liquides Organiques Radioactifs)[C]//Wm2013 Conference,1-16.
[34]方祥洪.模拟放射性有机废液的吸收法处理与作用机制研究[D].成都:成都理工大学,2017.
[35]花榕,张志宾,刘淑娟,等.碱矿渣胶凝材料固化废TBP的配方初步研究[J].原子能科学技术,2013,47(11):1956-1960.
[36]罗上庚,S Drobnik.废TBP-溶剂的固化研究[J].核科学与工程,1985,5(4):332-337.
[37]顾忠茂.核废物处理技术[M].北京:原子能出版社,2009.
[38]陈宝生,王维国,周秀珠,等.磷酸加合水解法分离TBP和煤油的研究[J].
[39]丁欢,李军,金央,等.磷酸三丁酯在碱中的降解研究[J].化学工程师,2015(11):51-53.
[40]严沧生,梁永丰,战仕全.放射性废树脂处理技术工程应用的选择[J].辐射防护,2016,36(4):232-239.