Patent US4908322A successfully refreshed from Google Patents.
US4908322A
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US
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Derivatization of amines for electrochemical detection
Assignee: United States Department of Health and Human Services
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Filing: 1988-12-27
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Granted: 1990-03-13
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Expires: 2008-12-27
Abstract
Abstract Primary and secondary amines in biological fluids are selectively derivitized by reaction with esters of N-hydroxysuccinimide or N-hydroxysulfosuccinimide to form an N-acylated derivative. Those N-acylated derivatives may then be extracted into a polar organic phase and extracted. Non-electroactive amines may be made suitable for coulometric analysis by selecting the ester used so as to attach an electroactive group to the amine. For example, histamine may be reacted with the Bolton-Hunter reagent to form a suitable derivative in high yield.
Inventors
- 👤 Kenneth A. Jacobson
- 👤 Kenneth L. Kirk
- 👤 Markku I. Linnoila
- 👤 Thomas Miller
- 👤 Kazunori Mine
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-09 03:57
CPC Classifications
G; G01; G01N; G01N33/00; G01N33/48; G01N33/50; G01N33/52; Y; Y10; Y10S; Y10S436/00; Y10S436/815; Y10S436/816; Y10S436/901; Y10T; Y10T436/00; Y10T436/17; Y10T436/173845; Y10T436/174614
Claims Analysis
Total Claims: 28
Claim 1
Independent Claim
106 words
A process for the quantitative detection of amines in a fluid sample, comprising: reacting a fluid sample, under a non-reactive atmosphere, with a reactive O-acyl N-hydroxysulfosuccinamide to form an N-acylated derivative of the amine to be detected, wherein said acyl group is selected so as to enhance the separability of said N-acylated amine derivative from polar substances in the remainder of the fluid which may interfere with electrochemical measuring; separating the N-acylated amine derivative from polar substances in the remainder of the fluid sample which may interfere with electrochemical measuring; and subjecting the separating N-acylated amine derivative to electrochemical detection coupled to high pressure liquid chromatography.
Claim 2
Dependent Claim
106 words
A process for the quantitative detection of amines in a fluid sample, comprising: reacting a fluid sample, under a non-reactive atmosphere, with a reactive O-acyl N-hydroxysulfosuccinamide to form an N-acylated derivative of the amine to be detected, wherein said acyl group is selected so as to enhance the separability of said N-acylated amine derivative from polar substances in the remainder of the fluid which may interfere with electrochemical measuring; separating the N-acylated amine derivative from polar substances in the remainder of the fluid sample which may interfere with electrochemical measuring; and subjecting the separating N-acylated amine derivative to electrochemical detection coupled to high pressure liquid chromatography.
Claim 3
Dependent Claim
15 words
A process in accordance with claim 1, wherein said fluid sample is a biological fluid.
Claim 4
Dependent Claim
46 words
A process in accordance with claim 1, wherein the acyl group of said reactive O-acyl N-hydroxysulfosuccinamide is selected so as to render said N-acylated amine derivative soluble in an organic solvent, and said separating step comprises extracting the N-acylated amine derivative with a suitable organic solvent.
Claim 5
Dependent Claim
53 words
A process in accordance with claim 1, wherein the acyl group of said reactive O-acyl hydroxysulfosuccinamide is selected so as to render said N-acylated amine derivative isolatable by chromatography from polar substances in the remainder of the fluid sample which may interfere with electrochemical measuring, and said separating step is achieved by chromatography.
Claim 6
Dependent Claim
15 words
A process in accordance with claim 1 wherein said reactive O-acyl N-hydroxysulfosuccinamide in water soluble.
Claim 7
Dependent Claim
178 words
In the process for the quantitative detection of electroactive amines in an aqueous fluid sample containing other polar substances, comprising electrochemical detection coupled to high pressure liquid chromatography, the improvement whereby the sensitivity of such process can be substantially increased, comprising the steps of, prior to said detection step: reacting the fluid sample, under a non-reactive atmosphere, with a reactive O-acyl hydroxlamine derivative to form an N-acylated derivative of the electroactive amine to be detected, wherein said reactive O-acyl hydroxylamine derivative is selected to have the property that it is not reactive toward the portion of the electroactive amine to be detected which renders the amine electroactive, and wherein said acyl group is selected so as to render said N-acylated amine derivative soluble in an organic solvent and thereby separable from polar substances in the remainder of the fluid which may interfere with electrochemical measuring; and separating the N-acylated amine derivative from polar substances in the remainder of the fluid sample which may interfere with electrochemical measuring by extracting the N-acylated amine derivative with a suitable organic solvent.
Claim 8
Dependent Claim
178 words
In the process for the quantitative detection of electroactive amines in an aqueous fluid sample containing other polar substances, comprising electrochemical detection coupled to high pressure liquid chromatography, the improvement whereby the sensitivity of such process can be substantially increased, comprising the steps of, prior to said detection step: reacting the fluid sample, under a non-reactive atmosphere, with a reactive O-acyl hydroxlamine derivative to form an N-acylated derivative of the electroactive amine to be detected, wherein said reactive O-acyl hydroxylamine derivative is selected to have the property that it is not reactive toward the portion of the electroactive amine to be detected which renders the amine electroactive, and wherein said acyl group is selected so as to render said N-acylated amine derivative soluble in an organic solvent and thereby separable from polar substances in the remainder of the fluid which may interfere with electrochemical measuring; and separating the N-acylated amine derivative from polar substances in the remainder of the fluid sample which may interfere with electrochemical measuring by extracting the N-acylated amine derivative with a suitable organic solvent.
Claim 9
Dependent Claim
35 words
A process in accordance with claim 6, further including the step of concentrating the derivative-containing organic solvent solution obtained by said separating step by evaporating a portion of said solvent prior to said detection step.
Claim 10
Dependent Claim
23 words
A process in accordance with claim 6, wherein said O-acyl hydroxylamine derivative is an ester of N-hydroxysuccinamide or an ester of an N-hydroxysulfosuccinamide.
Claim 11
Dependent Claim
63 words
A process in accordance with claim 8, wherein said O-acyl hydroxylamine derivative is a compound of the formula ##STR11## wherein R represents a straight chain alkyl group, a parasubstituted phenol, a hydroquinone, an aniline homolog, an aniline analog, a thiol, an oxidizable thioether, a quinone, a nitroaromatic, a disulfide or --CH 2 NHCONH 2 , and Y is --H or --SO 3 .
Claim 12
Dependent Claim
24 words
A process in accordance with claim 9, wherein R is --CH 3 , --CH 2 CH 3 , --CH 2 NHCONH 2 or ##STR12##
Claim 13
Dependent Claim
17 words
A process in accordance with claim 6, wherein said O-acyl hydroxylamine derivative is an ester of N-hydroxysulfosuccinamide.
Claim 14
Dependent Claim
15 words
A process in accordance with claim 11, wherein said ester of N-hydroxysulfosuccinamide is water soluble.
Claim 15
Dependent Claim
53 words
A process in accordance with claim 6, further including the steps of adding to the fluid sample, prior to said reacting step, a known quantity of an analog or homolog of said electroactive amine having essentially the same reactivity as said amine towards said O-acyl hydroxylamine derivative, thereby serving as an internal standard.
Claim 16
Dependent Claim
18 words
A process in accordance with claim 13, wherein the fluid of said fluid sample is a biological fluid.
Claim 17
Dependent Claim
18 words
A process in accordance with claim 6, wherein the fluid of said fluid sample is a biological fluid.
Claim 18
Dependent Claim
193 words
In the process for the quantitative detection of non-electroactive amines in an aqueous fluid sample containing other polar substances, comprising derivatizing said amines with an electroactive group and detecting said derivatized amine by electrochemical detection coupled to high pressure liquid chromatography, the improvement whereby such non-electroactive amines can be quantitatively detected in the fluid sample at substantial sensitivity, comprising the steps of, prior to said detecting step: reacting the fluid sample, under a non-reactive atmosphere, with a reactive O-acyl hydroxylamine derivative to form an N-acylated derivative of the non-electroactive amine to be detected, wherein said reactive O-acyl hydroxlamine derivative is selected to have the property that it is not reactive toward hydroxyl groups, and wherein said acyl group is selected so as to render said N-acylated amine derivative soluble in an organic solvent and thereby separable from polar substances in the remainder of the fluid sample which may interfere with electrochemical measuring and to render said N-acylated amine derivative electroactive; and separating the N-acylated amine derivative from polar substances in the remainder of the fluid sample which may interfere with electrochemical measuring by extracting the N-acylated amine derivative with a suitable organic solvent.
Claim 19
Dependent Claim
193 words
In the process for the quantitative detection of non-electroactive amines in an aqueous fluid sample containing other polar substances, comprising derivatizing said amines with an electroactive group and detecting said derivatized amine by electrochemical detection coupled to high pressure liquid chromatography, the improvement whereby such non-electroactive amines can be quantitatively detected in the fluid sample at substantial sensitivity, comprising the steps of, prior to said detecting step: reacting the fluid sample, under a non-reactive atmosphere, with a reactive O-acyl hydroxylamine derivative to form an N-acylated derivative of the non-electroactive amine to be detected, wherein said reactive O-acyl hydroxlamine derivative is selected to have the property that it is not reactive toward hydroxyl groups, and wherein said acyl group is selected so as to render said N-acylated amine derivative soluble in an organic solvent and thereby separable from polar substances in the remainder of the fluid sample which may interfere with electrochemical measuring and to render said N-acylated amine derivative electroactive; and separating the N-acylated amine derivative from polar substances in the remainder of the fluid sample which may interfere with electrochemical measuring by extracting the N-acylated amine derivative with a suitable organic solvent.
Claim 20
Dependent Claim
35 words
A process in accordance with claim 16, further including the step of concentrating the derivative-containing organic solvent solution obtained by said separating step by evaporating a portion of said solvent prior to said detection step.
Claim 21
Dependent Claim
23 words
A process in accordance with claim 16, wherein said O-acyl hydroxylamine derivative is an ester of N-hydroxysuccinamide or an ester of an N-hydroxysulfosuccinamide.
Claim 22
Dependent Claim
63 words
A process in accordance with claim 18, wherein said O-acyl hydroxylamine derivative is a compound of the formula ##STR13## wherein R represents a straight chain alkyl group, a parasubstituted phenol, a hydroquinone, an aniline homolog, an aniline analog, a thiol, an oxidizable thioether, a quinone, a nitroaromatic, a disulfide or --CH 2 NHCONH 2 , and Y is --H or --SO 3 .
Claim 23
Dependent Claim
24 words
A process in accordance with claim 19, wherein R is --CH 3 , --CH 2 CH 3 , --CH 2 NHCONH 2 or ##STR14##
Claim 24
Dependent Claim
17 words
A process in accordance with claim 16, wherein said O-acyl hydroxylamine derivative is an ester of N-hydroxysulfosuccinamide.
Claim 25
Dependent Claim
15 words
A process in accordance with claim 21, wherein said ester of N-hydroxysulfosuccinamide is water soluble.
Claim 26
Dependent Claim
53 words
A process in accordance with claim 16, further including the steps of adding to the fluid sample, prior to said reacting step, a known quantity of an analog or homolog of said non-electroactive amine having essentially the same reactivity as said amine towards said O-acyl hydroxylamine derivative, thereby serving as an internal standard.
Claim 27
Dependent Claim
18 words
A process in accordance with claim 23, wherein the fluid of said fluid sample is a biological fluid.
Claim 28
Dependent Claim
18 words
A process in accordance with claim 16, wherein the fluid of said fluid sample is a biological fluid.
References Cited (Backward Citations)
USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
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| 3.5 Years (Year 4) | 1993-03-12 | 1993-09-11 | 1994-03-13 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1997-03-12 | 1997-09-11 | 1998-03-13 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 2001-03-12 | 2001-09-11 | 2002-03-13 | $7700.00 | Window Closed / Lapsed |