Nitrogen doped carbon electrodes

• US 6,423,193 B1
• Filed: 08/30/1999
• Issued: 07/23/2002
• Est. Priority Date: 08/30/1999
• Status: Expired due to Fees

• Current Assignee: Case Western Reserve University
• Original Assignee: Case Western Reserve University
• Inventors: Kalish, Rafi, Miller, Barry, Shi, Xu
• Primary Examiner(s): Bell, Bruce F.
• Assistant Examiner(s): Nicolas, Wesley A.
• Application Number:
  US09/385,233
• Time in Patent Office: 1,058 Days
• Field of Search: 204/242, 204/290.01, 204/290.15, 204/294
• US Class Current: 204/242
• CPC Class Codes: C02F 1/46109 Electrodes
• CPC Class Codes: C23C 14/0605 Carbon
• CPC Class Codes: C25B 1/26 Chlorine; Compounds thereof by simultaneous production of alkali metal hydroxides and chlorine, oxyacids or salts of chlorine C25B1/34
• CPC Class Codes: C25B 11/073 characterised by the electrocatalyst material
• CPC Class Codes: G01N 27/308 at least partially made of carbon

Abstract

An electrode (22) formed from a layer (24) of tetrahedral carbon doped with nitrogen (taC:N) has both electroanalytical and electrosynthetic applications. The electrode includes a substrate material (26), such as a silicon wafer, for supporting the taC:N layer. The electrode has good durability under a high anodic potential and high selectivity for conversion of chloride ions to chlorine, and for other electron transfer reactions. The electrode is readily formed at ambient temperatures by vacuum deposition of carbon and nitrogen ions on to the substrate. Masking of the substrate during deposition allows the formation of microelectrode arrays.

Claims

1. An electrochemical system comprising:

an electrode at which an oxidation or reduction reaction takes place including;

a substrate, and

a layer of a material deposited on the substrate, the layer consisting essentially of carbon and nitrogen, the layer having a nitrogen concentration of at least about 5 atomic %;

an electrolyte in contact with the electrode; and

a counter electrode.

2. The system of claim 1, wherein the electrode comprises an anode.

3. The system of claim 1, wherein the substrate material is a silicon wafer.

4. The system of claim 1, wherein the layer is from about 10 nanometers to about 70 nanometers in thickness.

5. The system of claim 4, wherein the layer is from 30-50 nanometers in thickness.

8. The system of claim 1, wherein the layer has a nitrogen concentration of 8-12 atomic %.

9. The system of claim 2, further including:

a cathode, and wherein the system is capable of being used for one of detection and synthesis of at least one of the group consisting of;

i) a reaction involving a Cl⁻

/Cl₂ couple,

ii) a reaction involving a couple selected from the group consisting of a quinone/hydroquinone couple, other catechol derivatives, and combinations thereof;

iii) a reaction involving an outer sphere couple;

iv) a reaction involving one of hydrogen evolution and oxygen evolution.

11. The system of claim 1, wherein the layer of material is in the form of an array on the substrate.

6. An electrochemical system comprising:

an electrode including;

a substrate, and

a layer of a material on the substrate, the layer being primarily nitrogen-incorporated tetrahedral carbon;

an electrolyte in contact with the surface of the nitrogen-incorporated tetrahedral carbon layer; and

a counter electrode.

7. The system of claim 6, wherein the layer has a nitrogen concentration of from about 5-15 atomic %.

10. A chlorine generation system comprising:

an electrode including;

a substrate, and

a layer of a material on the substrate, the layer consisting essentially of carbon and nitrogen, the layer having a nitrogen concentration of from about 5-15 atomic %;

an electrolyte in contact with the layer, the electrolyte including chloride ions, chlorine being generated at the electrode; and

a counter electrode.

12. An electrochemical system comprising:

an electrode including;

a substrate, and

a layer of a material on the substrate, the layer consisting of carbon and nitrogen, the carbon having an atomic ratio of sp³/sp² of from about 70/30 to about 85/15;

an electrolyte in electrical contact with the layer; and

a counter electrode.