Electrode assembly for assaying glucose

• US 5,804,048 A
• Filed: 08/15/1996
• Issued: 09/08/1998
• Est. Priority Date: 08/15/1996
• Status: Expired due to Term

• Current Assignee: Segars California Partners, LP
• Original Assignee: VIA Medical Corporation (Medtronic Plc)
• Inventors: Lucisano, Joseph Y., Wong, David K.
• Primary Examiner(s): Gorgos, Kathryn L.
• Assistant Examiner(s): NOGUEROLA, ALEXANDER STEPHAN
• Application Number:
  US08/698,045
• Time in Patent Office: 754 Days
• Field of Search: 156/273.9, 427/2.11, 427/2.12, 427/2.13, 427/58, 204/403, 205/778, 205/72, 205/793, 438/817
• US Class Current: 204/403.09
• CPC Class Codes: C12Q 1/002 Electrode membranes
• CPC Class Codes: C12Q 1/006 for glucose
• CPC Class Codes: G01N 27/3271 Amperometric enzyme electrodes for analytes in body fluids, e.g. glucose in blood amperometry per se G01N27/49; aspects concerning the enzyme reagent C12Q1/001
• CPC Class Codes: Y10S 435/817 Enzyme or microbe electrode

Abstract

An improved electrode assembly is disclosed for use in assaying glucose in solution, e.g., in undiluted whole blood. The assembly includes a sensor electrode and a special overlaying multi-layer membrane that can be sterilized by gamma radiation without reducing the activity of a glucose oxidase enzyme located in an intermediate layer of the membrane. An outer layer of the membrane is formed with microscopic pores having a predetermined density and predetermined size, for reliably controlling the flux of glucose and oxygen from the solution to the intermediate layer, where they react in the presence of the glucose oxidase enzyme to form reactions products that include hydrogen peroxide. The outer layer thus functions as a diffusion barrier, to eliminate the adverse effects of any oxygen deficit that might be present. In addition, an inner layer of the membrane functions as an interference barrier, for controlling the permeation of the hydrogen peroxide reaction product to the underlying electrode. The inner layer includes a relatively thick, porous backing film, formed for example of porous polyester, and a relatively thin, porous overlaying film, formed for example of polysulfone.

Claims

1. An electrode assembly for use in assaying glucose in a solution, the electrode assembly comprising:

a sensor electrode; and

a membrane assembly overlaying the sensor electrode the membrane assembly including

an outer, diffusion-barrier layer positioned to contact the solution, the outer layer having a substantially uniform thickness and having a distribution of pores of a specific density and of a size in the range of 0.0125 to 0.0200 microns.

an inner, interference-barrier layer contacting a face of the sensor electrode and having a substantially uniform thickness, wherein the inner layer includes a relatively thick, porous backing film and a relatively thin, porous overlaying film that overlays the backing film, and

an immobilized glucose oxidase layer interposed between the outer and inner layers and having a substantially uniform thickness,

wherein the outer layer is configured to allow glucose and oxygen to diffuse through it to reach the glucose oxidase layer, where the glucose and oxygen react to form reaction products that include hydrogen peroxide,

and wherein the inner layer is configured to have a permeability sufficient to pass hydrogen peroxide from the glucose oxidase layer to the face of the sensor electrode.

2. An electrode assembly as defined in claim 1, wherein the outer layer is configured to allow the diffusion of oxygen from the solution to a substantially greater degree than it allows the diffusion of glucose from the solution.

3. An electrode assembly as defined in claim 2, wherein the outer layer is configured to be at least about 400 times more permeable to oxygen than it is to glucose.

4. An electrode assembly as defined in claim 2, wherein the outer layer is formed of polycarbonate.

5. An electrode assembly as defined in claim 2, wherein the outer layer has a thickness of about 6 microns.

6. An electrode assembly as defined in claim 2, wherein the pores in the outer layer contribute about 0.003 percent to about 0.015 percent of the outer layer'"'"'s total porosity.

7. An electrode assembly as defined in claim 1, wherein the pores of the outer layer have a substantially random distribution.

8. An electrode assembly as defined in claim 1, wherein the backing film of the inner layer is formed of polyester and the overlaying film of the inner layer is formed of polysulfone.

9. An electrode assembly as defined in claim 1, wherein the backing film and overlaying film of the inner layer have a combined thickness of about 15 microns.

10. An electrode assembly as defined in claim 1, wherein the immobilized glucose oxidase layer carries glucose oxidase and albumin, in prescribed relative proportions.

11. An electrode assembly as defined in claim 10, wherein the weight ratio of glucose oxidase:

albumin is about 85;

65.

12. An electrode assembly for use in assaying glucose in a solution, the electrode assembly comprising:

a sensor electrode; and

a membrane assembly overlaying the sensor electrode, the membrane assembly including

an outer, diffusion-barrier layer positioned to contact the solution, the outer layer having a uniform thickness and a distribution of pores of a specific density and a specific size,

an inner, interference-barrier layer contacting a face of the sensor electrode and including a relatively thick, porous backing film and a relatively thin, porous overlaying film that overlays the backing film, the two films together having a uniform thickness, and

an immobilized glucose oxidase layer interposed between the outer and inner layers,

wherein the outer layer is configured to allow glucose and oxygen to diffuse through it to reach the glucose oxidase layer, where the glucose and oxygen react to form reaction products that include hydrogen peroxide,

and wherein the inner layer is configured to have a permeability sufficient to pass hydrogen peroxide from the glucose oxidase layer to the face of the sensor electrode.

13. An electrode assembly as defined in claim 12, wherein the backing film of the inner layer is formed of polyester and the overlaying film of the inner layer is formed of polysulfone.

14. An electrode assembly as defined in claim 12, wherein the backing film and overlaying film of the inner layer have a combined thickness of about 15 microns.

15. An electrode assembly as defined in claim 12, wherein the pores in the outer layer have a size in the range of 0.0125 to 0.0200 microns.

16. An electrode assembly as defined in claim 12, wherein the immobilized glucose oxidase layer carries glucose oxidase and albumin, in prescribed relative proportions.

17. An electrode assembly as defined in claim 16, wherein the weight ratio of glucose oxidase:

albumin is about 85;

65.