IP Library Granted Patent US 8,592,617
Granted Patent B2
US 8,592,617 · App. 12/158,371 · Granted Nov 26, 2013

Redox mediators

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Quick Facts
Patent No.
US 8,592,617
App. No.
12/158,371
Granted
Nov 26, 2013
Kind
B2
Abstract

The present application is generally directed to ruthenium or osmium containing complexes and their use as redox mediators in electrochemical biosensors.

Claims (32)

1. A complex according to Formula I

[M(A) x (B) y ] m (X Z ) n   Formula I

wherein

M is ruthenium or osmium and has an oxidation state of 0, 1, 2, 3 or 4;

x, and n are independently an integer selected from 1 to 6; y is an integer selected from 1 to 5; m is an integer from −5 to +4 and z is an integer from −2 to +1;

A is a mono- or bidentate aromatic ligand containing 1 or 2 nitrogen atoms;

B is independently selected to be one or more ligands other than a heterocyclic nitrogen-containing ligand;

X comprises a combination of PF 6 − and CF 3 SO 3 − counterions;

wherein A is optionally substituted by 1 to 8 groups independently selected from the group consisting of substituted or unsubstituted alkyl, alkenyl, or aryl groups, —F, —Cl, —Br, —I, —NO 2 , —CN, —CO 2 H, —SO 3 H, —NHNH 2 , —SH, alkoxycarbonyl, alkylaminocarbonyl, dialkylaminocarbonyl, —OH, alkoxy, —NH 2 , alkylamino, dialkylamino, alkanoylamino, arylcarboxamido, hydrazino, alkylhydrazino, hydroxylamino, alkoxyamino, and alkylthio;

wherein the number of coordination atoms is 6.

2. A redox mediator comprising the complex as claimed in claim 1 .

3. The redox mediator as claimed in claim 2 wherein A is a monodentate ligand substituted by one or more CO 2 H groups, or a bidentate ligand optionally substituted by one or more CO 2 H groups.

4. The redox mediator as claimed in claim 2 wherein A is selected from the group consisting of nicotinic acid, isonicotinic acid, 2,2′ bipyridine, 2,2-bipyridyl-5,5′-dicarboxylic acid, 2,2-bipyridyl-4,4′-dicarboxylic acid, and 5-chloro-8-hydroxyquinoline.

5. The redox mediator as claimed in claim 2 wherein B is selected from the group consisting of amine ligands, CO, CN, halogen, acetylacetonate, 3-bromoacetylacetonate, oxalate, pyridine, and 5-chloro-8-hydroxyquinoline.

6. The redox mediator as claimed in claim 2 wherein the oxidation state of the metal is selected to be 3+.

7. The redox mediator as claimed in claim 2 wherein the ligands A and B are selected such that the overall charge on the complex is selected from the group consisting of +3, +2, +1, 0, −1, −2 and −3.

8. A complex as claimed in claim 1 wherein A is a monodentate ligand substituted by one or more CO 2 H groups, or a bidentate ligand optionally substituted by one or more CO 2 H groups wherein said one or more CO 2 H groups are each in a meta position relative to the co-ordinating heteroatom or heteroatoms.

9. A complex as claimed in claim 1 wherein A is selected from the group consisting of nicotinic acid, isonicotinic acid, 5-carboxynicotinic acid, 6-pyridyl-nicotinic acid, 2,2′-bipyridine-5,5′-bis-carboxylic acid, 2,2′-bipyridine-4,4′-bis-carboxylic acid, 2,2′-bipyridine, and 1,10-phenanthroline-3,9-bis-carboxylic acid.

10. A complex as claimed in claim 1 wherein B is selected from the group consisting of amine ligands; CO; CN; halogen, acetylacetonate, 3-bromoacetylacetonate, oxalate, and 5-chloro-8-hydroxyquinoline.

11. A complex as claimed in claim 1 wherein the ligands A and B are selected such that the overall charge on the complex is selected from the group consisting of +2, +1, 0, −1, −2 and −3.

12. A complex as claimed in claim 1 wherein said complex is [Ru III (NH 3 ) 5 (pyridine-3-COOH)](PF 6 ) 2 (CF 3 SO 3 ).

13. The redox mediator as claimed in claim 2 wherein said complex is [Ru III (NH 3 ) 5 (pyridine-3-COOH)](PF 6 ) 2 (CF 3 SO 3 ).

14. A complex according to Formula I

[M(A) x (B) y ] m (X Z ) n   Formula I

wherein

M is ruthenium or osmium and has an oxidation state of 0, 1, 2, 3 or 4;

x, and n are independently an integer selected from 1 to 6; y is an integer selected from 1 to 5; m is an integer from −5 to +4 and z is an integer from −2 to +1;

A is a mono- or bidentate aromatic ligand containing 1 or 2 nitrogen atoms;

B is independently selected to be one or more ligands other than a heterocyclic nitrogen-containing ligand;

X comprises a combination of two PF 6 − counterions and one CF 3 SO 3 − counterion;

wherein A is optionally substituted by 1 to 8 groups independently selected from the group consisting of substituted or unsubstituted alkyl, alkenyl, or aryl groups, —F, —Cl, —Br, —I, —NO 2 , —CN, —CO 2 H, —SO 3 H, —NHNH 2 , —SH, alkoxycarbonyl, alkylaminocarbonyl, dialkylaminocarbonyl, —OH, alkoxy, —NH 2 , alkylamino, dialkylamino, alkanoylamino, arylcarboxamido, hydrazino, alkylhydrazino, hydroxylamino, alkoxyamino, and alkylthio;

wherein the number of coordination atoms is 6.

Assignments (5)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 23, 2015
From: ROCHE DIAGNOSTICS OPERATIONS, INC.
To: ROCHE DIABETES CARE, INC.
Reel/Frame 036008/0670 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Apr 1, 2011
From: F. HOFFMANN-LA ROCHE AG A/K/A F. HOFFMAN-LA ROCHE LTD; F. HOFFMANN-LA ROCHE LTD
To: ROCHE DIAGNOSTICS OPERATIONS, INC.
Reel/Frame 026110/0749 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Mar 16, 2011
From: OXFORD BIOSENSORS LIMITED
To: F. HOFFMAN-LA ROCHE LTD A/K/A F. HOFFMANN-LA ROCHE AG AND HOFFMANN-LA ROCHE LTD
Reel/Frame 025993/0549 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 9, 2010
From: F. HOFFMANN-LA ROCHE AG
To: ROCHE DIAGNOSTICS OPERATIONS, INC.
Reel/Frame 024510/0706 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Oct 23, 2008
From: HILL, HUGH OLIVER ALLEN; NEWMAN, CHRISTOPHER PAUL; WONG, LUET LOK; LAU, TAI-CHU
To: OXFORD BIOSENSORS LTD.
Reel/Frame 021724/0001 →