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US4418148A Expired / Lapsed US ⏱️ 0.0 years remaining

Multilayer enzyme electrode membrane

Assignee: Bayer Corp
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Filing: 1981-11-05
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Granted: 1983-11-29
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Expires: 2001-11-05
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Abstract

Abstract A contiguous multilayer membrane for use with an electrochemical sensor is prepared comprising a first relatively nonporous dense polymer layer, a second polymer layer less dense and more porous than the first layer, a third layer containing an enzyme and a fourth polymer layer less dense and more porous than the first layer. The polymer is preferably cellulose acetate and the second and fourth layers are prepared with a solvent and nonsolvent for the polymer. The membrane may contain multiple enzyme layers separated by a polymer layer. The multilayer membrane provides advantages of higher substrate conversion, homogeneous distribution of enzyme and/or minimized interference with analyte diffusion.

Inventors

  • 👤 Bruce J. Oberhardt

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-10-25 14:43
CPC Classifications
C; C12; C12Q; C12Q1/00; C12Q1/001; C12Q1/002; G; G01; G01N; G01N27/00; G01N27/26; G01N27/28; G01N27/30; G01N27/327; G01N27/3271

Claims Analysis

Total Claims: 17
Claim 1
Independent Claim 273 words
A method of making a contiguous multilayer membrane of about 40 to about 100 microns in overall thickness suitable for use with an electrochemical sensor in the measurement of an unknown which comprises: providing as a first layer, a polymer dissolved in an inert organic solvent and casting said polymer in solution onto an inert support surface which is unreactive with said polymer and does not form a bond to said polymer; permitting said solution to form a film and thereby obtaining a first relatively nonporous dense polymer layer of about 2 to about 5 microns in thickness; providing as a second layer, a composition comprising a polymer dissolved in an inert organic solvent, mixing said polymer dissolved in solvent with a nonsolvent for said polymer to obtain a dispersion and thereafter casting said dispersion onto said first layer and thereafter permitting said second layer to dry to form a porous polymer layer of about 2 to about 20 microns in thickness and less dense and more porous than the first layer; providing a third layer comprising an enzyme solution or suspension and depositing said third layer onto the exposed surface of the second layer; providing as a fourth layer, a composition comprising a polymer dissolved in an inert organic solvent, mixing said polymer dissolved in solvent with a nonsolvent for said polymer to obtain a dispersion and thereafter casing said dispersion onto the exposed surface of the third layer to provide a fourth porous polymer layer of about 2 to about 20 microns in thickness and less dense and more porous than the first layer; and thereby forming said contiguous multilayer membrane.
Claim 2
Independent Claim 273 words
A method of making a contiguous multilayer membrane of about 40 to about 100 microns in overall thickness suitable for use with an electrochemical sensor in the measurement of an unknown which comprises: providing as a first layer, a polymer dissolved in an inert organic solvent and casting said polymer in solution onto an inert support surface which is unreactive with said polymer and does not form a bond to said polymer; permitting said solution to form a film and thereby obtaining a first relatively nonporous dense polymer layer of about 2 to about 5 microns in thickness; providing as a second layer, a composition comprising a polymer dissolved in an inert organic solvent, mixing said polymer dissolved in solvent with a nonsolvent for said polymer to obtain a dispersion and thereafter casting said dispersion onto said first layer and thereafter permitting said second layer to dry to form a porous polymer layer of about 2 to about 20 microns in thickness and less dense and more porous than the first layer; providing a third layer comprising an enzyme solution or suspension and depositing said third layer onto the exposed surface of the second layer; providing as a fourth layer, a composition comprising a polymer dissolved in an inert organic solvent, mixing said polymer dissolved in solvent with a nonsolvent for said polymer to obtain a dispersion and thereafter casing said dispersion onto the exposed surface of the third layer to provide a fourth porous polymer layer of about 2 to about 20 microns in thickness and less dense and more porous than the first layer; and thereby forming said contiguous multilayer membrane.
Claim 3
Dependent Claim 23 words
The method of claim 1 wherein each of said layers is deposited one or more times in sequence to obtain a multilayer membrane.
Claim 4
Dependent Claim 17 words
The method of claim 1 wherein the polymer is cellulose acetate or a copolymer of cellulose acetate.
Claim 5
Dependent Claim 13 words
The method of claim 1 wherein the inert organic solvent is a ketone.
Claim 6
Dependent Claim 16 words
The method of claim 1 wherein said second layer further includes an enzyme homogeneously dispersed therein.
Claim 7
Dependent Claim 16 words
The method of claim 1 wherein said second layer further contains an enzyme protectively encapsulated therein.
Claim 8
Dependent Claim 34 words
The method of claim 1 wherein said second layer is a phase inversion layer containing pores formed by dissolving said polymer in a solvent mixture, including a solvent and a nonsolvent for said polymer.
Claim 9
Dependent Claim 11 words
The method of claim 1 wherein the enzyme is glucose oxidase.
Claim 10
Independent Claim 244 words
A method of making a contiguous multilayer membrane of about 40 to about 100 microns in overall thickness suitable for use with an electrochemical sensor in the measurement of an unknown which comprises: (a) providing a first cellulose acetate polymer dissolved in an inert organic solvent; (b) casting said first polymer in solution onto an inert support surface which in unreactive with said cellulose acetate and does not form a bond to said cellulose acetate; (c) permitting said first polymer in solution to form a film and thereby obtain a first relatively nonporous dense layer of cellulose acetate of about 2 to about 5 microns in thickness; (d) providing a second cellulose acetate polymer dissolved in an inert organic solvent mixing said second polymer with a nonsolvent for said polymer to form a dispersion thereof; (e) casting said second cellulose acetate polymer dispersion onto said first layer of cellulose acetate and permitting said cellulose acetate polymer to form a porous second cellulose acetate layer of about 2 to about 20 microns in thickness and less dense and more porous than the first layer; (f) providing an aqueous solution or suspension of an enzyme and depositing said enzyme in a layer onto the surface of said second polymer; and (g) repeating (d), (e) and (f) at least once to deposit at least one additional said second cellulose acetate layer and at least one additional enzyme layer; thereby forming said contiguous multilayer cellulose acetate polymer membrane.
Claim 11
Independent Claim 244 words
A method of making a contiguous multilayer membrane of about 40 to about 100 microns in overall thickness suitable for use with an electrochemical sensor in the measurement of an unknown which comprises: (a) providing a first cellulose acetate polymer dissolved in an inert organic solvent; (b) casting said first polymer in solution onto an inert support surface which in unreactive with said cellulose acetate and does not form a bond to said cellulose acetate; (c) permitting said first polymer in solution to form a film and thereby obtain a first relatively nonporous dense layer of cellulose acetate of about 2 to about 5 microns in thickness; (d) providing a second cellulose acetate polymer dissolved in an inert organic solvent mixing said second polymer with a nonsolvent for said polymer to form a dispersion thereof; (e) casting said second cellulose acetate polymer dispersion onto said first layer of cellulose acetate and permitting said cellulose acetate polymer to form a porous second cellulose acetate layer of about 2 to about 20 microns in thickness and less dense and more porous than the first layer; (f) providing an aqueous solution or suspension of an enzyme and depositing said enzyme in a layer onto the surface of said second polymer; and (g) repeating (d), (e) and (f) at least once to deposit at least one additional said second cellulose acetate layer and at least one additional enzyme layer; thereby forming said contiguous multilayer cellulose acetate polymer membrane.
Claim 12
Dependent Claim 22 words
The method of claim 9 wherein the inert organic solvent used with said first and second cellulose acetate polymer is the same.
Claim 13
Dependent Claim 13 words
The method of claim 10 wherein the inert organic solvent is a ketone.
Claim 14
Dependent Claim 12 words
The method of claim 10 wherein the inert organic solvent is acetone.
Claim 15
Dependent Claim 21 words
The method of claim 9 wherein the enzyme is glucose oxidase and is present in a mixture of water and ethanol.
Claim 16
Dependent Claim 46 words
In a polarographic cell structure for use in electrochemical analysis of an unknown comprising an electrically insulating receptacle an electrode means mounted in said receptacle, and a membrane means, the improvement which comprises utilizing the multilayer membrane produced by the method of claim 1 or 9.
Claim 17
Dependent Claim 12 words
A multilayer membrane produced by the method of claim 1 or 9.

References Cited (Backward Citations)

US3715277A Cited
US3947325A Cited
US4004980A Cited
US3979274A Cited
US4092233A Cited
US4090022A Cited

USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1986-11-28 1987-05-30 1987-11-29 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1990-11-28 1991-05-30 1991-11-29 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 1994-11-28 1995-05-30 1995-11-29 $7700.00 Window Closed / Lapsed

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