Luminescent coordination compounds of lanthanides for light-emitting diodes

FIELD: chemistry.

SUBSTANCE: invention relates to complexes of lanthanides and organic ligands which are luminescent in the visible spectrum and are used in electroluminescent devices, means of protecting security paper and documents from falsification etc. Disclosed are novel luminescent coordination compounds of lanthanides of formula: where Ln is Eu3+, Tb3+, Dy3+, Sm3+, Gd3+.

EFFECT: said compounds have high luminescence intensity and considerable thermal tolerance of up to 400°C, which enables use thereof in modern production of light-emitting diodes.

4 dwg, 2 tbl

 

The invention relates to fluorescent in the visible spectrum of the complex compounds of lanthanides with organic ligands, which are used in electroluminescent devices, means of protection of securities and documents against falsification (Katkov M.A., Vituhnovskaya A.G., M. N. Bochkarev. // USP. 2005. So 74. No. 12. S-1215). This is because y complexes of lanthanides are fluorescence of the phosphors, quantum yield of luminescence which can reach 100%.

When using phosphors, for example, in the organic light-emitting diodes carry out layer-by-layer thermal spraying phosphor. While the sprayed substances are exposed to significant heat, so in addition to the high intensity of luminescence phosphors used should have high thermal stability.

Known phosphorescent phosphors, each representing a different coordination compounds of lanthanides with carboxylate ligands such as Tris-salicylates lanthanides. These coordination compounds have low intensity luminescence (V.Tsaryuk, K.Zhuravlev, V.Zolin, P.Gawryszewska, J.Legendziewicz, V.Kudryashova, I.Pekareva // Journal of Photochemistry and Photobiology A: Chemistry. 2006. V.177. P.314-323).

In part, this shortcoming is eliminated Tris-salicylates lanthanides, Ln(Sal)3Phen containing additional is hydrated neutral ligand 1,10-phenantroline (Phen) (Bing Yan, Hongjie Zhang, Shubin Wang, Jiazuan Ni // Journal of Photochemistry and Photobiology A: Chemistry. 1998. V.116. P.209-214) General formula:

where Ln Is Eu3+, Tb3+, Dy3+Sm3+, Gd3+.

Compared with the above analogs, it has a large quantum efficiency of luminescence, namely 10 times. This analogue is selected as the closest analogue of the prototype.

The disadvantages of the prototype is its low thermal stability, which makes its application in organic light-emitting diodes, due to the presence in its composition of 1,10-phenanthroline having a melting point of 117°C.

The technical result of the claimed invention to provide a thermally stable luminescent coordination compounds for use in light-emitting diodes.

To achieve a technical result are offered luminescent coordination compounds of lanthanides having the formula Ln2(Phdic)3·2H2O, namely:

where Ln Is Eu3+, Tb3+, Dy3+Sm3+, Gd3+.

As the ligand used heteroaromatic base, containing two carboxyl group - 1,10-phenanthroline-2,9-dicarboxylic acid (H2Phdic), the General formula:

It is known that ligand H 2Phdic we studied the complexation in solution with Eu3+, but was not selected coordination compounds in solid form (Eva F. Gudgin Templeton, Alfred Pollak // Journal of Luminescence, 1989. V.43, P.195-205). Data about the properties of solid coordination compounds of lanthanides with 1,10-phenanthroline-2,9-dicarboxylic acid in the literature were not found.

The figure 1 shows thermogram of the prototype, for example, Eu(Sal)3Phen; figure 2 is a thermogram of the inventive coordination compounds for example Eu2(Phdic)3·2H2O; figure 3 shows the luminescence spectrum coordination compounds samarium Sm2(Phdic)3·2H2O recorded at room temperature; the figure 4 presents the most informative part of the spectrum of luminescence of coordination compounds europium - Eu2(Phdic)3·2H2O recorded at room temperature.

Complex compounds of lanthanides with 1,10-phenanthroline-2,9-dicarboxylic acid were obtained by an ion exchange method (garnovsky A.D. Modern aspects of the synthesis of metal complexes. The main ligands and methods / Adherence, Isabelita, Dahanese. - Rostov-on-don: Lapo, 2000. - 335 S.).

Specific example

From setevogo acetate europium was preparing an aqueous solution with a concentration 0,048 mol/l 1,10-phenanthroline-2,9-dicarboxylic acid weight 0,g (2,71*10 -3mol) was dissolved in 150 ml of alcohol. In the prepared solution under stirring was added potassium hydroxide to pH 6, and then gradually added to the solution of acetate europium (9,03*10-4mol). The precipitate was filtered under vacuum and dried in a vacuum oven at a temperature of 90°C. and a residual pressure of 20 mm Hg In the received luminescent coordination compound Eu2(Phdic)3·2H2O elemental composition shown in table No. 1.

Similarly, were obtained luminescent coordination compounds with one of the lanthanides: Tb3+, Dy3+Sm3+, Gd3+representing stable on air light yellow substance, the composition of which satisfies the General formula: Ln2(Phdic)3·2H2O. the Elemental composition of the compounds obtained are presented in table 1.

Table No. 1
The data of elemental analysis of the obtained luminescent coordination compounds
ConnectionOutput %Brutto-formulaElemental composition (found/calculated), %
LnC NH2O
Eu2(Phdic)3·2H2O68C42H22N6O14Eu226,24/26,5743,51/44,067,25/7,343,55/3,15
Tb2(Phdic)3·2H2O74C42H22N6O14Tb227,11/27,4543,02/43,537,19/7,253,52/3,11
Dy2(Phdic)3·2H2O51C42H22N6O14Dy227,47/27,9042,73/43,267,14/7,213,51/3,09
Sm2(Phdic)3·2H2O82C42H22N6O14Sm226,03/26,3643,76/44,187,26/of 7.363,56/3,16
Gd2(Phdic)3·2H2O 54C42H22N6O14Cd226,77/27,2442,95/43,667,16/7,283,52/3,12

Table 2 presents data of the IR spectra of the obtained coordination compounds spectrometer spectrometer-02 confirming their identity.

Table 2
The assignment of the characteristic bands in the IR spectra of the ligand H2Phdic and luminescent coordination compounds of lanthanides with him
AssignmentWavenumber, cm-1
H2PhdicGd2Phdic3·2H2OEu2Phdic3·2H2OTb2Phdic3·2H2OSm2Phdic3·2H2ODy2Phdic3·2H2O
ν(O-H)3650-26703650-26403600-30003650-27003650-2800 3640-2700
ν(C=O)1738-----
νas(COO-)-16381638163316381634
ν(Cap=N)145414581463146314571463
νs(COO-)-13751368137113751375

In the infrared spectra of complex compounds observed the disappearance of the absorption bands of UN-ionized carboxyl group ν(C=O) at 1738 cm-1and the appearance of absorption bands of the ionized carboxyl group of the νas(COO-) and νs(COO-) in 1638 and 1368 cm-1respectively, indicating that both carboxyl groups in coordination with metal ion.

Presented at the Fig the arts 1 and 2 thermograms of the prototype and of the inventive luminescent coordination compounds characterize the dependence of the mass loss of the substance from the temperature and thermal stability. The claimed substance has a higher thermal stability (up to 400°C), compared with the prototype (up to 180°C), which will enable their use for the manufacture of organic light-emitting diodes by layer-by-layer thermal spraying in the currently used technologies of manufacturing light-emitting diodes.

From the spectra shown in figures 3 and 4, it is seen that the proposed coordination compounds intensively lumines cent in the visible region.

Based on the above we can conclude that the claimed compounds isolated in solid form, have a higher thermostability compared to the prototype, which makes them applicable for the production of organic light-emitting diodes.

Thus, the proposed luminescent coordination compounds of lanthanides inventive, are new and promising for industrial applications.

Luminescent coordination compounds of the lanthanides, including as a ligand 1,10-phenanthroline-2,9-dicarboxylic acid (H2Phdic) and having the General formula Ln2(Phdic)3·2H2O, namely:

where Ln Is Eu3+, Tb3+, Dy3+Sm3+, Gd3+.



 

Same patents:

FIELD: chemistry.

SUBSTANCE: colourless phosphorescing red glowing phosphor Eu(L2)3 is a product of reacting a europium (III) compound with [2-(aminocarbonyl)phenoxy]acetic acid (HL2) and subsequent vacuum drying in a furnace at residual pressure of 20 Pa. Said phosphor has phosphorescence maximum at 18636, 14360, 16180, 16860 cm-1 and provides considerable intensity of red luminescence which is 40.43 times higher than quantum efficiency of luminescence compared to existing colourless phosphorescing red glowing phosphor - a compound of europium (III) with salicylic acid.

EFFECT: improved properties.

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FIELD: chemistry.

SUBSTANCE: solution of rare-earth salts is prepared, for example, nitrates of gadolinium, europium, terbium and ytterbium, in non-polar solvents - oleyl amine, oleic acid or compositions thereof with concentration of rare-earth elements of 0.05-0.1 mol/l. The solution is heated in an inert atmosphere of argon to 80-100°C and held at that temperature for 15-30 minutes. Diphenyl ether is then added in amount of 5-10 moles of ether per mole of rare-earth elements. The mixture is heated to 250-300°C and held for 1-2 hours. Excess polar solvent - acetone - is added to the obtained mixture. The coagulated nanoparticles are separated from the solution by centrifuging and the residue is redispersed in excess heptane. Colloidal solutions of luminescent nanoplates of rare-earth oxides with average diameter of 8-17 nm and thickness of 1-15 nm are obtained.

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FIELD: chemistry.

SUBSTANCE: invention relates to metal-polymer complex of europium (Eu3+) and (co)poly-(methylmethacrylate)-(1-methacryloyl-2-(2-pyridyl)-4-carboxy quinolyl)hydrazine of formula: where: m:k = 80 - 95.5:20 - 3.9:0 - 0.6 mol %, MM from 17000 to 24000 Da, Lig denotes a low-molecular weight ligand selected from dibenzoyl methane, thenoyltrifluoroacetone, having Eu3+ ion content from 2.6 to 9.6 wt %.

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FIELD: chemistry.

SUBSTANCE: invention can be used to produce infrared luminophores, having radiation in the near infrared range (0.80-0.82 and 0.90-0.98 mcm) when excited. The yttrium ortho-phosphate-based infrared luminophore can be used to make hidden, machine-readable luminescent labels used to protect bond payer, as well as active medium for lasers which generate in the (1.5-1.6 mcm) spectral range which is safe for the human eye. The yttrium ortho-phosphate-based infrared luminophore contains only Yb3+, Er3+, Ce3+ ions as optically active ions in a cationic subarray and has chemical composition corresponding to the following empirical formula: Y1-x-y-zYbxEryCezPO4, where 0.1≤x≤0.88; 0.0001≤y≤0.1; 1*10-4≤z≤1*10-2. The luminophore has simultaneously high intensity of Stokes infrared luminescence in the 1.5-1.6 mcm range and minimum anti-Stokes luminescence. The method of producing the infrared luminophore involves thermal treatment of a mixture of oxides of yttrium, ytterbium, erbium and cerium, a phosphorus-containing compound and a mineralising agent in air, wherein the phosphorus-containing compound used is disubstituted ammonium phosphate, and the mineralising agent used is carbonates of alkali metals: Li, Na and K, and thermal treatment is carried out at temperature 900-1250°C, which, depending on the concentration of the mineralising agent and calcination conditions, ensures reproducible production of well-formed microcrystals of the yttriuim ortho-phosphate-based infrared luminophore with average particle size from 2 to 18 mcm.

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2 cl, 4 dwg, 11 ex

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10 cl, 3 dwg, 1 ex

FIELD: physics.

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EFFECT: reduced tendency to luminescence quenching, higher temperature and chemical stability.

11 cl, 6 dwg, 4 ex

FIELD: chemistry.

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3 dwg, 4 tbl, 12 ex

FIELD: physics.

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19 cl, 4 tbl, 2 dwg

FIELD: chemistry.

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EFFECT: invention provides reliable protection of the pigment from hydrolysis, enables regulation of the amount of polymer binder which affects colour characteristics and technological aspects, as well as the size of particles of the luminescent pigment, which is important when mixing the pigment with components of compositions or paints.

4 cl, 8 tbl, 58 ex

FIELD: chemistry.

SUBSTANCE: disclosed is a colourless phosphorescing luminophor, which is a coordination compound of terbium (III) with [2-(aminocarbonyl)phenoxy]acetic acid (HL2) and having formula Tb(L2)3, and specifically: , having high quantum efficiency of luminescence, considerable luminescence intensity and fluorescence maxima at 20500, 18300, 17000, 16000 cm-1.

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1 dwg, 1 ex

FIELD: chemistry.

SUBSTANCE: present invention relates to novel imidazopyridin-2-one derivatives of general formula or pharmacologically acceptable salts thereof, where (R1)n-A is a 1H-pyrrolo[2,3-b]pyridin-5-yl group, 3-chloro-1H-pyrrolo[2,3-b]pyridin-5-yl group, 4-chloro-1H-pyrrolo[2,3-b]pyridin-5-yl group, 3-fluoro-1H-pyrrolo[2,3-b]pyridin-5-yl group, 4-fluoro-1H-pyrrolo[2,3-b]pyridin-5-yl group, 3-methyl-1H-pyrrolo[2,3-b]pyridin-5-yl group, 4-methyl-1H-pyrrolo[2,3-b]pyridin-5-yl group, 3,4-dimethyl-1H-pyrrolo[2,3-b]pyridin-5-yl group, 3-fluoro-4-methyl-1H-pyrrolo[2,3-b]pyridin-5-yl group or 3-chloro-4-methyl-1H-pyrrolo[2,3-b]pyridin-5-yl group, B is a 3-6-member saturated or partially saturated monocyclic hydrocarbon group and can contain 1 or 2 oxygen atoms, a nitrogen atom and/or sulphonyl groups as ring components, B can have as substitutes identical or different R2 in amount of m, R2 is a substitute represented at a carbon atom or a nitrogen atom forming B, R2 is a substitute selected from a group consisting of a hydroxy group, a halogen atom, a cyano group, an oxo group, a C1-4alkyl group (where the C1-4 alkyl group can be substituted with 1 C1-4 alkoxy group) and a C1-4 alkoxy group, when R2 is a substitute represented at a carbon atom forming B, and R2 is a substitute selected from a group consisting of a C1-4 alkyl group and a C1-4 alkylcarbonyl group, when R2 is a substitute represented at a nitrogen atom forming B, m is any integer from 0 to 2, Q is a bond or a C1-4 alkylene group, R3 and R4 are identical or different and each denotes a hydrogen atom or a halogen atom, and R5 and R6 are identical or different and each denotes a hydrogen atom, a halogen atom or a C1-4 alkyl group. The invention also relates to specific compounds of formula (I), pharmacologically acceptable salts of compounds of formula (I), a pharmaceutical composition based on the compound of formula (I) and use of the compound of formula (I).

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21 cl, 161 ex

FIELD: medicine, pharmaceutics.

SUBSTANCE: present invention refers to new imidazo[4,5-b]pyrazine derivatives of general formula or to its pharmaceutically acceptable salt wherein: R1 represents either aryl unsubstituted or substituted by one of the groups: halogen, hydoxyl, C1-6alkyl, C1-6alkoxyl, NH2, NHC1-6alkyl, N(C1-6alkyl)2, NHC1-6alkylC1-6alkoxy, C1-6alkylhydroxy, -C(O)NH2, -C(O)OC1-6alkyl, -C(O)NH C1-6alkyl, cyano, carboxy, heteroaryl and heterocycloalkyl; or heteroaryl unsubstituted or substituted by one of the groups: C1-6alkoxy, hydroxy, -C1-6alkyl, NH2 and NHC1-6alkyl; heterocycloalkyl unsubstituted or substituted by one group =O; and R2 represents H; unsubstituted C3-4alkyl; C1-4alkyl substituted by C5-6cycloalkyl unsubstituted or substituted by one group specified in amino, hydroxyl, C1-6alkoxy, or heterocycloalkyl unsubstituted or substituted by 1-2 groups specified in =O, C1-6alkyl; or C5-6cycloalkyl substituted by one group specified in hydroxyl, C1-6alkoxyl, C1-6alkylC1-6alkoxy, C1-6alkylhydroxy, CONH2; or substituted ir unsubstituted heterocycloalkyl; wherein aryl represents an aromatic structure consisting of 6-10 carbon atoms containing one ring or two condensed rings; wherein heteroaryl represents a 5-10-member aryl ring system containing 1-2 heteroatoms specified in nitrogen, oxygen and sulphur; wherein heterocycloalkyl represents a 5-9-member nonaromatic cycloalkyl wherein 1-2 heteroatoms specified in nitrogen and oxygen; provided the compound does not represent 1,3-dihydro-5-phenyl-2H-imidazo[4,5-b]pyrazin-2-one. Also, the invention refers to the specific imidazo[4,5-b]pyrazine derivatives, to a based pharmaceutical composition, to a method of treating or preventing cancer, inflammatory conditions, immunological diseases, metabolic conditions, and to a method of kinase inhibition in a cell expressing said kinase.

EFFECT: there are produced new imidazo[4,5-b]pyrazine derivatives showing effective biological properties.

17 cl, 2 tbl, 210 ex

FIELD: medicine, pharmaceutics.

SUBSTANCE: invention refers to compounds of formula

and

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EFFECT: preparing the compounds possessing the protein kinase inhibitor property.

16 cl, 5 ex

FIELD: chemistry.

SUBSTANCE: invention relates to substituted N-phenylpyrrolidinyl methylpyrrolidine amides of formula , where R, R1, R2 and R3 are identical or different and independently denote H, (C1-C4)alkyl, CF3; R4 denotes phenyl, cyclohexyl, pyridinyl, furanyl, isoxazolyl, quinolinyl, naphthyridinyl, indolyl, benzoimidazolyl, benzofuranyl, chromanyl, 4-oxo-4H-chromenyl, 2,3-dihydrobenzofuranyl, benzo[1,3]dioxolyl and 2,5-dioxo-2,3,4,5-tetrahydro-1H-benzo[e]][1,4]diazepinyl; where said R4 is optionally substituted one to more times with a substitute selected from halogen, hydroxy, (C1-C4) alkyl, (C1-C4) alkoxy, CF3, hydroxymethyl, 2-hydroxyethylamino, methoxyethylamide, benzyloxymethyl, piperidinyl, N-acetylpiperidinyl, pyrrolyl, imidazolyl, 5-oxo-4,5-dihydropyrazolyl; or pharmaceutically acceptable salt thereof or enantiomer or diastereomer thereof.

EFFECT: compounds have modulating activity on histamine H3 receptor, which enables use thereof to prepare a pharmaceutical composition.

10 cl, 3 dwg, 29 ex

FIELD: chemistry.

SUBSTANCE: invention relates to substituted N-phenylbipyrrolidine carboxamides of formula , where values of R, R1, R2, R3 and R4 are given in claim 1.

EFFECT: compounds have activity which binds to the H3 ligand, which allows use thereof in pharmaceutical compositions for treating sleep disorder.

10 cl, 1 tbl, 4 dwg, 153 ex

FIELD: medicine, pharmaceutics.

SUBSTANCE: invention refers to (aza)indole derivatives of formula

wherein the values T, X1-X3, R1, Q, Y, J are presented in clause 1 of the patent claim.

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19 cl, 62 tbl, 332 ex

FIELD: medicine, pharmaceutics.

SUBSTANCE: claimed invention relates to novel derivatives of imidazo[4,5-c]chinoline of general formula or to its pharmaceutically acceptable salts, where R1 represents straight-chained C1-C6alkyl, possibly substituted with one substituent, selected from C1-C3alkoxy; Z1 represents C2-C6alkylene; X1 represents NR5 or >NCOR5; Y1 represents C1-C6alkylene; R3 represents C1-C6alkyl, possibly substituted with C1-C6alkoxy; R5 represents hydrogen, piperidinyl, possibly substituted by piperidinyl nitrogen with group R10, group C1-C6alkyl, where the last group is possibly substituted with one substituent, independently selected from NR7R8 or R9; or R5 represents C1-C6alkylene, which can be bound with carbon atom in C2-C6alkylene group Z1 with formation of piperidine ring; each of R7 and R8 independently represents tetrahydropyranyl, piperidinyl, possibly substituted by piperidinyl nitrogen atom with group R10a, C1-C6alkyl, where the last group is possibly substituted with one group, independently selected from OR12; or R7 and R8 together with nitrogen atom, to which they are bound, form 4-7-membered saturated heterocyclic ring, selected from asetidinyl, pyrrolidinyl, piperidinyl, piperazinyl, morpholinyl, azepanyl, 1,4-oxazepanyl and 1,4-diazepanyl, where heterocyclic ring is possibly substituted with one or two substituents, independently selected from S(O)qR15, OR15, CO2R15, COR15, CONR15R16, NR15CO2R16, pyrimidinyl and C1-C6alkyl, where the last group is possibly substituted with one group, independently selected from OR18 and CO2R18; R9 represents S(O)qR20; R10 and R10a independently represent COR2 or group C1-C6alkyl; each of R12, R15, R16, R18, R20 and R24 independently represents hydrogen or C1-C6alkyl; q equals 2; m and n both equal 0; and A represents phenyl. Invention also relates to method of obtaining formula (I) compound, based on it pharmaceutical composition, and to method of treating said pathological conditions.

EFFECT: obtained are novel derivatives of imidazo[4,5-c]chinoline, useful modulation of TLR7 activity.

17 cl, 18 dwg, 81 ex

FIELD: chemistry.

SUBSTANCE: invention relates to a novel heterocyclic amide compound of formula I: or a pharmaceutically acceptable salt thereof. Described also is a pharmaceutical composition containing said compound, having protein kinase inhibitor, regulator or modulator properties, which is acceptable in treating or preventing a proliferative disease, an anti-proliferative disorder, inflammation, arthritis, neurologic or neurodegenerative disease, cardiovascular disease, hair loss, neural disease, ischemic disorder, viral disease or fungal disease.

EFFECT: high efficiency of using the compounds.

2 cl, 20 tbl

FIELD: medicine, pharmaceutics.

SUBSTANCE: invention refers to new pyrrole nitrogen-containing heterocyclic derivatives of formula (I) or their pharmaceutically acceptable salts:

,

wherein: X means C, N; each R1,R2 means H; R3 means C1-10alkyl; R4 means -[CH2CH(OH)]rCH2NR9R10, -(CH2)nNR9R10; provided X means N, R5 is absent, each R6, R7, R8 means H, halogen; provided X means C, each R5, R6, R7, R8 means H, halogen, hydroxyC1-10alkyl, C1-10alkyl, phenyl, 6-member heteroaryl with one N, -OH, -OR9, -NR9R10, -(CH2)nCONR9R10, -NR9COR10, -SO2R9 and -NHCO2R10, wherein said phenyl is unsubstituted or additionally substituted by one or more group C1-10alkyl, C1-10alkoxyl, halogen; each R9, R10 means H, C1-10alkyl wherein C1-10alkyl is unsubstituted or additionally substituted by one or more group C1-10alkyl, phenyl, halogenophenyl, -OH, C1-10alkoxy, OH- C1-10alkyl; or R9 and R10 together with an attached atom form a 5-6-member heteroring which may contain one O; n is equal to 2- 6; z is equal to 1-2; r is equal to 1-6;.

EFFECT: compounds may be used as protein kinase inhibitors.

14 cl, 2 tbl, 67 ex

FIELD: chemistry.

SUBSTANCE: invention relates to novel derivatives of 2-heteroaryl-substituted benzothiophene and benzofuran, precursors thereof and therapeutic use of said compounds, having structural formula (1a) where R1, R2, X9 and Q assume values given in the description, and pharmaceutically acceptable salts thereof, which are suitable for imaging amyloid deposits in living patients. The invention also relates to pharmaceutical compositions based on compounds of formula 1a, use and methods of producing said compounds. More specifically, the present invention relates to a method of imaging brain amyloid deposits in vivo for intravital diagnosis of Alzheimer's disease, and measuring clinical efficiency of therapeutic agents against Alzheimer's disease.

EFFECT: high efficiency of using said compounds.

15 cl, 1 tbl, 14 ex

FIELD: metallurgy.

SUBSTANCE: method for obtaining pure lanthanum hexaboride is implemented by combined electrodeposition of lanthanum and boron from chloride molten metal on the cathode and their further interaction at atomic level. The process is performed in three-electrode quartz cell, where a tungsten bar serves as a cathode; a glassy carbon bar sealed in pyrex glass serves as a comparison electrode; a glassy carbon melting pot serves as anode and at the same time as a container. Synthesis of ultradisperse powder of lanthanum hexaboride is performed by means of controlled potential electrolysis from equimole KCl-NaCl melt containing lanthanum trichloride and potassium fluoroborate in the environment of cleaned and dried argon at potentials of -2.0 to -2.6 V relative to glassy carbon comparison electrode at the temperature of 700±10°C.

EFFECT: obtaining pure target product owing to good solubility of background electrolyte in water; reduction of electric power costs.

2 cl, 3 ex

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