CN117686299A - Method for extracting decay daughter of thorium element - Google Patents
Method for extracting decay daughter of thorium element Download PDFInfo
- Publication number
- CN117686299A CN117686299A CN202410143254.2A CN202410143254A CN117686299A CN 117686299 A CN117686299 A CN 117686299A CN 202410143254 A CN202410143254 A CN 202410143254A CN 117686299 A CN117686299 A CN 117686299A
- Authority
- CN
- China
- Prior art keywords
- sodium
- potassium
- leaching
- solution
- thorium
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
- 238000000034 method Methods 0.000 title claims abstract description 55
- 229910052776 Thorium Inorganic materials 0.000 title claims abstract description 46
- ZSLUVFAKFWKJRC-IGMARMGPSA-N 232Th Chemical compound [232Th] ZSLUVFAKFWKJRC-IGMARMGPSA-N 0.000 title claims abstract description 35
- 238000002386 leaching Methods 0.000 claims abstract description 174
- SFKTYEXKZXBQRQ-UHFFFAOYSA-J thorium(4+);tetrahydroxide Chemical compound [OH-].[OH-].[OH-].[OH-].[Th+4] SFKTYEXKZXBQRQ-UHFFFAOYSA-J 0.000 claims abstract description 90
- 239000002245 particle Substances 0.000 claims abstract description 83
- 239000007788 liquid Substances 0.000 claims abstract description 44
- 238000000926 separation method Methods 0.000 claims abstract description 26
- 238000002156 mixing Methods 0.000 claims abstract description 14
- 239000000243 solution Substances 0.000 claims description 113
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Chemical compound [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 claims description 42
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 39
- 235000010344 sodium nitrate Nutrition 0.000 claims description 21
- 239000004317 sodium nitrate Substances 0.000 claims description 21
- 238000001914 filtration Methods 0.000 claims description 17
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims description 16
- 230000032683 aging Effects 0.000 claims description 14
- 239000012266 salt solution Substances 0.000 claims description 14
- WCUXLLCKKVVCTQ-UHFFFAOYSA-M Potassium chloride Chemical compound [Cl-].[K+] WCUXLLCKKVVCTQ-UHFFFAOYSA-M 0.000 claims description 12
- 239000007864 aqueous solution Substances 0.000 claims description 12
- ZCCIPPOKBCJFDN-UHFFFAOYSA-N calcium nitrate Chemical compound [Ca+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ZCCIPPOKBCJFDN-UHFFFAOYSA-N 0.000 claims description 12
- 239000011259 mixed solution Substances 0.000 claims description 12
- FGIUAXJPYTZDNR-UHFFFAOYSA-N potassium nitrate Chemical compound [K+].[O-][N+]([O-])=O FGIUAXJPYTZDNR-UHFFFAOYSA-N 0.000 claims description 12
- -1 thorium ions Chemical class 0.000 claims description 11
- 229910002651 NO3 Inorganic materials 0.000 claims description 9
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 9
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 9
- NLKNQRATVPKPDG-UHFFFAOYSA-M potassium iodide Chemical compound [K+].[I-] NLKNQRATVPKPDG-UHFFFAOYSA-M 0.000 claims description 9
- FVAUCKIRQBBSSJ-UHFFFAOYSA-M sodium iodide Chemical compound [Na+].[I-] FVAUCKIRQBBSSJ-UHFFFAOYSA-M 0.000 claims description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 9
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 claims description 8
- 239000011780 sodium chloride Substances 0.000 claims description 8
- 239000003513 alkali Substances 0.000 claims description 7
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 claims description 6
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 6
- TWRXJAOTZQYOKJ-UHFFFAOYSA-L Magnesium chloride Chemical compound [Mg+2].[Cl-].[Cl-] TWRXJAOTZQYOKJ-UHFFFAOYSA-L 0.000 claims description 6
- VSCWAEJMTAWNJL-UHFFFAOYSA-K aluminium trichloride Chemical compound Cl[Al](Cl)Cl VSCWAEJMTAWNJL-UHFFFAOYSA-K 0.000 claims description 6
- 150000003863 ammonium salts Chemical class 0.000 claims description 6
- IWOUKMZUPDVPGQ-UHFFFAOYSA-N barium nitrate Chemical compound [Ba+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O IWOUKMZUPDVPGQ-UHFFFAOYSA-N 0.000 claims description 6
- NLSCHDZTHVNDCP-UHFFFAOYSA-N caesium nitrate Chemical compound [Cs+].[O-][N+]([O-])=O NLSCHDZTHVNDCP-UHFFFAOYSA-N 0.000 claims description 6
- VSGNNIFQASZAOI-UHFFFAOYSA-L calcium acetate Chemical compound [Ca+2].CC([O-])=O.CC([O-])=O VSGNNIFQASZAOI-UHFFFAOYSA-L 0.000 claims description 6
- 235000011092 calcium acetate Nutrition 0.000 claims description 6
- 239000001639 calcium acetate Substances 0.000 claims description 6
- 229960005147 calcium acetate Drugs 0.000 claims description 6
- 239000001110 calcium chloride Substances 0.000 claims description 6
- 229910001628 calcium chloride Inorganic materials 0.000 claims description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 claims description 6
- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(3+);trinitrate Chemical compound [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 claims description 6
- YIXJRHPUWRPCBB-UHFFFAOYSA-N magnesium nitrate Chemical compound [Mg+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O YIXJRHPUWRPCBB-UHFFFAOYSA-N 0.000 claims description 6
- SCVFZCLFOSHCOH-UHFFFAOYSA-M potassium acetate Chemical compound [K+].CC([O-])=O SCVFZCLFOSHCOH-UHFFFAOYSA-M 0.000 claims description 6
- XAEFZNCEHLXOMS-UHFFFAOYSA-M potassium benzoate Chemical compound [K+].[O-]C(=O)C1=CC=CC=C1 XAEFZNCEHLXOMS-UHFFFAOYSA-M 0.000 claims description 6
- IOLCXVTUBQKXJR-UHFFFAOYSA-M potassium bromide Chemical compound [K+].[Br-] IOLCXVTUBQKXJR-UHFFFAOYSA-M 0.000 claims description 6
- 239000001103 potassium chloride Substances 0.000 claims description 6
- 235000011164 potassium chloride Nutrition 0.000 claims description 6
- NROKBHXJSPEDAR-UHFFFAOYSA-M potassium fluoride Chemical compound [F-].[K+] NROKBHXJSPEDAR-UHFFFAOYSA-M 0.000 claims description 6
- 235000010333 potassium nitrate Nutrition 0.000 claims description 6
- 239000004323 potassium nitrate Substances 0.000 claims description 6
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 claims description 6
- JHJLBTNAGRQEKS-UHFFFAOYSA-M sodium bromide Chemical compound [Na+].[Br-] JHJLBTNAGRQEKS-UHFFFAOYSA-M 0.000 claims description 6
- PUZPDOWCWNUUKD-UHFFFAOYSA-M sodium fluoride Chemical compound [F-].[Na+] PUZPDOWCWNUUKD-UHFFFAOYSA-M 0.000 claims description 6
- LPXPTNMVRIOKMN-UHFFFAOYSA-M sodium nitrite Chemical compound [Na+].[O-]N=O LPXPTNMVRIOKMN-UHFFFAOYSA-M 0.000 claims description 6
- 159000000000 sodium salts Chemical class 0.000 claims description 6
- GEHJYWRUCIMESM-UHFFFAOYSA-L sodium sulfite Chemical compound [Na+].[Na+].[O-]S([O-])=O GEHJYWRUCIMESM-UHFFFAOYSA-L 0.000 claims description 6
- JIAARYAFYJHUJI-UHFFFAOYSA-L zinc dichloride Chemical compound [Cl-].[Cl-].[Zn+2] JIAARYAFYJHUJI-UHFFFAOYSA-L 0.000 claims description 6
- ONDPHDOFVYQSGI-UHFFFAOYSA-N zinc nitrate Chemical compound [Zn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ONDPHDOFVYQSGI-UHFFFAOYSA-N 0.000 claims description 6
- 159000000007 calcium salts Chemical class 0.000 claims description 5
- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-UHFFFAOYSA-N 0.000 claims description 4
- BIGPRXCJEDHCLP-UHFFFAOYSA-N ammonium bisulfate Chemical compound [NH4+].OS([O-])(=O)=O BIGPRXCJEDHCLP-UHFFFAOYSA-N 0.000 claims description 4
- 235000019270 ammonium chloride Nutrition 0.000 claims description 4
- 239000002585 base Substances 0.000 claims description 4
- 229910000389 calcium phosphate Inorganic materials 0.000 claims description 4
- GBAOBIBJACZTNA-UHFFFAOYSA-L calcium sulfite Chemical compound [Ca+2].[O-]S([O-])=O GBAOBIBJACZTNA-UHFFFAOYSA-L 0.000 claims description 4
- 235000010261 calcium sulphite Nutrition 0.000 claims description 4
- 230000001105 regulatory effect Effects 0.000 claims description 4
- BNGXYYYYKUGPPF-UHFFFAOYSA-M (3-methylphenyl)methyl-triphenylphosphanium;chloride Chemical compound [Cl-].CC1=CC=CC(C[P+](C=2C=CC=CC=2)(C=2C=CC=CC=2)C=2C=CC=CC=2)=C1 BNGXYYYYKUGPPF-UHFFFAOYSA-M 0.000 claims description 3
- XZXYQEHISUMZAT-UHFFFAOYSA-N 2-[(2-hydroxy-5-methylphenyl)methyl]-4-methylphenol Chemical compound CC1=CC=C(O)C(CC=2C(=CC=C(C)C=2)O)=C1 XZXYQEHISUMZAT-UHFFFAOYSA-N 0.000 claims description 3
- MFGOFGRYDNHJTA-UHFFFAOYSA-N 2-amino-1-(2-fluorophenyl)ethanol Chemical compound NCC(O)C1=CC=CC=C1F MFGOFGRYDNHJTA-UHFFFAOYSA-N 0.000 claims description 3
- JTNCEQNHURODLX-UHFFFAOYSA-N 2-phenylethanimidamide Chemical compound NC(=N)CC1=CC=CC=C1 JTNCEQNHURODLX-UHFFFAOYSA-N 0.000 claims description 3
- DDFHBQSCUXNBSA-UHFFFAOYSA-N 5-(5-carboxythiophen-2-yl)thiophene-2-carboxylic acid Chemical compound S1C(C(=O)O)=CC=C1C1=CC=C(C(O)=O)S1 DDFHBQSCUXNBSA-UHFFFAOYSA-N 0.000 claims description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 claims description 3
- USFZMSVCRYTOJT-UHFFFAOYSA-N Ammonium acetate Chemical compound N.CC(O)=O USFZMSVCRYTOJT-UHFFFAOYSA-N 0.000 claims description 3
- 239000005695 Ammonium acetate Substances 0.000 claims description 3
- ATRRKUHOCOJYRX-UHFFFAOYSA-N Ammonium bicarbonate Chemical compound [NH4+].OC([O-])=O ATRRKUHOCOJYRX-UHFFFAOYSA-N 0.000 claims description 3
- 229910000013 Ammonium bicarbonate Inorganic materials 0.000 claims description 3
- CBOCVOKPQGJKKJ-UHFFFAOYSA-L Calcium formate Chemical compound [Ca+2].[O-]C=O.[O-]C=O CBOCVOKPQGJKKJ-UHFFFAOYSA-L 0.000 claims description 3
- UNMYWSMUMWPJLR-UHFFFAOYSA-L Calcium iodide Chemical compound [Ca+2].[I-].[I-] UNMYWSMUMWPJLR-UHFFFAOYSA-L 0.000 claims description 3
- PQUCIEFHOVEZAU-UHFFFAOYSA-N Diammonium sulfite Chemical compound [NH4+].[NH4+].[O-]S([O-])=O PQUCIEFHOVEZAU-UHFFFAOYSA-N 0.000 claims description 3
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 claims description 3
- 229910021578 Iron(III) chloride Inorganic materials 0.000 claims description 3
- VMHLLURERBWHNL-UHFFFAOYSA-M Sodium acetate Chemical compound [Na+].CC([O-])=O VMHLLURERBWHNL-UHFFFAOYSA-M 0.000 claims description 3
- UIIMBOGNXHQVGW-DEQYMQKBSA-M Sodium bicarbonate-14C Chemical compound [Na+].O[14C]([O-])=O UIIMBOGNXHQVGW-DEQYMQKBSA-M 0.000 claims description 3
- DWAQJAXMDSEUJJ-UHFFFAOYSA-M Sodium bisulfite Chemical compound [Na+].OS([O-])=O DWAQJAXMDSEUJJ-UHFFFAOYSA-M 0.000 claims description 3
- 239000004280 Sodium formate Substances 0.000 claims description 3
- AZFNGPAYDKGCRB-XCPIVNJJSA-M [(1s,2s)-2-amino-1,2-diphenylethyl]-(4-methylphenyl)sulfonylazanide;chlororuthenium(1+);1-methyl-4-propan-2-ylbenzene Chemical compound [Ru+]Cl.CC(C)C1=CC=C(C)C=C1.C1=CC(C)=CC=C1S(=O)(=O)[N-][C@@H](C=1C=CC=CC=1)[C@@H](N)C1=CC=CC=C1 AZFNGPAYDKGCRB-XCPIVNJJSA-M 0.000 claims description 3
- 235000019257 ammonium acetate Nutrition 0.000 claims description 3
- 229940043376 ammonium acetate Drugs 0.000 claims description 3
- 235000012538 ammonium bicarbonate Nutrition 0.000 claims description 3
- SWLVFNYSXGMGBS-UHFFFAOYSA-N ammonium bromide Chemical compound [NH4+].[Br-] SWLVFNYSXGMGBS-UHFFFAOYSA-N 0.000 claims description 3
- 239000001099 ammonium carbonate Substances 0.000 claims description 3
- LFVGISIMTYGQHF-UHFFFAOYSA-N ammonium dihydrogen phosphate Chemical compound [NH4+].OP(O)([O-])=O LFVGISIMTYGQHF-UHFFFAOYSA-N 0.000 claims description 3
- 229910000387 ammonium dihydrogen phosphate Inorganic materials 0.000 claims description 3
- VZTDIZULWFCMLS-UHFFFAOYSA-N ammonium formate Chemical compound [NH4+].[O-]C=O VZTDIZULWFCMLS-UHFFFAOYSA-N 0.000 claims description 3
- HIVLDXAAFGCOFU-UHFFFAOYSA-N ammonium hydrosulfide Chemical compound [NH4+].[SH-] HIVLDXAAFGCOFU-UHFFFAOYSA-N 0.000 claims description 3
- 229940107816 ammonium iodide Drugs 0.000 claims description 3
- CAMXVZOXBADHNJ-UHFFFAOYSA-N ammonium nitrite Chemical compound [NH4+].[O-]N=O CAMXVZOXBADHNJ-UHFFFAOYSA-N 0.000 claims description 3
- VBIXEXWLHSRNKB-UHFFFAOYSA-N ammonium oxalate Chemical compound [NH4+].[NH4+].[O-]C(=O)C([O-])=O VBIXEXWLHSRNKB-UHFFFAOYSA-N 0.000 claims description 3
- UYJXRRSPUVSSMN-UHFFFAOYSA-P ammonium sulfide Chemical compound [NH4+].[NH4+].[S-2] UYJXRRSPUVSSMN-UHFFFAOYSA-P 0.000 claims description 3
- 239000001284 azanium sulfanide Substances 0.000 claims description 3
- WDIHJSXYQDMJHN-UHFFFAOYSA-L barium chloride Chemical compound [Cl-].[Cl-].[Ba+2] WDIHJSXYQDMJHN-UHFFFAOYSA-L 0.000 claims description 3
- 229910001626 barium chloride Inorganic materials 0.000 claims description 3
- RQPZNWPYLFFXCP-UHFFFAOYSA-L barium dihydroxide Chemical compound [OH-].[OH-].[Ba+2] RQPZNWPYLFFXCP-UHFFFAOYSA-L 0.000 claims description 3
- 229910001863 barium hydroxide Inorganic materials 0.000 claims description 3
- AIYUHDOJVYHVIT-UHFFFAOYSA-M caesium chloride Chemical compound [Cl-].[Cs+] AIYUHDOJVYHVIT-UHFFFAOYSA-M 0.000 claims description 3
- HUCVOHYBFXVBRW-UHFFFAOYSA-M caesium hydroxide Inorganic materials [OH-].[Cs+] HUCVOHYBFXVBRW-UHFFFAOYSA-M 0.000 claims description 3
- NKWPZUCBCARRDP-UHFFFAOYSA-L calcium bicarbonate Chemical compound [Ca+2].OC([O-])=O.OC([O-])=O NKWPZUCBCARRDP-UHFFFAOYSA-L 0.000 claims description 3
- 229910000020 calcium bicarbonate Inorganic materials 0.000 claims description 3
- YYRMJZQKEFZXMX-UHFFFAOYSA-L calcium bis(dihydrogenphosphate) Chemical compound [Ca+2].OP(O)([O-])=O.OP(O)([O-])=O YYRMJZQKEFZXMX-UHFFFAOYSA-L 0.000 claims description 3
- 229910001622 calcium bromide Inorganic materials 0.000 claims description 3
- 229940059251 calcium bromide Drugs 0.000 claims description 3
- WGEFECGEFUFIQW-UHFFFAOYSA-L calcium dibromide Chemical compound [Ca+2].[Br-].[Br-] WGEFECGEFUFIQW-UHFFFAOYSA-L 0.000 claims description 3
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 claims description 3
- 235000019255 calcium formate Nutrition 0.000 claims description 3
- 239000004281 calcium formate Substances 0.000 claims description 3
- 229940044172 calcium formate Drugs 0.000 claims description 3
- 239000000920 calcium hydroxide Substances 0.000 claims description 3
- 229910001861 calcium hydroxide Inorganic materials 0.000 claims description 3
- 229940046413 calcium iodide Drugs 0.000 claims description 3
- 229910001640 calcium iodide Inorganic materials 0.000 claims description 3
- JXRVKYBCWUJJBP-UHFFFAOYSA-L calcium;hydrogen sulfate Chemical compound [Ca+2].OS([O-])(=O)=O.OS([O-])(=O)=O JXRVKYBCWUJJBP-UHFFFAOYSA-L 0.000 claims description 3
- ORTQZVOHEJQUHG-UHFFFAOYSA-L copper(II) chloride Chemical compound Cl[Cu]Cl ORTQZVOHEJQUHG-UHFFFAOYSA-L 0.000 claims description 3
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 claims description 3
- 238000010908 decantation Methods 0.000 claims description 3
- ZPWVASYFFYYZEW-UHFFFAOYSA-L dipotassium hydrogen phosphate Chemical compound [K+].[K+].OP([O-])([O-])=O ZPWVASYFFYYZEW-UHFFFAOYSA-L 0.000 claims description 3
- 235000019797 dipotassium phosphate Nutrition 0.000 claims description 3
- 229910000396 dipotassium phosphate Inorganic materials 0.000 claims description 3
- IRXRGVFLQOSHOH-UHFFFAOYSA-L dipotassium;oxalate Chemical compound [K+].[K+].[O-]C(=O)C([O-])=O IRXRGVFLQOSHOH-UHFFFAOYSA-L 0.000 claims description 3
- BNIILDVGGAEEIG-UHFFFAOYSA-L disodium hydrogen phosphate Chemical compound [Na+].[Na+].OP([O-])([O-])=O BNIILDVGGAEEIG-UHFFFAOYSA-L 0.000 claims description 3
- 235000019800 disodium phosphate Nutrition 0.000 claims description 3
- 229910000397 disodium phosphate Inorganic materials 0.000 claims description 3
- 229960002089 ferrous chloride Drugs 0.000 claims description 3
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 3
- NMCUIPGRVMDVDB-UHFFFAOYSA-L iron dichloride Chemical compound Cl[Fe]Cl NMCUIPGRVMDVDB-UHFFFAOYSA-L 0.000 claims description 3
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 claims description 3
- 229910001629 magnesium chloride Inorganic materials 0.000 claims description 3
- 235000019837 monoammonium phosphate Nutrition 0.000 claims description 3
- 235000019691 monocalcium phosphate Nutrition 0.000 claims description 3
- 235000019796 monopotassium phosphate Nutrition 0.000 claims description 3
- 229910000402 monopotassium phosphate Inorganic materials 0.000 claims description 3
- 235000019799 monosodium phosphate Nutrition 0.000 claims description 3
- 229910000403 monosodium phosphate Inorganic materials 0.000 claims description 3
- RAFRTSDUWORDLA-UHFFFAOYSA-N phenyl 3-chloropropanoate Chemical compound ClCCC(=O)OC1=CC=CC=C1 RAFRTSDUWORDLA-UHFFFAOYSA-N 0.000 claims description 3
- PJNZPQUBCPKICU-UHFFFAOYSA-N phosphoric acid;potassium Chemical compound [K].OP(O)(O)=O PJNZPQUBCPKICU-UHFFFAOYSA-N 0.000 claims description 3
- 235000011056 potassium acetate Nutrition 0.000 claims description 3
- 239000011736 potassium bicarbonate Substances 0.000 claims description 3
- 235000015497 potassium bicarbonate Nutrition 0.000 claims description 3
- 229910000028 potassium bicarbonate Inorganic materials 0.000 claims description 3
- 229910000343 potassium bisulfate Inorganic materials 0.000 claims description 3
- DJEHXEMURTVAOE-UHFFFAOYSA-M potassium bisulfite Chemical compound [K+].OS([O-])=O DJEHXEMURTVAOE-UHFFFAOYSA-M 0.000 claims description 3
- 239000011698 potassium fluoride Substances 0.000 claims description 3
- 235000003270 potassium fluoride Nutrition 0.000 claims description 3
- WFIZEGIEIOHZCP-UHFFFAOYSA-M potassium formate Chemical compound [K+].[O-]C=O WFIZEGIEIOHZCP-UHFFFAOYSA-M 0.000 claims description 3
- 235000010259 potassium hydrogen sulphite Nutrition 0.000 claims description 3
- TYJJADVDDVDEDZ-UHFFFAOYSA-M potassium hydrogencarbonate Chemical compound [K+].OC([O-])=O TYJJADVDDVDEDZ-UHFFFAOYSA-M 0.000 claims description 3
- 235000010289 potassium nitrite Nutrition 0.000 claims description 3
- 239000004304 potassium nitrite Substances 0.000 claims description 3
- DPLVEEXVKBWGHE-UHFFFAOYSA-N potassium sulfide Chemical compound [S-2].[K+].[K+] DPLVEEXVKBWGHE-UHFFFAOYSA-N 0.000 claims description 3
- BHZRJJOHZFYXTO-UHFFFAOYSA-L potassium sulfite Chemical compound [K+].[K+].[O-]S([O-])=O BHZRJJOHZFYXTO-UHFFFAOYSA-L 0.000 claims description 3
- 235000019252 potassium sulphite Nutrition 0.000 claims description 3
- UMPKMCDVBZFQOK-UHFFFAOYSA-N potassium;iron(3+);oxygen(2-) Chemical compound [O-2].[O-2].[K+].[Fe+3] UMPKMCDVBZFQOK-UHFFFAOYSA-N 0.000 claims description 3
- 229910001961 silver nitrate Inorganic materials 0.000 claims description 3
- 239000011734 sodium Substances 0.000 claims description 3
- 229910052708 sodium Inorganic materials 0.000 claims description 3
- 235000015424 sodium Nutrition 0.000 claims description 3
- 239000001632 sodium acetate Substances 0.000 claims description 3
- 235000017281 sodium acetate Nutrition 0.000 claims description 3
- 229960004249 sodium acetate Drugs 0.000 claims description 3
- WBHQBSYUUJJSRZ-UHFFFAOYSA-M sodium bisulfate Chemical compound [Na+].OS([O-])(=O)=O WBHQBSYUUJJSRZ-UHFFFAOYSA-M 0.000 claims description 3
- 229910000342 sodium bisulfate Inorganic materials 0.000 claims description 3
- AJPJDKMHJJGVTQ-UHFFFAOYSA-M sodium dihydrogen phosphate Chemical compound [Na+].OP(O)([O-])=O AJPJDKMHJJGVTQ-UHFFFAOYSA-M 0.000 claims description 3
- 239000011775 sodium fluoride Substances 0.000 claims description 3
- 235000013024 sodium fluoride Nutrition 0.000 claims description 3
- HLBBKKJFGFRGMU-UHFFFAOYSA-M sodium formate Chemical compound [Na+].[O-]C=O HLBBKKJFGFRGMU-UHFFFAOYSA-M 0.000 claims description 3
- 235000019254 sodium formate Nutrition 0.000 claims description 3
- 235000010267 sodium hydrogen sulphite Nutrition 0.000 claims description 3
- 235000009518 sodium iodide Nutrition 0.000 claims description 3
- 235000010288 sodium nitrite Nutrition 0.000 claims description 3
- ZNCPFRVNHGOPAG-UHFFFAOYSA-L sodium oxalate Chemical compound [Na+].[Na+].[O-]C(=O)C([O-])=O ZNCPFRVNHGOPAG-UHFFFAOYSA-L 0.000 claims description 3
- 229940039790 sodium oxalate Drugs 0.000 claims description 3
- 229910052979 sodium sulfide Inorganic materials 0.000 claims description 3
- GRVFOGOEDUUMBP-UHFFFAOYSA-N sodium sulfide (anhydrous) Chemical compound [Na+].[Na+].[S-2] GRVFOGOEDUUMBP-UHFFFAOYSA-N 0.000 claims description 3
- 235000010265 sodium sulphite Nutrition 0.000 claims description 3
- 239000011592 zinc chloride Substances 0.000 claims description 3
- 235000005074 zinc chloride Nutrition 0.000 claims description 3
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 2
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 2
- 235000011114 ammonium hydroxide Nutrition 0.000 claims description 2
- 239000011575 calcium Substances 0.000 claims description 2
- 229910052791 calcium Inorganic materials 0.000 claims description 2
- MNNHAPBLZZVQHP-UHFFFAOYSA-N diammonium hydrogen phosphate Chemical compound [NH4+].[NH4+].OP([O-])([O-])=O MNNHAPBLZZVQHP-UHFFFAOYSA-N 0.000 claims description 2
- 238000004062 sedimentation Methods 0.000 claims description 2
- 238000000605 extraction Methods 0.000 abstract description 20
- 230000000694 effects Effects 0.000 description 33
- 239000007791 liquid phase Substances 0.000 description 30
- 239000007790 solid phase Substances 0.000 description 17
- 238000012360 testing method Methods 0.000 description 15
- 239000000203 mixture Substances 0.000 description 9
- 239000011347 resin Substances 0.000 description 8
- 229920005989 resin Polymers 0.000 description 8
- 239000007787 solid Substances 0.000 description 8
- 229910052705 radium Inorganic materials 0.000 description 7
- 238000002791 soaking Methods 0.000 description 7
- 238000000975 co-precipitation Methods 0.000 description 6
- 230000007774 longterm Effects 0.000 description 6
- 238000002360 preparation method Methods 0.000 description 6
- HCWPIIXVSYCSAN-UHFFFAOYSA-N radium atom Chemical compound [Ra] HCWPIIXVSYCSAN-UHFFFAOYSA-N 0.000 description 6
- 238000005119 centrifugation Methods 0.000 description 5
- 238000004519 manufacturing process Methods 0.000 description 5
- 230000005012 migration Effects 0.000 description 5
- 238000013508 migration Methods 0.000 description 5
- 238000003860 storage Methods 0.000 description 5
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 230000007935 neutral effect Effects 0.000 description 4
- 230000008569 process Effects 0.000 description 4
- 229910001426 radium ion Inorganic materials 0.000 description 4
- ZSLUVFAKFWKJRC-AHCXROLUSA-N thorium-228 Chemical compound [228Th] ZSLUVFAKFWKJRC-AHCXROLUSA-N 0.000 description 4
- 230000002378 acidificating effect Effects 0.000 description 3
- 229910052788 barium Inorganic materials 0.000 description 3
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 3
- 239000000706 filtrate Substances 0.000 description 3
- HLGOSPFVTORIQZ-UHFFFAOYSA-N thorium(4+) tetranitrate hexahydrate Chemical compound O.O.O.O.O.O.[N+](=O)([O-])[O-].[Th+4].[N+](=O)([O-])[O-].[N+](=O)([O-])[O-].[N+](=O)([O-])[O-] HLGOSPFVTORIQZ-UHFFFAOYSA-N 0.000 description 3
- VGBPIHVLVSGJGR-UHFFFAOYSA-N thorium(4+);tetranitrate Chemical compound [Th+4].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VGBPIHVLVSGJGR-UHFFFAOYSA-N 0.000 description 3
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 2
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 2
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 2
- 229910021529 ammonia Inorganic materials 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 229910052732 germanium Inorganic materials 0.000 description 2
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 description 2
- 238000011031 large-scale manufacturing process Methods 0.000 description 2
- 229910017604 nitric acid Inorganic materials 0.000 description 2
- BWHMMNNQKKPAPP-UHFFFAOYSA-L potassium carbonate Chemical compound [K+].[K+].[O-]C([O-])=O BWHMMNNQKKPAPP-UHFFFAOYSA-L 0.000 description 2
- 239000002244 precipitate Substances 0.000 description 2
- 238000001556 precipitation Methods 0.000 description 2
- 239000012217 radiopharmaceutical Substances 0.000 description 2
- 229940121896 radiopharmaceutical Drugs 0.000 description 2
- 230000002799 radiopharmaceutical effect Effects 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 238000005070 sampling Methods 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 238000010998 test method Methods 0.000 description 2
- 230000007704 transition Effects 0.000 description 2
- LWIHDJKSTIGBAC-UHFFFAOYSA-K tripotassium phosphate Chemical compound [K+].[K+].[K+].[O-]P([O-])([O-])=O LWIHDJKSTIGBAC-UHFFFAOYSA-K 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 description 1
- 150000001218 Thorium Chemical class 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 229960005069 calcium Drugs 0.000 description 1
- 229910000019 calcium carbonate Inorganic materials 0.000 description 1
- 235000010216 calcium carbonate Nutrition 0.000 description 1
- 229940062672 calcium dihydrogen phosphate Drugs 0.000 description 1
- FUFJGUQYACFECW-UHFFFAOYSA-L calcium hydrogenphosphate Chemical compound [Ca+2].OP([O-])([O-])=O FUFJGUQYACFECW-UHFFFAOYSA-L 0.000 description 1
- QXDMQSPYEZFLGF-UHFFFAOYSA-L calcium oxalate Chemical compound [Ca+2].[O-]C(=O)C([O-])=O QXDMQSPYEZFLGF-UHFFFAOYSA-L 0.000 description 1
- 239000001506 calcium phosphate Substances 0.000 description 1
- 229960001714 calcium phosphate Drugs 0.000 description 1
- 235000011010 calcium phosphates Nutrition 0.000 description 1
- JGIATAMCQXIDNZ-UHFFFAOYSA-N calcium sulfide Chemical compound [Ca]=S JGIATAMCQXIDNZ-UHFFFAOYSA-N 0.000 description 1
- 235000011132 calcium sulphate Nutrition 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 150000003983 crown ethers Chemical class 0.000 description 1
- 230000003013 cytotoxicity Effects 0.000 description 1
- 231100000135 cytotoxicity Toxicity 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 235000019700 dicalcium phosphate Nutrition 0.000 description 1
- 229940079593 drug Drugs 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 230000000155 isotopic effect Effects 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- VCXNHCBXRKRKSO-UHFFFAOYSA-J oxalate;thorium(4+) Chemical compound [Th+4].[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O VCXNHCBXRKRKSO-UHFFFAOYSA-J 0.000 description 1
- LZMJNVRJMFMYQS-UHFFFAOYSA-N poseltinib Chemical compound C1CN(C)CCN1C(C=C1)=CC=C1NC1=NC(OC=2C=C(NC(=O)C=C)C=CC=2)=C(OC=C2)C2=N1 LZMJNVRJMFMYQS-UHFFFAOYSA-N 0.000 description 1
- 229910000027 potassium carbonate Inorganic materials 0.000 description 1
- 235000011181 potassium carbonates Nutrition 0.000 description 1
- 229910000160 potassium phosphate Inorganic materials 0.000 description 1
- 235000011009 potassium phosphates Nutrition 0.000 description 1
- OTYBMLCTZGSZBG-UHFFFAOYSA-L potassium sulfate Chemical compound [K+].[K+].[O-]S([O-])(=O)=O OTYBMLCTZGSZBG-UHFFFAOYSA-L 0.000 description 1
- 229910052939 potassium sulfate Inorganic materials 0.000 description 1
- 235000011151 potassium sulphates Nutrition 0.000 description 1
- 238000004321 preservation Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 230000002285 radioactive effect Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000012216 screening Methods 0.000 description 1
- 229910000029 sodium carbonate Inorganic materials 0.000 description 1
- 235000017550 sodium carbonate Nutrition 0.000 description 1
- 239000004289 sodium hydrogen sulphite Substances 0.000 description 1
- 239000001488 sodium phosphate Substances 0.000 description 1
- 229910000162 sodium phosphate Inorganic materials 0.000 description 1
- 235000011008 sodium phosphates Nutrition 0.000 description 1
- 229910052938 sodium sulfate Inorganic materials 0.000 description 1
- 235000011152 sodium sulphate Nutrition 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 239000006228 supernatant Substances 0.000 description 1
- MZQZQKZKTGRQCG-UHFFFAOYSA-J thorium tetrafluoride Chemical compound F[Th](F)(F)F MZQZQKZKTGRQCG-UHFFFAOYSA-J 0.000 description 1
- IPIGTJPBWJEROO-UHFFFAOYSA-B thorium(4+);tetraphosphate Chemical compound [Th+4].[Th+4].[Th+4].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O IPIGTJPBWJEROO-UHFFFAOYSA-B 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- QORWJWZARLRLPR-UHFFFAOYSA-H tricalcium bis(phosphate) Chemical compound [Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O QORWJWZARLRLPR-UHFFFAOYSA-H 0.000 description 1
- RYFMWSXOAZQYPI-UHFFFAOYSA-K trisodium phosphate Chemical compound [Na+].[Na+].[Na+].[O-]P([O-])([O-])=O RYFMWSXOAZQYPI-UHFFFAOYSA-K 0.000 description 1
Classifications
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P10/00—Technologies related to metal processing
- Y02P10/20—Recycling
Abstract
The present application provides a method of extracting decay daughter of thorium element, wherein the method comprises the steps of leaching: mixing thorium hydroxide particles with a leaching solution so that decaying daughter of thorium element in the thorium hydroxide particles is dissolved in the leaching solution; and (3) solid-liquid separation: the thorium hydroxide particles mixed with the leaching solution are separated from the liquid to obtain a solution of decaying daughter containing thorium element. The method can achieve higher leaching efficiency, and the leaching efficiency of multiple times of extraction is up to 88%.
Description
Technical Field
The present application relates to the field of radioactive elements, in particular to a method of extracting decay daughter of thorium element, more particularly by thorium hydroxide particles.
Background
In recent years, the field of alpha-therapeutic isotope radiopharmaceuticals has grown rapidly, and many studies on the preparation of radiopharmaceuticals and nuclides for alpha nuclides have been widely conducted. Wherein, 212 Pb（ 212 bi) is an important representation of emerging alpha nuclides, a daughter thereof 212 Bi (6.05 MVe) and 212 po (8.78 Mev) exhibits excellent cytotoxicity as an alpha emitter which ultimately gives rise to toxicity (drug efficacy). Meanwhile, the production of the nuclide does not depend on the long-term reserve of national nuclide, and can be extracted from natural thorium elements. 232 Natural decay chain of Th, in this chain 212 Pb and 212 bi is composed of 232 Th is produced by continuous decay.
Wherein, 232 th is the major isotopic component of natural thorium. 228 Th is also distributed in natural thorium or obtained by other enrichment means. From what is known as 212 In terms of Pb production mode, by natural means 232 Preparation of nuclide on Th stepwise extraction decay chain 212 Pb being the most predominant 212 Pb production mode. However, due to 232 The Th half-life was very long (1.4X10) 10 Years), 5 years of shelf life 232 Th contains only 2×10 -10 (w/w) 228 Ra (Ra). Thus, how to get from a large number of 232 Extraction from Th 228 Ra, i.e. all 212 The starting point of Pb preparation production is also the most critical technical difficulty. Known slave 232 Extraction from Th 228 The method for Ra comprises the following steps: barium coprecipitation, selective radium resin extraction, and the like. The methods in the prior art have the advantages and the disadvantages, such as high single waste liquid content of the barium coprecipitation method; the selective radium resin extraction method requires expensive selective resins. And both methods require long-term storage of large amounts of strongly acidic Th (IV) solutions.
Disclosure of Invention
The technical problem to be solved by the application is the deficiency in the background technology and provides a method for extracting decay daughter of thorium element.
The technical scheme of the application is as follows:
a method of extracting a decay daughter of thorium element, wherein the method comprises,
leaching: mixing thorium hydroxide particles with a leaching solution so that decaying daughter of thorium element in the thorium hydroxide particles is dissolved in the leaching solution;
and (3) solid-liquid separation: the thorium hydroxide particles mixed with the leaching solution are separated from the liquid to obtain a solution of decaying daughter containing thorium element.
In some embodiments, an aging process is performed prior to the leaching step, wherein the aging step comprises: the thorium hydroxide particles are left for a period of time to enrich the decay daughter of the thorium element.
In some embodiments, the leaching solution is selected from one or more of water, nitrate solution, hydrochloride solution, sodium salt solution, potassium salt solution, calcium salt solution, ammonium salt solution.
In some embodiments of the present invention, in some embodiments, the nitrate is selected from sodium nitrate, potassium nitrate, silver nitrate, magnesium nitrate, calcium nitrate, copper nitrate, ferric nitrate, zinc nitrate, barium nitrate, aluminum nitrate, cesium nitrate,And one or more than two of ferrous nitrate;
the hydrochloride is selected from sodium chloride, potassium chloride, magnesium chloride, calcium chloride, copper chloride, ferric chloride, zinc chloride, barium chloride, aluminum chloride, cesium chloride, and,And one or more than two of ferrous chloride;
the sodium salt is one or more than two of sodium chloride, sodium bicarbonate, sodium bisulfate, sodium nitrate, sodium hydrogen phosphate, sodium dihydrogen phosphate, sodium sulfide, sodium sulfite, sodium bisulfite, sodium nitrite, sodium ferrate, sodium fluoride, sodium bromide, sodium iodide, sodium formate, sodium acetate and sodium oxalate;
the potassium salt is selected from one or more than two of potassium chloride, potassium bicarbonate, potassium bisulfate, potassium nitrate, potassium hydrogen phosphate, potassium dihydrogen phosphate, potassium sulfide, potassium sulfite, potassium hydrogen sulfite, potassium nitrite, potassium ferrate, potassium fluoride, potassium bromide, potassium iodide, potassium formate, potassium acetate and potassium oxalate;
the calcium salt is one or more than two of calcium chloride, calcium bicarbonate, calcium bisulfate, calcium nitrate, calcium hydrophosphate, calcium biphosphate, calcium sulfite, calcium nitrite, calcium bromide, calcium iodide, calcium formate, calcium acetate and calcium acetate;
the ammonium salt is selected from one or more than two of ammonium chloride, ammonium bicarbonate, ammonium bisulfate, ammonium nitrate, ammonium hydrogen phosphate, ammonium dihydrogen phosphate, ammonium sulfide, ammonium sulfite, ammonium bisulfide, ammonium nitrite, ammonium ferrate, ammonium fluoride, ammonium bromide, ammonium iodide, ammonium formate, ammonium acetate and ammonium oxalate.
In some embodiments, the leaching solution is a sodium chloride solution and/or a sodium nitrate solution.
In some embodiments, the pH of the leaching solution is 4-12.
In some embodiments, the pH of the leaching solution is 6 to 8.
In some embodiments, the leaching solution is 0.5 to 20 volumes compared to 1 volume of thorium hydroxide particles.
In some embodiments, the leaching solution is 1-3 volumes compared to 1 volume of thorium hydroxide particles.
In some embodiments, the leaching step, the solid-liquid separation step, are repeated to further extract the decay daughter.
In some embodiments, the thorium hydroxide particles are prepared as follows:
adding alkali containing hydroxyl or aqueous solution thereof into the solution containing thorium ions to obtain a mixed solution, regulating the pH value of the mixed solution to 4-14, and carrying out solid-liquid separation to obtain thorium hydroxide particles.
In some embodiments, the thorium hydroxide particles have a diameter of from 100 nm mm to 1mm.
In some embodiments, the pH of the mixed solution is 4-10.
In some embodiments, the hydroxide-containing base is selected from one or more of ammonia, sodium hydroxide, calcium hydroxide, potassium hydroxide, barium hydroxide, cesium hydroxide.
In some embodiments, the hydroxide-containing base is sodium hydroxide.
In some embodiments, the means for solid-liquid separation is selected from one or more of filtration, centrifugation, decantation, or natural settling.
In some embodiments, the means of solid-liquid separation is filtration.
The prior art has been a Ra/Th separation method (Ra-selective adsorption resin method) using specific crown ether resin to selectively adsorb Ra (II) without adsorbing Th (IV), or a method (BaSO) for enriching Ra (II) from Th (IV) using co-precipitation method of homogeneous Ba (II) and Ra (II) 4 Coprecipitation method), the methods in the prior art have various advantages and various disadvantages, such as high single waste liquid content in the barium coprecipitation method; the selective radium resin extraction method requires expensive selective resins, and both methods require long-term storage of large amounts of strongly acidic Th (IV) solutions.
In order to solve these problems, the applicant of the present application has made a great deal of attempts and innovations, from the practice it has been concluded that the decay daughter of thorium is more soluble in aqueous solutions, whereas the thorium ions (Th 4+ ) The characteristic of poor solubility is that decay daughter is selectively extracted into aqueous solution.
Furthermore, in the screening of a large amount of thorium solids, the applicant of the application finds that the thorium hydroxide contains a higher proportion of water, and the characteristic can greatly improve the migration speed of the decay daughter and quickly complete the migration of the decay daughter from the solid phase to the liquid phase.
In addition, the chemical form and morphology of the thorium hydroxide are not affected in the extraction process, so that the thorium hydroxide particles can be stored in an aqueous solution for a long time, and decay daughter can be repeatedly extracted from the thorium hydroxide.
Meanwhile, in order to increase the contact area of thorium hydroxide and leaching solution, the leaching efficiency is further improved by preparing thorium hydroxide into particles.
Methods in the prior art (Ra Selective adsorption resin method and BaSO) 4 Coprecipitation method) requires long-term preservation of a strongly acidic Th (IV) solution, and the long-term storage of thorium hydroxide particles in this application is in the form of neutral wet solids, which is easier for large-scale storage.
The method has simple extraction operation process, is beneficial to realizing large-scale production, and is easy to store thorium hydroxide. Most importantly, the method has high efficiency of extracting the decay daughter and low thorium element residue.
The application is suitable for direct extraction of natural thorium 228 Ra from containing 228 Extraction of natural thorium from Th 224 Ra (b); from containing 228 Extraction of natural thorium from Th 224 Ra。
The method is used for extracting radium ions (Ra 2+ ) When the laser ion (Ra) 2+ ) The solid-liquid transition agent is easier to dissolve in aqueous solution, can rapidly finish transition from a solid phase to a liquid phase, and has high efficiency and low thorium element residue. For example, a single step operation obtained from natural thorium 228/224 In Ra solution 232 The proportion of Th is increased to 10 -4 ~10 -2 (w/w). The thorium hydroxide particles of the application have high water content, and can effectively realize the effect of radium ion (Ra 2+ ) In the solid phase migration, high leaching efficiency is realized, for example, the leaching rate of the first leaching can reach 52% and above, and the leaching efficiency of the repeated leaching can reach 88% and above.
The application firstly completes the extraction of radium ions (Ra 2+ ) According to the scheme, the storage difficulty can be effectively reduced.
Drawings
FIG. 1 shows 232 Decay chain of Th.
Detailed Description
The present application is further illustrated below with reference to examples, it being understood that the examples are for further illustration and explanation of the application only and are not intended to limit the application.
Unless defined otherwise, technical and scientific terms used in this specification have the same meaning as commonly understood by one of ordinary skill in the art. Although methods and materials similar or equivalent to those described herein can be used in the practice or testing of the present invention, the materials and methods are described herein below. In case of conflict, the present specification, including definitions therein, will control and materials, methods, and examples, will control and be in no way limiting. The present application is further illustrated below in conjunction with specific examples, but is not intended to limit the scope of the present application.
In the present application, the source of thorium hydroxide particles is not limited, and is commercially available or can be obtained by self-preparation. The person skilled in the art can choose the way of obtaining the thorium hydroxide particles on demand. For example, in some modes of acquisition, it may be obtained by means of self-preparation, such as by the action of thorium salts with alkali or concentrated ammonia, to precipitate thorium hydroxide particles.
In the present application, the decay daughter of thorium element means 232 Th decays to give a material, as shown in FIG. 1, which may be 228 Ac、 228 Ra、 228 Th、 224 Ra、 220 Rn、 216 Po、 212 Pb、 212 Bi、 208 One or more of Pb. The decay daughter of thorium element has different properties and applications, and a person skilled in the art can select a suitable mode to extract the decay daughter according to actual needs.
The present application provides a process for extracting decay daughter of thorium element by thorium hydroxide particles, wherein the process comprises: leaching: mixing thorium hydroxide particles with a leaching solution so that decaying daughter of thorium element in the thorium hydroxide particles is dissolved in the leaching solution; and (3) solid-liquid separation: the thorium hydroxide particles mixed with the leaching solution are separated from the liquid to obtain a solution of decaying daughter containing thorium element.
In some embodiments of the present application, prior to leaching, an aging treatment is performed, wherein the aging step comprises: and placing the thorium hydroxide particles for a period of time to enrich the decay daughter of the thorium element, and leaching the aged thorium hydroxide particles after the decay daughter reaches a certain concentration.
In some embodiments of the present application, the decay daughter may also be leached directly without aging.
In the present application, whether to perform the aging treatment is mainly determined according to actual needs. It will be appreciated by those skilled in the art that the concentration of decay gas will further increase after aging. However, without aging treatment, the decay daughter can also be extracted efficiently using the method of the present application.
In the present application, the inventors have found that decay species of thorium are more soluble in aqueous solutions, whereas thorium ions (Th 4+ ) Is not easily dissolved in the aqueous solution, so that the decay daughter can be selectively extracted into the aqueous solution, for example 228 Ra and/or 224 Ra is selectively extracted to an aqueous solution.
In the present application, leaching solution refers to decay-type bodies that readily dissolve thorium element, but not to thorium ions (Th 4+ ) I.e. Th (IV) in the insoluble thorium hydroxide particles.
In the application, the thorium hydroxide particles are neutral wet solids and contain a higher proportion of water, so that the migration speed of radium ions can be improved, and the migration from a solid phase to a liquid phase can be completed quickly. In addition, the chemical form and morphology of the thorium hydroxide are not affected in the extraction process, so that the thorium hydroxide particles can be stored in an aqueous solution for a long time, and radium can be repeatedly extracted from the thorium hydroxide particles.
In some embodiments of the present application, the decay daughter is selected from the group consisting of 228 Ac， 228 Ra， 224 Ra， 220 Rn， 212 Pb， 212 One or more of Bi; preferably is 228 Ra and/or 224 Ra。
In the present application, 228 ra and/or 224 Ra has a longer half-life than other decay daughter, and is easy to carry out more complex purification processes, generally in medical isotopes 212 Pb/ 212 Bi is independently used as a key intermediate nuclide in the production of Bi.
In the present application, the leaching rate refers to the proportion of decay species to be leached that dissolve into the leaching solution after mixing the thorium hydroxide particles with the leaching solution.
In this application, the leaching rate is calculated as follows:
224 ra content test method: the sample is taken and directly tested by a high purity germanium (HPGe) gamma spectrometer, and the energy peak count of 240.0 keV is used for determining 224 Ra content;
228 ra content test method: taking a proper amount of sample, placing the sample to be tested at not lower than 24 h, and taking the sample 228 Ra and its daughter 228 After Ac reaches equilibrium, it is directly tested by high purity germanium (HPGe) gamma spectrometer and determined by 911.1 keV energy peak count 228 Ac content of 228 Ra activity is equal to 228 Activity of Ac.
Leaching rate: leaching rate = Ra activity in liquid phase/(Ra activity in liquid phase+ra activity in solid phase).
In this application, the inventors have found that the pH of the leaching solution has a great influence on the leaching rate. When the pH does not meet the specific conditions, the leaching rate is low or substantially 0. The pH value of the leaching solution is 4-12; for example, the pH of the leaching solution may be 4, 5, 6, 7, 8, 9, 10, 11, 12 or any range therebetween.
In some preferred embodiments of the present application, the pH of the leaching solution is 6 to 8. The inventors found that the leaching rate was the highest when the pH of the leaching solution was 6 to 8, 228 ra and/or 224 The Ra leaching rates were all highest.
In this application, the inventors have found that the choice of leaching solution can further affect leaching rates, e.g., some insoluble salts or salts that cause precipitation of Ra, cannot be used as leaching solutions, e.g., sodium carbonate, sodium sulfate, sodium phosphate, potassium carbonate, potassium sulfate, potassium phosphate, calcium carbonate, calcium sulfate, calcium phosphate, calcium sulfide, calcium sulfite, calcium oxalate, and the like. Some leachates may help 228 Ra and/or 224 Leaching effect of Ra. The leaching solution is selected from water, nitrate solution, hydrochloride solution, sodium salt solution, potassium salt solution, and calciumOne or more of salt solution and ammonium salt solution.
In some embodiments of the present application, the nitrate is selected from sodium nitrate, potassium nitrate, silver nitrate, magnesium nitrate, calcium nitrate, copper nitrate, ferric nitrate, zinc nitrate, barium nitrate, aluminum nitrate, cesium nitrate,And one or more than two of ferrous nitrate.
In some embodiments of the present application, the hydrochloride is selected from the group consisting of sodium chloride, potassium chloride, magnesium chloride, calcium chloride, copper chloride, ferric chloride, zinc chloride, barium chloride, aluminum chloride, cesium chloride,And one or more than two of ferrous chloride.
In some embodiments of the present application, the sodium salt is selected from one or more of sodium chloride, sodium bicarbonate, sodium bisulfate, sodium nitrate, sodium hydrogen phosphate, sodium dihydrogen phosphate, sodium sulfide, sodium sulfite, sodium bisulphite, sodium nitrite, sodium ferrate, sodium fluoride, sodium bromide, sodium iodide, sodium formate, sodium acetate, and sodium oxalate.
In some embodiments of the present application, the potassium salt is selected from one or more of potassium chloride, potassium bicarbonate, potassium bisulfate, potassium nitrate, potassium hydrogen phosphate, potassium dihydrogen phosphate, potassium sulfide, potassium sulfite, potassium hydrogen sulfite, potassium nitrite, potassium ferrate, potassium fluoride, potassium bromide, potassium iodide, potassium formate, potassium acetate, and potassium oxalate.
In some embodiments of the present application, the calcium salt is selected from one or more of calcium chloride, calcium bicarbonate, calcium bisulfate, calcium nitrate, calcium hydrogen phosphate, calcium dihydrogen phosphate, calcium sulfite, calcium nitrite, calcium bromide, calcium iodide, calcium formate, calcium acetate, and calcium acetate.
In some embodiments of the present application, the ammonium salt is selected from one or more of ammonium chloride, ammonium bicarbonate, ammonium bisulfate, ammonium nitrate, ammonium bisulfate, ammonium dihydrogen phosphate, ammonium sulfide, ammonium sulfite, ammonium bisulfide, ammonium nitrite, ammonium ferrate, ammonium fluoride, ammonium bromide, ammonium iodide, ammonium formate, ammonium acetate, and ammonium oxalate.
In some preferred embodiments of the present application, the leaching solution is a sodium chloride solution and/or a sodium nitrate solution.
In some embodiments of the present application, the leaching solution is 0.5 to 20 volumes, preferably 1 to 3 volumes, compared to 1 volume of thorium hydroxide particles; for example, the leaching solution may be 0.5, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20 or any range therebetween, compared to 1 volume of thorium hydroxide particles. The volume of the leaching solution is further increased, so that the leaching rate is not improved, and the cost of raw materials is increased.
In some embodiments of the present application, the leaching step, the solid-liquid separation step, are repeated to further extract the decay daughter. The method can be repeated for a plurality of times, and the leaching rate can be further improved. The number of repetitions can be chosen by the person skilled in the art according to the actual needs. Wherein, the repeated leaching step and the solid-liquid separation step in the application can be divided into multiple leaching and multi-round leaching. Wherein, the multi-round leaching is to repeat the leaching step and the solid-liquid separation step after the aging step, and further extract the decay daughter. The leaching step and the solid-liquid separation step are directly repeated for a plurality of times, and the decay daughter is further extracted. It will be appreciated by those skilled in the art that multiple leaches may be performed in a single round of leaching. The number of times and the number of rounds of leaching can be selected according to actual needs.
In the present application, the term "leaching" means that the leaching step is repeated after one aging step and then the solid-liquid separation step is performed, or that the leaching step is repeated and then the solid-liquid separation step is performed, that is, the leaching is performed a plurality of times in one round of leaching.
In the present application, multiple rounds of leaching refers to completion of a complete aging step, leaching step, solid-liquid separation step, referred to as one round of leaching, or completion of a complete leaching step, solid-liquid separation step, referred to as one round of leaching, multiple rounds of leaching being repeated.
In some embodiments of the present application, an aging process is performed prior to the leaching step.
In some embodiments of the present application, the thorium hydroxide particles are prepared as follows: adding alkali containing hydroxyl or aqueous solution thereof into the solution containing thorium ions to obtain a mixed solution, regulating the pH value of the mixed solution to 4-14, and carrying out solid-liquid separation to obtain thorium hydroxide particles.
In the present application, the source of thorium ions is not limited as long as it is known to those skilled in the art, and for example, the solution containing thorium ions may be thorium fluoride, thorium nitrate, thorium oxalate and thorium phosphate or other solutions containing thorium ions.
In the present application, the inventors have found that the pH of the mixed solution can directly influence the generation of thorium hydroxide particles, and that it is difficult to produce thorium hydroxide particles when the pH of the mixed solution does not satisfy specific conditions. For example, when acidity rises to a certain degree, precipitation cannot be generated. The pH of the mixed solution may be 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14 or any range therebetween.
In some preferred embodiments of the present application, the pH of the mixed solution is between 4 and 10.
In some embodiments of the present application, the thorium hydroxide particles have a diameter of from 100 nm mm to 1mm; for example, the thorium hydroxide particles can have a diameter of 100 nm, 200 nm, 300 nm, 400 nm, 500 nm, 600 nm, 700 nm, 800 nm, 900 nm, 1000nm, 0.01mm, 0.1mm, 1mm, or any range therebetween.
In the present application, the source of the hydroxide-containing base is not limited in any way, as long as it is known to those skilled in the art and satisfies the actual demand. Wherein the hydroxide-containing alkali is selected from one or more of ammonia water, sodium hydroxide, calcium hydroxide, potassium hydroxide, barium hydroxide and cesium hydroxide; sodium hydroxide is preferred.
In some embodiments of the present application, the solid-liquid separation method is not limited in any way, as long as the purpose is satisfied, and a person skilled in the art may select a desired solid-liquid separation method according to actual needs, for example, one or more of filtration, centrifugal separation, decantation, and natural sedimentation; preferably filtration.
In one embodiment of the present application, the thorium hydroxide particles are prepared as follows: dissolving thorium nitrate hexahydrate into water; dropwise adding sodium hydroxide solution, and testing the pH value of the solution by using a pH meter; sampling under different pH conditions, and adjusting the pH to be neutral to prepare the thorium hydroxide particles.
In one embodiment of the present application, the method of extracting the decay daughter by thorium hydroxide particles is as follows: adding sodium nitrate solution into thorium hydroxide particles, mixing, centrifuging, and testing liquid phase and solid 224 Ra content, leaching rate was calculated.
In one embodiment of the present application, thorium nitrate hexahydrate is taken and dissolved in water; dropwise adding sodium hydroxide solution, and testing the pH value of the solution by using a pH meter; sampling under different pH conditions, regulating pH to neutrality, preparing thorium hydroxide particles, centrifuging, and testing liquid phase and solid 224 Ra content, calculating the first leaching rate; adding sodium nitrate solution into thorium hydroxide particles, mixing, centrifuging, and testing liquid phase (combined with first leaching) and solid phase 224 Ra content, calculating the second leaching rate; after adding 1 mL of sodium nitrate solution with ph=7 to thorium hydroxide particles, mixing well, centrifuging and testing the liquid phase (combined with the first and second leaching) and the solid phase respectively 224 Ra content, the third leaching rate was calculated.
The method has simple extraction operation process, is beneficial to realizing large-scale production, and is easy to store thorium hydroxide. The method for extracting radium has high efficiency and low thorium element residue. For example, a single step operation obtained from natural thorium 228/ 224 In Ra solution 232 The proportion of Th is increased to 10 -4 ~10 -2 （w/w）。
The application is suitable for direct extraction of natural thorium 228 Ra from containing 228 Extraction of natural thorium from Th 224 Ra (b); from containing 228 Extraction of natural thorium from Th 224 Ra。
Examples
Example 1 thorium hydroxide particles prepared at different pH conditions
1) Dissolving 10.4. 10.4 g of thorium nitrate hexahydrate in 30 mL of water;
2) Stirring, dripping 1.72-M sodium hydroxide solution, and testing the pH value of the solution by using a pH meter;
3) Samples were taken at different pH values according to Table 1 (examples 1-10 only for different pH values in the preparation of thorium hydroxide particles) of about 1.5. 1.5 mL, pH was adjusted to neutral to prepare thorium hydroxide particles, and after centrifugation, the liquid phase and the solid phase were tested separately 224 Ra content, calculating the first leaching rate;
4) 1 mL of sodium nitrate solution with pH=7 was added to the solid, after mixing, centrifuged and tested for liquid phase (combined with the first leaching) and solid phase, respectively 224 Ra content, calculating the second leaching rate;
5) Adding 1 mL of sodium nitrate solution with pH=7 into the solid, uniformly mixing, centrifuging, and respectively testing the liquid phase and the solid phase 224 Ra content, calculating the leaching rate of the third time;
6) Testing in the combined solution 232 Th residual amount.
Examples 2-10 differ from example 1 only in the pH at which the thorium hydroxide particles are prepared, see in particular Table 1, the remainder being the same as in example 1.
In this embodiment, the multiple leaching is performed continuously in time, so that the overall efficiency of the multiple leaching is more effectively represented, and the following calculation formulas include "the second leaching rate" and "the third leaching rate" which include "the second leaching rate". The leaching rate for multiple leaches was calculated as follows:
first leaching rate = Ra activity in liquid phase after first leaching/(Ra activity in liquid phase after first leaching + Ra activity in solid phase after first leaching)
Second leaching rate = Ra activity in liquid phase after second leaching/(Ra activity in liquid phase after first leaching + Ra activity in solid phase after first leaching) +first leaching rate
Third leaching rate = Ra activity in liquid phase after third leaching/(Ra activity in liquid phase after first leaching + Ra activity in solid phase after first leaching) +second leaching rate
TABLE 1
。
As can be seen from table 1, at pH <3.7, thorium ions are unable to produce thorium hydroxide particle precipitates, which occur as the acidity decreases. After three leaching, the leaching rate of the thorium hydroxide particles obtained under the condition that the pH is 4.77-12.2 is 72% -88%. The precipitate of thorium hydroxide particles, which is produced in a weakly basic form (pH 10.7, 12.2), has a significantly lower leaching rate in the first leaching, which may be affected by the residual alkali in the thorium hydroxide particles. In the second leaching and the third leaching, the leaching rates reached similar rates to those of the thorium hydroxide particles prepared in examples 6-7.
Examples 11 to 18
Example 11
1) Weighing thorium hydroxide particles prepared in example 7, adding leaching solutions according to the weight ratio of 1:1, wherein the leaching solutions are sodium nitrate solutions, and the pH values of the leaching solutions are shown in Table 2, (examples 11-18 only refer to the difference in pH values of the leaching solutions, wherein the pH values are adjusted by nitric acid or sodium hydroxide);
2) After mixing evenly, testing the liquid phase and the solid phase after centrifugation 224 Ra content, calculating a round of leaching rate;
3) The same leaching solution as in step 1) is added to the thorium hydroxide particles again, and after mixing, the mixture is left for about 7 days. Testing liquid phase and solid phase after centrifugation 224 Ra content, two rounds of leaching rate was calculated.
Examples 12-18 differ from example 11 only in the pH of the leach solution, which is adjusted by nitric acid or sodium hydroxide, see in particular Table 2, with the remainder being the same as in example 11.
In this example, the multi-round leaching rate is calculated as follows:
first round leaching rate = Ra activity in liquid phase after first round leaching/(Ra activity in liquid phase after first round leaching + Ra activity in solid phase after first round leaching)
Second round leaching rate = Ra activity in liquid phase after second round leaching/(Ra activity in supernatant after second round leaching + Ra activity in solid phase after second round leaching)
TABLE 2
。
As is clear from Table 2, the leaching solutions of different pH values hardly leach under slightly alkaline conditions (pH 10.76, 12.08) when leaching the thorium hydroxide particles of example 7, especially at pH 12.8. Wherein the optimal leaching rate is at pH 6.35 and pH 6.92, so that pH 6-8 is considered to be the optimal leaching solution interval. As can be seen from examples 13-18, the leaching efficiency did not decrease after two rounds of leaching.
Examples 19-34 different salt solutions leaching
Example 19
1) Weighing thorium hydroxide particles prepared in example 7, adding leaching solution with pH of 6-7 in a weight ratio of 1:1, mixing the leaching solution with salt solution specified in Table 3, and standing for one week;
2) After mixing evenly, testing the liquid phase and the solid after centrifugation 224 Ra content, leaching rate was calculated.
Examples 20-34 differ from example 19 only in the leaching solution, see in particular Table 3, and the remainder are the same as in example 19.
TABLE 3 Table 3
。
Example 35 Single-round multiple leaching of thorium hydroxide particles 228 Ra
1) 1L of 200g/L natural thorium nitrate solution is taken, 2.2 mol/L sodium hydroxide solution is added into the solution until the pH of the solution reaches 6-8, and the solution is removed by filtration to obtain about 1L of thorium hydroxide particles of about 0.5L;
2) Adding sodium nitrate solution 0.5-L with pH of 6-7 into the thorium hydroxide particles obtained in step 1), soaking, and standing for two years (initial solid-liquid mixture contains 228 Ra 69327 Bq）；
3) Filtering to obtain filtrate containing 228 Solution 0.5. 0.5L of Ra, which is designated solution 1-1; filtering to obtain thorium hydroxide particles;
4) Adding sodium nitrate solution with pH of 6-7 into the thorium hydroxide particles obtained by filtering in the step 3) to 0.5-L, and soaking;
5) Filtering to obtain filtrate containing 228 Solution 0.5. 0.5L of Ra, which is designated as solution 1-2; filtering to obtain thorium hydroxide particles;
6) Adding sodium nitrate solution with pH of 6-7 into the thorium hydroxide particles obtained by filtering in the step 5) to 0.5-L, and soaking;
7) Filtering to obtain filtrate containing 228 Solution 0.5. 0.5L of Ra, which is designated as solutions 1-3.
Through testing, in solution 1-1 228 Ra total content 38347 Bq, in solution 1-2 228 Ra total content 14828 Bq, in solution 1-3 228 The total Ra content 7481, bq, 60656, bq and leaching rate 87%.
Example 35 shows that: the sum of the three leaching rates can reach 87 percent.
The leaching rate of the multiple leaching in this example was calculated as follows:
leaching rate= (Ra activity in liquid phase after first leaching + Ra activity in liquid phase after second leaching + Ra activity in liquid phase after third leaching)/Ra activity in initial solid-liquid mixture.
In the examples, the unit of activity is Bq, the same as below.
EXAMPLE 36 Long-term Multi-round leaching of thorium hydroxide particles 224 Ra
1) 1000 mL of 200g/L natural thorium nitrate (containing approximately 1600 Bq/g) 228 Th) solution, adding 2.2 mol/L sodium hydroxide solution to the solution until the pH of the solution reaches 6-8, centrifuging by a low-speed centrifuge, and recovering the liquid to obtain about 400 mL of thorium hydroxide particles;
2) Adding 500-mL of sodium nitrate solution with the pH of 6-7 into the thorium hydroxide particles obtained in the step 1), and soaking;
3) Left for about 1 week (wherein the initial solid-liquid mixture contains 241218 Bq 224 Ra）；
4) Centrifuging by a low-speed centrifuge to recover liquid, wherein the liquid is named as solution 2-1; filtering to obtain thorium hydroxide particles;
5) Adding 500-mL of sodium nitrate solution with pH of 6-7 into the thorium hydroxide particles obtained in the step 4), and soaking;
6) Left for about 1 week (wherein the initial solid-liquid mixture contains 240678 Bq 224 Ra）；
7) Centrifuging by a low-speed centrifuge to recover liquid, wherein the liquid is denoted as solution 2-2; filtering to obtain thorium hydroxide particles;
8) Adding 500-mL of sodium nitrate solution with the pH of 6-7 into the thorium hydroxide particles obtained in the step 7), and soaking;
9) Left for about 1 week (wherein the initial solid-liquid mixture contains 220889 Bq 224 Ra）；
10 Low-speed centrifuge to recover the liquid, which is designated as solution 2-3; filtering to obtain thorium hydroxide particles;
11 Adding 500 mL of sodium nitrate solution with pH of 7 to the thorium hydroxide particles obtained in the step 10), and soaking;
through testing, in solution 2-1 224 Ra total content 123834 Bq (first round leaching rate 51%), solution 2-2 224 Ra Total content 108273 Bq (second round leaching rate 45%), solution 2-3 224 Ra total content 103532 Bq (47% leaching rate on the third round).
In this embodiment:
first round leaching rate = Ra activity in the liquid phase after the first round leaching/Ra activity in the initial solid-liquid mixture of the first round
Second round leaching rate = Ra activity in liquid phase after the second round leaching/Ra activity in initial solid-liquid mixture of the second round
Third leaching rate = Ra activity in the liquid phase after the third leaching/Ra activity in the initial solid-liquid mixture of the third leaching
Example 36 shows that: the method can be used for continuous multi-round radium extraction, the extraction rate is 45% -51%, and no obvious reduction of leaching efficiency is seen.
Although the present invention has been described with reference to the above embodiments, it should be understood that the invention is not limited thereto, but rather is capable of modification and variation without departing from the spirit and scope of the present invention as defined in the following claims.
Claims (15)
1. A method of extracting a decay daughter of thorium element, wherein the method comprises,
leaching: mixing thorium hydroxide particles with a leaching solution so that decaying daughter of thorium element in the thorium hydroxide particles is dissolved in the leaching solution;
and (3) solid-liquid separation: the thorium hydroxide particles mixed with the leaching solution are separated from the liquid to obtain a solution of decaying daughter containing thorium element.
2. The method of claim 1, wherein,
before the leaching step, an aging treatment is carried out, wherein the aging step comprises the following steps: the thorium hydroxide particles are left for a period of time to enrich the decay daughter of the thorium element.
3. The method of claim 1, wherein,
the leaching solution is one or more than two selected from water, nitrate solution, hydrochloride solution, sodium salt solution, potassium salt solution, calcium salt solution and ammonium salt solution.
4. The method of claim 3, wherein,
the nitrate is selected from one or more than two of sodium nitrate, potassium nitrate, silver nitrate, magnesium nitrate, calcium nitrate, copper nitrate, ferric nitrate, zinc nitrate, barium nitrate, aluminum nitrate, cesium nitrate, ammonium nitrate and ferrous nitrate;
the hydrochloride is one or more than two of sodium chloride, potassium chloride, magnesium chloride, calcium chloride, copper chloride, ferric chloride, zinc chloride, barium chloride, aluminum chloride, cesium chloride, ammonium chloride and ferrous chloride;
the sodium salt is one or more than two of sodium chloride, sodium bicarbonate, sodium bisulfate, sodium nitrate, sodium hydrogen phosphate, sodium dihydrogen phosphate, sodium sulfide, sodium sulfite, sodium bisulfite, sodium nitrite, sodium ferrate, sodium fluoride, sodium bromide, sodium iodide, sodium formate, sodium acetate and sodium oxalate;
the potassium salt is selected from one or more than two of potassium chloride, potassium bicarbonate, potassium bisulfate, potassium nitrate, potassium hydrogen phosphate, potassium dihydrogen phosphate, potassium sulfide, potassium sulfite, potassium hydrogen sulfite, potassium nitrite, potassium ferrate, potassium fluoride, potassium bromide, potassium iodide, potassium formate, potassium acetate and potassium oxalate;
the calcium salt is one or more than two of calcium chloride, calcium bicarbonate, calcium bisulfate, calcium nitrate, calcium hydrophosphate, calcium biphosphate, calcium sulfite, calcium nitrite, calcium bromide, calcium iodide, calcium formate, calcium acetate and calcium acetate;
the ammonium salt is selected from one or more than two of ammonium chloride, ammonium bicarbonate, ammonium bisulfate, ammonium nitrate, ammonium hydrogen phosphate, ammonium dihydrogen phosphate, ammonium sulfide, ammonium sulfite, ammonium bisulfide, ammonium nitrite, ammonium ferrate, ammonium fluoride, ammonium bromide, ammonium iodide, ammonium formate, ammonium acetate and ammonium oxalate.
5. The method of claim 1, wherein,
the pH value of the leaching solution is 4-12.
6. The method of claim 5, wherein,
the pH value of the leaching solution is 6-8.
7. The method of claim 1, wherein,
the leaching solution is 0.5-20 volumes compared with 1 volume of thorium hydroxide particles.
8. The method according to claim 1 or 2, wherein,
and repeating the leaching step and the solid-liquid separation step, and further extracting the decay daughter.
9. The method of claim 1, wherein,
the thorium hydroxide particles were prepared as follows:
adding alkali containing hydroxyl or aqueous solution thereof into the solution containing thorium ions to obtain a mixed solution, regulating the pH value of the mixed solution to 4-14, and carrying out solid-liquid separation to obtain thorium hydroxide particles.
10. The method of claim 1, wherein,
the diameter of the thorium hydroxide particles is 100 nm-1mm.
11. The method of claim 9, wherein,
the pH of the mixed solution is 4-10.
12. The method of claim 9, wherein,
the hydroxide-containing alkali is selected from one or more of ammonia water, sodium hydroxide, calcium hydroxide, potassium hydroxide, barium hydroxide and cesium hydroxide.
13. The method of claim 12, wherein,
the hydroxide-containing base is sodium hydroxide.
14. The method of claim 1, wherein,
the solid-liquid separation mode is one or more than two selected from filtration, centrifugal separation, decantation or natural sedimentation.
15. The method of claim 14, wherein,
the solid-liquid separation mode is filtration.
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