CN102167813B - Fluorescent tracing nanometer magnetic resonance imaging contrast agent - Google Patents
Fluorescent tracing nanometer magnetic resonance imaging contrast agent Download PDFInfo
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- CN102167813B CN102167813B CN2011100244888A CN201110024488A CN102167813B CN 102167813 B CN102167813 B CN 102167813B CN 2011100244888 A CN2011100244888 A CN 2011100244888A CN 201110024488 A CN201110024488 A CN 201110024488A CN 102167813 B CN102167813 B CN 102167813B
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- dtpaa
- qdtpagd
- sherwood oil
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Abstract
The invention discloses a compound and a preparation method and application thereof. The expression of the compound is F3O4-PEG-QDTPAGd and the structure of the compound is shown in the specification. The compound can be used in the magnetic resonance imaging detection, the fluorescent tracing of fluorescer, the nanometer magnetic resonance imaging and the contrast agent with liver targeting.
Description
Technical field
The present invention relates to a kind of compound that can be used as contrast medium, particularly a kind ofly be used for that nuclear magnetic resonance detects, have the fluorescent tracing nano magnetic resonance imaging contrast agent of fluorescent agent.
Background technology
Nuclear magnetic resonance (MRI) technology is to tumour, and the early diagnosis of malignant changes such as cardiovascular and cerebrovascular diseases is very effective, so be widely used in medical science and high-new scientific research field.Because the instrumental resolution that the MRI technology is used is always limited, so need be used contrast medium in many cases to increase image definition.But the development of contrast medium can not be satisfied the required of clinical diagnosis far away.Still micro-clinically now at the horse root that uses, a kind of many carboxyls polyamines base Gd (III) title complex, or the German product of the eighties in last century.The micro-no target property of existing horse root, its imaging effect still remains to be improved under some use occasion.Seek that new than existing contrast medium the target MRI compound of better effect to be arranged be the focus of association area worker research.
Summary of the invention
The present invention provides the preparation method of a kind of compound and this compound; This compound can be used as the contrast medium that nuclear magnetic resonance detects; And this contrast medium has a better effect than existing horse root is micro-; And have target fluorescent tracing group, Gd (III) title complex is through δ-amino polyoxamide methyl-3, and the 4-dihydroxy-benzene is bonded on the nano ferriferrous oxide carrier.
Compound of the present invention, its expression formula are F
3O
4-PEG-QDTPAGd, structure is as shown in the formula showing:
PEG is δ-amino polyoxamide methyl-3 in the expression formula, and 4-dihydroxy-benzene, QDTPAGd are that diethylenetriamine-acetyl (8 '-quinoline) amine-ethanoyl-nitrilotriacetic closes gadolinium (III).F is existing fluorophor in the structural formula, and for example fluorophor F can be ready-made flavones fluorophor, and preferred F is a 8-quinolylamine fluorophor.
The preparation method of the preferred compound of the present invention is: with ferriferrous oxide nano-particle and δ-amino polyoxamide methyl-3; 4-dihydroxy-benzene (PEG) is a raw material; Earlier with 60mg δ-amino polyoxamide methyl-3; The 4-dihydroxy-benzene is scattered in the chloroform, and the 150mg ferriferrous oxide nano-particle is dissolved in the solution of chloroform, fully stirs the back under the mixture room temperature and makes product Fe at adorned nanoparticle through adding sherwood oil
3O
4-PEG-NH
2Be precipitated out, spinning goes out product, with a spot of trichloromethane dissolving, adds sherwood oil more therein and produces deposition and recentrifuge separation, carries out purifying three times so repeatedly, will be dispersed among the DMF by the decorated nanometer particle then, uses in order to next step reaction; Weighing 239mg diethylene triamine pentacetic acid (DTPA) dianhydride (DTPAA) is dissolved in dry DMF with it, stirs moments later; Add the 0.8mL anhydrous triethylamine, DTPAA is dissolved in DMF fully, then gets the 8-quinolylamine that 69mg is dissolved in the 10mL dry DMF; In 2 hours, it is slowly joined in the DTPAA solution again; After fully stirring under the room temperature, the mixed solution rotary evaporation is removed unnecessary solvent, obtain saturated 8-AQ-DTPAA DMF solution; Get DMF liquid and the Fe of the saturated 8-AQ-DTPAA of equimolar amount
3O
4-PEG-NH
2Mix and stir diel; Add sherwood oil more therein and make by the decorated nanometer particle precipitation, spinning goes out post precipitation again with a spot of trichloromethane dissolving, continues to add sherwood oil and produces deposition; Spinning so obtains by decorated nanometer particle Fe behind the triplicate purifying
3O
4-PEG-DTPA-8-AQ is dispersed in the water it for use; Get equimolar Gadolinium trinitrate and join the Fe that has prepared
3O
4In-PEG-DTPA-8-AQ the dispersion liquid, the stirring at room diel behind the filtering reacting liquid, adds sherwood oil more therein and makes F
3O
4-PEG-QDTPAGd is precipitated out, and dissolves with a spot of trichloromethane through the spinning after product, continues to add sherwood oil and makes F
3O
4-PEG-QDTPAGd is precipitated out, and spinning again is so repeatedly after the purification process three times, with last products therefrom nanometer F
3O
4-PEG-QDTPAGd is dispersed in the water.
This compound of the present invention can be used as the fluorescent tracing nano magnetic resonance imaging contrast agent and uses.Test according to relevant shows that compound of the present invention has the liver target, and it is micro-that its longitudinal relaxation efficient is superior to existing MRI contrast medium horse root, and compound of the present invention also has the advantage that fluorescence shows simultaneously.
Description of drawings
Accompanying drawing 2 is Fe
3O
4-PEG-NH
2The IR spectrogram.
Accompanying drawing 3 is the IR spectrogram of 8-AQ-DTPAA.
Accompanying drawing 4 is Fe
3O
4The IR spectrogram of-PEG-DTPA-8-AQ.
Accompanying drawing 5 is the UV-vis spectrogram of 8-AQ-DTPAA.
Accompanying drawing 6 is Fe
3O
4The UV-vis spectrogram of-PEG-DTPA-8-AQ.
Accompanying drawing 7 is .Fe
3O
4-PEG-DTPA-8-AQ (peak 1) and Fe
3O
4-PEG-NH
2The fluorescence spectrum figure at (peak 2).
Accompanying drawing 8 is Fe
3O
4The transmission electron microscope picture of-PEG-QDTPAGd.
Accompanying drawing 9 is not with the mouse liver MRI of contrast medium figure (contrast).
Accompanying drawing 10 is the mouse liver MRI figure of contrast medium for adopting compound of the present invention.
Embodiment
Below provide the preparation and the corresponding test situation of compound of the present invention.
One, the preparation of compound and sign
1. buy or prepare a certain amount of ferriferrous oxide nano-particle raw material.
2. buy or preparation δ-amino polyoxamide methyl-3 the 4-dihydroxy-benzene.
3.PEG the magnetic nano-particle of modifying preparation
Weighing 60mg δ-amino polyoxamide methyl-3, the 4-dihydroxy-benzene is scattered in it in chloroform, and the solution that then ferriferrous oxide nano-particle is dissolved in chloroform adds above-mentioned reaction system.Stir diel under the mixture room temperature, then, adorned nanoparticle is separated out deposition through adding sherwood oil, and spinning gets product (Fe
3O
4-PEG-NH
2), with a spot of trichloromethane dissolving, continue to add sherwood oil and separate out deposition again, spinning, it is inferior to give a baby a bath on the third day after its birth so repeatedly, will be dispersed among the DMF by the decorated nanometer particle at last, uses in order to next step reaction, and synthetic route is following:
4. the preparation that has the nanoparticle of fluorescence
Weighing 239mg diethylene triamine pentacetic acid (DTPA) dianhydride (DTPAA) is dissolved in dry DMF with it, stirs moments later; Add the 0.8mL anhydrous triethylamine, DTPAA is dissolved in DMF fully, then gets the 8-quinolylamine (8-AQ) that 69mg is dissolved in the 10mL dry DMF; In 2h, slowly join in the DTPAA solution through constant pressure funnel, stir under the room temperature 1 round the clock after, with the mixed solution rotary evaporation; Obtain small amount of liquid, its note is 8-AQ-DTPAA.The take a morsel DMF liquid of 8-AQ-DTPAA is with Fe
3O
4-PEG-NH
2Mix and stir diel.Last adorned nanoparticle is separated out post precipitation through adding sherwood oil, spinning, and product dissolves with a spot of trichloromethane, and continue to add sherwood oil and separate out deposition again, spinning, repetitive scrubbing is three times like this, then will be by decorated nanometer particle Fe
3O
4-PEG-DTPA-8-AQ is dispersed in the water for use, and synthetic route is following:
5. the preparation of targeted contrast agent
With Gadolinium trinitrate add prepared by decorated nanometer Fe
3O
4In-PEG-DTPA-8-AQ the dispersion liquid, the stirring at room diel.After using the cotton filtering reacting liquid then, and then adorned nanoparticle is separated out deposition, back spinning through adding sherwood oil; Product dissolves with a spot of trichloromethane; Continue to add sherwood oil and separate out deposition again, spinning, repetitive scrubbing is three times like this; At last adorned nanoparticle is dispersed in the water, its expression formula is F
3O
4-PEG-QDTPAGd, structure is suc as formula showing that as 1 wherein: F is a 8-quinolylamine fluorophor; F
3O
4Be nano ferriferrous oxide; PEG is δ-amino polyoxamide methyl-3, the 4-dihydroxy-benzene; QDTPAGd is that diethylenetriamine-acetyl (8 '-quinoline) amine-ethanoyl-nitrilotriacetic closes gadolinium (III).
Two, sample is formed sign:
1. sample appearance: brown oily solid is dispersed in the water and did not precipitate in 6 months.
2.Fe
3O
4Each integral part characteristic of-PEG-QDTPAGd
3. compound characterizes
Accompanying drawing 4 is Fe
3O
4The IR spectrogram of-PEG-DTPA-8-AQ, 3424cm
-1Be amino v (N-H), 1731cm
-1Be the v (C=O) of DTPAA, 1634cm
-1Be the skeletal vibration peak of quinoline ring and phenyl ring, 616cm
-1Be that pyrocatechol closes Fe
3O
4V (Fe-O), above characteristic peak is consistent with precursor I R characteristic peak, proves that made sample is correct.
Accompanying drawing 5,6 is respectively 8-AQ-DTPAA and Fe
3O
4The UV-vis spectrogram of-PEG-DTPA-8-AQ, the UV maximum absorption band of 8-AQ-DTPAA is at 280nm and 350nm, Fe
3O
4The UV maximum absorption band of-PEG-DTPA-8-AQ has proved further that at 280nm and 300nm the conclusion of IR (accompanying drawing 2,3) is correct.
Accompanying drawing 7 is Fe
3O
4The fluorescence spectrum figure of-PEG-DTPA-8-AQ, 358nm place cutting edge of a knife or a sword 1 is Fe among the figure
3O
4The fluorescence emission peak of-PEG-DTPA-8-AQ (connecting F), the peak 2 at 450nm place is Fe
3O
4-PEG-NH
2The fluorescence emission peak of (not connecting F), the former fluorescent emission intensity is stronger about 60 times than the latter, and the latter does not have fluorescence basically.Fluorescent emission intensity significantly strengthens after proving compound introducing F of the present invention.
Three, mouse living imaging contrast experiment
Accompanying drawing 9 is not for scheming (being control group) with the mouse liver MRI of contrast medium.Accompanying drawing 10 is the mouse liver MRI figure of contrast medium for adopting compound of the present invention, and wherein the same position of same reference numeral is used the MRI figure of the micro-medicine of existing horse root and used compound F 17-hydroxy-corticosterone of the present invention among Fig. 9 and 10
3O
4-PEG-QDTPAGd MRI figure.Accompanying drawing 9 and 10 imaging picture all are on MiniMR-60 animal magnetic resonance imager, to accomplish, and the imaging sequence that makes is the multilayer spin-echo sequence.Compound of the present invention adopts and is tried the mouse subcutaneous administration in the test, and the result shows and uses the mouse of being tried of compound of the present invention only to look like to have clear improvement at the liver station diagram.Comparison diagram 9,10 can be known, uses F
3O
4The mouse liver image definition is obviously improved behind-the PEG-QDTPAGd, and this proves that compound of the present invention is the MRI contrast medium that liver is had target, and its effect to be superior to existing MRI contrast medium horse root micro-, this point can be by the R of The compounds of this invention
1Be able to proof (seeing the following form) for micro-high 7.69 times than horse root.
The sample title | T 1(ms) | C(mmol/L) | R 1(Mm -1s -1) |
Horse root micro-(control group) | 104.11 | 1.10 | 8.14 |
Fe 3O 4-PEG-QDTPAGd | 30.2 | 0.531 | 62.58 |
H 2O | 3771.84 |
It is the Fe of 0.531mmol/L that last tabular has gone out concentration
3O
4Micro-and the neat solvent (H of the horse root of-PEG-QDTPAGd and 1.10mmol/L
2O) longitudinal relaxation time (T
1) measured value, according to T
1Calculate Fe
3O
4The relaxation efficient R of-PEG-QDTPAGd
1=62.58Mm
-1s
-1, the R that the horse root is micro-
1=8.14Mm
-1s
-1It is thus clear that the R of The compounds of this invention
1Micro-higher 7.69 times than horse root, it is micro-to prove that its imaging effect is superior to existing MRI contrast medium horse root.
Claims (4)
1. compound, its expression formula is Fe
3O
4-PEG-QDTPAGd, structure is as shown in the formula showing:
PEG is amino polyoxamide methyl-3 in the expression formula, and 4-dihydroxy-benzene, QDTPAGd are that diethylenetriamine-acetyl (8 '-quinoline) amine-ethanoyl-nitrilotriacetic closes gadolinium (III), and F is a fluorophor in the structural formula, Fe
3O
4Be nano ferriferrous oxide.
2. the described compound of claim 1 is characterized in that F is a 8-quinolylamine fluorophor.
3. the preparation method of the compound of claim 2; It is characterized in that: with ferriferrous oxide nano-particle and δ-amino polyoxamide methyl-3; The 4-dihydroxy-benzene is a raw material, and earlier with 60mg δ-amino polyoxamide methyl-3, the 4-dihydroxy-benzene is scattered in the chloroform; The 150mg ferriferrous oxide nano-particle is dissolved in the solution of chloroform, fully stirs the back under the mixture room temperature and makes product Fe through adding sherwood oil at adorned nanoparticle
3O
4-PEG-NH
2Be precipitated out, spinning goes out product, with a spot of trichloromethane dissolving, adds sherwood oil more therein and produces deposition and recentrifuge separation, carries out purifying three times so repeatedly, will be dispersed among the DMF by the decorated nanometer particle then, uses in order to next step reaction; Weighing 239mg diethylene triamine pentacetic acid (DTPA) dianhydride (DTPAA) is dissolved in dry DMF with it, stirs moments later; Add the 0.8mL anhydrous triethylamine, DTPAA is dissolved in DMF fully, then gets the 8-quinolylamine that 69mg is dissolved in the 10mL dry DMF; In 2 hours, it is slowly joined in the DTPAA solution again; After fully stirring under the room temperature, the mixed solution rotary evaporation is removed unnecessary solvent, obtain the DMF solution of the 8-AQ-DTPAA of saturated solution; Get DMF liquid and the Fe of the saturated 8-AQ-DTPAA of equimolar amount
3O
4-PEG-NH
2Mix and stir diel, add sherwood oil more therein and make by the decorated nanometer particle precipitation, spinning goes out post precipitation again with a spot of trichloromethane dissolving; Continue to add sherwood oil and produce deposition; Spinning, behind the triplicate purifying like this, will be by decorated nanometer particle Fe
3O
4-PEG-DTPA-8-AQ is dispersed in the water for use; Equimolar Gadolinium trinitrate is joined the Fe that has prepared
3O
4-PEG-DTPA-8-AQ is by in the decorated nanometer particle dispersion, and the stirring at room diel behind the filtering reacting liquid, adds sherwood oil more therein and makes Fe
3O
4-PEG-QDTPAGd is precipitated out, and dissolves with a spot of trichloromethane through the spinning after product, continues to add sherwood oil and makes Fe
3O
4-PEG-QDTPAGd is precipitated out, and spinning again is so repeatedly after the purification process three times, at last with adorned nanoparticle Fe
3O
4-PEG-QDTPAGd is dispersed in the water.
4. claim 1 or the 2 described compounds application that is to prepare the fluorescent tracing nano magnetic resonance imaging contrast agent.
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CN102516822B (en) * | 2011-11-04 | 2014-08-06 | 昆明理工大学 | Surface-functionalized Fe3O4 nanoparticles as well as preparation method and application thereof |
CN103980297B (en) * | 2014-04-15 | 2016-11-23 | 大连大学 | A kind of Multifunctional imaging probe detecting mercury ion |
CN107007843A (en) * | 2017-03-03 | 2017-08-04 | 广州军区广州总医院 | PET/MRI bimodal developer SPIO NOTA68Ga and preparation method thereof and purposes |
CN109568666B (en) * | 2018-12-10 | 2021-02-02 | 锦州医科大学附属第一医院 | Gd:Fe3O4Method for repairing spinal nerve injury by using @ RA composite nano molecule and MRI (magnetic resonance imaging) contrast method |
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CN1684710A (en) * | 2002-09-23 | 2005-10-19 | 通用电气公司 | Bifunctional contrast agent comprising a fluorescent dye and an MRI contrast agent |
CN101912623A (en) * | 2010-08-24 | 2010-12-15 | 上海师范大学 | Preparation and application of Fe-Gd double-mode magnetic resonance contrast agent with targeting function |
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CN1684710A (en) * | 2002-09-23 | 2005-10-19 | 通用电气公司 | Bifunctional contrast agent comprising a fluorescent dye and an MRI contrast agent |
CN101912623A (en) * | 2010-08-24 | 2010-12-15 | 上海师范大学 | Preparation and application of Fe-Gd double-mode magnetic resonance contrast agent with targeting function |
Non-Patent Citations (2)
Title |
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Ki Hyun Bae,etal..Bioinspired Synthesis and Characterization of Gadolinium-Labeled Magnetite Nanoparticles for Dual Contrast T1- and T2-Weighted Magnetic Resonance Imaging.《Bioconjugate Chemistry》.2010,第21卷(第3期),第506-507页. * |
汪宝堆.磁性纳米粒子为载体的色酮衍生物及配合物的合成和药理活性研究.《中国博士学位论文全文数据库 工程科技I辑》.2009,(第12期),第二章第27-30页,第四章第52-55页. * |
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