U(Ⅵ)在处置场地质环境中迁移规律的模拟研究
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摘要
以西南某极低放射性废物处置场土壤为研究对象,采用静态吸附和动态吸附实验获取处置场地质特征参数,结合PHREEQC软件和地下水数值模拟系统(GMS)预测U(Ⅵ)在处置场环境中的化学种态和迁移规律。结果表明:U(Ⅵ)在处置场土壤中的吸附平衡时间为20 d,吸附分配系数为358 m L/g;U(Ⅵ)在处置场地下水环境中主要以UO_2(CO_3)_2~(2-)和UO_2(CO_3)_3~(4-)形式存在;处置场关闭后安全运行30 a,处置场中心U(Ⅵ)质量浓度下降4.20%,外围50 m与下游河流边界处U(Ⅵ)质量浓度分别为初始给定值的3.40%和1.32%;在12 a时有0.10%的U(Ⅵ)到达河边。
Using the soil from a very low level radioactive waste disposal site in southwestern of China as research object,the geologic parameters of the disposal site were obtained by static and dynamic adsorption experiments,and combined with PHREEQC software and groundwater modeling system(GMS),the chemical species and migration of U(Ⅵ)in the disposal site soil were predicted. The research result showed that:The adsorption equilibrium time of U(Ⅵ)in the disposal site soil was 20 d with 358 m L/g of the adsorption partition coefficient;U(Ⅵ)in groundwater of the disposal site was mainly in the form of UO_2(CO_3)_2~(2-) and UO_2(CO_3)_3~(4-); In 30 a of safe operation of the closed disposal site,the U(Ⅵ)mass concentration of soil in the disposal site centre will decrease by 4.20%,and that of soil at outer-ring 50 m and downstream boundary will be 3.40% and 1.32% of the initial value respectively;After 12 a of operation,only 0.10% of U(Ⅵ)will arrive at the riverside.
Using the soil from a very low level radioactive waste disposal site in southwestern of China as research object,the geologic parameters of the disposal site were obtained by static and dynamic adsorption experiments,and combined with PHREEQC software and groundwater modeling system(GMS),the chemical species and migration of U(Ⅵ)in the disposal site soil were predicted. The research result showed that:The adsorption equilibrium time of U(Ⅵ)in the disposal site soil was 20 d with 358 m L/g of the adsorption partition coefficient;U(Ⅵ)in groundwater of the disposal site was mainly in the form of UO_2(CO_3)_2~(2-) and UO_2(CO_3)_3~(4-); In 30 a of safe operation of the closed disposal site,the U(Ⅵ)mass concentration of soil in the disposal site centre will decrease by 4.20%,and that of soil at outer-ring 50 m and downstream boundary will be 3.40% and 1.32% of the initial value respectively;After 12 a of operation,only 0.10% of U(Ⅵ)will arrive at the riverside.
引文
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[20]徐真,陆春海,陈敏,等.铀在不同地区地下水中的种态模拟[J].核化学与放射化学,2015,37(3):184-188.
[21]易立新,徐鹤.地下水数值模拟:GMS应用基础与实例[M].北京:化学工业出版社,2009:98-99.
[2]Agency I A E.The safety case and safety assessment for the predisposal management of radioactive waste:General safety guide[M].Austria:International Atomic Energy Agency,2013:25-40.
[3]核工业标准化研究所.GB/T 28178—2011极低水平放射性废物的填埋处置[S].北京:中国标准出版社,2011.
[4]杨彬,方祥洪,王棋赟,等.国内外低、中水平放射性固体废物处置技术研究[J].核科学与技术,2015,3(2):17-21.
[5]赵杨军,李洋,顾志杰.低、中放固体废物处置场关闭后的景象分析[J].辐射防护通讯,2015,35(3):29-32.
[6]徐建华,赵昱龙,杜良,等.典型放射性核素在某极低放填埋场特定场址的迁移预测[J].核化学与放射化学,2015,37(2):105-109.
[7]杜良,王萍,李士诚,等.极低放废物填埋场防渗层对60Co和63Ni的阻滞性能[J].核技术,2017,40(3):39-45.
[8]Zhang Henghua,Zhao Xuan,Wei Jiying,et al.Removal of cesium from low-level radioactive wastewaters using magnetic potassium titanium hexacyanoferrate[J].Chem Eng J,2015,275:262-270.
[9]Ding Dexing,Xin Xin,Li Le,et al.Removal and recovery of U(Ⅵ)from low concentration radioactive wastewater by ethylenediamine-modified biomass of aspergillus niger[J].Water,Air,Soil Pollut,2014,225(12):1-16.
[10]韩非,侯若昕,顾平.亚铁氰化铜的制备及其对铯的吸附[J].化工环保,2015,35(1):84-88.
[11]罗洁,张海军,刘璟,等.碱激发粉煤灰对Cs+的吸附行为[J].化工环保,2015,35(2):192-198.
[12]杜浪,李玉香,马雪,等.偶氮胂Ⅲ分光光度法测定微量铀[J].冶金分析,2015,35(1):68-71.
[13]岳萍,庹先国,宿吉龙,等.239Pu在膨润土中的吸附和迁移实验研究[J].科学技术与工程,2014,14:168-172.
[14]邓晓颖,庹先国,李哲,等.238U、239Pu在板岩和土壤中迁移速度的实验模拟[J].环境化学,2012,31(12):1948-1952.
[15]窦妍,刘传富,鲁茹,等.水中溴离子含量测定方法的研究[J].应用化工,2013,42(5):936-938.
[16]中国地质调查局.水文地质手册[M].2版.北京:地质出版社,2012:241-253.
[17]地质矿产部地质环境管理司.GB/T 14848—1993地下水质量标准[S].北京:中国标准出版社,1994.
[18]Guillaumont R,Moman F J.Update on the chemical thermodynamics of uranium,neptunium,plutonium,americium and technetium[M].France:OECD Nuclear Energy Agence,2003:10-95.
[19]Parkhurst D L,Appelo C A J.User's guide to PHREEQC:A computer program for speciation,batchreaction,one-dimensional transport,and inverse geochemical calculations[R].Denver:U.S.Geological Survey,Earth Science Information Center,Open-File Reports Section,1999:99-4259.
[20]徐真,陆春海,陈敏,等.铀在不同地区地下水中的种态模拟[J].核化学与放射化学,2015,37(3):184-188.
[21]易立新,徐鹤.地下水数值模拟:GMS应用基础与实例[M].北京:化学工业出版社,2009:98-99.