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US4746507A Expired / Lapsed US ⏱️ 0.0 years remaining

EDHPA based contrast agents for MR imaging, apparatus and methods

Assignee: Amersham Health Salutar Inc
•
Filing: 1985-04-02
•
Granted: 1988-05-24
•
Expires: 2005-04-02
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Abstract

Abstract Ethylene Diamine Hydroxy Phenylacetic Acid (EDHPA) type chelators strongly bind paramagnetic metal ions to provide excellent contrast agents for magnetic resonance (MR) imaging. The magnetic dipole generated by unpaired electrons within the paramagnetic (PM) atom, causes a local reduction in the bulk magnetic field of the MR system. The resulting shortening of the T1 (spin lattice) relaxation time in the hydrogen protons within the area of interest, causes an intense "free induction signal" and a corresponding modulation in the collected scanning data. The tissue of organ of interest appears on the MR display as a high intensity of white area. Background tissue is displayed as darker or lower intensity greys. Each member chelator EDHPA' of the EDHPA family of chelators, is a phenolic analog of EDTA, with variations in the para position radical (PR) of the phenol ring. Each EDHPA' chelator is formed by twin amino acid molecules (phenylalanine etc), which provide twin chelation units having three coordination points each for binding the paramagnetic metal.

Inventors

  • 👤 Steven C. Quag

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-11-02 20:04
CPC Classifications
G; G01; G01R; G01R33/00; G01R33/20; G01R33/44; G01R33/48; G01R33/54; G01R33/56; G01R33/5601; A; A61; A61K; A61K49/00; A61K49/06

Claims Analysis

Total Claims: 42
Claim 1
Independent Claim 181 words
An EDHPA based contrast agent in a solid state form, for use in an in vivo solution during diagnostic magnetic resonance (MR) imaging, to enhance the MR image of the region of interest of a subject within the magnetic field of the MR system, having the general formula: ##STR2## where: "PM" is a paramagnetic metal ion bound by chelation within the EDHPA; "B" is a benzene ring bonded to the acetic carbon, with only the "O - " phenol radical at the ortho position, or, a benzene ring bonded to the acetic carbon, with the "O - " phenol radical plus a para position phenol radical selected from the group consisting of ______________________________________ alkyl: --(CH.sub.2)--CH.sub.3, carboxyl: --COO.sup.-, nitro: --NO.sub.2, and sulfonic acid: --SO.sub.3.sup.- ; ______________________________________ "n" is, from 2 to 4 inclusive, methyl groups within the methyl chain connecting the two Nitrogen atoms; and "IN + " is a chemically inert cation for balancing the charge of the contrast agent molecule; whereby the contrast agent causes a reduction in the T1 relaxation timer near the region of interest within the subject.
Claim 2
Dependent Claim 181 words
An EDHPA based contrast agent in a solid state form, for use in an in vivo solution during diagnostic magnetic resonance (MR) imaging, to enhance the MR image of the region of interest of a subject within the magnetic field of the MR system, having the general formula: ##STR2## where: "PM" is a paramagnetic metal ion bound by chelation within the EDHPA; "B" is a benzene ring bonded to the acetic carbon, with only the "O - " phenol radical at the ortho position, or, a benzene ring bonded to the acetic carbon, with the "O - " phenol radical plus a para position phenol radical selected from the group consisting of ______________________________________ alkyl: --(CH.sub.2)--CH.sub.3, carboxyl: --COO.sup.-, nitro: --NO.sub.2, and sulfonic acid: --SO.sub.3.sup.- ; ______________________________________ "n" is, from 2 to 4 inclusive, methyl groups within the methyl chain connecting the two Nitrogen atoms; and "IN + " is a chemically inert cation for balancing the charge of the contrast agent molecule; whereby the contrast agent causes a reduction in the T1 relaxation timer near the region of interest within the subject.
Claim 3
Dependent Claim 36 words
The family of contrast agents of claim 1, wherein "IN + " is at least one inert cation selected from the group consisting of: Methyl Glucamine, N-Methyl Glucamine, and a first periodic group mineral salt cation.
Claim 4
Dependent Claim 15 words
The family of contrast agents of claim 1, wherein "n" is the whole integer 3.
Claim 5
Dependent Claim 90 words
The contrast agent of claim 1, wherein the paramagnetic metal ion "PM" is an ion selected from the group consisting of: ______________________________________ Cr + 3 Co + 2 Mn + 2 Ni + 2 Fe + 3 Fe + 2 Cu + 2 La + 3 Gd + 3 Ce + 3 Tb + 3 Pr + 3 Dy + 3 Nd + 3 Ho + 3 Pm + 3 Er + 3 Sm + 3 Tm + 3 Eu + 3 Yb + 3 and Lu + 3. ______________________________________
Claim 6
Dependent Claim 48 words
THe contrast agent of claim 1, wherein the paramagnetic metal ion "PM" is an ion selected from the group consisting of: ______________________________________ Cr + 3 Co + 2 Mn + 2 Ni + 2 Fe + 3 Fe + 2 Cu + 2 and Gd + 3. ______________________________________
Claim 7
Dependent Claim 39 words
The contrast agent of claim 1, wherein the paramagnetic metal ion "PM" is an ion selected from the group consisting of: ______________________________________ Fe + 3 Co + 2 Mn + 2 Cu + 2 and Gd + 3. ______________________________________
Claim 8
Dependent Claim 190 words
An EDHPA based contrast agent in a pharmacological solution form, for use in vivo solution during diagnostic magnetic resonance (MR) imaging, to enhance the MR image of the region of interest of a subject within the magnetic field of the MR system, having the general formula: ##STR3## where: "PM" is a paramagnetic metal ion bound by chelation within the EDHPA; "B" is a benzene ring bonded to the acetic carbon, with only the "O - " phenol radical at the ortho position, or, a benzine ring bonded to the acetic carbon, with the "O - " phenol radical plus a para position phenol radical selected from the group consisting of ______________________________________ alkyl: --(CH.sub.2)--CH.sub.3, carboxyl: --COO.sup.-, nitro: --NO.sub.2, and sulfonic acid: --SO.sub.3.sup.- ; ______________________________________ "n" is, from 2 to 4 inclusive, methyl groups within the methyl chain connecting the two Nitrogen atoms; and "IN + " is a chemically inert cation for balancing the charge the contrast agent molecule; and a pharmaceutically acceptable vehicle means for dispersing the EDHPA(PM) contrast agent; whereby the contrast agent causes a reduction in the T1 relaxation time near the region of interest within the subject.
Claim 9
Dependent Claim 190 words
An EDHPA based contrast agent in a pharmacological solution form, for use in vivo solution during diagnostic magnetic resonance (MR) imaging, to enhance the MR image of the region of interest of a subject within the magnetic field of the MR system, having the general formula: ##STR3## where: "PM" is a paramagnetic metal ion bound by chelation within the EDHPA; "B" is a benzene ring bonded to the acetic carbon, with only the "O - " phenol radical at the ortho position, or, a benzine ring bonded to the acetic carbon, with the "O - " phenol radical plus a para position phenol radical selected from the group consisting of ______________________________________ alkyl: --(CH.sub.2)--CH.sub.3, carboxyl: --COO.sup.-, nitro: --NO.sub.2, and sulfonic acid: --SO.sub.3.sup.- ; ______________________________________ "n" is, from 2 to 4 inclusive, methyl groups within the methyl chain connecting the two Nitrogen atoms; and "IN + " is a chemically inert cation for balancing the charge the contrast agent molecule; and a pharmaceutically acceptable vehicle means for dispersing the EDHPA(PM) contrast agent; whereby the contrast agent causes a reduction in the T1 relaxation time near the region of interest within the subject.
Claim 10
Dependent Claim 14 words
The contrast agent of claim 7, wherein the vehicle means is a water solution.
Claim 11
Dependent Claim 36 words
The family of contrast agents of claim 7, wherein "IN + " is at least one inert cation selected from the group consisting of Methyl Glucamine, N-Methyl Glucamine, and a first periodic group mineral salt cation.
Claim 12
Dependent Claim 15 words
The family of contrast agents of claim 7, wherein "n" is the whole integer 3.
Claim 13
Dependent Claim 90 words
The contrast agent of claim 7, wherein the paramagnetic metal ion "PM" is an ion selected from the group consisting of: ______________________________________ Cr + 3 Co + 2 Mn + 2 Ni + 2 Fe + 3 Fe + 2 Cu + 2 La + 3 Gd + 3 Ce + 3 Tb + 3 Pr + 3 Dy + 3 Nd + 3 Ho + 3 Pm + 3 Er + 3 Sm + 3 Tm + 3 Eu + 3 Yb + 3 and Lu + 3. ______________________________________
Claim 14
Dependent Claim 48 words
The contrast agent of claim 7, wherein the paramagnetic metal ion "PM" is an ion selected from the group consisting of: ______________________________________ Cr + 3 Co + 2 Mn + 2 Ni + 2 Fe + 3 Fe + 2 Cu + 2 and Gd + 3. ______________________________________
Claim 15
Dependent Claim 39 words
The contrast agent of claim 7, wherein the paramagnetic metal ion "PM" is an ion selected from the group consisting of: ______________________________________ Fe + 3 Co + 2 Mn + 2 Cu + 2 and Gd + 3. ______________________________________
Claim 16
Independent Claim 320 words
A method of manufacture of a chemically stable physiologically tolerable contrast agent EDHPA'(PM) by deprotonating and chelating the corresponding EDHPA based chelator, for use in vivo solution during diagnostic magnetic resonance (MR) imaging, to enhance the MR image of the region of interest of a subject within the magnetic field of the MR system, comprising: PROVIDING INITIAL SOLVENT for the deprotonating and chelating steps; PROVIDING to the solvent EDHPA based chelator having the general form: ##STR4## where: "B" is a benzene ring bonded to the acetic carbon, with only the "OH" phenol radical at the ortho position, or, a benzene ring bonded to the acetic carbon, bonded with the "OH" phenol radical plus a para position phenol radical selected from the group consisting of ______________________________________ alkyl: --(CH.sub.2)--CH.sub.3, carboxyl: --COOH, nitro: --NO.sub.2, and sulfonic acid: --SO.sub.3 H; ______________________________________ and "n" is, from 2 to 4 inclusive, methyl groups within the methyl chain connecting the two Nitrogen atoms; DEPROTONATING THE EDHPA' by adding a strong base deprotonating agent for removing the protons from the four oxygen coordinate sites: ______________________________________ EDHPA Based Chelator Plus Deprotonating Agent EDHPA'(-4) - (H.sup.+).sub.4 4(Dcat.sup.+ Dan.sup.-) Yields Deprotonated EDHPA' Plus Deprotonation By-Product EDHPA'(-4) + 4Dcat.sup.+ 4(H-Dan) (EDHPA' salt) ______________________________________ where: Dan - is a deprotonating anion for pulling the protons away from the EDHPA' chelator, and Dcat + is a deprotonating cation which occupies the four negatively charged coordination points, to provide the EDHPA'(-4) ion in solution; CHELATING THE EDHPA'(-) to form EDHPA'(PM) by adding the paramagnetic metal ion in the form of a metal salt: ______________________________________ Deprotonated EDHPA' Plus Metal Salt EDHPA'(-4) + 4Dcat.sup.+ PM + 2 - 2(Can.sup.-) Yields Chelated EDHPA' Plus Chelation By-Product EDHPA'(PM).sup.-- + 2Dcat.sup.+ 2(Can-Dcat) ______________________________________ where: PM is a paramagnetic metal cation from the added metal salt, and Can - is the counter anion from the added metal salt, to provide the EDHPA based chelator in the contrast agent form of EDHPA'(PM).
Claim 17
Independent Claim 320 words
A method of manufacture of a chemically stable physiologically tolerable contrast agent EDHPA'(PM) by deprotonating and chelating the corresponding EDHPA based chelator, for use in vivo solution during diagnostic magnetic resonance (MR) imaging, to enhance the MR image of the region of interest of a subject within the magnetic field of the MR system, comprising: PROVIDING INITIAL SOLVENT for the deprotonating and chelating steps; PROVIDING to the solvent EDHPA based chelator having the general form: ##STR4## where: "B" is a benzene ring bonded to the acetic carbon, with only the "OH" phenol radical at the ortho position, or, a benzene ring bonded to the acetic carbon, bonded with the "OH" phenol radical plus a para position phenol radical selected from the group consisting of ______________________________________ alkyl: --(CH.sub.2)--CH.sub.3, carboxyl: --COOH, nitro: --NO.sub.2, and sulfonic acid: --SO.sub.3 H; ______________________________________ and "n" is, from 2 to 4 inclusive, methyl groups within the methyl chain connecting the two Nitrogen atoms; DEPROTONATING THE EDHPA' by adding a strong base deprotonating agent for removing the protons from the four oxygen coordinate sites: ______________________________________ EDHPA Based Chelator Plus Deprotonating Agent EDHPA'(-4) - (H.sup.+).sub.4 4(Dcat.sup.+ Dan.sup.-) Yields Deprotonated EDHPA' Plus Deprotonation By-Product EDHPA'(-4) + 4Dcat.sup.+ 4(H-Dan) (EDHPA' salt) ______________________________________ where: Dan - is a deprotonating anion for pulling the protons away from the EDHPA' chelator, and Dcat + is a deprotonating cation which occupies the four negatively charged coordination points, to provide the EDHPA'(-4) ion in solution; CHELATING THE EDHPA'(-) to form EDHPA'(PM) by adding the paramagnetic metal ion in the form of a metal salt: ______________________________________ Deprotonated EDHPA' Plus Metal Salt EDHPA'(-4) + 4Dcat.sup.+ PM + 2 - 2(Can.sup.-) Yields Chelated EDHPA' Plus Chelation By-Product EDHPA'(PM).sup.-- + 2Dcat.sup.+ 2(Can-Dcat) ______________________________________ where: PM is a paramagnetic metal cation from the added metal salt, and Can - is the counter anion from the added metal salt, to provide the EDHPA based chelator in the contrast agent form of EDHPA'(PM).
Claim 18
Dependent Claim 24 words
The method of claim 14, further comprising the additional step of adding an inert cation for balancing the charge on the contrast agent EDHPA'(PM).
Claim 19
Dependent Claim 57 words
The method of claim 15, further comprising the additional step of: FORMING A STABLE EDHPA'(PM) SOLID from the deprotonated chelated EDHPA'(PM) and inert cation by removing: the initial solvent, the unused deprotonating agent (Dcat + -Dan - ), the by-products (H-Dan and Can-Dcat), and the Dcat + ions from the O═C--O - coordination points on the EDHPA'(PM).
Claim 20
Dependent Claim 22 words
The method of claim 16, wherein the step of forming a stable EDHPA'(PM) solid is accomplished by heating the deprotonated chelated solution.
Claim 21
Dependent Claim 26 words
The method of claim 18, wherein the step of forming a stable EDHPA'(PM) solid is accomplished by heating the deprotonated chelated solution under a partial vacuum.
Claim 22
Dependent Claim 30 words
The method of claim 18, wherein the step of forming a stable EDHPA'(PM) solid is accomplished by heating the deprotonated chelated solution under a partial vacuum in a rotary evaporator.
Claim 23
Dependent Claim 38 words
The method of claim 16, further comprising the additional step of: FORMING A STABLE EDHPA'(PM) SOLUTION by dissolving the stable solid EDHPA'(PM)-IN in a pharmacologically suitable solvent yielding EDHPA'(PM) -- 2IN + , in a stable pharmacological solution.
Claim 24
Dependent Claim 12 words
The method of claim 20, wherein the pharmacologically suitable solvent is water.
Claim 25
Dependent Claim 20 words
The method of claim 14, wherein the initial solvent provided for the deprotonating and chelating steps is a volatile liquid.
Claim 26
Dependent Claim 13 words
The method of claim 22, wherein the initial volatile solvent is an alcohol.
Claim 27
Dependent Claim 12 words
The method of claim 23, wherein the initial volatile solvent is methanol.
Claim 28
Dependent Claim 30 words
The method of claim 14, wherein the strong base deprotonating agent is at least one member selected from the group consisting of NaOH, NH 4 OH, LiOH, KOH, and CaOH.
Claim 29
Dependent Claim 14 words
The method of claim 14, wherein the strong base deprotonating agent is ammonium hydroxide.
Claim 30
Dependent Claim 18 words
The method of claim 1, wherein the Can - anion in the metal salt is a halide ion.
Claim 31
Dependent Claim 12 words
The method of claim 1, wherein Can - is Cl - .
Claim 32
Dependent Claim 90 words
The contrast agent of claim 14, wherein the paramagnetic metal ion "PM" is an ion selected from the group consisting of: ______________________________________ Cr + 3 Co + 2 Mn + 2 Ni + 2 Fe + 3 Fe + 2 Cu + 2 La + 3 Gd + 3 Ce + 3 Tb + 3 Pr + 3 Dy + 3 Nd + 3 Ho + 3 Pm + 3 Er + 3 Sm + 3 Tm + 3 Eu + 3 Yb + 3 and Lu + 3. ______________________________________
Claim 33
Dependent Claim 48 words
The contrast agent of claim 14, wherein the paramagnetic metal ion "PM" is an ion selected from the group consisting of: ______________________________________ Cr + 3 Co + 2 Mn + 2 Ni + 2 Fe + 3 Fe + 2 Cu + 2 and Gd + 3. ______________________________________
Claim 34
Dependent Claim 39 words
The contrast agent of claim 14, wherein the paramagnetic metal ion "PM" is an ion selected from the group consisting of: ______________________________________ Fe + 3 Co + 2 Mn + 2 Cu + 2 and Gd + 3. ______________________________________
Claim 35
Dependent Claim 33 words
The method of claim 14, wherein "IN + " is at least one inert cation selected from the group consisting of: Methyl Glucamine, N-Methyl Glucamine, and a first periodic group mineral salt cation.
Claim 36
Dependent Claim 19 words
The method of claim 14, further comprising the step of freeze drying the EDHPA'(PM) to form a stable crystal.
Claim 37
Dependent Claim 25 words
The method of claim 33, further comprising the step of adding a pharmaceutically acceptable vehicle means for dispersing the EDHPA'(PM) crystal forming the contrast agent.
Claim 38
Independent Claim 208 words
The method of imaging a subject with a magnetic resonance (MR) imaging system employing an EDHPA based paramagnetic contrast agent EDHPA'(PM), comprising the steps of: PROVIDING a physiologically tolerable contrast agent EDHPA'(PM) having the general form: ##STR5## where: "PM" is a paramagnetic metal ion bound by chelation within the EDHPA'; "B" is a benzene ring bonded to the acetic carbon, with only the "O - " phenol radical at the ortho position, or, a benzene ring bonded to the acetic carbon, with the "O - " phenol radical plus a para position phenol radical selected from the group consisting of ______________________________________ alkyl: --(CH.sub.2)--CH.sub.3, carboxyl: --COO.sup.-, nitro: --NO.sub.2, and sulfonic acid: --SO.sub.3.sup.- ; ______________________________________ "n" is, from 2 to 4 inclusive, methyl groups within the methyl chain connecting the two Nitrogen atoms; and "IN + " is a chemically inert cation for balancing the charge the contrast agent molecule; whereby the contrast agent causes a reduction in the T1 relaxation time near the region of interest within the subject; INTRODUCING the EDHPA'(PM) contrast agent into the subject; WAITING for the phenol radicals to cooperate with the in vivo environment; and IMAGING the region of interest within a subject with the MR system to obtain a contrast agent enhanced image.
Claim 39
Independent Claim 208 words
The method of imaging a subject with a magnetic resonance (MR) imaging system employing an EDHPA based paramagnetic contrast agent EDHPA'(PM), comprising the steps of: PROVIDING a physiologically tolerable contrast agent EDHPA'(PM) having the general form: ##STR5## where: "PM" is a paramagnetic metal ion bound by chelation within the EDHPA'; "B" is a benzene ring bonded to the acetic carbon, with only the "O - " phenol radical at the ortho position, or, a benzene ring bonded to the acetic carbon, with the "O - " phenol radical plus a para position phenol radical selected from the group consisting of ______________________________________ alkyl: --(CH.sub.2)--CH.sub.3, carboxyl: --COO.sup.-, nitro: --NO.sub.2, and sulfonic acid: --SO.sub.3.sup.- ; ______________________________________ "n" is, from 2 to 4 inclusive, methyl groups within the methyl chain connecting the two Nitrogen atoms; and "IN + " is a chemically inert cation for balancing the charge the contrast agent molecule; whereby the contrast agent causes a reduction in the T1 relaxation time near the region of interest within the subject; INTRODUCING the EDHPA'(PM) contrast agent into the subject; WAITING for the phenol radicals to cooperate with the in vivo environment; and IMAGING the region of interest within a subject with the MR system to obtain a contrast agent enhanced image.
Claim 40
Dependent Claim 20 words
The method of imaging a subject as specified in claim 35, wherein the contrast agent is introduced by intravenous injection.
Claim 41
Dependent Claim 24 words
The method of imaging a subject as specified in claim 35, wherein the waiting step last from about fifteen minutes to about thirty minutes.
Claim 42
Dependent Claim 40 words
The method of imaging a subject as specified in claim 35, further comprising: the initial step of providing data from a prior MR imaging: and the final step of subtraction comparing the prior MR image with the current MR image.

References Cited (Backward Citations)

US2795550A Cited
AU8633082A Cited
US4647447A Cited
US4442305A Cited

USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1991-05-24 1991-11-23 1992-05-24 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1995-05-24 1995-11-23 1996-05-24 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 1999-05-24 1999-11-23 2000-05-24 $7700.00 Window Closed / Lapsed

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