The effects of the acid leaching and alkali fusion on the leaching efficiency of Y,Eu,Ce,and Tb from the waste rare earth fluorescent powders were investigated in this paper.The results show that hydrochloric acid is ...The effects of the acid leaching and alkali fusion on the leaching efficiency of Y,Eu,Ce,and Tb from the waste rare earth fluorescent powders were investigated in this paper.The results show that hydrochloric acid is better than sulfuric acid in the first acid leaching,and NaOH is better than Na2CO3in the alkali fusion.In the first acid leaching,the Wloss is 20.94%when the waste rare earth fluorescent powders are acid leached in H?concentration 3 mol L-1and S/L ratio 1:3 for 4 h due to red powders dissolved.The better results of the alkali fusion can be got at 800℃ for 2 h when the NaOH is used.The blue powders and the green powders can be dissolved into NaAlO2and oxides such as rare earth oxide(REO).The REO can be dissolved in H?concentration 5 mol L-1,S/L1:10 for 3 h in the second acid leaching.The leaching rates of the Y,Eu,Ce,and Tb are 99.06%,97.38%,98.22%,and 98.15%,respectively.The leaching rate of the total rare earth is 98.60%.展开更多
Low radioactive rare earth waste (containing 232 Th,specific activity 5 000 8 000 Bq·kg -1 ) were diluted 20 times by cement,sand and carbide ash and were made into special cement.The radioactivity of...Low radioactive rare earth waste (containing 232 Th,specific activity 5 000 8 000 Bq·kg -1 ) were diluted 20 times by cement,sand and carbide ash and were made into special cement.The radioactivity of this special cement complied with the healthy protect standard for radioactive materials (GB6566 86).Test results showed that this special cement could lower COD,the degradation rate increased as the time went on.In acidic medium,this special cement could remove E Coli effectively.Applying aeration and adding lumps of cement,the degradation of COD versus time complied with Logistic model through fitting by computer.The two “S” curves indicated that aeration and adding lumps of cement had synergistic action on sewage treatment.展开更多
In this study,a novel hydrometallurgical process consisting of hydrochloric acid three-stage countercurrent leaching and solvent extraction was proposed to recover rare earth oxide(REO)from the rare earth polishing po...In this study,a novel hydrometallurgical process consisting of hydrochloric acid three-stage countercurrent leaching and solvent extraction was proposed to recover rare earth oxide(REO)from the rare earth polishing powder waste(REPPW).The effects of HCl concentration,liquid-solid ratio(L/S ratio),temperature and time on the leaching yields of rare earths(in REO)and aluminum(in Al2O3)were studied.The result shows that the leaching yields of REO and Al2O3 are 90.96%and 43.89%respectively under the optimum leaching parameters of HCl concentration=8.00 mol/L,L/S ratio=4 mL/g,leaching temperature=353 K and leaching time=180 min.Meanwhile,the leaching kinetics of REO and Al2O3 were investigated in this study.The leaching behaviors of REO and Al2O3 follow a shrinking sphere/core model and the general leaching process is controlled by the surface chemical reaction.The leaching activation energies of REO and Al2O3 are 9.86 and 13.68 kJ/mol,respectively.The leaching yield of each substance in three-stage countercurrent leaching is improved substantially compared with single-stage leaching,with a change from 90.96%to 95.38%for REO and from 43.89%to 46.22%for Al2O3,respectively.Especially,the total concentration of REO in three-stage countercurrent leaching solution is greatly increased to above 300 g/L,and the acidity of which is decreased to ca.pH=2,which is conducive to subsequent solvent extraction directly.High purity REO(99.92%)is obtained by solvent extraction separation,oxalate precipitation and calcination.The total recovery yield of REO is 85.13%.展开更多
This study described a hydrometallurgical method to investigate the separation of rare earth elements(REEs)from rare earth polishing powder wastes(REPPWs)containing large amounts of rare earth oxides with a major ...This study described a hydrometallurgical method to investigate the separation of rare earth elements(REEs)from rare earth polishing powder wastes(REPPWs)containing large amounts of rare earth oxides with a major phase of CeO2 and minor phases of La2O3,Pr2O3,and Nd2O3 using a process devised by the authors.The suggested approach consisted of five processes:the synthesis of NaR E(SO4)2·xH2O from rare earth oxides in Na2SO4-H2SO4-H2 O solutions(Process 1),the conversion of NaR E(SO4)2·xH2O into RE(OH)3 using NaO H(Process 2),and the oxidation of Ce(OH)3 into Ce(OH)4 using air with O2 injection(Process 3),followed by Processes 4 and 5 for separation of REEs by acid leaching using HCl and H2SO4,respectively.To confirm the high yield of NaR E(SO4)2·xH2O in Process 1,experiments were carried out under various Na2SO4 concentrations(0.4–2.5 mol/L),sulfuric acid concentrations(6–14 mol/L),and reaction temperatures(95–125 oC).In addition,the effect of the pH value on the separation of Ce(OH)4 in HCl-H2 O solutions with Ce(OH)4,La-,Pr-,and Nd(OH)3 in Process 4 was also investigated.On the basis of above results,the possibility of effective separation of REEs from REPPWs could be confirmed.展开更多
Waste management of rare earth metals(REMs) containing materials and recycling of rare earth metals(REM) from waste materials are becoming more and more important due to high demand and resource exhaustion. Howeve...Waste management of rare earth metals(REMs) containing materials and recycling of rare earth metals(REM) from waste materials are becoming more and more important due to high demand and resource exhaustion. However, extraction of REM from waste fluorescent powder materials is difficult because of their special aluminate structure. A novel "alkaline roasting-acid leaching" process was developed in this study. The alkaline roasting process mechanism was examined using differential thermal analysis(DTA)-thermogravimetric(TG) measurements, and the roasting product was characterized by XRD analysis. In this process, Al_2O_3 was converted into water soluble NaAlO_2 via alkaline roasting, and NaAlO_ 2 in the roasting product could be easily dissolved in water, while the rare earth oxide(REOs) remained as solid. After filtration, REOs cake was leached using hydrochloric acid to achieve 99.8% of REM recovery. It was concluded that the alkaline roasting-acid leaching process could effectively separate Al_2O_3 and REOs with high REM recovery.展开更多
Leaching behavior and gastrointestinal bioaccessibility of rare earth elements (REEs) from hospital waste incineration (HWI) fly and bottom ash samples collected from Beijing and Nanjing Cities were assessed. In t...Leaching behavior and gastrointestinal bioaccessibility of rare earth elements (REEs) from hospital waste incineration (HWI) fly and bottom ash samples collected from Beijing and Nanjing Cities were assessed. In the same ash sample, the leaching concentrations of individual REEs determined by the Toxicity Characteristic Leaching Procedure (TCLP) were higher than those detected by the European standard protocol (EN-type test), thereby suggesting that the low pH value of leaching solution was an important factor influencing the leacha(bility-of REE. The REE bioaccessibility results, which were evaluated using the physiologically based extraction test (PBET), indicated that REEs were highly absorbed during fgastric phase by dissolution; and subsequently precipitated and/or re-adsorbed in small intestinal phase. The relative amounts of the total REEs extracted by the TCLP method, EN-type test and PBET test were compared. In addition to the pH value of extraction solutions, the chelating role of REEs witllt organic ligands used in the PBET method was also an important parameter affecting REE adsorption in human body. Additionally, this study showed that REEs were extracted by these methods as concomitants of heavy metals and anions (NO3^-, F^-, SO4^2- , and Cl^-) from HWI ash, which probably caused the remarkably complex toxicity on human body by the exposure pathway.展开更多
The chemical stability of simulated waste forms Zr_(1–x)Nd_xSiO_(4–x/2) was investigated using the static leach test(MCC-1) with lixiviants of three pH values(pH=4, 6.7 and 10) at three temperature points(4...The chemical stability of simulated waste forms Zr_(1–x)Nd_xSiO_(4–x/2) was investigated using the static leach test(MCC-1) with lixiviants of three pH values(pH=4, 6.7 and 10) at three temperature points(40, 90 and 150 oC) for periods ranging from 1 to 42 d, and the influence of temperature, pH, as well as their combined effects were explored in detail. The results showed that all the normalized release rate of Nd firstly decreased with leaching time and closed to equilibrium after 14 d. As the temperature increased, the normalized release rate of Nd also increased, but it was no more than 3×10^(–5) g/(m^2·d). And, the normalized release rate of Nd reached the highest values(~5×10^(–5) g/(m^2·d)) when pH=4, whilst the normalized release rate of Nd remained the lowest value(~1×10^(–5) g/(m^2·d)) near neutral environment(pH=6.7).展开更多
Zircon was employed to immobilize simulated tetravalentactinide nuclide(Ce^4+). Zr_(1–x)Ce_xSiO_4(0≤x≤0.10) ceramics were synthesized and their chemical durabilities were investigated systematically. The eff...Zircon was employed to immobilize simulated tetravalentactinide nuclide(Ce^4+). Zr_(1–x)Ce_xSiO_4(0≤x≤0.10) ceramics were synthesized and their chemical durabilities were investigated systematically. The effects of p H and temperature on the chemical durability of the as-prepared compounds were investigated using the MCC-1 static leaching test, and their coupling effects were also explored. It was found that the normalized release rates of Ce in deionized water and alkaline solutions(pH=10) were smaller than those in acid solutions(p H=4). At a certain p H value, the normalized release rate of Ce(LR Ce) increased with the temperature in the initial period. However, the leaching progress almost reached a balance after 14 days, and both of the p H and the temperature had slight impact on the leaching of Ce element. Moreover, the LR_(Ce) were below 10^(–5)g/m^2/d after 42 days, which was lower than those of other nuclear waste forms in all discussed leachates.展开更多
基金supported by the National Hi-Tech R&D Program of China (No. 2012AA063202)National Key Project of Scientific and Technical Support Program of China (Nos. 2011BAE13B07, 2012BAC02B01, and 2011BAC10B02)National Natural Science Foundation of China (Nos. 51174247 and 50972013)
文摘The effects of the acid leaching and alkali fusion on the leaching efficiency of Y,Eu,Ce,and Tb from the waste rare earth fluorescent powders were investigated in this paper.The results show that hydrochloric acid is better than sulfuric acid in the first acid leaching,and NaOH is better than Na2CO3in the alkali fusion.In the first acid leaching,the Wloss is 20.94%when the waste rare earth fluorescent powders are acid leached in H?concentration 3 mol L-1and S/L ratio 1:3 for 4 h due to red powders dissolved.The better results of the alkali fusion can be got at 800℃ for 2 h when the NaOH is used.The blue powders and the green powders can be dissolved into NaAlO2and oxides such as rare earth oxide(REO).The REO can be dissolved in H?concentration 5 mol L-1,S/L1:10 for 3 h in the second acid leaching.The leaching rates of the Y,Eu,Ce,and Tb are 99.06%,97.38%,98.22%,and 98.15%,respectively.The leaching rate of the total rare earth is 98.60%.
文摘Low radioactive rare earth waste (containing 232 Th,specific activity 5 000 8 000 Bq·kg -1 ) were diluted 20 times by cement,sand and carbide ash and were made into special cement.The radioactivity of this special cement complied with the healthy protect standard for radioactive materials (GB6566 86).Test results showed that this special cement could lower COD,the degradation rate increased as the time went on.In acidic medium,this special cement could remove E Coli effectively.Applying aeration and adding lumps of cement,the degradation of COD versus time complied with Logistic model through fitting by computer.The two “S” curves indicated that aeration and adding lumps of cement had synergistic action on sewage treatment.
基金Project supported by National High-tech Research and Development Program(2017AA031002)。
文摘In this study,a novel hydrometallurgical process consisting of hydrochloric acid three-stage countercurrent leaching and solvent extraction was proposed to recover rare earth oxide(REO)from the rare earth polishing powder waste(REPPW).The effects of HCl concentration,liquid-solid ratio(L/S ratio),temperature and time on the leaching yields of rare earths(in REO)and aluminum(in Al2O3)were studied.The result shows that the leaching yields of REO and Al2O3 are 90.96%and 43.89%respectively under the optimum leaching parameters of HCl concentration=8.00 mol/L,L/S ratio=4 mL/g,leaching temperature=353 K and leaching time=180 min.Meanwhile,the leaching kinetics of REO and Al2O3 were investigated in this study.The leaching behaviors of REO and Al2O3 follow a shrinking sphere/core model and the general leaching process is controlled by the surface chemical reaction.The leaching activation energies of REO and Al2O3 are 9.86 and 13.68 kJ/mol,respectively.The leaching yield of each substance in three-stage countercurrent leaching is improved substantially compared with single-stage leaching,with a change from 90.96%to 95.38%for REO and from 43.89%to 46.22%for Al2O3,respectively.Especially,the total concentration of REO in three-stage countercurrent leaching solution is greatly increased to above 300 g/L,and the acidity of which is decreased to ca.pH=2,which is conducive to subsequent solvent extraction directly.High purity REO(99.92%)is obtained by solvent extraction separation,oxalate precipitation and calcination.The total recovery yield of REO is 85.13%.
文摘This study described a hydrometallurgical method to investigate the separation of rare earth elements(REEs)from rare earth polishing powder wastes(REPPWs)containing large amounts of rare earth oxides with a major phase of CeO2 and minor phases of La2O3,Pr2O3,and Nd2O3 using a process devised by the authors.The suggested approach consisted of five processes:the synthesis of NaR E(SO4)2·xH2O from rare earth oxides in Na2SO4-H2SO4-H2 O solutions(Process 1),the conversion of NaR E(SO4)2·xH2O into RE(OH)3 using NaO H(Process 2),and the oxidation of Ce(OH)3 into Ce(OH)4 using air with O2 injection(Process 3),followed by Processes 4 and 5 for separation of REEs by acid leaching using HCl and H2SO4,respectively.To confirm the high yield of NaR E(SO4)2·xH2O in Process 1,experiments were carried out under various Na2SO4 concentrations(0.4–2.5 mol/L),sulfuric acid concentrations(6–14 mol/L),and reaction temperatures(95–125 oC).In addition,the effect of the pH value on the separation of Ce(OH)4 in HCl-H2 O solutions with Ce(OH)4,La-,Pr-,and Nd(OH)3 in Process 4 was also investigated.On the basis of above results,the possibility of effective separation of REEs from REPPWs could be confirmed.
基金Supported by National Natural Science Foundation of China(51464012)Natural Science Foundation of Jiangxi(20114 bab206031)the Natural Science Foundation of Jiangxi University of Science and Technology(NSFJ2015-G09)
文摘Waste management of rare earth metals(REMs) containing materials and recycling of rare earth metals(REM) from waste materials are becoming more and more important due to high demand and resource exhaustion. However, extraction of REM from waste fluorescent powder materials is difficult because of their special aluminate structure. A novel "alkaline roasting-acid leaching" process was developed in this study. The alkaline roasting process mechanism was examined using differential thermal analysis(DTA)-thermogravimetric(TG) measurements, and the roasting product was characterized by XRD analysis. In this process, Al_2O_3 was converted into water soluble NaAlO_2 via alkaline roasting, and NaAlO_ 2 in the roasting product could be easily dissolved in water, while the rare earth oxide(REOs) remained as solid. After filtration, REOs cake was leached using hydrochloric acid to achieve 99.8% of REM recovery. It was concluded that the alkaline roasting-acid leaching process could effectively separate Al_2O_3 and REOs with high REM recovery.
基金Acknowledgements We would like to acknowledge all of the participators who collected HWI ash samples for this study from both the Beijing and Nanjing sites. This work was financially supported by the National Natural Science Foundation of China (Grant No. 51378180), the Technology Department of the Henan Science and Technology Fund Project (Nos. 142102210457 and 142102210456), and the Fundamental Research Funds for the Central Universities (No. 30916014102).
文摘Leaching behavior and gastrointestinal bioaccessibility of rare earth elements (REEs) from hospital waste incineration (HWI) fly and bottom ash samples collected from Beijing and Nanjing Cities were assessed. In the same ash sample, the leaching concentrations of individual REEs determined by the Toxicity Characteristic Leaching Procedure (TCLP) were higher than those detected by the European standard protocol (EN-type test), thereby suggesting that the low pH value of leaching solution was an important factor influencing the leacha(bility-of REE. The REE bioaccessibility results, which were evaluated using the physiologically based extraction test (PBET), indicated that REEs were highly absorbed during fgastric phase by dissolution; and subsequently precipitated and/or re-adsorbed in small intestinal phase. The relative amounts of the total REEs extracted by the TCLP method, EN-type test and PBET test were compared. In addition to the pH value of extraction solutions, the chelating role of REEs witllt organic ligands used in the PBET method was also an important parameter affecting REE adsorption in human body. Additionally, this study showed that REEs were extracted by these methods as concomitants of heavy metals and anions (NO3^-, F^-, SO4^2- , and Cl^-) from HWI ash, which probably caused the remarkably complex toxicity on human body by the exposure pathway.
基金Project supported by the National Natural Science Foundation of China(41302028,41302029,21507105)Thousand Youth Talents Plan(Y42H831301)+3 种基金Key Project of Sichuan Education Department(14ZA0099,15ZB0116)Foundation of Laboratory of National Defense Key Discipline for Nuclear Waste and Environmental Safety,Southwest University of Science and Technology(15yyhk10)the Doctor Foundation in Southwest University of Science and Technology(10zx7126)Hebei Science and Technology Support Program(15211121)
文摘The chemical stability of simulated waste forms Zr_(1–x)Nd_xSiO_(4–x/2) was investigated using the static leach test(MCC-1) with lixiviants of three pH values(pH=4, 6.7 and 10) at three temperature points(40, 90 and 150 oC) for periods ranging from 1 to 42 d, and the influence of temperature, pH, as well as their combined effects were explored in detail. The results showed that all the normalized release rate of Nd firstly decreased with leaching time and closed to equilibrium after 14 d. As the temperature increased, the normalized release rate of Nd also increased, but it was no more than 3×10^(–5) g/(m^2·d). And, the normalized release rate of Nd reached the highest values(~5×10^(–5) g/(m^2·d)) when pH=4, whilst the normalized release rate of Nd remained the lowest value(~1×10^(–5) g/(m^2·d)) near neutral environment(pH=6.7).
基金Project supported by the National Natural Science Foundation of China(21507105,41302029)Thousand Youth Talents Plan(Y42H831301)+3 种基金Key Project of Sichuan Education Department(15ZB0116)Foundation of Laboratory of National Defense Key Discipline for Nuclear Waste and Environmental Safety,Southwest University of Science and Technology(15yyhk10)the Doctor Foundation in Southwest University of Science and Technology(10zx7126)Sichuan’s Training Program of Innovation and Entrepreneurship for Undergraduate(201610619039)
文摘Zircon was employed to immobilize simulated tetravalentactinide nuclide(Ce^4+). Zr_(1–x)Ce_xSiO_4(0≤x≤0.10) ceramics were synthesized and their chemical durabilities were investigated systematically. The effects of p H and temperature on the chemical durability of the as-prepared compounds were investigated using the MCC-1 static leaching test, and their coupling effects were also explored. It was found that the normalized release rates of Ce in deionized water and alkaline solutions(pH=10) were smaller than those in acid solutions(p H=4). At a certain p H value, the normalized release rate of Ce(LR Ce) increased with the temperature in the initial period. However, the leaching progress almost reached a balance after 14 days, and both of the p H and the temperature had slight impact on the leaching of Ce element. Moreover, the LR_(Ce) were below 10^(–5)g/m^2/d after 42 days, which was lower than those of other nuclear waste forms in all discussed leachates.