A new kind of diamide N,N,N’,N’-tetrahexylsuccinylamide(THSA) was synthesized, characterized and used for the extraction of HNO3, U(VI) and TI(IV) in a diluent composed of 0.5 volume fraction 1,2,4-trimethy be...A new kind of diamide N,N,N’,N’-tetrahexylsuccinylamide(THSA) was synthesized, characterized and used for the extraction of HNO3, U(VI) and TI(IV) in a diluent composed of 0.5 volume fraction 1,2,4-trimethy benzene(TMB) and 0.5 volume fraction kerosene(OK). Extraction distribution coefficients of U(VI) and TI(IV) as functions of aque- ous nitric acid concentration, extractant concentration, temperature and salting-out agent (LiNO3 ) have been studied, and it is found that THSA as an extractant is superior to TBP for extraction of U(VI) and TI(IV). Back extraction was also studied. At low acidity, the main adduct of THSA and HNO3 is HNO3.THSA. THSA.(HNO3)2 and THSA.(HNO3)3 are also found at high acidity. The compositions of extracted species, apparent equilibrium constants and enthalpies of extraction reactions have also been calculated.展开更多
Extraction behavior of thorium(Ⅳ) and uranium(Ⅵ) from nitric acid(HNO_3) was studied using N,N,N',N'-tetraoctyldiglycolamide(TODGA) as extractant in different ionic liquids, and isooctane as comparison.Slope...Extraction behavior of thorium(Ⅳ) and uranium(Ⅵ) from nitric acid(HNO_3) was studied using N,N,N',N'-tetraoctyldiglycolamide(TODGA) as extractant in different ionic liquids, and isooctane as comparison.Slope analyses with varying HNO_3 concentrations and diluents revealed the extraction mechanism. With increasing length of alkyl chain and HNO_3 concentration, the extraction mechanism of TODGA/IL system changed from cation exchange to neutral complex and/or anion exchange,and the molar ratio between TODGA and metal ions varied gradually from 2:1 to 1:1 for Th(Ⅳ) and 3:1 to 1:1 for U(Ⅵ). The kinetics and thermodynamic studies of Th(Ⅳ)and U(Ⅵ) by the best TODGA/[C_2mim][NTf_2] system showed that the extraction equilibrium was reached within 2 h and extraction reactions were endothermic. Compared to TODGA/isooctane system, TODGA/[C_2mim][NTf_2]system presented higher radiation stability under c-irradiation. Therefore, it would have a promising application in spent fuel reprocessing.展开更多
文摘A new kind of diamide N,N,N’,N’-tetrahexylsuccinylamide(THSA) was synthesized, characterized and used for the extraction of HNO3, U(VI) and TI(IV) in a diluent composed of 0.5 volume fraction 1,2,4-trimethy benzene(TMB) and 0.5 volume fraction kerosene(OK). Extraction distribution coefficients of U(VI) and TI(IV) as functions of aque- ous nitric acid concentration, extractant concentration, temperature and salting-out agent (LiNO3 ) have been studied, and it is found that THSA as an extractant is superior to TBP for extraction of U(VI) and TI(IV). Back extraction was also studied. At low acidity, the main adduct of THSA and HNO3 is HNO3.THSA. THSA.(HNO3)2 and THSA.(HNO3)3 are also found at high acidity. The compositions of extracted species, apparent equilibrium constants and enthalpies of extraction reactions have also been calculated.
基金financially supported by the National Natural Science Foundation of China(No.11475112)the Ph.D. Programs Foundation of Ministry of Education of China(No.20130073120051)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning
文摘Extraction behavior of thorium(Ⅳ) and uranium(Ⅵ) from nitric acid(HNO_3) was studied using N,N,N',N'-tetraoctyldiglycolamide(TODGA) as extractant in different ionic liquids, and isooctane as comparison.Slope analyses with varying HNO_3 concentrations and diluents revealed the extraction mechanism. With increasing length of alkyl chain and HNO_3 concentration, the extraction mechanism of TODGA/IL system changed from cation exchange to neutral complex and/or anion exchange,and the molar ratio between TODGA and metal ions varied gradually from 2:1 to 1:1 for Th(Ⅳ) and 3:1 to 1:1 for U(Ⅵ). The kinetics and thermodynamic studies of Th(Ⅳ)and U(Ⅵ) by the best TODGA/[C_2mim][NTf_2] system showed that the extraction equilibrium was reached within 2 h and extraction reactions were endothermic. Compared to TODGA/isooctane system, TODGA/[C_2mim][NTf_2]system presented higher radiation stability under c-irradiation. Therefore, it would have a promising application in spent fuel reprocessing.