Method for producing a device for electrochemical detection of molecules by way of redox cycling, device therefor and the use thereof

Patent metadata

Field	Value
Publication number	US-10739298-B2
Application number	US-201615567752-A
Country	US
Kind code	B2
Filing date	Apr 9, 2016
Priority date	May 8, 2015
Publication date	Aug 11, 2020
Grant date	Aug 11, 2020

Abstract

The invention relates to a method for producing a device for the electrochemical detection of molecules by way of redox cycling, to a device therefor, and to the use thereof. A porous dielectric layer is present between two electrode layers, which is able to receive redox-active molecules and may be biofunctionalized. The individual layers are preferably applied by way of an ink jet printing method.

First claim

The invention claimed is:

1. A device for electrochemical detection of redox-active molecules by way of redox cycling, comprising:
a first electrically conductive electrode disposed on a substrate,
a passivation layer covering the first electrically conductive electrode at a surface opposite the substrate, the passivation layer having a through-opening;
a dielectric layer permeable by said redox-active molecules disposed in the through opening on the first electrically conductive electrode, and
a second electrically conductive electrode, having no electrical contact with the first electrode, disposed on the passivation layer and covering the dielectric layer, the second electrically conductive electrode having an access for or being permeable to said redox-active molecules,
wherein redox cycling of redox-active molecules permeating the dielectric layer takes place at least at portions of the first electrically conductive electrode and second electrically conductive electrode that are in contact with the dielectric layer,
wherein the dielectric layer is a reservoir for the redox-active molecules present in a solution, a pathway for the redox-active molecules to enter the reservoir being comprised by the second electrically conductive electrode through which said redox-active molecules migrate from an exposed surface of the second electrically conductive electrode through the second electrically conductive electrode into the dielectric layer,
wherein at least one of the first electrically conductive electrode and second electrically conductive electrode comprises printed electrically conductive particles, and wherein the passivation layer comprises printed electrically insulating particles, and
wherein the first electrically conductive electrode and the second electrically conductive electrode of the device are working electrodes in a potentiostat, which are in contact with either one or both of a reference electrode and a counter electrode.

2. A device according to claim 1 , wherein the dielectric layer has a surface area between at least 1 μm 2 and no more than 1 cm 2 .

3. The device according to claim 1 operated by a method comprising:
introducing said solution comprising redox-active molecules into the dielectric layer, and
applying a voltage to the electrodes so causing alternating reduction and oxidation of the redox-active molecules at the first and second electrically conductive electrodes.

4. The device according to claim 3 , wherein said introducing comprises migrating redox-active molecules in solution through pores of the second electrically conductive layer into the dielectric layer.

5. The device according to claim 4 , wherein the first electrode has a pore size that is 0 to 50 nm in diameter, the dielectric layer has a pore size that is 10 to 1000 nm in diameter, and the second electrode has a pore size that is 100 to 10000 nm in diameter.

6. The device according to claim 1 ,
wherein the first electrode comprises conductive particles made of gold, platinum, silver, carbon poly(3,4-ethylenedioxythiophene)polystyrene sulfonate or polyaniline; and
wherein the second electrode comprises conductive particles made of gold, platinum, silver, carbon, poly(3,4-ethylenedioxythiophene)polystyrene sulfonate or polyaniline.

7. The device according to claim 1 , wherein the dielectric layer comprises insulating particles, to which enzymes, antibodies, receptors or other biomolecules can bind.

8. A method for electrochemically detecting redox-active molecules by way of redox cycling comprising:
providing a device comprising:
a first electrically conductive electrode disposed on a substrate;
a passivation layer covering the first electrically conductive electrode at a surface opposite the substrate, the passivation layer having a through-opening;
a dielectric layer permeable by said redox-active molecules disposed in the through opening on the first electrically conductive electrode; and
a second electrically conductive electrode, having no electrical contact with the first electrode, disposed on the passivation layer and covering the dielectric layer, the second electrically conductive electrode having an access for or being permeable to said redox-active molecules;
wherein redox cycling of redox-active molecules permeating the dielectric layer takes place at least at portions of the first electrically conductive electrode and second electrically conductive electrode that are in contact with the dielectric layer;
wherein the dielectric layer is a reservoir for the redox-active molecules present in a solution, a pathway for the redox-active molecules to enter the reservoir being comprised by the second electrically conductive electrode through which said redox-active molecules migrate from an exposed surface of the second electrically conductive electrode through the second electrically conductive electrode into the dielectric layer;
wherein at least one of the first electrically conductive electrode and second electrically conductive electrode comprises printed electrically conductive particles;
wherein the passivation layer comprises printed electrically insulating particles; and

wherein the method comprises:
introducing said solution comprising redox-active molecules into the dielectric layer, and
applying a voltage to the electrodes so causing alternating reduction and oxidation of the redox-active molecules at the first and second electrically conductive electrodes.

9. The method according to claim 8 , wherein said introducing comprises migrating redox-active molecules in solution through pores of the second electrically conductive layer into the dielectric layer.

10. The method according to claim 9 , wherein the first electrode has a pore size that is 0 to 50 nm in diameter, the dielectric layer has a pore size that is 10 to 1000 nm in diameter, and the second electrode has a pore size that is 100 to 10000 nm in diameter.

11. The device method according to claim 8 ,
wherein the first electrode comprises conductive particles made of gold, platinum, silver, carbon, poly(3,4-ethylenedioxythiophene)polystyrene sulfonate or polyaniline; and
wherein the second electrode comprises conductive particles made of gold, platinum, silver, carbon poly(3,4-ethylenedioxythiophene)polystyrene sulfonate or polyaniline.

12. The method according to claim 8 , wherein the dielectric layer comprises insulating particles, to which enzymes, antibodies, receptors or other biomolecules can bind.

13. A device for electrochemical detection of redox-active molecules by way of redox cycling, comprising:
a first electrically conductive electrode disposed on a substrate;
a passivation layer covering the first electrically conductive electrode at a surface opposite the substrate, the passivation layer having a through-opening;
a dielectric layer permeable by said redox-active molecules disposed in the through opening on the first electrically conductive electrode; and
a second electrically conductive electrode, having no electrical contact with the first electrode, disposed on the passivation layer and covering the dielectric layer, the second electrically conductive electrode having an access for or being permeable to said redox-active molecules;
wherein redox cycling of redox-active molecules permeating the dielectric layer takes place at least at portions of the first electrically conductive electrode and second electrically conductive electrode that are in contact with the dielectric layer;
wherein the dielectric layer is a reservoir for the redox-active molecules present in a solution, a pathway for the redox-active molecules to enter the reservo

Assignees

• Forschungszentrum Juelich Gmbh

Inventors

• Yakushenko Alexey
• Wolfrum Bernhard
• Adly Hassan Nouran Yehia
• Offenhausser Andreas

Classifications

• G01N27/3278

  involving nanosized elements, e.g. nanogaps or nanoparticles (nanopores G01N33/48721; magnetic beads G01N27/745) · CPC title

• H05K1/00

  Printed circuits · CPC title

• C12Q1/68

  involving nucleic acids · CPC title

• C12Q1/001

  Enzyme electrodes · CPC title

• C09D11/54

  Inks based on two liquids, one liquid being the ink, the other liquid being a reaction solution, a fixer or a treatment solution for the ink · CPC title