# US 12,595,575 B2 · Electrochemical oxidation of methane towards methanol on mixed metal oxides

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- Number: US 12,595,575 B2
- Document ID: US12595575B2
- Status: Granted
- Kind: B2
- Application number: 18/273,381
- Filed: 2022-01-27
- Published: 2024-09-19
- Granted: 2026-04-07
- Earliest claimed: 2021-01-27
- Assignees: The Board of Trustees of the University of Illinois
- Applicants: The Board of Trustees of the University of Illinois
- Inventors: Meenesh R. Singh; Aditya Prajapati
- Web page: https://patentgrep.com/patent/US12595575B2

## CPC

- C25B 3/01: Products
- C25B 3/07: Oxygen containing compounds
- C25B 3/23: Oxidation (halogenation C25B3/27)
- C25B 9/15: Flow-through cells
- C25B 9/19: with diaphragms
- C25B 9/21: two or more diaphragms
- C25B 11/032: Gas diffusion electrodes
- C25B 11/054: Electrodes comprising electrocatalysts supported on a carrier
- C25B 11/073: characterised by the electrocatalyst material
- C25B 11/089: Alloys
- Y02E 60/50: Fuel cells
- C25B: ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR (anodic or cathodic protection C23F13/00; single-crystal growth C30B)
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

An electrochemical cell for conversion of methane to methanol includes a bimetallic catalyst having alternating regions of first and second metals thereby providing interfaces at which methane is converted to methanol or formate.

## Claims

### Claim 1

An electrochemical cell for conversion of methane to methanol and/or formate, comprising:
an anode compartment comprising an anode, the anode comprising or having dispose thereon a bimetallic catalyst, the bimetallic catalyst comprising a patterned arrangement of a first metal region and a second metal region disposed on a support, wherein methane is converted to methanol and/or formate when methane contacts the bimetallic catalysts;
a gas inlet in fluid communication with the anode compartment for introduction of methane into the anode compartment and arranged such that methane flows in contact with and/or through the bimetallic catalyst;
a cathode compartment comprising a cathode;
a membrane separating the anode compartment and the cathode compartment;
one or more electrolytes disposed in and/or flowed through the anode and cathode compartments; and
a product outlet in fluid communication with the anode compartment for collection of the methanol and/or formate after conversion;
wherein in the patterned arrangement the first and second metal regions are arranged in a uniform alternating fashion across the catalyst with an interface defined between adjacent ones of the first and second metal regions, wherein each of the first metal regions comprises one or more of Cu, Pd, Ag, and Ni, and each of the second metal regions comprises one or more of Ti, Ir, Ru, Sn, Pb, and Pt.

### Claim 2 (depends on 1)

The electrochemical cell of claim 1, wherein the electrolyte comprises Cl ions.

### Claim 3 (depends on 1)

The electrochemical cell of claim 1, wherein each of the first and second metal regions is square-shaped, triangular, hexagonal, and/or circular.

### Claim 4 (depends on 1)

The electrochemical cell of claim 1, wherein each of the first metal regions is copper and each of the second metal regions is titanium.

### Claim 5 (depends on 1)

The electrochemical cell of claim 1, wherein the cell is a flow-through cell and comprises a catholyte tank in fluid communication with the cathode compartment to circulate electrolyte through the cathode compartment and an anolyte tank in fluid communication with the anode compartment to circulate electrolyte through the anode compartment.

### Claim 6 (depends on 1)

The electrochemical cell of claim 1, wherein the membrane is an ion exchange membrane.

### Claim 7 (depends on 1)

The electrochemical cell of claim 1, wherein the anode comprises a sectioned anode having two or more sections each comprising the bimetallic catalyst.

### Claim 8 (depends on 1)

The electrochemical cell of claim 1, wherein the anode compartment surrounds the cathode compartments and the membrane disposed between the anode and cathode compartments and wherein the anode comprises a sectioned anode having two more sections each comprising the bimetallic catalyst.

### Claim 9 (depends on 8)

The electrochemical cell of claim 8, wherein the membrane is a semi-permeable membrane.

### Claim 10 (depends on 1)

The electrochemical cell of claim 1, wherein the support is a gas diffusion layer.

### Claim 11 (depends on 1)

The electrochemical cell of claim 1, wherein the cell has a faradaic efficiency of methanol production of about 6% to about 20%.

### Claim 12 (depends on 1)

The electrochemical cell of claim 1, wherein each of the first metal regions comprises copper and each of the second metal regions comprises one or more of Ti, Ir, Pb, and Pt.

### Claim 13 (depends on 1)

A process for converting methane to methanol and/or formate using the electrochemical cell of claim 1, comprising:
flowing methane and/or a methane containing source in contact with the bimetallic catalyst, wherein upon contact with the bimetallic catalyst the methane is converted to methanol and/or formate at the interface between the first and second metal regions.

### Claim 14 (depends on 13)

The process of claim 13, wherein the process has a faradic efficiency of methanol production of about 6% to about 20% and/or wherein the process has a faradic efficiency of methane oxidation reaction of about 10% to about 80%.

### Claim 15 (depends on 13)

The process of claim 13, comprising applying a potential of about 1.5V to about 3V while flowing the methane in contact with the bimetallic catalyst.

### Claim 16 (depends on 13)

The process of claim 13, comprising performing the process at room temperature.

### Claim 17 (depends on 13)

The process of claim 13, wherein the methane containing source is biogas, natural gas, and/or mining gas.
