PHREEQC在Pu的种态分布及废水处理中的应用
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摘要
为了探究不同水化学条件下Pu的种态分布,对含Pu废水的处理提供指导,通过地球化学软件PHREEQC对Pu的种态进行了模拟。结果表明:Pu对环境的氧化还原条件十分敏感,p H在2～12范围内增加时,Pu的主要价态不断升高,水解程度变大;随着pe的提高,Pu的主要价态不断升高。不同价态Pu的络合(水解)能力大小为:Pu(IV)>Pu(VI)≈Pu(Ⅲ)>Pu(Ⅴ);对于指定价态Pu,与各离子络合能力大小为:OH~-、CO_3~(2-)>F~-、SO_4~(2-)>Cl~-、NO_3~-;反渗透对离子半径大、所带电荷高的种态截留率更高。
In order to explore the distribution of Pu species under different hydrochemical conditions and provide guidance for the treatment of Pu containing wastewater,the species of Pu was simulated by geochemical software PHREEQC.Pu is very sensitive to the redox conditions of the environment.With the increase of p H in the range of 2～12,the main valence state of Pu increases and the degree of hydrolysis increases.The complexation(hydrolysis)ability of different valence Pu is:Pu(Ⅳ)>Pu(Ⅵ)≈Pu(Ⅲ)>Pu(Ⅴ).For the specified valence of Pu,the complexation ability of various ions is:OH~-,CO~(2-)_3>F~-,SO~(2-)_4>Cl~-,NO~-_3.Reverse osmosis membrane has higher rejection rate for species with large ion radius and high charge.
In order to explore the distribution of Pu species under different hydrochemical conditions and provide guidance for the treatment of Pu containing wastewater,the species of Pu was simulated by geochemical software PHREEQC.Pu is very sensitive to the redox conditions of the environment.With the increase of p H in the range of 2～12,the main valence state of Pu increases and the degree of hydrolysis increases.The complexation(hydrolysis)ability of different valence Pu is:Pu(Ⅳ)>Pu(Ⅵ)≈Pu(Ⅲ)>Pu(Ⅴ).For the specified valence of Pu,the complexation ability of various ions is:OH~-,CO~(2-)_3>F~-,SO~(2-)_4>Cl~-,NO~-_3.Reverse osmosis membrane has higher rejection rate for species with large ion radius and high charge.
引文
1 Boggs M A,Dai Z,Kersting A B,et al. Plutonium(Ⅳ)sorption to montmorillonite in the presence of organic matter[J]. Journal of Environmental Radioactivity,2015,141(141C):90-96
2 Ruhela R,Panja S,Singh A K,et al. BenzoDODA grafted polymeric resin—Plutonium selective solid sorbent[J]. Journal of Hazardous Materials,2016,318:186-193
3 Bhanushali R D,Pathak S S,Pius I C,et al. Recovery of plutonium from aqueous waste solutions using porous zirconia spherical particles[J]. Journal of Radioanalytical&Nuclear Chemistry,2010,285(3):647-651
4 SchulteHerbrüggen H M A,Semio A J C,Chaurand P,et al. Effect of pH and pressure on Uranium removal from drinking water using NF/RO membranes[J]. Environmental Science&Technology,2016,50(11):5817-5824
5 成建峰,冷阳春,庹先国,等. pH对U、Pu的吸附影响[J].核化学与放射化学,2017,39(3):213-217Cheng Jianfeng,Leng Yangchun,Tuo Xianguo,et al. Effect of pH on adsorption characteristics of Uranium and Plutonium[J]. Journal of Nuclear and Radiochemistry,2017,39(3):213-217
6 成建峰,冷阳春,朱杉,等. Pu在处置库地下水中的种态模拟及影响特征[J].环境工程,2017,35(8):11-14Cheng Jianfeng,Leng Yangchun,Zhu Shan,et al. Speciation simulation and influence of plutonium in groundwater of disposal repository[J]. Environment Engineering,2017,35(8):11-14
7 蒋京呈,王晓丽,蒋美玲,等.利用CHEMSPEC模拟计算Np和Pu在北山地下水中的种态分布及其在水合氧化铁上的吸附[J].中国科学(化学),2016,46(8):816-822Jiang Jingcheng,Wang Xiaoli,Jiang Meiling,et al. Speciation distribution of Np and Pu in beishan groundwater and sorption on hydrous ferric oxide calculated by CHEMSPEC[J]. Science ChinaChemistry,2016,46(8):816-822
8 Guillaumont R,Fanghanel T H,Neck V,et al. Update on the chemical thermodynamics of uranium,neptunium,plutonium,americium and technetium[M]. New York:Elsevier B V,2003
9 Lemire R J,Fuger J,Nitsche H,et al. Chemical thermodynamics of neptunium and plutonium[M]. Amsterdam:North Holland Elsevier Science Publisher B V,2001:37-83
10 Zhao P,Begg J D,Zavarin M,et al. Plutonium(Ⅳ)and(Ⅴ)sorption to Goethite at sub-femtomolar to micromolar concentrations:Redox transformations and surface precipitation[J]. Environmental Science&Technology,2016,50(13):6948-6956
11 Kaplan D I,Powell B A,Duff M C,et al. Influence of sources on plutonium mobility and oxidation state transformations in vadose zone sediments[J]. Environmental Science&Technology,2007,41(21):7417-7423
12 Choppin G R. Redox speciation of plutonium in natural waters[J].Journal of Radioanalytical&Nuclear Chemistry,1991,147(1):109-116
2 Ruhela R,Panja S,Singh A K,et al. BenzoDODA grafted polymeric resin—Plutonium selective solid sorbent[J]. Journal of Hazardous Materials,2016,318:186-193
3 Bhanushali R D,Pathak S S,Pius I C,et al. Recovery of plutonium from aqueous waste solutions using porous zirconia spherical particles[J]. Journal of Radioanalytical&Nuclear Chemistry,2010,285(3):647-651
4 SchulteHerbrüggen H M A,Semio A J C,Chaurand P,et al. Effect of pH and pressure on Uranium removal from drinking water using NF/RO membranes[J]. Environmental Science&Technology,2016,50(11):5817-5824
5 成建峰,冷阳春,庹先国,等. pH对U、Pu的吸附影响[J].核化学与放射化学,2017,39(3):213-217Cheng Jianfeng,Leng Yangchun,Tuo Xianguo,et al. Effect of pH on adsorption characteristics of Uranium and Plutonium[J]. Journal of Nuclear and Radiochemistry,2017,39(3):213-217
6 成建峰,冷阳春,朱杉,等. Pu在处置库地下水中的种态模拟及影响特征[J].环境工程,2017,35(8):11-14Cheng Jianfeng,Leng Yangchun,Zhu Shan,et al. Speciation simulation and influence of plutonium in groundwater of disposal repository[J]. Environment Engineering,2017,35(8):11-14
7 蒋京呈,王晓丽,蒋美玲,等.利用CHEMSPEC模拟计算Np和Pu在北山地下水中的种态分布及其在水合氧化铁上的吸附[J].中国科学(化学),2016,46(8):816-822Jiang Jingcheng,Wang Xiaoli,Jiang Meiling,et al. Speciation distribution of Np and Pu in beishan groundwater and sorption on hydrous ferric oxide calculated by CHEMSPEC[J]. Science ChinaChemistry,2016,46(8):816-822
8 Guillaumont R,Fanghanel T H,Neck V,et al. Update on the chemical thermodynamics of uranium,neptunium,plutonium,americium and technetium[M]. New York:Elsevier B V,2003
9 Lemire R J,Fuger J,Nitsche H,et al. Chemical thermodynamics of neptunium and plutonium[M]. Amsterdam:North Holland Elsevier Science Publisher B V,2001:37-83
10 Zhao P,Begg J D,Zavarin M,et al. Plutonium(Ⅳ)and(Ⅴ)sorption to Goethite at sub-femtomolar to micromolar concentrations:Redox transformations and surface precipitation[J]. Environmental Science&Technology,2016,50(13):6948-6956
11 Kaplan D I,Powell B A,Duff M C,et al. Influence of sources on plutonium mobility and oxidation state transformations in vadose zone sediments[J]. Environmental Science&Technology,2007,41(21):7417-7423
12 Choppin G R. Redox speciation of plutonium in natural waters[J].Journal of Radioanalytical&Nuclear Chemistry,1991,147(1):109-116