Glucose sensor

• US 5,522,977 A
• Filed: 10/07/1994
• Issued: 06/04/1996
• Est. Priority Date: 10/07/1994
• Status: Expired due to Fees

• Current Assignee: Biomedix, Inc.
• Original Assignee: Biomedix, Inc.
• Inventors: Shieh, Paul
• Primary Examiner(s): TUNG, TA HSUNG
• Application Number:
  US08/319,618
• Time in Patent Office: 606 Days
• Field of Search: 204/403, 204/416, 204/418, 204/419, 204/153.12
• US Class Current: 204/403.06
• CPC Class Codes: C12Q 1/006 for glucose
• CPC Class Codes: Y10S 435/817 Enzyme or microbe electrode

Abstract

A redox electrode for the rapid detection of glucose in aqueous media and a method for its use are provided. The redox electrode comprises an electrically conductive member such as copper, and a redox membrane in direct contact with said electrically conductive member. The redox membrane comprises a polymer matrix such as PVC containing a plasticizer, and a complex of 7,7,8,8 -tetracyanoquinodimethane and tetrathiafulvalene with the complex having a burgundy-red coloration and characterized by a broad absorption from about 340 nm to about 550 nm and weaker absorption between about 650 nm to about 800 nm having about six small peaks with an absorption maximum at about 750nm. Glucose is rapidly assayed by bringing the redox electrode and a reference electrode into simultaneous contact with an aqueous medium containing KCl, phosphate buffer, glucose oxidase, peroxidase, and 3,3'"'"',5,5'"'"'-tetramethylbenzidine dihydrochloride. The potential of the redox membrane is then monitored until it is stable. A sample containing glucose is added to the aqueous medium, and the change of potential of the redox electrode, which is related to glucose concentration, is then observed. In a variant of this method, the redox electrode is treated with ascorbic acid before a glucose oxidation to magnify the potential difference generated, and after oxidation to rapidly collapse the potential and prepare the electrode for another analysis.

Claims

1. An electrode for the potentiometric determination of glucose in aqueous media comprising:

an electrically conductive member, and

a redox membrane indirect contact with said electrically conductive member, said redox membrane comprising;

a polymer matrix, said polymer matrix containing;

a plasticizer, and

a complex of 7,7,8,8-tetracyanoquinodimethane and tetrathiafulvalene comprising a complex having a burgundy-red color.

2. The electrode of claim 1 in which the complex of 7,7,8,8-tetracyanoquinodimethane and tetrathiafulvalene comprises a complex having an ultraviolet absorption spectrum with broad absorption from about 340 nanometers to about 550 nanometers.

3. The electrode of claim 1 in which said polymer matrix comprises polyvinylchloride and the plasticizer comprises dibutylphthalate.

4. The electrode of claim 3 in which said electrically conductive member comprises a wire having a tip, with said redox membrane in direct contact with said tip.

5. The electrode of claim 4 in which the wire comprises copper.

6. The electrode of claim 5 in which said wire further comprises a layer of insulation with said layer of insulation sheathing said copper wire along its length.

7. The electrode of claim 6 in which said polymer matrix adheres to said layer of insulation sheathing the copper wire.

8. A polymeric redox membrane for potentiometric determination of glucose, the membrane to interface with a test solution containing glucose, the membrane in direct contact with a conductive substrate or in electrical contact with an internal reference electrode element, said membrane comprising:

a polymeric matrix, the polymeric matrix containing;

a plasticizer, and

a complex of 7,7,8,8-tetracyanoquinodimethane and tetrathiafulvalene comprising a complex having a burgundy-red color.

9. The polymeric redox membrane of claim 8 in which the complex of 7,7,8,8-tetracyanoquinodimethane and tetrathiafulvalene comprises a complex having an ultraviolet absorption spectrum with broad absorption from about 340 nanometers to about 550 nanometers.

10. The polymeric redox membrane of claim 8 in which the polymeric matrix comprises polyvinylchloride.

11. The polymeric redox membrane of claim 10 in which the plasticizer comprises dibutylphthalate.

12. A redox membrane for the potentiometric assay of glucose in aqueous solution, fabricated in steps comprising:

a) preparing a liquid solution of polyvinylchoride, dibutylphthalate and equal weights of 7,7,8,8-tetracyanoquinodimethane and tetrathiafulvalene in a solvent;

b) adding a particle of solid 7,7,8,8-tetracyanoquinodimethane to the solution of step a);

c) concentrating the solution of step b) at ambient temperature until the solution has a burgundy-red coloration and a higher viscosity;

d) coating the solution of step c) on a substrate;

e) evaporating the solvent from the coating of step d) to form a redox membrane.

13. The redox membrane of claim 12 in which the solvent of step a) is tetrahydrofuran.

14. A complex useful as a component of redox membranes for potentiometric glucose sensors comprising:

a complex of 7,7,8,8-tetracyanoquinodimethane and tetrathiafulvalene formed in solution in the presence of undissolved 7,7,8,8-tetracyanoquinodimethane, the complex having a burgundy-red color in solution and an absorption spectrum in solution with broad absorption from about 340 nanometers to about 550 nanometers.