Ionic hydrophilic high molecular weight redox polymers for use in enzymatic electrochemical-based sensors

• US 7,351,770 B2
• Filed: 09/30/2004
• Issued: 04/01/2008
• Est. Priority Date: 09/30/2004
• Status: Active Grant

• Current Assignee: Cilag Gmbh International (Johnson & Johnson)
• Original Assignee: Lifescan Incorporated (Duv Holding Corporation)
• Inventors: Lillie, Geoffrey, Rodgers, James Iain, Cardosi, Marco Fabio, Liu, Zuifang
• Primary Examiner(s): Gulakowski; Randy
• Assistant Examiner(s): BERNSHTEYN, MICHAEL
• Application Number:
  US10/957,441
• Publication Number:
  US 20060069211A1
• Time in Patent Office: 1,279 Days
• Field of Search: 526/241, 525/279, 525/283, 525/297, 525/298, 435/4
• US Class Current: 525/283
• CPC Class Codes: C12Q 1/004 mediator-assisted

Abstract

Ionic hydrophilic high molecular weight redox polymers for use in enzymatic electrochemical-based sensors include a hydrophilic polymer (such as a hydrophilic polymer backbone) with ionic portions (e.g., cationic monomers incorporated in the hydrophilic polymer backbone) and a plurality of attached redox mediators. The redox mediators can be, for example, covalently attached to the hydrophilic polymer in a pendant manner. An exemplary cationic hydrophilic high molecular weight redox polymer is synthesized by co-polymerization of a hydrophilic acrylamide monomer, [2-(acryloyloxy)ethyl]trimethyl ammonium chloride and vinyl ferrocene.

Claims

1. An ionic hydrophilic high molecular weight redox polymer for use in enzymatic electrochemical-based sensors employing a charged redox enzyme, the ionic hydrophilic high molecular weight redox polymer comprising:

a hydrophilic polymer backbone that includes ionic portions; and

a plurality of attached redox mediators covalently attached to the hydrophilic polymer backbone in a flexible pendant manner such that the redox mediators can segmentally diffuse between the charged redox enzyme and an electrode of the enzymatic electrochemical-based sensor,

wherein the molecular weight of the ionic hydrophilic high molecular weight polymer is greater than 16 Kg/mol as a weight average molecular weight, and

wherein an ionic charge of the ionic portions is predetermined to result in an affinity between the ionic portions and the charged redox enzyme of an enzymatic electrochemical-based sensor and that minimizes leaching of the redox enzyme and fosters activity between the redox enzyme and redox mediator.

2. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein the hydrophilic polymer backbone is formed at least partially from a hydrophilic acrylamide monomer (AAM).

3. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein the hydrophilic polymer backbone is formed at least partially from at least one of hydrophilic monomers with an acrylate polymerizable group and hydrophilic monomers with a vinyl polymerizable group.

4. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein the ionic portions are cationic portions.

5. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein the ionic portion is formed of [2-(acryloyloxy)ethyl]trimethyl ammonium chloride (AETMAC).

6. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein the ionic portion is formed of at least one of a quaternary ammonium cationic monomer and a tertiary ammonium cationic monomer.

7. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein the redox mediator is ferrocene (Fc).

8. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein:

the hydrophilic polymer is a hydrophilic polymer backbone formed at least partially from hydrophilic acrylamide monomer (AAM);

the ionic portion is formed at least partially from [2-(acryloyloxy)ethyl]trimethyl ammonium chloride (AETMAC) incorporated in the hydrophilic polymer backbone; and

the redox mediator is ferrocene (Fc) covalently attached to the hydrophilic polymer backbone in the form of vinyl ferrocene (VFc).

9. The ionic hydrophilic high molecular weight redox polymer of claim 8, wherein the molecular weight is approximately 110 Kg/mol as a weight average molecular weight.

10. The ionic hydrophilic high molecular weight redox polymer of claim 8, wherein the relative molar portion of AAM is in the range of about 84 to about 99, the relative molar portion of VFc is in the range of about 1 to about 6 and the relative molar portion of AETMAC is in the range of from nearly zero to about 10.

11. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein the ionic portion is formed of a carboxylic acid monomer.

12. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein the ionic hydrophilic high molecular weight redox polymer is a cationic hydrophilic high molecular weight redox polymer.

13. The ionic hydrophilic high molecular weight redox polymer of claim 1, wherein the ionic hydrophilic high molecular weight redox polymer is an anionic hydrophilic high molecular weight redox polymer.