CN101862463A - Preparation method of 18F-labeled nano particle and application thereof - Google Patents
Preparation method of 18F-labeled nano particle and application thereof Download PDFInfo
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- CN101862463A CN101862463A CN 201010202271 CN201010202271A CN101862463A CN 101862463 A CN101862463 A CN 101862463A CN 201010202271 CN201010202271 CN 201010202271 CN 201010202271 A CN201010202271 A CN 201010202271A CN 101862463 A CN101862463 A CN 101862463A
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- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- 239000002105 nanoparticle Substances 0.000 title abstract description 12
- 238000000034 method Methods 0.000 claims abstract description 69
- 239000002245 particle Substances 0.000 claims abstract description 63
- 150000001768 cations Chemical class 0.000 claims abstract description 16
- 150000001450 anions Chemical class 0.000 claims abstract description 7
- 230000003993 interaction Effects 0.000 claims abstract description 6
- 239000002086 nanomaterial Substances 0.000 claims description 80
- 229910010252 TiO3 Inorganic materials 0.000 claims description 31
- 238000003384 imaging method Methods 0.000 claims description 30
- 238000002600 positron emission tomography Methods 0.000 claims description 19
- -1 oxides Substances 0.000 claims description 15
- 229910019142 PO4 Inorganic materials 0.000 claims description 11
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 claims description 11
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 claims description 6
- 229910052691 Erbium Inorganic materials 0.000 claims description 6
- 229910052769 Ytterbium Inorganic materials 0.000 claims description 6
- 150000003839 salts Chemical class 0.000 claims description 6
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 5
- 239000002131 composite material Substances 0.000 claims description 5
- 229910003443 lutetium oxide Inorganic materials 0.000 claims description 5
- KLZUFWVZNOTSEM-UHFFFAOYSA-K Aluminium flouride Chemical compound F[Al](F)F KLZUFWVZNOTSEM-UHFFFAOYSA-K 0.000 claims description 4
- 229910020186 CeF4 Inorganic materials 0.000 claims description 4
- 229910002319 LaF3 Inorganic materials 0.000 claims description 4
- 150000001449 anionic compounds Chemical class 0.000 claims description 4
- AYJRCSIUFZENHW-UHFFFAOYSA-L barium carbonate Chemical compound [Ba+2].[O-]C([O-])=O AYJRCSIUFZENHW-UHFFFAOYSA-L 0.000 claims description 4
- 229910000019 calcium carbonate Inorganic materials 0.000 claims description 4
- 150000001767 cationic compounds Chemical class 0.000 claims description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 claims description 4
- 229910015805 BaWO4 Inorganic materials 0.000 claims description 3
- 229910052684 Cerium Inorganic materials 0.000 claims description 3
- 229910052692 Dysprosium Inorganic materials 0.000 claims description 3
- 229910052693 Europium Inorganic materials 0.000 claims description 3
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 3
- 229910052689 Holmium Inorganic materials 0.000 claims description 3
- 229910021159 KSmF4 Inorganic materials 0.000 claims description 3
- 229910010896 LiLaF4 Inorganic materials 0.000 claims description 3
- 229910018966 NaNdF4 Inorganic materials 0.000 claims description 3
- 229910052779 Neodymium Inorganic materials 0.000 claims description 3
- 229910052777 Praseodymium Inorganic materials 0.000 claims description 3
- 229910052772 Samarium Inorganic materials 0.000 claims description 3
- 229910018096 ScF3 Inorganic materials 0.000 claims description 3
- 229910052771 Terbium Inorganic materials 0.000 claims description 3
- 229910052775 Thulium Inorganic materials 0.000 claims description 3
- 229910010342 TiF4 Inorganic materials 0.000 claims description 3
- 229910002113 barium titanate Inorganic materials 0.000 claims description 3
- 229910001634 calcium fluoride Inorganic materials 0.000 claims description 3
- 229910052735 hafnium Inorganic materials 0.000 claims description 3
- 229910052746 lanthanum Inorganic materials 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- 229910052706 scandium Inorganic materials 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 229910052727 yttrium Inorganic materials 0.000 claims description 3
- 229910000164 yttrium(III) phosphate Inorganic materials 0.000 claims description 3
- 229910052726 zirconium Inorganic materials 0.000 claims description 3
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 2
- 229910002971 CaTiO3 Inorganic materials 0.000 claims description 2
- 229910004829 CaWO4 Inorganic materials 0.000 claims description 2
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 2
- 229910002493 Ce2(CO3)3 Inorganic materials 0.000 claims description 2
- 229910020187 CeF3 Inorganic materials 0.000 claims description 2
- 229910020197 CePO4 Inorganic materials 0.000 claims description 2
- 229910016468 DyF3 Inorganic materials 0.000 claims description 2
- 229910016495 ErF3 Inorganic materials 0.000 claims description 2
- 229910016653 EuF3 Inorganic materials 0.000 claims description 2
- KRHYYFGTRYWZRS-UHFFFAOYSA-M Fluoride anion Chemical compound [F-] KRHYYFGTRYWZRS-UHFFFAOYSA-M 0.000 claims description 2
- 229910005561 Gd2(CO3)3 Inorganic materials 0.000 claims description 2
- 229910003337 Gd2Ti2O7 Inorganic materials 0.000 claims description 2
- 229910005693 GdF3 Inorganic materials 0.000 claims description 2
- 229910004504 HfF4 Inorganic materials 0.000 claims description 2
- 229910004650 HoF3 Inorganic materials 0.000 claims description 2
- 229910021023 KLaF4 Inorganic materials 0.000 claims description 2
- 229910021053 KNdF4 Inorganic materials 0.000 claims description 2
- 229910020854 La(OH)3 Inorganic materials 0.000 claims description 2
- 229910017569 La2(CO3)3 Inorganic materials 0.000 claims description 2
- 229910002248 LaBO3 Inorganic materials 0.000 claims description 2
- 229910001477 LaPO4 Inorganic materials 0.000 claims description 2
- 229910013666 LiNdF4 Inorganic materials 0.000 claims description 2
- 229910012378 LiSmF4 Inorganic materials 0.000 claims description 2
- 229910013482 LuF3 Inorganic materials 0.000 claims description 2
- 229910052765 Lutetium Inorganic materials 0.000 claims description 2
- 229910017676 MgTiO3 Inorganic materials 0.000 claims description 2
- 229910017672 MgWO4 Inorganic materials 0.000 claims description 2
- 229910021266 NaErF4 Inorganic materials 0.000 claims description 2
- 229910019264 NaLaF4 Inorganic materials 0.000 claims description 2
- 229910019431 NaSmF4 Inorganic materials 0.000 claims description 2
- 229910017512 Nd2(CO3)3 Inorganic materials 0.000 claims description 2
- 229910017557 NdF3 Inorganic materials 0.000 claims description 2
- 229910019322 PrF3 Inorganic materials 0.000 claims description 2
- 229910021181 Sm2(CO3)3 Inorganic materials 0.000 claims description 2
- 229910021175 SmF3 Inorganic materials 0.000 claims description 2
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims description 2
- 229910004299 TbF3 Inorganic materials 0.000 claims description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 2
- 229910008903 TmF3 Inorganic materials 0.000 claims description 2
- 229910009454 Y(OH)3 Inorganic materials 0.000 claims description 2
- 229910009440 Y2(CO3)3 Inorganic materials 0.000 claims description 2
- 229910009372 YVO4 Inorganic materials 0.000 claims description 2
- 229910009544 Yb(OH)3 Inorganic materials 0.000 claims description 2
- 229910009520 YbF3 Inorganic materials 0.000 claims description 2
- 229910008243 Zr3(PO4)4 Inorganic materials 0.000 claims description 2
- 229910007998 ZrF4 Inorganic materials 0.000 claims description 2
- 229910000147 aluminium phosphate Inorganic materials 0.000 claims description 2
- RQPZNWPYLFFXCP-UHFFFAOYSA-L barium dihydroxide Chemical compound [OH-].[OH-].[Ba+2] RQPZNWPYLFFXCP-UHFFFAOYSA-L 0.000 claims description 2
- 229910001632 barium fluoride Inorganic materials 0.000 claims description 2
- WAKZZMMCDILMEF-UHFFFAOYSA-H barium(2+);diphosphate Chemical compound [Ba+2].[Ba+2].[Ba+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O WAKZZMMCDILMEF-UHFFFAOYSA-H 0.000 claims description 2
- 239000004327 boric acid Substances 0.000 claims description 2
- WUKWITHWXAAZEY-UHFFFAOYSA-L calcium difluoride Chemical compound [F-].[F-].[Ca+2] WUKWITHWXAAZEY-UHFFFAOYSA-L 0.000 claims description 2
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 claims description 2
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 claims description 2
- DPUCLPLBKVSJIB-UHFFFAOYSA-N cerium;tetrahydrate Chemical compound O.O.O.O.[Ce] DPUCLPLBKVSJIB-UHFFFAOYSA-N 0.000 claims description 2
- NLQFUUYNQFMIJW-UHFFFAOYSA-N dysprosium(III) oxide Inorganic materials O=[Dy]O[Dy]=O NLQFUUYNQFMIJW-UHFFFAOYSA-N 0.000 claims description 2
- VQCBHWLJZDBHOS-UHFFFAOYSA-N erbium(III) oxide Inorganic materials O=[Er]O[Er]=O VQCBHWLJZDBHOS-UHFFFAOYSA-N 0.000 claims description 2
- RSEIMSPAXMNYFJ-UHFFFAOYSA-N europium(III) oxide Inorganic materials O=[Eu]O[Eu]=O RSEIMSPAXMNYFJ-UHFFFAOYSA-N 0.000 claims description 2
- CMIHHWBVHJVIGI-UHFFFAOYSA-N gadolinium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Gd+3].[Gd+3] CMIHHWBVHJVIGI-UHFFFAOYSA-N 0.000 claims description 2
- CJNBYAVZURUTKZ-UHFFFAOYSA-N hafnium(IV) oxide Inorganic materials O=[Hf]=O CJNBYAVZURUTKZ-UHFFFAOYSA-N 0.000 claims description 2
- JYTUFVYWTIKZGR-UHFFFAOYSA-N holmium oxide Inorganic materials [O][Ho]O[Ho][O] JYTUFVYWTIKZGR-UHFFFAOYSA-N 0.000 claims description 2
- 210000000003 hoof Anatomy 0.000 claims description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum oxide Inorganic materials [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims description 2
- 239000001095 magnesium carbonate Substances 0.000 claims description 2
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 claims description 2
- 229910000021 magnesium carbonate Inorganic materials 0.000 claims description 2
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical compound [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 claims description 2
- 229910001635 magnesium fluoride Inorganic materials 0.000 claims description 2
- 239000000347 magnesium hydroxide Substances 0.000 claims description 2
- 229910001862 magnesium hydroxide Inorganic materials 0.000 claims description 2
- PLDDOISOJJCEMH-UHFFFAOYSA-N neodymium oxide Inorganic materials [O-2].[O-2].[O-2].[Nd+3].[Nd+3] PLDDOISOJJCEMH-UHFFFAOYSA-N 0.000 claims description 2
- 229910052759 nickel Inorganic materials 0.000 claims description 2
- KTUFCUMIWABKDW-UHFFFAOYSA-N oxo(oxolanthaniooxy)lanthanum Chemical compound O=[La]O[La]=O KTUFCUMIWABKDW-UHFFFAOYSA-N 0.000 claims description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 2
- 239000010452 phosphate Substances 0.000 claims description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N phosphoric acid Substances OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 claims description 2
- FKTOIHSPIPYAPE-UHFFFAOYSA-N samarium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Sm+3].[Sm+3] FKTOIHSPIPYAPE-UHFFFAOYSA-N 0.000 claims description 2
- OEKDNFRQVZLFBZ-UHFFFAOYSA-K scandium fluoride Chemical compound F[Sc](F)F OEKDNFRQVZLFBZ-UHFFFAOYSA-K 0.000 claims description 2
- RPACBEVZENYWOL-XFULWGLBSA-M sodium;(2r)-2-[6-(4-chlorophenoxy)hexyl]oxirane-2-carboxylate Chemical compound [Na+].C=1C=C(Cl)C=CC=1OCCCCCC[C@]1(C(=O)[O-])CO1 RPACBEVZENYWOL-XFULWGLBSA-M 0.000 claims description 2
- 239000000126 substance Substances 0.000 claims description 2
- 150000003568 thioethers Chemical class 0.000 claims description 2
- ZIKATJAYWZUJPY-UHFFFAOYSA-N thulium (III) oxide Inorganic materials [O-2].[O-2].[O-2].[Tm+3].[Tm+3] ZIKATJAYWZUJPY-UHFFFAOYSA-N 0.000 claims description 2
- XROWMBWRMNHXMF-UHFFFAOYSA-J titanium tetrafluoride Chemical compound [F-].[F-].[F-].[F-].[Ti+4] XROWMBWRMNHXMF-UHFFFAOYSA-J 0.000 claims description 2
- QGJSAGBHFTXOTM-UHFFFAOYSA-K trifluoroerbium Chemical compound F[Er](F)F QGJSAGBHFTXOTM-UHFFFAOYSA-K 0.000 claims description 2
- FDIFPFNHNADKFC-UHFFFAOYSA-K trifluoroholmium Chemical compound F[Ho](F)F FDIFPFNHNADKFC-UHFFFAOYSA-K 0.000 claims description 2
- BYMUNNMMXKDFEZ-UHFFFAOYSA-K trifluorolanthanum Chemical compound F[La](F)F BYMUNNMMXKDFEZ-UHFFFAOYSA-K 0.000 claims description 2
- LKNRQYTYDPPUOX-UHFFFAOYSA-K trifluoroterbium Chemical compound F[Tb](F)F LKNRQYTYDPPUOX-UHFFFAOYSA-K 0.000 claims description 2
- PBYZMCDFOULPGH-UHFFFAOYSA-N tungstate Chemical class [O-][W]([O-])(=O)=O PBYZMCDFOULPGH-UHFFFAOYSA-N 0.000 claims description 2
- LSGOVYNHVSXFFJ-UHFFFAOYSA-N vanadate(3-) Chemical class [O-][V]([O-])([O-])=O LSGOVYNHVSXFFJ-UHFFFAOYSA-N 0.000 claims description 2
- FIXNOXLJNSSSLJ-UHFFFAOYSA-N ytterbium(III) oxide Inorganic materials O=[Yb]O[Yb]=O FIXNOXLJNSSSLJ-UHFFFAOYSA-N 0.000 claims description 2
- 229910021512 zirconium (IV) hydroxide Inorganic materials 0.000 claims description 2
- OMQSJNWFFJOIMO-UHFFFAOYSA-J zirconium tetrafluoride Chemical compound F[Zr](F)(F)F OMQSJNWFFJOIMO-UHFFFAOYSA-J 0.000 claims description 2
- 150000002500 ions Chemical class 0.000 claims 1
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- 230000000694 effects Effects 0.000 abstract description 5
- 102000004169 proteins and genes Human genes 0.000 abstract description 3
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- 239000007788 liquid Substances 0.000 description 6
- BDJRBEYXGGNYIS-UHFFFAOYSA-N nonanedioic acid Chemical compound OC(=O)CCCCCCCC(O)=O BDJRBEYXGGNYIS-UHFFFAOYSA-N 0.000 description 6
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 3
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- 229910052906 cristobalite Inorganic materials 0.000 description 3
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- 239000000377 silicon dioxide Substances 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 3
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- 229910052905 tridymite Inorganic materials 0.000 description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 238000000376 autoradiography Methods 0.000 description 2
- 238000003759 clinical diagnosis Methods 0.000 description 2
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- 238000011503 in vivo imaging Methods 0.000 description 2
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- 229910001845 yogo sapphire Inorganic materials 0.000 description 2
- NSTREUWFTAOOKS-UHFFFAOYSA-N 2-fluorobenzoic acid Chemical class OC(=O)C1=CC=CC=C1F NSTREUWFTAOOKS-UHFFFAOYSA-N 0.000 description 1
- 206010028980 Neoplasm Diseases 0.000 description 1
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- 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
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Abstract
The invention belongs to the technical field of an 18F label, in particular to a preparation method of a nano particle which is labeled by the strong interaction between 18F anion and 18F cation, and 18F-labbled nano contrast agent which is prepared by the method and can be used for the tomoscan development of the cation. Compared with the known 18F label organic chemical reaction labeling method, the method is simple and fast, and has high labeling efficiency. The prepared 18F-labbled nano contrast agent can label a plurality of 18Fs on one particle, and achieves the good effect for firstly connecting with protein and nucleic acid and secondly labeling the 18 F.
Description
Technical Field
The invention belongs to18The field of F marking technology, more specifically, the invention relates to a method for marking18Method for labeling nano particles with strong force between F anions and cations and nano particles prepared by method and used for positron emission tomography imaging18F-labelled nano-contrast agents, with known agents18Compared with the F organic chemical reaction labeling method, the method is simple and rapid, has high labeling efficiency, and the prepared F organic chemical reaction labeling method18The F-labeled nano contrast agent has multiple labels on one particle18F, and effecting ligation of the protein and the nucleic acid first and labeling thereafter18And F is excellent.
Background
Ultrasensitive molecular imaging techniques are playing an increasingly important role in determining trace molecular events relevant to biomedical research and clinical diagnostics. Positron Emission Tomography (PET) technology has the highest in vivo imaging sensitivity and has been used for clinical diagnosis. Among the numerous species of positive electron species,18the half-life of F is about 110min, which is very suitable for clinical diagnosis. At present, the number of the current day,18F-FDG has been widely used in clinical diagnostics such as tumor screening and post-operative evaluation.
In a large number18In the F labeling method, all the components are in the form of covalent bonds18F is attached to a probe molecule, the method is based on organic chemistry, and the preparation is carried out at present18The reaction conditions of the F probe are harsh (such as heating, organic solvent and the like); usually, a plurality of reactions are needed, HPLC is adopted for separating and purifying products, and the total reaction yield is very low; the reaction time is relatively long, and the reaction time is relatively long,18the utilization of F is low. For example, in the case of the conventional intermediate N-succinimide-4-, [ in the case of a marker polypeptide and protein18F]The total reaction time for fluorobenzoic acid esters was about 120 min. Thus developing fast and high efficiency18The F labeling method has important significance.
Disclosure of Invention
The invention aims to provide a quick, simple and efficient method18The F labeling method and the probe prepared by the method can be used for Positron Emission Tomography (PET) imaging. In particular, the invention makes use of18F strong force between anion and cation18F is combined with the surface of the nano material to prepare18F-labeled nano material for positron emission tomography imaging. The method has the advantages of simplicity, rapidness, high efficiency and low cost.
It is an object of the present invention to provide positron emission tomography imaging18Method for labeling cationic-containing nanomaterial by using F anion, and it can be used for preparing18F markThe nano contrast agent can be used for Positron Emission Tomography (PET) imaging.
According to the invention18The F labeling method is based on strong interaction between anions and cations18The F nuclide is attached to a nano contrast agent, wherein:18the strong interaction of the cation and cation of the F nuclide comprises a first main group (Li, Na, K), a second main group element (comprising Ca, Mg, Ba), a third main group element (comprising B, Al), a first auxiliary group element (comprising Sc, Y, La, Ce, Pr, Nd Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu), a second auxiliary group element (comprising Ti, Zr, Hf) and18the effect of an F-species, preferably a second main group element, a first subgroup element, a second subgroup element, most preferably a first subgroup element;
the probe refers to a metal complex and a nano material containing the elements;
the nanomaterial is particles having a size of 1-1000nm and containing the above elements, and the particles containing the above elements may be fluoride particles, oxides, complex oxides, hydroxide particles, sulfides, carbonate particles, phosphate particles, titanate particles, borate particles, vanadate compounds, tungstate compounds, complex cationic compounds, complex anionic compounds. Wherein,
the fluoride compound includes at least: a first main group: such as LiF, NaF, KF; second main group: such as CaF2，MgF2，BaF2(ii) a Third main group: such as BF3，AlF3The first subgroup: ScF3，YF3，LaF3，CeF3，CeF4，PrF3，NdF3，SmF3，EuF3，GdF3，TbF3，DyF3，HoF3，ErF3，TmF3，YbF3，LuF3(ii) a A second subgroup: such as TiF4，ZrF4，HfF4；
The oxide at least comprises: third main group: such as Al2O3(ii) a A first subgroup: such asSc2O3，La2O3，CeO2，Pr2O3，Nd2O3，Sm2O3，Eu2O3，Gd2O3，Tb2O3，Dy2O3，Ho2O3，Er2O3，Tm2O3，Yb2O3，Lu2O3(ii) a A second subgroup: such as TiO2，ZrO2，HfO2；
The composite oxide includes at least: sr2CeO4，Gd2Ti2O7，Sm2Sn(2-x)B′xO7，Ce2Sn(2-x)B′xO7，(B’＝Fe，Co，Ni；x＝0～1.0)，Dy(1-x)SrxCoO(3-y)，(Y0.97Eu0.03)2O3；
The hydroxide includes at least: second main group: such as Ca (OH)2，Mg(OH)2，Ba(OH)2(ii) a A first subgroup: sc (OH)3，Y(OH)3，La(OH)3，Ce(OH)3，Ce(OH)4，Pr(OH)3，Nd(OH)3，Sm(OH)3，Eu(OH)3，Gd(OH)3，Tb(OH)3，Dy(OH)3，Ho(OH)3，Er(OH)3，Tm(OH)3，Yb(OH)3，Lu(OH)3(ii) a A second subgroup: such as Ti (OH)4，Zr(OH)4，Hf(OH)4；
The sulfide includes at least: second main group: such as CaS, MgS, BaS;
the carbonic acid compound at least comprises: second main group: such as CaCO3，MgCO3，BaCO3(ii) a A first subgroup: such as Sc2(CO3)3，Y2(CO3)3，La2(CO3)3，Ce2(CO3)3，Pr2(CO3)3，Nd2(CO3)3，Sm2(CO3)3，Eu2(CO3)3，Gd2(CO3)3，Tb2(CO3)3，Dy2(CO3)3，Ho2(CO3)3，Er2(CO3)3，Tm2(CO3)3，Yb2(CO3)3，Lu2(CO3)3(ii) a A second subgroup: such as Ti (CO)3)2，Zr(CO3)2，Hf(CO3)2；
The phosphoric acid compound at least includes: second main group: such as Ca3(PO4)2，Mg3(PO4)2，Ba3(PO4)2(ii) a A first subgroup: such as ScPO4，YPO4，LaPO4，CePO4，PrPO4，NdPO4，SmPO4，EuPO4，GdPO4，TbPO4，DyPO4，HoPO4，ErPO4，TmPO4，YbPO4，LuPO4(ii) a A second subgroup: such as Ti3(PO4)4，Zr3(PO4)4，Hf3(PO4)4；
The titanic acid compound includes at least: second main group: such as CaTiO3，MgTiO3，BaTiO3(ii) a A first subgroup: such as Sc2(TiO3)3，La2(TiO3)3，Ce2(TiO3)3，Pr2(TiO3)3，Nd2(TiO3)3，Sm2(TiO3)3，Eu2(TiO3)3，Gd2(TiO3)3，Tb2(TiO3)3，Dy2(TiO3)3，Ho2(TiO3)3，Er2(TiO3)3，Tm2(TiO3)3，Yb2(TiO3)3，Lu2(TiO3)3(ii) a A second subgroup: such as ZrTiO3，HfTiO3；
The boric acid compound includes at least: second main group: such as Ca3(BO3)2，Mg3(BO3)2，Ba3(BO3)2(ii) a A first main group: such as LaBO3，CeBO3，PrBO3，NdBO3，SmBO3，EuBO3，GdBO3，TbBO3，DyBO3，HoBO3，ErBO3，TmBO3，YbBO3，LuBO3(ii) a A second subgroup: such as Ti (BO)3)2，Zr(BO3)2，Hf(BO3)2；
The vanadate compound at least comprises: second main group: such as Ca3(VO4)2，Mg3(VO4)2，Ba3(VO4)2The first subgroup: ScVO4，YVO4，LaVO4，CeVO4，PrVO4，NdVO4，SmVO4，EuVO4，GdVO4，TbVO4，DyVO4，HoVO4，ErVO4，TmVO4，YbVO4，LuVO4(ii) a A second subgroup: such as Ti3(VO4)4，Zr3(VO4)4，Hf3(VO4)4；
The tungstic acid compound at least comprises: second main group: such as CaWO4，MgWO4，BaWO4(ii) a A first subgroup: such as La6W2O15，Ce2WO6，Pr2(WO4)3，Nd2WO6，Sm2WO6，Eu2(WO4)3，Gd2WO6，Tb2(WO4)3，Dy2WO6，Ho2(WO4)3，Er2WO6，Tm2(WO4)3，Yb2WO6，Lu2(WO4)3(ii) a A second subgroup: such as Ti3(WO4)4，Zr3(WO4)4，Hf3(WO4)4；
The complex cationic compound includes at least: first subgroup Li salt: such as LiScF4，LiLaF4，LiCeF4，LiPrF4，LiNdF4，LiSmF4，LiEuF4，LiGdF4，LiTbF4，LiDyF4，LiHoF4，LiErF4，LiTmF4，LiYbF4，LiLuF4(ii) a First subgroup Na salt: such as NaScF4，NaLaF4，NaCeF4，NaPrF4，NaNdF4，NaSmF4，NaEuF4，NaGdF4，NaTbF4，NaDyF4，NaHoF4，NaErF4，NaTmF4，NaYbF4，NaLuF4(ii) a First subgroup K salts: such as KScF4，KLaF4，KCeF4，KPrF4，KNdF4，KSmF4，KEuF4，KGdF4，KTbF4，KDyF4，KHoF4，KErF4，KTmF4，KYbF4，KLuF4(ii) a First subgroup NH4Salt: NH (NH)4ScF4，NH4LaF4，NH4CeF4，NH4PrF4，NH4NdF4，NH4SmF4，NH4EuF4，NH4GdF4，NH4TbF4，NH4DyF4，NH4HoF4，NH4ErF4，NH4TmF4，NH4YbF4，NH4LuF4；
CompoundingThe anionic compound includes at least: first subgroup OF salts: such as ScOF, YOF, LaOF, CeOF, PrOF, NdOF, SmOF, EuOF, GdOF, TbOF, DyOF, HoOF, ErOF, TmOF, YbOF, LuOF; first subgroup (OH) CO3Salt, Sc (OH) CO3，Y(OH)CO3，La(OH)CO3，Ce(OH)CO3，Pr(OH)CO3，Nd(OH)CO3，Sm(OH)CO3，Eu(OH)CO3，Gd(OH)CO3，Tb(OH)CO3，Dy(OH)CO3，Ho(OH)CO3，Er(OH)CO3，Tm(OH)CO3，Yb(OH)CO3，Lu(OH)CO3；
The preparation process of the metal complex and the nanometer material of the elements comprises the following steps: at a certain temperature, the nano material containing the elements is mixed with18Mixing the F nuclide solution for 0-2 hours to prepare the product18And F, marking the nano material at the certain temperature from normal temperature to the highest temperature without damaging the physical and chemical properties of the nano material.
The objective material prepared by the above method does not need to be purified, or can be purified by a separation and purification method (such as centrifugation) which is conventional in the art.
Synthesized according to the method of the invention18The F-labeled nano material has a good positron imaging function and can be used for in-vivo imaging.
In order to study several nanoparticles18F labelling ability, water-soluble Lu2O3Nano particle, NaLuF with azelaic acid surface4Nanocrystalline and 20 mol% Yb doped with azelaic acid on the surface3+And 2 mol% Er2+NaLuF (R) 24Nanocrystals (UCNPs, particle size 14nm) are respectively mixed with18F-Mixing, and standing at room temperature for 10 min. Get18F-And the UCNPs mixed solution was spotted on a TLC strip (polyamide thin film), developed with physiological saline, and visualized by autoradiography (see fig. 1):18F-and UCNPs mixture has strong radioactive signal at the point origin, and is free18F-The radioactive signal is located inSolvent front. This phenomenon is illustrated by the fact that UCNPs do not stay at the point of origin as the developer moves forward18F-And most of the UCNPs18F-Have been bound to UCNPs. Centrifuging and repeatedly washing to remove18F-After separation of the nanoparticles, Lu2O3、NaLuF4And UCNP nanoparticles exhibit strong radioactive signals that can be directly imaged using radioisotope imaging methods (fig. 2). The radioactive intensities of the solid (nanoparticles) and the liquid were measured to be 45.3%, 89.8% and 89.4%, respectively18F-Bound to Lu2O3、NaLuF4And on UCNP nanoparticles (fig. 2).
In control experiments, several other materials such as SiO2Mesoporous SiO2Nano vesicle, ZnO and ZrO2The nano particles and the active carbon are subjected to the same condition18F-The radioactivity intensity after treatment was low (fig. 2). Of particular note are mesoporous SiO's with high adsorption capacity2Nano vesicle (pore volume 0.9 cm)3Per g, specific surface area 300m2Per gram) and activated carbon18The labeling rates of F are 2.05 percent and 5.23 percent respectively, which shows that the physical adsorption improves the nano material18The F labelling rate had no significant effect. Furthermore, SiO2Method for preparing coated UCNPs18F mark rate is also low, which indicates18F-And UCNPs surface Lu3+Is directly acting on18F-The bonding is very critical. Therefore, the temperature of the molten metal is controlled,18F-is obtained by18F-And Lu3+Is rapidly and efficiently coupled to the surface of the material.
Drawings
Fig. 1.18F-Marking surface of azelaic acid doped with 20 mol% Yb3+And 2 mol% Er2+NaLuF (R) 24Autoradiography of the nanocrystals;
FIG. 2 shows several nanomaterials (5 mg each) separately combined with18F-(～11.1MBq，1.75×10-10mol) are mixed in distilled water, placed for 10min at room temperature, centrifuged and washed for three times to obtain solid radionuclide imaging;
fig. 3.18F-labeled NaGdF4The nano material is used for positron emission tomography imaging;
fig. 4.18F-marker Gd (OH)3The nano material is used for positron emission tomography imaging;
fig. 5.18F-labeled NaLuF4The nano material is used for positron emission tomography imaging;
fig. 6.18F-labeled LaF3The nano material is used for positron emission tomography imaging.
Detailed Description
Specific examples of the compounds of the present invention are given below, which illustrate the invention in detail by way of examples, without restricting it in any way. The starting materials used in this example are all known materials and are commercially available or may be prepared according to methods known in the art.
Example 1:18f-labelled CaF2Synthesis of nanomaterials
5mg CaF with a particle size distribution of about 100nm2Adding the nano material into 500 mu L18F-After shaking the solution (. about.1.0 mCi) for 1min, the solution was centrifuged at 14,000 rpm and the supernatant was aspirated. Marking rate is solid/(solid + liquid) × 100%.
Adding 1mL of distilled water into the solid, oscillating for 1min, centrifuging at a rotating speed of 14,000 rpm, and sucking out the supernatant; the radioactivity of the solid and liquid fractions was measured separately by an activity meter. Purity ═ solid/(solid + liquid) × 100%.
The samples were added to 1mL PBS, dispersed by sonication, centrifuged separately after 2h, the supernatant aspirated and the radioactivity in the solid and liquid fractions measured separately using an activity meter. 2 hours stability ═ solid/(solid + liquid) × 100%.
The results showed a labeling rate of 89.36%, a purity of 90.0%, and a 2h stability of 70.0%.
Example 2:18synthesis of F-labeled LiF nanomaterial
The particle size of the material is 70nm, and the marking temperature is 62 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 61.76%, a purity of 72.1%, and a 2h stability of 81.0%.
Example 3:18f-labelled AlF3Synthesis of nanomaterials
The particle size of the material is 10nm, and the marking temperature is 100 ℃. The rest of the labeling process was the same as in example 1.
The results showed 78.76% labeling, 92.1% purity and 90.1% 2h stability.
Example 4:18f-tag ScF3Synthesis of nanomaterials
The particle size of the material is 50nm, and the marking temperature is 45 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labelling rate of 56.76%, a purity of 77.4% and a 2h stability of 31.0%.
Example 5:18f-labelled TiF4Synthesis of nanomaterials
The particle size of the material is 60nm, and the marking temperature is 40 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 63.66%, a purity of 77.6%, and a 2h stability of 68.0%.
Example 6:18f-labeled Al2O3Synthesis of nanomaterials
The particle size of the material is 500nm, and the marking temperature is 60 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 63.43%, a purity of 72.5%, and a 2h stability of 71.3%.
Example 7:18f-mark Sc2O3Synthesis of nanomaterials
The particle size of the material is 700nm, and the marking temperature is 20 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 63.46%, a purity of 88.15%, and a 2h stability of 84.0%.
Example 8:18f-labelled TiO2Synthesis of Ce nano material
The particle size of the material is 900nm, and the marking temperature is 20 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labelling rate of 73.76%, a purity of 62.4% and a 2h stability of 61.1%.
Example 9:18f-labelled Sr2CeO4Synthesis of nanomaterials
The particle size of the material is 550nm, and the marking temperature is 30 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 53.76%, a purity of 72.1%, and a 2h stability of 71.1%.
Example 10:18f-marker Ca (OH)2Synthesis of nanomaterials
The particle size of the material is 950nm, and the marking temperature is 40 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 63.46%, a purity of 72.6%, and a 2h stability of 41.0%.
Example 11:18f-marker Gd (OH)3Synthesis of nanomaterials
The particle size of the material is 580nm, and the marking temperature is 60 ℃. The rest of the labeling process was the same as in example 1.
The results showed 63.56% labeling, 72.7% purity, and 71.0% 2h stability.
Example 12:18f-mark Ti (OH)4Synthesis of nanomaterials
The particle size of the material is 540nm, and the marking temperature is 90 ℃. The rest of the labeling process was the same as in example 1.
The results showed 53.56% labeling, 72.8% purity, and 66.5% 2h stability.
Example 13:18synthesis of F-labeled LiF nanomaterial
The particle size of the material is 150nm, and the marking temperature is 90 ℃. The rest of the labeling process was the same as in example 1.
The results showed 55.76% labeling, 72.7% purity, and 61.7% 2h stability.
Example 14:18synthesis of F-labeled CaS nanomaterial
The particle size of the material is 350nm, and the marking temperature is 70 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labelling rate of 66.76%, a purity of 72.7% and a 2h stability of 71.0%.
Example 15:18f-marking of CaCO3Synthesis of nanomaterials
The particle size of the material is 660nm, and the marking temperature is 40 ℃. The rest of the labeling process was the same as in example 1.
The results showed 53.56% labeling, 62.1% purity and 71.6% 2h stability.
Example 16:18f-mark Sc2(CO3)3Of nanometric materialSynthesis of
The particle size of the material is 800nm, and the marking temperature is 40 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 77.5%, a purity of 62.1%, and a 2h stability of 71.6%.
Example 17:18f-labelling of Zr (CO)3)2Synthesis of nanomaterials
The particle size of the material is 850nm, and the marking temperature is 20 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 63.76%, a purity of 52.5%, and a 2h stability of 73.2%.
Example 18:18f-labelled Mg3(PO4)2Synthesis of nanomaterials
The particle size of the material is 760nm, and the marking temperature is 90 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labelling rate of 43.56%, a purity of 72.1% and a 2h stability of 81.0%.
Example 19:18f-mark YPO4Synthesis of nanomaterials
The particle size of the material is 770nm, and the marking temperature is 60 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 92.99%, a purity of 98.19%, and a 2h stability of 84.17%.
Example 20:18f-mark Hf3(PO4)4Synthesis of nanomaterials
The particle size of the material was 460nm, and the labeling temperature was 70 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 97.91%, a purity of 99.29%, and a 2h stability of 73.27%.
Example 21:18f-marking of CaCO3Synthesis of nanomaterials
The particle size of the material is 590nm, and the marking temperature is 50 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 75.91%, a purity of 79.21%, and a 2h stability of 73.57%.
Example 22:18f-labelled BaTiO3Synthesis of nanomaterials
The particle size of the material is 790nm, and the marking temperature is 100 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 92.91%, a purity of 96.21%, and a 2h stability of 75.57%.
Example 23:18f-mark Sm2(TiO3)3Synthesis of nanomaterials
The particle size of the material is 540nm, and the marking temperature is 90 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 95.91%, a purity of 97.28%, and a 2h stability of 77.17%.
Example 24:18f-labeled ZrTiO3Synthesis of nanomaterials
The particle size of the material is 380nm, and the marking temperature is 80 ℃. The rest of the labeling process was the same as in example 1.
The results showed 88.91% labelling, 93.28% purity and 71.97% 2h stability.
Example 25:18f-labelled Mg3(BO3)2Synthesis of nanomaterials
The particle size of the material is 260nm, and the marking temperature is 30 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 89.91%, a purity of 95.98%, and a 2h stability of 65.27%.
Example 26:18f-tag PrBO3Synthesis of nanomaterials
The particle size of the material is 290nm, and the marking temperature is 70 ℃. The rest of the labeling process was the same as in example 1.
The results showed 85.91% labeling, 93.98% purity, and 71.27% 2h stability.
Example 27:18f-labelled Zr (BO)3)2Synthesis of nanomaterials
The particle size of the material is 670nm, and the marking temperature is 60 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 86.91%, a purity of 94.98%, and a 2h stability of 93.27%.
Example 28:18f-labelled Mg3(VO4)2Synthesis of nanomaterials
The particle size of the material is 920nm, and the marking temperature is 50 ℃. The rest of the labeling process was the same as in example 1.
The results showed 87.91% labeling, 97.98% purity and 73.17% 2h stability.
Example 29:18f-labeled LaVO4Synthesis of nanomaterials
The particle size of the material is 110nm, and the marking temperature is 20 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 83.21%, a purity of 97.58%, and a 2h stability of 93.12%.
Example 30:18f-labeling of Zr3(VO4)4Synthesis of nanomaterials
The particle size of the material is 20nm, and the marking temperature is 10 ℃. The rest of the labeling process was the same as in example 1.
The results showed 86.41% labeling, 92.58% purity, and 80.12% 2h stability.
Example 31:18f-labeling of Zr3(VO4)4Synthesis of nanomaterials
The particle size of the material is 40nm, and the marking temperature is 30 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 83.11%, a purity of 92.32%, and a 2h stability of 77.17%.
Example 32:18f-labelled BaWO4Synthesis of nanomaterials
The particle size of the material is 90nm, and the marking temperature is 20 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 81.11%, a purity of 82.32%, and a 2h stability of 81.17%.
Example 33:18f-mark Nd2WO6Synthesis of nanomaterials
The particle size of the material is 160nm, and the marking temperature is 90 ℃. The rest of the labeling process was the same as in example 1.
The results showed 89.11% labelling, 92.32% purity and 77.17% 2h stability.
Example 34:18f-labelled Ti3(WO4)4Synthesis of nanomaterials
The particle size of the material is 450nm, and the marking temperature is 100 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 87.16%, a purity of 90.12%, and a 2h stability of 87.29%.
Example 35:18f-labeled LiLaF4Synthesis of nanomaterials
The particle size of the material is 230nm, and the marking temperature is 50 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 83.19%, a purity of 88.12%, and a 2h stability of 80.27%.
Example 36:18f-labeled NaNdF4Synthesis of nanomaterials
The particle size of the material is 270nm, and the marking temperature is 80 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 85.11%, a purity of 97.62%, and a 2h stability of 71.63%.
Example 37:18f-tag KSmF4Synthesis of nanomaterials
The particle size of the material is 820nm, and the marking temperature is 70 ℃. The rest of the labeling process was the same as in example 1.
The results showed 97.11% labelling, 97.62% purity and 72.54% 2h stability.
Example 38:18f-labelled NH4GdF4Synthesis of nanomaterials
The particle size of the material is 770nm, and the marking temperature is 30 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 97.51%, a purity of 97.83%, and a 2h stability of 74.83%.
Example 39:18f-labeled NaGdF4Synthesis of Yb and Er nano material
The particle size of the material is 730nm, and the marking temperature is 60 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 93.04%, a purity of 89.55%, and a 2h stability of 88.54%.
Example 40:18f-labelled Eu (OH) CO3Synthesis of nanomaterials
The particle size of the material is 220nm, and the marking temperature is 70 ℃. The rest of the labeling process was the same as in example 1.
The results showed a labeling rate of 62.11%, a purity of 85.0%, and a 2h stability of 77.54%.
Example 41:18F-label NaGdF4Use of nano material in positron emission tomography imaging
The particle size of the material is 30nm, and the marking temperature is 20 ℃. The rest of the labeling process was the same as in example 1. The results showed a labeling rate of 89.36%, a purity of 90.0%, and a 2h stability of 87.27%.
18F-The labeled sample solid is added with 0.25mL of physiological saline to prepare a solution of 200 mu Ci/100 mu L, namely the radioactive nano material for the imaging experiment. After tail vein injection, the micro PET imaging detection result shows that the materials are mainly distributed in two tissues of the liver and the spleen, the result is the same as the fluorescent living body imaging result, and the nano material after the prompt mark can be used as a positron emission tomography imaging contrast agent (figure 3).
Example 42:18F-marker Gd (OH)3Use of nano material in positron emission tomography imaging
The particle size of the material is 30nm, and the marking temperature is 20 ℃. The rest of the labeling process was the same as in example 1. The results showed 86.04% labeling, 88.53% purity, and 76.04% 2h stability.
18F-The labeled sample solid is added with 0.25mL of physiological saline to prepare a solution of 200 mu Ci/100 mu L, namely the radioactive nano material for the imaging experiment. The in vivo experimental process is the same as that of example 23, and the detection result of microPET imaging shows that the material can be used as a positron emission tomography imaging contrast agent (figure 4).
Example 43:18F-labeled NaLuF4Use of nano material in positron emission tomography imaging
The particle size of the material is 40nm, and the marking temperature is 20 ℃. The rest of the labeling process was the same as in example 1. The results showed a labeling rate of 93.04%, a purity of 89.55%, and a 2h stability of 88.54%.
18F-The labeled sample solid is added with 0.25mL of physiological saline to prepare a solution of 200 mu Ci/100 mu L, namely the radioactive nano material for the imaging experiment. The in vivo experimental process is the same as that of example 23, and the detection result of microPET imaging shows that the material can be used as a positron emission tomography imaging contrast agent (figure 5).
Example 44:18F-label LaF3Use of nano material in positron emission tomography imaging
The particle size of the material is 220nm, and the marking temperature is 70 ℃. The rest of the labeling process was the same as in example 1. The results showed a labeling rate of 91.55%, a purity of 88.15%, and a 2h stability of 81.54%.
18F-The labeled sample solid is added with 0.25mL of physiological saline to prepare a solution of 200 mu Ci/100 mu L, namely the radioactive nano material for the imaging experiment. The in vivo experimental process is the same as that of example 23, and the detection result of microPET imaging shows that the material can be used as a positron emission tomography imaging contrast agent (figure 6).
The positive effects are as follows:
according to the invention18F-Labeling positron-emitting nano-contrast agents based on18F is a strong interaction with some elements contained in the nanomaterial, such as second main group elements (including Ca, Mg, Ba), third main group elements (including B, Al), first auxiliary group elements (including Sc, Y, La, Ce, Pr, Nd, Pm, Sm, Eu, Tb, Gd, Dy, Ho, Er, Tm, Yb), and second auxiliary group elements (including Ti, Zr, Hf). The nano material containing the above elements has high surface area and is easy to adsorb18F-And are18F-Form strong interaction so that18F-Can be quickly and efficiently combined with the surface of the nano material, thereby preparing18F, labeling the nano contrast agent. As given in example 418The mark F reaches 93.04%, and the preparation processSimple, add18F-Can be used after shaking up at room temperature without separation,18F-the most convenient and time-saving preparation method of the labeled positron emission contrast agent. Thus, use of18The F-labeling method can produce more abundant18F-Labeling the positron emitting contrast agent.
Claims (7)
1. A kind of18The preparation method of the F-labeled nano material is characterized by comprising the following steps of: at a certain temperature, the nano material containing cation elements is mixed with18Mixing the F nuclide solution for 0-2 hours to prepare the product18And F, marking the nano material, wherein the certain temperature is from normal temperature to the highest temperature without damaging the physical and chemical properties of the nano material.
2. The method of claim 118The preparation method of the F-marked nano material is characterized in thatIs characterized in that18F is connected to the nano material through strong interaction of anions and cations.
3. The method of claim 118The preparation method of the F-marked nano material is characterized in that18The cation of F nuclide is interacted with the anion and cation, and the cation comprises second main group elements of Ca, Mg and Ba; a third main group element of B, Al; the first subgroup element is Sc, Y, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb and Lu; the second subgroup element is the positive ions of Ti, Zr and Hf.
4. The method of claim 318The preparation method of the F-marked nano material is characterized in that18Cation of the F species is preferably cation of the second main group element, the first sub-group element or the second sub-group element.
5. The method of claim 418The preparation method of the F-marked nano material is characterized in that18The cation of the F species, preferably the cation of the first subgroup element, interacts with the cation of the F species.
6. The method of claim 118The preparation method of the F-marked nano material is characterized in that the nano material is particles which have the size of 1-1000nm and contain the elements, the particles containing the elements can be fluoride particles, oxides, composite oxides, hydroxide particles, sulfides, carbonate particles, phosphate particles, titanate particles, borate particles, vanadate compounds, tungstate compounds, composite cationic compounds or composite anionic compounds, wherein,
the fluoride compound includes at least: a first main group: LiF, NaF, KF; second main group: CaF2、MgF2、BaF2(ii) a Third main group: BF (BF) generator3、AlF3(ii) a A first subgroup: ScF3、YF3、LaF3、CeF3、CeF4、PrF3、NdF3、SmF3、EuF3、GdF3、TbF3、DyF3、HoF3、ErF3、TmF3、YbF3、LuF3(ii) a A second subgroup: TiF4、ZrF4、HfF4；
The oxide at least comprises: third main group: al (Al)2O3(ii) a A first subgroup: sc (Sc)2O3、La2O3、CeO2、Pr2O3、Nd2O3、Sm2O3、Eu2O3、Gd2O3、Tb2O3、Dy2O3、Ho2O3、Er2O3、Tm2O3、Yb2O3、Lu2O3(ii) a A second subgroup: TiO 22、ZrO2、HfO2；
The composite oxide includes at least: sr2CeO4、Gd2Ti2O7、Sm2Sn(2-x)B′xO7、Ce2Sn(2-x)B′xO7、(B’＝Fe，Co，Ni；x＝0～1.0)、Dy(1-x)SrxCoO(3-y)、(Y0.97Eu0.03)2O3；
The hydroxide includes at least: second main group: ca (OH)2、Mg(OH)2、Ba(OH)2(ii) a A first subgroup: sc (OH)3、Y(OH)3、La(OH)3、Ce(OH)3、Ce(OH)4、Pr(OH)3、Nd(OH)3、Sm(OH)3、Eu(OH)3、Gd(OH)3、Tb(OH)3、Dy(OH)3、Ho(OH)3、Er(OH)3、Tm(OH)3、Yb(OH)3、Lu(OH)3(ii) a A second subgroup: ti (OH)4、Zr(OH)4、Hf(OH)4；
The sulfide includes at least: second main group: CaS, MgS, BaS;
the carbonic acid compound at least comprises: second main group: CaCO3、MgCO3、BaCO3(ii) a A first subgroup: sc (Sc)2(CO3)3、Y2(CO3)3、La2(CO3)3、Ce2(CO3)3、Pr2(CO3)3、Nd2(CO3)3、Sm2(CO3)3、Eu2(CO3)3、Gd2(CO3)3、Tb2(CO3)3、Dy2(CO3)3、Ho2(CO3)3、Er2(CO3)3、Tm2(CO3)3、Yb2(CO3)3、Lu2(CO3)3(ii) a A second subgroup: ti (CO)3)2、Zr(CO3)2、Hf(CO3)2；
The phosphoric acid compound at least includes: second main group: ca3(PO4)2、Mg3(PO4)2、Ba3(PO4)2(ii) a A first subgroup: ScPO4、YPO4、LaPO4、CePO4、PrPO4、NdPO4、SmPO4、EuPO4、GdPO4、TbPO4、DyPO4、HoPO4、ErPO4、TmPO4、YbPO4、LuPO4(ii) a A second subgroup: ti3(PO4)4、Zr3(PO4)4、Hf3(PO4)4；
The titanic acid compound includes at least: second main group: CaTiO3、MgTiO3、BaTiO3(ii) a A first subgroup: sc (Sc)2(TiO3)3、La2(TiO3)3、Ce2(TiO3)3、Pr2(TiO3)3、Nd2(TiO3)3、Sm2(TiO3)3、Eu2(TiO3)3、Gd2(TiO3)3、Tb2(TiO3)3、Dy2(TiO3)3、Ho2(TiO3)3、Er2(TiO3)3、Tm2(TiO3)3、Yb2(TiO3)3、Lu2(TiO3)3(ii) a A second subgroup: ZrTiO3、HfTiO3；
The boric acid compound includes at least: second main group: ca3(BO3)2、Mg3(BO3)2、Ba3(BO3)2(ii) a A first main group: LaBO3、CeBO3、PrBO3、NdBO3、SmBO3、EuBO3、GdBO3、TbBO3、DyBO3、HoBO3、ErBO3、TmBO3、YbBO3、LuBO3(ii) a A second subgroup: ti (BO)3)2、Zr(BO3)2、Hf(BO3)2；
The vanadate compound at least comprises: second main group: ca3(VO4)2、Mg3(VO4)2、Ba3(VO4)2(ii) a A first subgroup: ScVO4、YVO4、LaVO4、CeVO4、PrVO4、NdVO4、SmVO4、EuVO4、GdVO4、TbVO4、DyVO4、HoVO4、ErVO4、TmVO4、YbVO4、LuVO4(ii) a A second subgroup: ti3(VO4)4、Zr3(VO4)4、Hf3(VO4)4；
The tungstic acid compound at least comprises: second main group: CaWO4、MgWO4、BaWO4(ii) a A first subgroup: la6W2O15、Ce2WO6、Pr2(WO4)3、Nd2WO6、Sm2WO6、Eu2(WO4)3、Gd2WO6、Tb2(WO4)3、Dy2WO6、Ho2(WO4)3、Er2WO6、Tm2(WO4)3、Yb2WO6、Lu2(WO4)3(ii) a A second subgroup: ti3(WO4)4、Zr3(WO4)4、Hf3(WO4)4；
The complex cationic compound includes at least: first subgroup Li salt: LiScF4、LiLaF4、LiCeF4、LiPrF4、LiNdF4、LiSmF4、LiEuF4、LiGdF4、LiTbF4、LiDyF4、LiHoF4、LiErF4、LiTmF4、LiYbF4、LiLuF4(ii) a First subgroup Na salt: NaScF4、NaLaF4、NaCeF4、NaPrF4、NaNdF4、NaSmF4、NaEuF4、NaGdF4、NaTbF4、NaDyF4、NaHoF4、NaErF4、NaTmF4、NaYbF4、NaLuF4(ii) a First subgroup K salts: KScF4、KLaF4、KCeF4、KPrF4、KNdF4、KSmF4、KEuF4、KGdF4、KTbF4、KDyF4、KHoF4、KErF4、KTmF4、KYbF4、KLuF4(ii) a First subgroup NH4Salt: NH (NH)4ScF4、NH4LaF4、NH4CeF4、NH4PrF4、NH4NdF4、NH4SmF4、NH4EuF4、NH4GdF4、NH4TbF4、NH4DyF4、NH4HoF4、NH4ErF4、NH4TmF4、NH4YbF4、NH4LuF4；
The complex anionic compound includes at least: first subgroup OF salts: ScOF, YOF, LaOF, CeOF, PrOF, NdOF, SmOF, EuOF, GdOF, TbOF, DyOF, HoOF, ErOF, TmOF, YbOF, LuOF; first subgroup (OH) CO3Salt: sc (OH) CO3、Y(OH)CO3、La(OH)CO3、Ce(OH)CO3、Pr(OH)CO3、Nd(OH)CO3、Sm(OH)CO3、Eu(OH)CO3、Gd(OH)CO3、Tb(OH)CO3、Dy(OH)CO3、Ho(OH)CO3、Er(OH)CO3、Tm(OH)CO3、Yb(OH)CO3、Lu(OH)CO3。
7. A process as claimed in claims 1 to 618Prepared by the preparation method of F-marked nano material18The use of an F-labeled nanomaterial preparation for positron emission tomography imaging.
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| CN103007306A (en) * | 2012-12-27 | 2013-04-03 | 复旦大学 | Method and application for marking anion-cation type inorganic nano material through samarium-153 and/or lutecium-177 |
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| CN102676172A (en) * | 2012-04-24 | 2012-09-19 | 中国科学院福建物质结构研究所 | Rare earth-doped fluoride lanthanum potassium nano fluorescent marking material and preparation method thereof |
| CN103007306A (en) * | 2012-12-27 | 2013-04-03 | 复旦大学 | Method and application for marking anion-cation type inorganic nano material through samarium-153 and/or lutecium-177 |
| CN112472827A (en) * | 2020-11-27 | 2021-03-12 | 中国科学院大学宁波华美医院 | Novel bimodal PET/CT imaging material and preparation method and application thereof |
| CN115259206A (en) * | 2022-07-22 | 2022-11-01 | 承德莹科精细化工股份有限公司 | Preparation method of high-purity thulium carbonate and high-purity thulium trifluoride |
| CN115259206B (en) * | 2022-07-22 | 2024-02-20 | 承德莹科精细化工股份有限公司 | Preparation method of high-purity thulium carbonate and high-purity thulium trifluoride |
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