Method for isolating and purifying 90Y From 90strontium in multi-curie quantities

Information

  • Patent Grant
  • 6309614
  • Patent Number
    6,309,614
  • Date Filed
    Friday, April 14, 2000
    24 years ago
  • Date Issued
    Tuesday, October 30, 2001
    22 years ago
Abstract
The invention relates to a process for separating and purifying multi-curie quantities 90Y of sufficient chemical and radiochemical purity suitable for use in medical applications without a series of 90Sr selective extraction chromatographic columns while minimizing loss of radioactive 90Sr parent and waste stream. The process includes dissolving a nitrate salt of an original 90Sr stock solution in H2O creating a strontium nitrate solution; acidifying the strontium nitrate solution containing 90Y with concentrated nitric acid; evaporating the strontium nitrate solution; filtering or centrifuging strontium nitrate solution to separate crystalline 90Sr nitrate salt from the solution; evaporating the remaining 90Y enriched supernate to dryness; dissolving the remaining 90Y enriched supernate in a strong acid; passing the solution through an yttrium selective extraction chromatographic column; rinsing the yttrium selective extraction chromatographic column with strong acid; and eluting yttrium from yttrium selective extraction column with strong acid.
Description




FIELD OF THE INVENTION




This invention relates to a new process of separating and purifying multi-curie quantities of yttrium-90 from strontium-90 and other trace elements and impurities while minimizing loss of strontium and amount of waste generated.




BACKGROUND OF THE INVENTION




Although the possibility of treating rheumatoid arthritis, other inflamed joints, and cancer with yttrium-90 (


90




39


Y) is well known, a cost effective way to separate


90


Y of sufficient purify that minimizes loss of radioactive Sr and does not generate a large waste stream is still needed.


90


Y results from the decay of strontium-90 and


90


Y decays to stable


90


Zr according to the following scheme:










38
90


Sr














29





Years
















39
90


Y

+


B
-







(

0.54





MeV

)




;







39
90


Y














64.0





hours












40
90


Zr

+


B
-







(

2.28





MeV

)















90


Y has a relatively short half-life (64.0 h) and maximum beta energy (2.28 MeV) which makes it suitable for a variety of therapeutic uses such as radiolabeling antibodies for tumor therapy or treating liver malignancies.




Although it is known that


90


Y is suitable for immuno radiotherapy, scientists and doctors have encountered numerous difficulties using


90


Y for medical treatments because of the absence of a cost effective way to separate


90


Y of sufficient purity while minimizing loss of radioactive Sr without generating a large waste stream. The following non-exclusive non-exhaustive list of difficulties in separating and purifying


90


Y have limited the application of


90


Y for medical treatment. Although the half-life and decay scheme of


90


Y is appropriate for various radio therapy applications,


90


Y must be capable of being produced in sufficient multi-curie quantities. Furthermore, before


90


Y can be safely used in clinical applications,


90


Y must be essentially free of


90


Sr and any other trace elements.


90


Y must be free of


90


Sr by at least a factor of 10


7


because


90


Sr can suppress bone marrow production.


90


Y must also be free from any trace elements, such as Ca, Cu, Fe, Zn, and Zr, and other impurities because trace elements could interfere with the radio labeling process by competing with


90


Y for binding sites. All of these difficulties must be overcome in a cost effective manner while minimizing loss of valuable radioactive Sr without generating large amounts of waste.




In the past,


90


Y has been separated from


90


Sr by solvent extraction, ion-exchange, precipitation, and various forms of chromatography, all of which fail to separate


90


Y of sufficient quantity and purity in a cost effective manner that minimizes loss of radioactive Sr and does not generate a large waste stream. Numerous procedures use a cation exchange resin (e.g. Dowex 50) to retain


90


Sr, while the


90


Y is eluted with an aqueous solution such as lactate, acetate, citrate, oxalate, or EDTA. Several of these procedures have been proposed as the basis for a


90


Y generator system.




U.S. Pat. No. 5,100,585, and U.S. Pat. No. 5,344,623 describe processes for recovering strontium and technetium from acidic feed solutions containing other fission products.




Another process for separating


90


Y from


90


Sr involves extracting


90


Y from a dilute acid solution of


90


Sr/


90


Y using bis 2-ethylhexyl phosphoric acid in dodecane. This procedure has the disadvantages of having a limited generator lifespan and accumulating radiolytic by-products in the


90


Sr stock. This process also has the disadvantage of requiring repeated stripping of the initial extractant solution to reduce trace impurities and repeated washing of stock solution to destroy dissolved organic phosphates.




Kanapilly and Newton (1971) have described a process for separating multi-curie quantities of


90


Y from


90


Sr by precipitating


90


Y as a phosphate. This process, however, requires adding nonradioactive yttrium as a carrier, yielding


90


Y which are obviously not carrier free and hence unsuitable for site specific binding. This and other prior art teach the addition of only nonradioactive yttrium. This and other prior art do not teach the addition of nonradioactive strontium. In fact, the prior art teaches away from adding nonradioactive strontium.




U.S. Pat. No. 5,368,736 describes a process for isolating


90


Y from a stock solution of


90


Sr. The


90


Sr solution is stored for a sufficient period of time to allow


90


Y ingrowth to occur. This process teaches the use of a series of Sr selective columns at the initial stages of the process. A major disadvantage is that


90


Sr must be stripped off from each of the strontium-selective extraction chromatographic column because


90


Sr is very valuable and it must be recycled to allow for new


90


Y growth.




Unfortunately, all the various methods mentioned above suffer from one or more of the following disadvantages. The first disadvantage of these methods is that the concentration of trace elements is too high and the trace elements thereby compete with


90


Y for binding sites, resulting in a decrease in


90


Y labeling. Thus, it is necessary to either remove trace elements and other impurities prior to antibody labeling or carry out postlabeling purification. The second disadvantage is that ion-exchange resins gradually lose capacity due to radiation damage. As a result, ion-exchange is considered suitable only for purifying and separating subcurie quantities of


90


Y, which is less than the multi quantities of


90


Y needed for clinical applications. The third disadvantage is that separating


90


Y in acceptable purity and quantity while minimizing


90


Sr breakthrough often requires using a series of long ion-exchange columns and impractically large volumes of eluent. A need still exists for a cost effective process of separating


90


Y of sufficient quality and quantity without a series of


90


Sr selective extraction chromatographic columns while minimizing loss of


90


Sr and without generating large amounts of waste and using large volumes of eluent.




SUMMARY OF THE INVENTION




This invention relates to a new process for separating and purifying multi-curie quantities


90


Y of sufficient chemical and radiochemical purity suitable for use in medical applications without a series of


90


Sr selective extraction chromatographic columns while minimizing loss of radioactive


90


Sr parent and waste stream.




It is an object of the invention to separate


90


Y from Sr by a highly selective and efficient Sr precipitation procedure and using Y selective resins and no Sr selective resins. Another object of this invention is to provide a process for separating


90


Y from Sr where


90


Sr activity in


90


Y is reduced by >10


7


. It is a further object of the invention to provide a process for separating


90


Y with an overall recovery of


90


Y>95%. Furthermore, another object of the invention is to provide a process for separating


90


Y with an overall recovery of


90


Sr>99.9% and improved purity with each processing run. Furthermore, another object of the invention is to provide a rapid process for separating


90


Y such that waste generation and radiation damage is minimum.











BRIEF DESCRIPTION OF THE DRAWINGS




The above-mentioned and other features of the invention will become more apparent and be best understood, together with the description, by reference to the accompanying drawings, in which:





FIG. 1

shows a single column arrangement for isolating


90


Y from


90


Sr in accordance with the following steps: dissolving strontium nitrate in H


2


O; acidifying the strontium nitrate solution with concentrated nitric acid; evaporating said solution; separating


90


Sr from solution by filtering or centrifuging; evaporating the remaining


90


Y enriched supemate; dissolving the remaining


90


Y enriched supernate in 0.1 to 0.2M HCL; passing the supernate through an yttrium selective extraction chromatographic column containing alkyl alkylphosphonic acid; rinsing the yttriun selective extraction chromatographic column with HCL; and removing yttrium from yttrium selective extraction column with 1 to 2M HCL.





FIG. 2

shows a single column arrangement for isolating


90


Y similar to

FIG. 1

except that the yttrium selective extraction chromatographic column contains dialkylphosphinic acid instead of alkyl alkylphosphonic acid.











DESCRIPTION OF THE PREFERRED EMBODIMENTS





FIG. 1

depicts the new simplified process, with only one chromatographic column, for separating


90


Y of sufficient purify and multi-curie quantity while minimizing loss of radioactive


90


Sr. Initially,


90


Y is separated from approximately 99.7% of the


90


Sr by precipitating the strontium as a nitrate salt from a nitric acid eutectic (16M). Essentially all of the yttrium remains in solution together with any ferric iron and zirconium while the strontium is selectively precipitated out. To reduce the loss of valuable


90


Sr to the yttrium supernate and to increase the ease of handling radioactive multi curie quantities of


90


Y, stable strontium is added to the


90


Sr. At least 80 to 90% of the mass of strontium that is present in the initial


90


Sr/


90


Y stock solution should be stable Sr, i.e.,


86,87,88


Sr isotopes. Requiring that 80-90% of the strontium mass be stable strontium isotopes, as opposed to radioactive


90


Sr, reduces the specific activity of the mixture. Minimizing amounts of


90


Sr is crucial if one desires


90


Y suitable for radio therapeutic applications. When


90


Sr is present in great quantity, more steps and materials are needed to separate and purify


90


Y. For example, three Sr selective chromatography columns are used in the process disclosed in U.S. Pat. No. 5,368,736. By contrast, this new process, which minimizes amounts of radioactive


90


Sr, does not require any


90


Sr selective chromatography. This new process thus saves money, space, time, and waste while decreasing


90


Sr contamination.




As shown in

FIG. 1

, precipitating strontium as a nitrate salt is achieved by first dissolving the strontium nitrate salt in H


2


O, 1 FIG.


1


. Approximately 10 mL of H


2


O is used for one gram of Sr as the nitrate salt. If the initial weight of


90


Sr is 20% by mass, one has 28 curies (200 mg) of radioactivity which is a very substantial amount. After dissolving the strontium nitrate in H


2


O, 5 mL of concentrated nitric acid is added, 2 (FIG.


1


), the volume is reduced to 5 mL by evaporating, 3 (FIG.


1


). Centrifuging or filtering, 4 (FIG.


1


), the mixture precipitates approximately 99.7% of the Sr as strontium nitrate. Having started out with 1 g of Sr (=1000 mg), this means that 99.7% or better of 1 g Sr precipitates out. (99.7% of 1 g=997 mg). Hence 997 mg of Sr precipitates out and 3 mg of the original starting Sr remains in the supernate. Of the 3 mg Sr remaining in the supernate, only 0.3 to 0.6 mg are radioactive


90


Sr if the initial mixture contained 10 to 20%


90


Sr, respectively (10% of 3 mg=0.3 mg and 20% of 3 mg=0.6 mg).




The concentrated nitric acid supernate is evaporated to dryness, 5 (FIG.


1


), and the residue dissolved in 2 to 4 mL of 0.05-0.4 M HCL, preferably 0.1M HCL, 6. The acid does not have to be HCL. The acid may be a strong acid consisting of nitric acid (HNO


3


), perchloric acid (HCLO


4


), and sulfuric acid (H


2


SO


4


). The resultant supernate load, 7, (

FIG. 1

) is passed through only one extraction chromatographic column, 10 (FIG.


1


), (usually only one mL in bed volume) containing an alkyl alkylphosphonic acid extractant sorbed on an inert polymeric support. The extraction chromatographic column containing the alkyl alkylphosphonic acid extractant is highly selective for


90


Y. The alkyl alkylphosphonic acid column selectively retains yttrium while all alkali and alkaline earth metal ions (including valuable


90


Sr) and divalent transition and post transition metal ions pass through and are recycled back to the


90


Sr stock solution, 7 and 8 (FIG.


1


). The yttrium-selective extractant may be obtained from commercially available 2-ethylhexyl 2-ethylhexylphosphonic acid. However, extraction chromatographic columns prepared from the material must undergo extensive purification using selected complexing agents and acids. The length of the carbon chain (C


n


) in alkyl alkylphosphonic acid can vary. The alkyl alkylphosphophonic acid is preferably selected from any alkyls consisting of C


5


, C


6


, C


7


, C


8


, C


9


, C


10


and C


11


. This description of alkyl alkylphosphonic acid is for purposes of illustration. The description of alkyl alkylphosphonic acid is not exhaustive and does not limit the invention to the chemical structure disclosed. For example, an alkyl alkylphosphonic acid with alkyls greater than eleven carbons or less than five carbons may be used.




Extensive rinsing (e.g. 20 bed volumes) of the alkyl alkylphosphonic acid extraction chromatographic column is carried out with 0.05-0.4 M, preferably 0.1M HCL, 8 (FIG.


1


), to reduce any


90


Sr present by at least 10


4


and reduce the overall


90


Sr activity by a factor of 10


7


. The acid to remove


90


Sr does not have to be HCL. The acid may be a strong acid consisting of nitric acid (HNO


3


), perchloric acid (HCLO


4


), and sulfuric acid (H


2


SO


4


). Before recycling the


90


Sr that passes thru the yttrium selective column, this very small quantity of Sr can be purified by adding sufficient concentrated nitric acid to bring the final nitrate concentration to 3M HNO


3


and then passing the resultant solution through a Sr selective column. The addition of the


90


Sr recovered from step 7 and 8 (

FIG. 1

) to that recovered from step 4 (

FIG. 1

) gives an overall recovery of


90


Sr >99.9%. After rinsing the column,


90


Y is eluted from the yttrium selective column in 4 bed volumes using 0.5-3.0 M, preferably 1 M HCL, 9 (

FIG. 1

) with an overall recovery of


90


Y >95%. Ferric iron and zirconium (IV) are retained on the column. The acid does not have to be HCL. The acid to elute yttrium may be a strong acid consisting of nitric acid (HNO


3


), perchloric acid (HCLO


4


), and sulfuric acid (H


2


SO


4


). Any trace of organic extractant or degradation products present in the purified


90


Y are removed by passing the solution through a bed of a polymeric support such as Amberchrom XAD-7, step 11 (FIG.


1


). Clinical applications require that the


90


Y product be in ≦0.05M HC1 making a final evaporation of the


90


Y column strip necessary.




A small variation of the above process may be carried out by replacing the extraction chromatographic column containing the alkyl alkylphosphonic acid extractant 12 (FIG.


1


), with a column containing a dialkylphosphinic acid extractant 21 (FIG.


2


). The length of the carbon chain (C


n


) in dialkylphosphinic acid may vary. Similar to alkyl alkylphosphonic acid, the dialkylphosphinic is preferably selected from any alkyls consisting of C


5


, C


6


, C


7


, C


8


, C


9


, C


10


and C


11


. The alkyls may be straight chained or branched. This description of dialkylphosphinic acid is for purposes of illustration. The description of dialkylphosphinic acid is not exhaustive and does not limit the invention to the chemical structure disclosed. For example, a dialkylphosphinic acid with alkyls greater than eleven carbons or less than five carbons may be used. Phosphinic acid extractant is more stable to hydrolysis and radiolysis but requires a much lower acidity to effectively retain yttrium. To effectively retain


90


Y (III), a solution containing only 0.01M hydrogen ion must be used.




The load for the dialkylphosphinic acid column is prepared by dissolving the residue obtained from evaporating the supernate in 0.05-0.4 HCL, preferably 0.1 M HCl, 13 (FIG.


2


), and passing this solution through a small (1 to 2 mL) bed volume column containing a conventional strong base anion exchange resin on the acetate cycle. The acid does not have to be HCL. The acid may be a strong acid consisting of nitric acid (HNO


3


), perchloric acid (HCLO


4


), and sulfuric acid (H


2


SO


4


). The chloride in the load solution is replaced by acetate which in turn produces acetic acid. Acetic acid solutions are in the correct pH range for loading the phosphinic acid containing resin.




After loading the yttrium containing solution onto the dialkylphosphinic acid extraction chromatographic column, the column is rinsed with 0.005-0.04 HCL, preferably 0.01M HCL, 19 (

FIG. 2

) to remove all traces of


90


Sr to give an overall recovery of


90


Sr>99.9% and reduce


90


Sr activity by a factor of 10


4


. The acid to remove


90


Sr does not have to be HCL. The acid may be a strong acid consisting of nitric acid (HNO


3


), perchloric acid (HCLO


4


), and sulfuric acid (H


2


SO


4


). Yttrium is then eluted from the column using 0.05-0.3 HCL, preferably 0.1M HCl, 20 (FIG.


2


), with an overall recovery of


90


Y>95%. The acid to elute does not have to be HCL. The acid may be a strong acid consisting of nitric acid (HNO


3


), perchloric acid (HCLO


4


), and sulfuric acid (H


2


SO


4


). Any traces of extractant or organic degradation products are removed by passing the solution through a bed of polymeric support. Preparation of the final 0.05M HCl solution may be carried out by dilution.




The following tables 1 and 2 describe the behavior of selected metal ions on yttrium selective resins. The following data about


90


Y were used to calculate some of the information in Tables 1 and 2: Specific activity of


90


Sr (t


½


=28.6 y) (λ=4.61×10


−8


min


−1


). 139 Ci/g or 139 milli-Ci/mg. One Curie of


90


Sr=7.20 mg if pure. Specific activity of


90


Y (t


½


=64.1 hrs.) (λ=1.80×10


−4


min


−1


). 0.544 Ci/μg. One curie of


90


Y=1.84 μg. Table 1 corresponds to

FIG. 1

when the extractant is alkyl alkylphosphonic acid. Table 1 data was collected under the following conditions: Alkyl Alkylphosphonic Acid on Amberchrom CG-71, Particle Size 50-100 μm, Load 4.0 mL of 0.1 M HCL, Rinse 2.0 mL of 0.1 M HCI/fraction, and Strip 2.0 mL of 1.0 M HCL/fraction. Table 2 corresponds to

FIG. 2

when the extractant is dialklyphosphinic acid. Table 2 data was collected under the following conditions: Dialkylphosphinic Acid on Amberchrom CG-71, Particle Size 50-100 μm, Bed Volume=1.0 mL, 0.7 cm diameter, Flow Rate=1.0 mL/sq. cm/min, Load 9 mL of ˜1M Acetic Acid, Rinse 2.0 mL of 0.01M HCI/fraction, and Strip 2.0 mL of 0.1 M HCI/fraction.












TABLE 1











Behavior of Selected Metal Ions on Yttrium Selective Resin






Percent of Total Measured in Each Fraction (for FIG. 1)














RINSE




STRIP





















LOAD




1




2




3




4




5




1




2




3




4




5

























Al




96




3




1














































Fe




0.1




0.03



















































Mn




97




3



















































Cu




96




3




1














































Zn




95




4




0.2




0.1









































Sr




93




7



















































Y


































83




17




0.1
















Zr





























































Cd




97




3



















































Pb




96




3




0.3




0.3




0.2









0.4


































Alkyl Alkylphosphonic Acid on Amberchrom CG-71, Particle Size 50-100 μm, Load 4.0 mL of 0.1M HCI, Rinse 2.0 mL of 1.0 M HCL/fraction, and Strip 2.0 ml of 0.1M HCL/fraction.












TABLE 2











Behavior of Selected Metal Ions on Yttrium Selective Resin






Percent of Total Measured in Each Fraction (for FIG. 2)














RINSE




STRIP





















LOAD




1




2




3




4




5




1




2




3




4




5

























Al




75




14




8




3









































Fe




89




11



















































Mn




89




11



















































Cu




91




9



















































Zn




4




74




10%




2




1




































Sr




94




6



















































Y


































76




12




4




5











Zr




48
























































Cd




90




10



















































Pb




88




12



























































Dialkylphosphinic Acid on Amberchrom CG-71, Particle Size 50-100 μm, Bed Volume=1.0 mL, 0.7 cm diameter, Flow Rate=1.0 mL/sq. cm/min, Load 9 mL of ˜1M Acetic Acid, Rinse 2.0 mL of 0.01 M HCI/fraction, and Strip 2.0 mL of 0.1 M HCL/fraction.




The foregoing description of preferred embodiments of the invention has been presented for purposes of illustration and description. It is not intended to be exhaustive or to limit the invention to the precise form disclosed. Many modifications and variations are possible in light of the above teaching. For example,


91


Y may be used for other therapeutic uses not mentioned. Various isotopes of yttrium, such as yttrium-87 and yttrium-91, may be purified using the yttrium selective resin as described herein, although modifications of various acid and extractant concentrations and columnar figure might be necessary. The embodiments were chosen and described to best explain the principles of the invention and its practical application and thereby enable others of ordinary skill in the art to best utilize the invention.



Claims
  • 1. A process for separating and purifying yttrium isotope consisting of 87Y, 90Y, or 91Y from strontium-90, comprising:a. dissolving a nitrate salt of an original 90Sr stock solution in H2O creating a strontium nitrate solution; b. acidifying said strontium nitrate solution containing 90Y with concentrated nitric acid; c. evaporating said acidified strontium nitrate solution; d. filtering or centrifuging said evaporated strontium nitrate solution to separate crystalline 90Sr nitrate salt from said solution to make an yttrium enriched supernate; e. evaporating said yttrium enriched supernate to dryness; f. dissolving said dried yttrium enriched supernate which is free of nitric acid in a strong acid; g. passing said dissolved yttrium enriched supernate through an yttrium selective extraction chromatographic column such that essentially all said yttrium isotope is retained while all other trace metals and impurities pass through and are recycled back to said original 90Sr stock solution; h. rinsing said yttrium selective extraction chromatographic column with a strong acid to remove any remaining 90Sr which is recycled back to said original 90Sr stock solution; and i. eluting said yttrium isotope from said yttrium selective extraction chromatographic column with a strong acid.
  • 2. A process for separating and purifying said Y isotope as in claim 1 wherein at least 80-90% of the mass of strontium in the original 90Sr stock solution is stable Sr.
  • 3. A process for separating and purifying said Y isotope as in claim 1 wherein said strong acids are selected from a group consisting of HCL, sulfuric acid, perchloric acid, and nitric acid.
  • 4. A process for separating and purifying said Y isotope as in claim 1 wherein extractant for said yttrium selective extraction chromatographic column is alkyl alkylphosphonic acid.
  • 5. A process for separating and purifying said Y isotope as in claim 4 wherein 90Y enriched nitric acid residue is dissolved in said strong acid being 0.05-0.4M HCL.
  • 6. A process for separating and purifying said Y isotope as in claim 4 wherein any remaining said 90Sr is recovered from said yttrium selective extraction chromatographic column with said strong acid being 0.05M-0.4M HCL which is recycled back to said original 90Sr stock solution.
  • 7. A process for separating and purifying said Y isotope as in claim 4 wherein said yttrium isotape is eluted from said yttrium selective extraction chromatographic column with said strong acid being 0.5-3.0 HCL.
  • 8. A process for separating and purifying said Y isotope as in claim 4 wherein the alkyl in said alkyl alkylphosphonic acid is selected from alkyls consisting of C5, C6, C7, C8, C9, C10 and C11 straight chained alkanes.
  • 9. A process for separating and purifying said Y isotope as in claim 4 wherein the alkyl in said alkyl alkylphosphonic acid is selected from alkyls consisting of C5, C6, C7, C8, C9, C10 and C11 branched alkanes.
  • 10. A process for separating and purifying said Y isotope as in claim 4 wherein the alkyl in said alkyl alkylphosphonic acid are alkyls with Cn greater than 11.
  • 11. A process for separating and purifying said Y isotope as in claim 4 wherein the alkyl in said alkyl alkylphosphonic acid are alkyls with Cn less than 5.
  • 12. A process for separating and purifying said Y isotope as in claim 1 wherein extractant for said yttrium selective extraction chromatographic column is dialkylphosphinic acid.
  • 13. A process for separating and purifying said Y isotope as in claim 12 wherein 90Y enriched nitric acid residue is dissolved in said strong acid being 0.05-0.4M HCL.
  • 14. A process for separating and purifying said Y isotope as in claim 12 wherein any remaining said 90Sr is recovered from said yttrium selective extraction chromatographic column with said strong acid being 0.005-0.04M HCL which is recycled back to said original 90Sr stock solution.
  • 15. A process for separating and purifying said Y isotope as in claim 12 wherein said wherein said yttrium isotope is eluted from said yttrium selective extraction chromatographic column with said strong acid being 0.05-0.3 M HCL.
  • 16. A process for separating and purifying said Y isotope as in claim 12 wherein 90Y enriched nitric acid residue is dissolved in said strong acid being 0.05-0.4M HCL.
  • 17. A process for separating and purifying said Y isotope as in claim 12 wherein the alkyl in said dialkylphosphinic acid is selected from alkyls consisting of C5, C6, C7, C8, C9, C10 and C11 straight chained alkanes.
  • 18. A process for separating and purifying said Y isotope as in claim 12 wherein the alkyl in said dialkylphosphinic acid is selected from alkyls consisting of C5, C6, C7, C8, C9, C10 and C11 branched alkanes.
  • 19. A process for separating and purifying said Y isotope as in claim 12 wherein the alkyl in said dialkylphosphinic acid are alkyls with Cn greater than 11.
  • 20. A process for separating and purifying said Y isotope as in claim 12 wherein the alkyl in said dialkylphosphinic acid are alkyls with Cn less than 5.
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4835107 Horwitz et al. May 1989
5100585 Horwitz et al. Mar 1992
5110474 Horwitz et al. May 1992
5154897 Ehrhardt et al. Oct 1992
5225173 Wai Jul 1993
5344623 Horwitz et al. Sep 1994
5368736 Horwitz et al. Nov 1994
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5512256 Bray et al. Apr 1996
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Number Date Country
60-097300 May 1985 JP
753037 Sep 1983 SU
9323854 Nov 1993 WO