Pu在地下水溶液中的形态及吸附行为
|
摘要
以GMZ膨润土为吸附介质,纯水和阿拉善某地下水为溶液,研究了Pu在GMZ膨润土中的吸附平衡时间关系、Pu初始浓度与吸附量的关系、不同浓度pH值对Pu的吸附影响.用PHREEQC软件模拟计算了水溶液中Pu的形态.研究表明,实验条件下GMZ膨润土对Pu的吸附平衡时间为20 h,中性环境中吸附效果大于酸性环境中的吸附效果,纯水溶液中的吸附效果大于阿拉善某地下水溶液中的吸附效果,通过模拟形态分析,溶液中的形态对吸附效果产生一定影响,在酸性溶液中主要是Pu~(3+),中性溶液中主要是Pu(OH)~(+3),碱性溶液中主要是Pu(OH)_4.
Adsorption kinetics of Pu in GMZ bentonite was studied in pure water and Alashan groundwater. The effect of initial concentration and p H on the adsorption of Pu in GMZ bentonite was investigated. Speciation of Pu in water was also calculated by PHREEQC simulation software. The results showed that adsorption of Pu in GMZ bentonite reached equilibrium after 20 h,and the adsorption of Pu in GMZ bentonite in neutral solution and pure water were better than that in acidic solution and Alashan groundwater,respectively. Simulation analysis results showed that speciation of Pu in acidic, neutral and alkaline solution were mainly Pu~(3+),Pu(OH)_3~+,and Pu( OH)_4,respectively.
Adsorption kinetics of Pu in GMZ bentonite was studied in pure water and Alashan groundwater. The effect of initial concentration and p H on the adsorption of Pu in GMZ bentonite was investigated. Speciation of Pu in water was also calculated by PHREEQC simulation software. The results showed that adsorption of Pu in GMZ bentonite reached equilibrium after 20 h,and the adsorption of Pu in GMZ bentonite in neutral solution and pure water were better than that in acidic solution and Alashan groundwater,respectively. Simulation analysis results showed that speciation of Pu in acidic, neutral and alkaline solution were mainly Pu~(3+),Pu(OH)_3~+,and Pu( OH)_4,respectively.
引文
[1]王孝强,李平川,冷阳春,等.水相环境中p H对Pu在膨润土中吸附行为的影响[J].原子能科学技术,2013,47(4):523-528.WANG X Q,LI P C,LENG Y C,et al.Effect of p H on the adsorption behavior of pu in bentonite in aqueous environment[J].Atomic Energy Science and Technology.2013,47(4):523-528(in Chinese).
[2]FRANCIS A J,DODGE C J.Microbial mobilization of plutonium and other actinides from contaminated soil[J].Journal of Environmental Radioactivity,2015,150:277-285.
[3]CHO H R,YOUN Y S,JUNG E C,et al.Hydrolysis of trivalent plutonium and solubility of Pu(OH)3(am)under electrolytic reducing conditions[J].Dalton Transactions,2016,45(48):19449-19457
[4]BANIK N L,BUDA R A,BRGER S.Speciation and interactions of plutonium with humic substances and kaolinite in aquifer systems[J].Journal of Alloys&Compounds,2007,444(24):522-525.
[5]MATSUNAGA T,NAGAO S,UENO T,et al.Association of dissolved radionuclides released by the Chernobyl accident with colloidal materials in surface water[J].Applied Geochemistry,2004,19(10):1581-1599.
[6]LUJANIEN G,BENE2 P,VOPALKA K,et al.Study of Pu(IV)and Am(III)sorption to clay minerals:Laboratory experiments and modeling[J].A Supplement to Radiochimica Acta,2011,1(1):237-244.
[7]PARKHURST D L,APPELO C A J.User's guide to phreeqc(version 2)-a compute program for speciation,batch-reaction,onedimensional transport,and inverse geochemical calculations[R].U.S.Geological Survey Water-Resources Investiations Report,1999,99.
[8]ALTMAIER M,GAONA X,FANGHNEL T.Recent advances in aqueous actinide chemistry and thermodynamics[J].Chemical Reviews,2013,113(2):901-943.
[9]GECKEIS H,LüTZENKIRCHEN J,POLLY R,et al.Mineral-water interface reactions of actinides[J].Chemical Reviews,2013,113(2):1016-1062.
[10]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,2016,48(8):816-822.JIANG C J,WANG X L,JIANG M L,et al.Using CHEMSPEC to simulate the distribution of Np and Pu in groundwater of Beishan and its adsorption on hydrated iron oxide[J].Chinese Science:Chemistry,2016,48(8):816-822(in Chinese).
[11]曾路,李予晋,王宗霞,等.有机膨润土在有机溶剂中微观形貌的研究[J].电子显微学报,2006,(S1):330.ZENG L,LI Y J,WANG Z X,et al.Study on micro-morphology of organic bentonite in organic solvents[J].Journal of Electron Microscopy,2006,(B08):330-330(in Chinese).
[12]SABODINA M N,KALMYKOV S N,SAPOZHNIKOV Y A.Neptunium,plutonium and 137 Cs sorption by bentonite clays and their speciation in pore waters[J].Journal of Radioanalytical and Nuclear Chemistry,2006,270(2):349-355
[13]SANTSCHI J M,SCHWANTES PETER H.Mechanisms of plutonium sorption to mineral oxide surfaces:New insights with implications for colloid-enhanced migration[J].Radiochimica Acta,2010,98(9-11):737-742.
[14]DZOMBAK D A,MOREL F.Surface complexation modeling:Hydrous ferric oxide[J].Surface Complexation Modeling Hydrous Ferric.Oxide,1990:97-108.
[2]FRANCIS A J,DODGE C J.Microbial mobilization of plutonium and other actinides from contaminated soil[J].Journal of Environmental Radioactivity,2015,150:277-285.
[3]CHO H R,YOUN Y S,JUNG E C,et al.Hydrolysis of trivalent plutonium and solubility of Pu(OH)3(am)under electrolytic reducing conditions[J].Dalton Transactions,2016,45(48):19449-19457
[4]BANIK N L,BUDA R A,BRGER S.Speciation and interactions of plutonium with humic substances and kaolinite in aquifer systems[J].Journal of Alloys&Compounds,2007,444(24):522-525.
[5]MATSUNAGA T,NAGAO S,UENO T,et al.Association of dissolved radionuclides released by the Chernobyl accident with colloidal materials in surface water[J].Applied Geochemistry,2004,19(10):1581-1599.
[6]LUJANIEN G,BENE2 P,VOPALKA K,et al.Study of Pu(IV)and Am(III)sorption to clay minerals:Laboratory experiments and modeling[J].A Supplement to Radiochimica Acta,2011,1(1):237-244.
[7]PARKHURST D L,APPELO C A J.User's guide to phreeqc(version 2)-a compute program for speciation,batch-reaction,onedimensional transport,and inverse geochemical calculations[R].U.S.Geological Survey Water-Resources Investiations Report,1999,99.
[8]ALTMAIER M,GAONA X,FANGHNEL T.Recent advances in aqueous actinide chemistry and thermodynamics[J].Chemical Reviews,2013,113(2):901-943.
[9]GECKEIS H,LüTZENKIRCHEN J,POLLY R,et al.Mineral-water interface reactions of actinides[J].Chemical Reviews,2013,113(2):1016-1062.
[10]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,2016,48(8):816-822.JIANG C J,WANG X L,JIANG M L,et al.Using CHEMSPEC to simulate the distribution of Np and Pu in groundwater of Beishan and its adsorption on hydrated iron oxide[J].Chinese Science:Chemistry,2016,48(8):816-822(in Chinese).
[11]曾路,李予晋,王宗霞,等.有机膨润土在有机溶剂中微观形貌的研究[J].电子显微学报,2006,(S1):330.ZENG L,LI Y J,WANG Z X,et al.Study on micro-morphology of organic bentonite in organic solvents[J].Journal of Electron Microscopy,2006,(B08):330-330(in Chinese).
[12]SABODINA M N,KALMYKOV S N,SAPOZHNIKOV Y A.Neptunium,plutonium and 137 Cs sorption by bentonite clays and their speciation in pore waters[J].Journal of Radioanalytical and Nuclear Chemistry,2006,270(2):349-355
[13]SANTSCHI J M,SCHWANTES PETER H.Mechanisms of plutonium sorption to mineral oxide surfaces:New insights with implications for colloid-enhanced migration[J].Radiochimica Acta,2010,98(9-11):737-742.
[14]DZOMBAK D A,MOREL F.Surface complexation modeling:Hydrous ferric oxide[J].Surface Complexation Modeling Hydrous Ferric.Oxide,1990:97-108.