湿法氧化处理放射性废离子交换树脂的方法
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摘要
本文对放射性废离子交换树脂湿法氧化处理方法的反应机理、工艺特点、工业应用情况进行了总结。主要对酸煮解法、蒸汽重整工艺、超临界水氧化法(SCWO)及芬顿湿法氧化法进行了对比,通过分析国内外研究现状及工业应用情况,同时结合各个方法的优缺点及后处理难易程度,考虑到核安全及经济性,认为芬顿湿法氧化法处理放射性废离子交换树脂是较为可行的方案之一。
Radioactive waste ion-exchange resins have been treated by cement solidification directly,however,the effect of cement is unsatisfactory.In order to find other proper treatment methods,many investigations have been carried out.Especially,wet oxidation treatment technology is favored by many researchers because of its short treatment cycle and high volume reduction ratio.In this work,the reaction mechanism,process characteristics and industrial application of the wet oxidation treatment of radioactive spent ion-exchange resins were summarized.The analysis of the acid boiling degradation,Fenton wet oxidation technology,steam reforming process and supercritical water oxidation method had been focused.Mainly for the acid digestion,steam reforming process,supercritical water oxidation and Fenton wet oxidation were compared by the status of research at home and abroad and industrial applications,combined with the advantages and disadvantages of each method and the ease of post-processing,and considering the perspective of nuclear safety and convenient for subsequent processing,four treatment methods were briefly analyzed by comparing the advantages and disadvantages of each method.The results indicated that Fenton wet oxidation treatment of radioactive spent ion exchange resin was one of the feasible schemes.
Radioactive waste ion-exchange resins have been treated by cement solidification directly,however,the effect of cement is unsatisfactory.In order to find other proper treatment methods,many investigations have been carried out.Especially,wet oxidation treatment technology is favored by many researchers because of its short treatment cycle and high volume reduction ratio.In this work,the reaction mechanism,process characteristics and industrial application of the wet oxidation treatment of radioactive spent ion-exchange resins were summarized.The analysis of the acid boiling degradation,Fenton wet oxidation technology,steam reforming process and supercritical water oxidation method had been focused.Mainly for the acid digestion,steam reforming process,supercritical water oxidation and Fenton wet oxidation were compared by the status of research at home and abroad and industrial applications,combined with the advantages and disadvantages of each method and the ease of post-processing,and considering the perspective of nuclear safety and convenient for subsequent processing,four treatment methods were briefly analyzed by comparing the advantages and disadvantages of each method.The results indicated that Fenton wet oxidation treatment of radioactive spent ion exchange resin was one of the feasible schemes.
引文
[1]中国国家发展改革委员会.核电中长期发展规划(2005-2020年)[R].北京:中国国家发展改革委员会,2007.
[2]罗上庚.放射性废离子交换树脂的处理技术[J].辐射防护,1992,12(5):398-404.Luo Shanggeng.Treating technique of radioactive spent ion exchange resin[J].Radiation Protection,1992,12(5):398-404(in Chinese).
[3]陈斌.核电厂低中放废树脂处理工艺[J].辐射防护通讯,2010,(1):13-16.Chen Bin.Process research of spent resin treatment from NPP[J].Radiation Protection Bulletion,2010,(1):13-16(in Chinese).
[4]IAEA.The principles of radioactive waste management[R].Vienna:IAEA,1995.
[5]罗上庚.废离子交换树脂的优化处理[J].核科学与工程,2003,(12):165-172.Luo Shanggeng.Optimizing the management of spent ion exchange resin[J].Chinese Journal of Nuclear Science and Engineering,2003,(12):165-172(in Chinese).
[6]方祥洪,马若霞,杨彬,等.放射性废树脂处理研究方法[J].广州化工,2015,43(3):6-7.Fang Xianghong,Ma Ruoxia,Yang Bin,et al.Study on the method of radioactive waste resintreatment[J].Guangzhou Chemical Industry,2015,43(3):6-7(in Chinese).
[7]郭喜良,冯文东,高超,等.废树脂湿法氧化减容处理技术路线及问题探讨[J].辐射防护,2015,35(5):267-273.Guo Xiliang,Feng Wendong,Gao Chao,et al.A roadmap and key issues of spent resin wetoxidation research[J].Radiation Protection,2015,35(5):267-273(in Chinese).
[8]高超,安鸿翔,梁栋,等.桶内微波干燥废树脂可行性研究[J].干燥技术与设备,2012,10(3):20-25.Gao Chao,An Hongxiang,Liang Dong,et al.The pilot study on microwave drum drying technology for waste resin[J].Drying Technology&Equipment,2012,10(3):20-25(in Chinese).
[9]高超,贾梅兰,王亚东.放射性废物微波处理装置有效输出功率的测定[J].广东微量元素科学,2015,22(3):48-51.Gao Chao,Jia Meilan,Wang Yadong.The effective output power of radioactive waste microwave treatment equipment[J].Guangdong Trace Elements Science,2015,22(3):48-51(in Chinese).
[10]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.Chen Juan,Li Quanwei.New research progress on the oxidative decomposition technology for spent radioative ion exchange resin[J].Journal of Isotopes,2012,25(2):124-128(in Chinese).
[11]罗上庚.放射性废物处理与处置[M].北京:中国环境科学出版社,2007.
[12]Yoshii K,Hideo M,Jokun A,et al.Acid digestion of radioactive combustible wastes[J].Journal of Nuclear Science and Technology,1980,17(11):865-868.
[13]孙才济.酸蒸煮放射性废物[J].国外核新闻,1981,(12):24.
[14]李斗,华伟,廖能斌,等.蒸汽重整处理核电厂放射性废树脂的探讨[J].广州化工,2015,43(15):157-158.Li Dou,Hua Wei,Liao Nengbin,et al.Discussion on treatment of radioactive spent resins in nuclear power plant by steam reforming[J].Guangdong Chemical Industry,2015,43(15):157-158(in Chinese).
[15]林力,马兴均,陈先林,等.放射性废物蒸汽重整处理及矿化技术发展现状及展望[J].科技创新导报,2015,18:6-10.
[16]Bradley M J,Thoms W O,Marty P C,et al.Studsvik processing facility pyrolysis/steam reforming technology for volume and weight reduction and stabilization of LLRW and mixed wastes[C]∥WM’99conference.Columbia(USA):WM Symposia,Inc.,1999.
[17]Carol M J.Engineering study of the Hanford Low Activity Waste(LAW)steam reforming process(U)[M].Savannah River(USA):Savannah River Technology Center,2002.
[18]Medoll M.Treatment for oxidation of organic material in supercriti-cal water:US,4338199[P].1984-05.
[19]Lixiong L,Peishi C,Earnest F G.Generalized kinetic model for wet oxidation of organic compounds[J].AIChE Journal,1991,37(11):1 687-1 697.
[20]Juan R P,Lopez J,Nebot E,et al.Elimination of cutting oil wastes by promoted hydrothermal oxidation[J].Hazardous Materials,2001,88(1):95-106.
[21]Kyeongsook K,Soon H S,KwangSin K,et al.Treatment of radioactive ionic exchange resin by super-and sub-critical water oxidation(SCWO)[J].Nuclear Engineering and Design,2010,240:3 654-3 659.
[22]Leybros A,Roubaud A,Guichardon P,et al.Ion exchange resins destruction in a stirred supercritical warter oxidation rector[J].J of Supercritical Fluids,2010,51:369-375.
[23]王亮,何辉,唐洪斌.超临界水氧化技术处理放射性有机废物的应用与展望[J].中国原子能科学研究院年报,2007,1:259-259.Wang Liang,He Hui,Tang Hongbin.Application and Prospect of supercritical water oxidation technology for treatment of radioactive organic waste[J].Annual Report of China Institute of Atomic Energy,2007,1:259-259(in Chinese).
[24]蹇兴超,云桂春.放射性废离子交换树脂的过氧化氢湿法催化氧化技术研究[J].辐射防护,1993,13(3):203-210.Jian Xingchao,Yun Guichun.A study on wet catalysis oxidation of spent radioactive ion exchange resin by hydrogen peroxide[J].Radiation Protection,1993,13(3):203-210(in Chinese).
[25]Wang Jianlong,Wan Zhong.Treatment and disposal of spent radioactive ion-exchange resins produced in the nuclear industry[J].Progress in Nuclear Energy,2015,78:47-55.
[26]Taylor P A.Destruction of ion-exchange resin in waste from the HFIR,T1,and T2tanks using Fenton’s reagent[M].Tennessee(USA):Oak Ridge National Laboratory,2002.
[27]Bibler N E,Orebaugh E G.Iron-catalysed dissolution of polystyrenesulfonate cation-exchange resin in hydrogen peroxide[J].Ind Eng Chem Prod Res Dev,1976,15:136.
[28]Lee S C.Dissolution of ion-exchange resin by hydrogen peroxide[M].South Carolina(USA):Savannah River Laboratory,1981.
[29]Srinivas C.Wet oxidative destruction of spent ion-exchange resins using hydrogen peroxide[M].Bombay(India):Bhabha Atomic Research Centre,1994.
[30]Srinivas C,Sugilal G,Wattal P K.Management of spent organic ion-exchange resins by photochemical oxidation[C]∥WM’03 conference.Tucson,Arizona(USA):WM Symposia,Inc.,2003.
[31]Feng Jiyun,Hu Xijun,Po Lock Y.Degradation of salicylic acid by photo-assisted fenton reaction using Fe ions on strongly acidic ion exchange resin as catalyst[J].Chemical Engineering Journal,2004,100:159-165.
[32]Hwan-Young K,In-Tae K,Gi-Hong K,et al.Wet oxidation of mixed resins by a modified Fenton’s reaction with an electrochemical potential[J].J Ind Eng Chem,2004,13(05):665-668.
[33]Monika Z,Romuald B,Esther O,et al.Application of the Fenton process to the dissolution and mineralization of ion exchange resins[J].Catalysis Today,2007,129:200-206.
[34]黄慶村.放射性廢離子交換樹脂減容與安定化技術之建立[C]∥第五届两岸核能学术交流研讨会.中国台湾台北:中国核学会,2005.
[35]梁志荣,吴玉生,刘学军.芬顿氧化法预处理放射性废离子交换树脂[J].核化学与放射化学,2007,29(2):71-74.Liang Zhirong,Wu Yusheng,Liu Xuejun.Pretreatment of radioactive spent ion exchange resin by Fenton process[J].Journal of Nuclear and Radiochemistry,2007,29(2):71-74(in Chinese).
[36]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,2009,148:371-377.
[37]Wan Zhong,Xu Lejin,Wang Jianlong.Disintegration and dissolution of spent radioactive cationic exchange resins using Fenton-like oxidation process[J].Nuclear Engineering and Design,2015,291:101-108.
[38]Charman R G,Twissell M A.Wet oxidation mobile pilot demonstration on organic radioactive wastes[R].EUR:Nuclear Science and Technology,1999.
[39]高帅,郭喜良,高超,等.放射性废树脂处理技术[J].辐射防护通讯,2014,34(1):28-33.Gao Shuai,Guo Xiliang,Gao Chao,et al.The process of spent resin treatment[J].Radiation Protection Bulletion,2014,34(1):28-33(in Chinese).
[40]Miyamoto T,Motoyama M,Shibuya M.Development of wet-oxidation treatment system for filter backwash sludge and ion exchange resins[C]∥WM’03conference.Tucson,Arizona(USA):WM Symposia,Inc.,2003.
[41]李庆瑞.核二厂低放射性废弃物管理成效与精进简报[C]∥2011年两岸核电管理研讨会.北京:中国核学会,2011.
[42]陈义平,田景光,罗任瀚,等.湿式氧化暨高效率固化系统之建置[C]∥第三届两岸放射性废物管理研讨会会议论文集.成都:中国核学会,2013.
[2]罗上庚.放射性废离子交换树脂的处理技术[J].辐射防护,1992,12(5):398-404.Luo Shanggeng.Treating technique of radioactive spent ion exchange resin[J].Radiation Protection,1992,12(5):398-404(in Chinese).
[3]陈斌.核电厂低中放废树脂处理工艺[J].辐射防护通讯,2010,(1):13-16.Chen Bin.Process research of spent resin treatment from NPP[J].Radiation Protection Bulletion,2010,(1):13-16(in Chinese).
[4]IAEA.The principles of radioactive waste management[R].Vienna:IAEA,1995.
[5]罗上庚.废离子交换树脂的优化处理[J].核科学与工程,2003,(12):165-172.Luo Shanggeng.Optimizing the management of spent ion exchange resin[J].Chinese Journal of Nuclear Science and Engineering,2003,(12):165-172(in Chinese).
[6]方祥洪,马若霞,杨彬,等.放射性废树脂处理研究方法[J].广州化工,2015,43(3):6-7.Fang Xianghong,Ma Ruoxia,Yang Bin,et al.Study on the method of radioactive waste resintreatment[J].Guangzhou Chemical Industry,2015,43(3):6-7(in Chinese).
[7]郭喜良,冯文东,高超,等.废树脂湿法氧化减容处理技术路线及问题探讨[J].辐射防护,2015,35(5):267-273.Guo Xiliang,Feng Wendong,Gao Chao,et al.A roadmap and key issues of spent resin wetoxidation research[J].Radiation Protection,2015,35(5):267-273(in Chinese).
[8]高超,安鸿翔,梁栋,等.桶内微波干燥废树脂可行性研究[J].干燥技术与设备,2012,10(3):20-25.Gao Chao,An Hongxiang,Liang Dong,et al.The pilot study on microwave drum drying technology for waste resin[J].Drying Technology&Equipment,2012,10(3):20-25(in Chinese).
[9]高超,贾梅兰,王亚东.放射性废物微波处理装置有效输出功率的测定[J].广东微量元素科学,2015,22(3):48-51.Gao Chao,Jia Meilan,Wang Yadong.The effective output power of radioactive waste microwave treatment equipment[J].Guangdong Trace Elements Science,2015,22(3):48-51(in Chinese).
[10]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.Chen Juan,Li Quanwei.New research progress on the oxidative decomposition technology for spent radioative ion exchange resin[J].Journal of Isotopes,2012,25(2):124-128(in Chinese).
[11]罗上庚.放射性废物处理与处置[M].北京:中国环境科学出版社,2007.
[12]Yoshii K,Hideo M,Jokun A,et al.Acid digestion of radioactive combustible wastes[J].Journal of Nuclear Science and Technology,1980,17(11):865-868.
[13]孙才济.酸蒸煮放射性废物[J].国外核新闻,1981,(12):24.
[14]李斗,华伟,廖能斌,等.蒸汽重整处理核电厂放射性废树脂的探讨[J].广州化工,2015,43(15):157-158.Li Dou,Hua Wei,Liao Nengbin,et al.Discussion on treatment of radioactive spent resins in nuclear power plant by steam reforming[J].Guangdong Chemical Industry,2015,43(15):157-158(in Chinese).
[15]林力,马兴均,陈先林,等.放射性废物蒸汽重整处理及矿化技术发展现状及展望[J].科技创新导报,2015,18:6-10.
[16]Bradley M J,Thoms W O,Marty P C,et al.Studsvik processing facility pyrolysis/steam reforming technology for volume and weight reduction and stabilization of LLRW and mixed wastes[C]∥WM’99conference.Columbia(USA):WM Symposia,Inc.,1999.
[17]Carol M J.Engineering study of the Hanford Low Activity Waste(LAW)steam reforming process(U)[M].Savannah River(USA):Savannah River Technology Center,2002.
[18]Medoll M.Treatment for oxidation of organic material in supercriti-cal water:US,4338199[P].1984-05.
[19]Lixiong L,Peishi C,Earnest F G.Generalized kinetic model for wet oxidation of organic compounds[J].AIChE Journal,1991,37(11):1 687-1 697.
[20]Juan R P,Lopez J,Nebot E,et al.Elimination of cutting oil wastes by promoted hydrothermal oxidation[J].Hazardous Materials,2001,88(1):95-106.
[21]Kyeongsook K,Soon H S,KwangSin K,et al.Treatment of radioactive ionic exchange resin by super-and sub-critical water oxidation(SCWO)[J].Nuclear Engineering and Design,2010,240:3 654-3 659.
[22]Leybros A,Roubaud A,Guichardon P,et al.Ion exchange resins destruction in a stirred supercritical warter oxidation rector[J].J of Supercritical Fluids,2010,51:369-375.
[23]王亮,何辉,唐洪斌.超临界水氧化技术处理放射性有机废物的应用与展望[J].中国原子能科学研究院年报,2007,1:259-259.Wang Liang,He Hui,Tang Hongbin.Application and Prospect of supercritical water oxidation technology for treatment of radioactive organic waste[J].Annual Report of China Institute of Atomic Energy,2007,1:259-259(in Chinese).
[24]蹇兴超,云桂春.放射性废离子交换树脂的过氧化氢湿法催化氧化技术研究[J].辐射防护,1993,13(3):203-210.Jian Xingchao,Yun Guichun.A study on wet catalysis oxidation of spent radioactive ion exchange resin by hydrogen peroxide[J].Radiation Protection,1993,13(3):203-210(in Chinese).
[25]Wang Jianlong,Wan Zhong.Treatment and disposal of spent radioactive ion-exchange resins produced in the nuclear industry[J].Progress in Nuclear Energy,2015,78:47-55.
[26]Taylor P A.Destruction of ion-exchange resin in waste from the HFIR,T1,and T2tanks using Fenton’s reagent[M].Tennessee(USA):Oak Ridge National Laboratory,2002.
[27]Bibler N E,Orebaugh E G.Iron-catalysed dissolution of polystyrenesulfonate cation-exchange resin in hydrogen peroxide[J].Ind Eng Chem Prod Res Dev,1976,15:136.
[28]Lee S C.Dissolution of ion-exchange resin by hydrogen peroxide[M].South Carolina(USA):Savannah River Laboratory,1981.
[29]Srinivas C.Wet oxidative destruction of spent ion-exchange resins using hydrogen peroxide[M].Bombay(India):Bhabha Atomic Research Centre,1994.
[30]Srinivas C,Sugilal G,Wattal P K.Management of spent organic ion-exchange resins by photochemical oxidation[C]∥WM’03 conference.Tucson,Arizona(USA):WM Symposia,Inc.,2003.
[31]Feng Jiyun,Hu Xijun,Po Lock Y.Degradation of salicylic acid by photo-assisted fenton reaction using Fe ions on strongly acidic ion exchange resin as catalyst[J].Chemical Engineering Journal,2004,100:159-165.
[32]Hwan-Young K,In-Tae K,Gi-Hong K,et al.Wet oxidation of mixed resins by a modified Fenton’s reaction with an electrochemical potential[J].J Ind Eng Chem,2004,13(05):665-668.
[33]Monika Z,Romuald B,Esther O,et al.Application of the Fenton process to the dissolution and mineralization of ion exchange resins[J].Catalysis Today,2007,129:200-206.
[34]黄慶村.放射性廢離子交換樹脂減容與安定化技術之建立[C]∥第五届两岸核能学术交流研讨会.中国台湾台北:中国核学会,2005.
[35]梁志荣,吴玉生,刘学军.芬顿氧化法预处理放射性废离子交换树脂[J].核化学与放射化学,2007,29(2):71-74.Liang Zhirong,Wu Yusheng,Liu Xuejun.Pretreatment of radioactive spent ion exchange resin by Fenton process[J].Journal of Nuclear and Radiochemistry,2007,29(2):71-74(in Chinese).
[36]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,2009,148:371-377.
[37]Wan Zhong,Xu Lejin,Wang Jianlong.Disintegration and dissolution of spent radioactive cationic exchange resins using Fenton-like oxidation process[J].Nuclear Engineering and Design,2015,291:101-108.
[38]Charman R G,Twissell M A.Wet oxidation mobile pilot demonstration on organic radioactive wastes[R].EUR:Nuclear Science and Technology,1999.
[39]高帅,郭喜良,高超,等.放射性废树脂处理技术[J].辐射防护通讯,2014,34(1):28-33.Gao Shuai,Guo Xiliang,Gao Chao,et al.The process of spent resin treatment[J].Radiation Protection Bulletion,2014,34(1):28-33(in Chinese).
[40]Miyamoto T,Motoyama M,Shibuya M.Development of wet-oxidation treatment system for filter backwash sludge and ion exchange resins[C]∥WM’03conference.Tucson,Arizona(USA):WM Symposia,Inc.,2003.
[41]李庆瑞.核二厂低放射性废弃物管理成效与精进简报[C]∥2011年两岸核电管理研讨会.北京:中国核学会,2011.
[42]陈义平,田景光,罗任瀚,等.湿式氧化暨高效率固化系统之建置[C]∥第三届两岸放射性废物管理研讨会会议论文集.成都:中国核学会,2013.