Electrochemical sensor

• US 5,437,999 A
• Filed: 02/22/1994
• Issued: 08/01/1995
• Est. Priority Date: 02/22/1994
• Status: Expired due to Term

• Current Assignee: Roche Diabetes Care Inc. (Roche Holding AG)
• Original Assignee: Boehringer Mannheim Corporation
• Inventors: Kordal, Richard J., Diebold, Eric R., Wilsey, Christopher D., Surridge, Nigel A.
• Primary Examiner(s): Beisner, William H.
• Application Number:
  US08/200,174
• Time in Patent Office: 525 Days
• Field of Search: 435/288, 435/291, 435/817, 422/82.01, 422/82.02, 204/400, 204/403, 204/434, 204/435, 204/153.12
• US Class Current: 204/403.11
• CPC Class Codes: C12Q 1/001 Enzyme electrodes
• CPC Class Codes: G01N 27/3272 Test elements therefor, i.e. disposable laminated substrates with electrodes, reagent and channels optical biosensors G01N33/52
• CPC Class Codes: Y10S 435/817 Enzyme or microbe electrode

Abstract

A method for fabricating high-resolution, biocompatible electrodes is disclosed, allowing production of an electrochemical sensor which is capable of precise analyte concentration determination on a very small sample size. Electrically conducting material is affixed to a first insulating substrate. A second insulating substrate is then affixed to the electrically conducting material and patterned using photolithography to define an electrode area. Alternatively, the electrically conducting material may be screen printed directly onto a standard printed circuit board substrate in the case of a counter or reference electrode. In either case, the substrate may be rigid or flexible. When the electrodes produced in accordance with the present invention are then used in an electrochemical sensor which includes a reagent, the small and highly-defined electrode areas permit highly-accurate electrochemical analyte measurements to be performed on very small sample sizes.

Claims

1. An electrochemical sensor useful for measuring the concentration of an analyte in a fluid sample, comprising:

(a) opposing working and counter electrode elements, spatially displaced by a spacer having a first cutout portion forming a capillary space between the working and counter electrode elements and a second cutout portion allowing electrical connection between the counter electrode element and a meter and power source, wherein the capillary space is vented by a port in the working or counter electrode elements, the working electrode element including

1) a first insulating substrate,

2) an electrically conducting material affixed to the first insulating substrate, and

3) a second insulating substrate affixed to the electrically conducting material and the spacer, the second insulating substrate having a first cutout portion for exposing a portion of the electrically conducting material to the capillary space and a second cutout portion which allows contact between the electrically conducting material and the meter and power source,

the counter electrode element including

1) an insulating substrate, and

2) an electrically conducting material affixed to the insulating substrate and the spacer; and

(b) a reagent disposed in the capillary space, the reagent being specifically reactive with the analyte in the fluid sample to produce an electrochemically-measurable signal which can be correlated to the concentration of the analyte in the fluid sample.

2. The electrochemical sensor of claim 1, wherein the vent port extends through the working electrode element and the counter electrode element.

3. The electrochemical sensor of claim 2, wherein the counter electrode element further comprises:

3) a second insulating substrate affixed to the electrically conducting material and the spacer, the second insulating substrate having a first cutout portion for exposing a portion of the electrically conducting material to the capillary space and a second cutout portion which overlays the second cutout portion of the spacer.

4. The electrochemical sensor of claim 3, wherein the electrically conducting material of the working electrode element is a noble metal or carbon.

5. The electrochemical sensor of claim 4, wherein the electrically conducting material of the counter electrode element is a noble metal or carbon.

6. The electrochemical sensor of claim 5, wherein the second insulating substrate is a solder resist.

7. The electrochemical sensor of claim 6, further comprising:

(d) the power source in electrical connection with the working and counter electrode elements; and

(e) the meter in electrical connection with the working and counter electrode elements and capable of measuring current.

8. The electrochemical sensor of claim 7, wherein the reagent comprises a mediator and an enzyme.

9. The electrochemical sensor of claim 8, wherein the reagent further comprises a buffer, a film former, and a surfactant.

10. The electrochemical sensor of claim 9, wherein the analyte is glucose, the mediator is [Os(II)(bpy)₂ (im)Cl]⁺ [Cl]^-, the enzyme is glucose oxidase, the buffer is MES buffer, the film former is polyvinyl alcohol, and the surfactant is a nonionic surfactant.

11. The electrochemical sensor of claim 8, wherein the mediator is Os(II)(bpy)₂ (im)Cl]⁺ [Cl]^- and the enzyme is glucose oxidase.

12. An electrochemical sensor useful for measuring the concentration of an analyte in a fluid sample, comprising:

(a) opposing working and reference electrode elements, spatially displaced by a spacer having a first cutout portion forming a capillary space between the working and reference electrode elements and a second cutout portion allowing electrical connection between the reference electrode element and a meter and power source, wherein the capillary space is vented by a port in the working or reference electrode elements, the working electrode element including

1) a first insulating substrate,

2) an electrically conducting material affixed to the first insulating substrate, and

3) a second insulating substrate affixed to the electrically conducting material and the spacer, the second insulating substrate having a first cutout portion for exposing a portion of the electrically conducting material to the capillary space and a second cutout portion which allows contact between the electrically conducting material and the meter and power source,

the reference electrode element including

1) an insulating substrate,

2) an electrically conducting reference material affixed to the insulating substrate and the spacer; and

(b) a reagent disposed in the capillary space, the reagent being specifically reactive with the analyte in the fluid sample to produce an electrochemically-measurable signal which can be correlated to the concentration of the analyte in the fluid sample.

13. The electrochemical sensor of claim 12, wherein the vent port extends through the working electrode element and the reference electrode element.

14. The electrochemical sensor of claim 13, wherein the reference electrode element further comprises:

4) a second insulating substrate affixed to the reference electrode material and the spacer, the second insulating substrate having a first cutout portion for exposing a portion of the electrically conducting material to the capillary space and a second cutout portion which overlays the second cutout portion of the spacer.

15. The electrochemical sensor of claim 14, wherein the electrically conducting material of the working electrode element is a noble metal or carbon.

16. The electrochemical sensor of claim 15, wherein the electrically conducting reference material of the reference electrode element is silver/silver chloride.

17. The electrochemical sensor of claim 16, wherein the second insulating substrate is a solder resist.

18. The electrochemical sensor of claim 17, further comprising:

(d) the power source in electrical connection with the working and reference electrode elements; and

(e) the meter in electrical connection with the working and reference electrode elements and capable of measuring current.

19. The electrochemical sensor of claim 18, wherein the reagent comprises a redox mediator and an enzyme.

20. The electrochemical sensor of claim 19, wherein the reagent further comprises a buffer, a film former, and a surfactant.

21. The electrochemical sensor of claim 20, wherein the analyte is glucose, the redox mediator is [Os(II)(bpy)₂ (im)Cl]⁺ [Cl]^-, the enzyme is glucose oxidase, the buffer is MES buffer, the film former is polyvinyl alcohol, and the surfactant is a nonionic surfactant.

22. The electrochemical sensor of claim 19, wherein the redox mediator is [Os(II)(bpy)₂ (im)Cl]⁺ [Cl]^- and the enzyme is glucose oxidase.