Separation of the minor actinides(Am and Cm)from lanthanides in high-level liquid wastes(HLLW)is one of the most challenging chemical separation tasks known owing to their chemical similarities and is highly significa...Separation of the minor actinides(Am and Cm)from lanthanides in high-level liquid wastes(HLLW)is one of the most challenging chemical separation tasks known owing to their chemical similarities and is highly significant in nuclear fuel reprocessing plants because it could practically lead to sustainable nuclear energy by closing the nuclear fuel cycle.The solid phase extraction is proposed to be a possible strategy but all reported sorbent materials severely suffer from limited stability and/or efficiency caused by the harsh conditions of high acidity coupled with intense irradiation.Herein,a phenanthroline-based polymeric organic framework(PhenTAPB-POF)was designed and tested for the separation of trivalent americium from lanthanides for the first time.Due to its fully conjugated structure,PhenTAPB-POF exhibits previously unachieved stability under the combined extreme conditions of strong acids and high irradiation field.The americium partitioning experiment indicates that PhenTAPB-POF possesses an ultrahigh adsorption selectivity towards Am(Ⅲ)over lanthanides(e.g.,SFAm(Ⅲ)/Eu(Ⅲ)=3326)in highly acidic simulated HLLW and relatively fast adsorption kinetics in both static and dynamic experiments.Am(Ⅲ)can be almost quantitatively eluted from the PhenTAPB-POF packed-column using a concentrated nitric acid elution.The high stability and superior separation performance endow PhenTAPB-POF with the promising alternative for separating minor actinides over lanthanides from highly acidic HLLW streams.展开更多
A process for actinide(Ⅲ)and lanthanum(Ⅲ)extraction separation from high-level liquid waste(HLLW)was proposed,with N,N,N’,N’-tetraoctyl diglycolamide(TODGA)as the extractant,tri-n–butyl phosphate(TBP)as the phase...A process for actinide(Ⅲ)and lanthanum(Ⅲ)extraction separation from high-level liquid waste(HLLW)was proposed,with N,N,N’,N’-tetraoctyl diglycolamide(TODGA)as the extractant,tri-n–butyl phosphate(TBP)as the phase modifier and 2,6-bis[1-(propan-1-ol)-1,2,3-triazol-4-yl]pyridine(PyTri-Diol or PTD)as hydrophilic stripping agent.This‘hot test’was successfully carried out,achieving 99.92%removal of americium-241(^(241)Am)with a separation factor SF(Eu/Am)of 3.8×10^(3)in the actinide(Ⅲ)product solution.The results show that bisamide podand extractants can effectively realize the extraction and separation of actinide(Ⅲ)and lanthanum(Ⅲ)from Chinese commercial HLLW and thus have a bright practical application potential for the treatment of commercial HLLW.展开更多
基金supported by the grants from the National Natural Science Foundation of China(Nos.21825601,21790374,and 21806117)。
文摘Separation of the minor actinides(Am and Cm)from lanthanides in high-level liquid wastes(HLLW)is one of the most challenging chemical separation tasks known owing to their chemical similarities and is highly significant in nuclear fuel reprocessing plants because it could practically lead to sustainable nuclear energy by closing the nuclear fuel cycle.The solid phase extraction is proposed to be a possible strategy but all reported sorbent materials severely suffer from limited stability and/or efficiency caused by the harsh conditions of high acidity coupled with intense irradiation.Herein,a phenanthroline-based polymeric organic framework(PhenTAPB-POF)was designed and tested for the separation of trivalent americium from lanthanides for the first time.Due to its fully conjugated structure,PhenTAPB-POF exhibits previously unachieved stability under the combined extreme conditions of strong acids and high irradiation field.The americium partitioning experiment indicates that PhenTAPB-POF possesses an ultrahigh adsorption selectivity towards Am(Ⅲ)over lanthanides(e.g.,SFAm(Ⅲ)/Eu(Ⅲ)=3326)in highly acidic simulated HLLW and relatively fast adsorption kinetics in both static and dynamic experiments.Am(Ⅲ)can be almost quantitatively eluted from the PhenTAPB-POF packed-column using a concentrated nitric acid elution.The high stability and superior separation performance endow PhenTAPB-POF with the promising alternative for separating minor actinides over lanthanides from highly acidic HLLW streams.
文摘A process for actinide(Ⅲ)and lanthanum(Ⅲ)extraction separation from high-level liquid waste(HLLW)was proposed,with N,N,N’,N’-tetraoctyl diglycolamide(TODGA)as the extractant,tri-n–butyl phosphate(TBP)as the phase modifier and 2,6-bis[1-(propan-1-ol)-1,2,3-triazol-4-yl]pyridine(PyTri-Diol or PTD)as hydrophilic stripping agent.This‘hot test’was successfully carried out,achieving 99.92%removal of americium-241(^(241)Am)with a separation factor SF(Eu/Am)of 3.8×10^(3)in the actinide(Ⅲ)product solution.The results show that bisamide podand extractants can effectively realize the extraction and separation of actinide(Ⅲ)and lanthanum(Ⅲ)from Chinese commercial HLLW and thus have a bright practical application potential for the treatment of commercial HLLW.
