# US 10,309,020 B2 · Electrolytic cell for the production of ammonia

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- Number: US 10,309,020 B2
- Document ID: US10309020B2
- Status: Granted
- Kind: B2
- Application number: 14/905,510
- Filed: 2014-07-18
- Published: 2016-07-07
- Granted: 2019-06-04
- Earliest claimed: 2013-07-18
- Assignees: Technische Universiteit Delft
- Applicants: Technische Universiteit Delft
- Inventors: Fokko Marten Mulder
- Web page: https://patentgrep.com/patent/US10309020B2

## CPC

- C25B 1/27: Ammonia
- C25B 9/17: Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
- C25B 1/00: Electrolytic production of inorganic compounds or non-metals
- C25B 9/19: with diaphragms
- C25B 9/23: comprising ion-exchange membranes in or on which electrode material is embedded
- C25B 11/02: characterised by shape or form
- C25B 11/031: Porous electrodes
- C25B 11/032: Gas diffusion electrodes
- C25B 11/04: characterised by the material
- C25B 11/051: Electrodes formed of electrocatalysts on a substrate or carrier
- C25B 11/052: Electrodes comprising one or more electrocatalytic coatings on a substrate
- C25B 11/075: consisting of a single catalytic element or catalytic compound
- C25B 11/077: the compound being a non-noble metal oxide
- C25B 11/081: the element being a noble metal
- C25B 11/089: Alloys
- H01M 8/222: {Fuel cells in which the fuel is based on compounds containing nitrogen, e.g. hydrazine, ammonia}
- Y02E 60/50: Fuel cells
- Y02P 70/50: Manufacturing or production processes characterised by the final manufactured product
- 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)
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

The invention provides an electrolytic cell 10 for the production of ammonia (NH3), comprising an electrolytic cell unit 100 comprising a first electrode 110, a second electrode 120, and an electrolyte 133, further a voltage generator 210, a supply 220 of a dinitrogen comprising fluid 221, and a supply 230 of a water comprising fluid 231. The electrolyte is configured to allow transport of protons. The first electrode is permeable for protons, wherein the first electrode is at first side in contact with the electrolyte and at second side is in fluid contact with the supply of the dinitrogen comprising fluid. The second electrode is permeable for protons but impermeable to O2 and H2O. The second electrode is at first side also in contact with the electrolyte, and at second side in fluid contact with the supply of the water comprising fluid. The ammonia can be produced and stored in liquid form.

## Claims

### Claim 1

An electrolytic cell for the production of ammonia (NH3) from N2 and H2O, the electrolytic cell comprising (i) an electrolytic cell unit comprising a first electrode, a second electrode, and an electrolyte, (ii) a voltage generator, (iii) a supply of a dinitrogen (N2) comprising fluid, and (iv) a supply of a water comprising fluid, wherein the voltage generator is configured to apply a negative potential to the first electrode and a positive potential to the second electrode, wherein the electrolyte is configured to allow transport of protons, wherein the first electrode is permeable for protons and non-permeable for O2 and H2O, wherein the first electrode is at first side in contact with the electrolyte and at second side is in fluid contact with the supply of the dinitrogen comprising fluid, and wherein the second electrode is permeable for protons, and non-permeable for O2, or H2O, wherein the second electrode is at first side also in contact with the electrolyte, and at second side in fluid contact with the supply of the water comprising fluid, and wherein the electrolyte is contained in a compartment between the first side of the first electrode and the first side of the second electrode.

### Claim 2 (depends on 1)

The electrolytic cell of claim 1, wherein the first electrode comprises a metal or an alloy of one or more of Ni and Fe, or Ni, Fe, Mn, Mo, W, Cu, V, Ti, Ta, Nb, Zr, Hf, and wherein the second electrode comprises nickel metal or an alloy of nickel.

### Claim 3 (depends on 2)

The electrolytic cell of claim 2, wherein the second electrode comprises one or more of Ni, Fe, Mn, Mo, Ru, W, Cu, V, Ti, Ta, Nb, Zr, Hf, Pt and Pd.

### Claim 4 (depends on 1)

The electrolytic cell of claim 1, wherein the first electrode comprises one or more of a nickel metal foil and an iron metal foil, and wherein the second electrode comprises a nickel metal foil.

### Claim 5 (depends on 1)

The electrolytic cell of claim 1, wherein the electrolyte comprises an anhydrous proton transporting ionic liquid.

### Claim 6 (depends on 1)

The electrolytic cell of claim 1, wherein the first electrode is permeable to hydrogen gas and wherein the second electrode is non-permeable for oxygen (O2), dinitrogen and water.

### Claim 7 (depends on 1)

The electrolytic cell of claim 1, wherein the first electrode further comprises a dinitrogen binding catalyst and wherein the second electrode further comprises an oxygen evolution catalyst.

### Claim 8 (depends on 1)

The electrolytic cell of claim 1, wherein the second electrode has a permeability at 25° C. for oxygen of less than 0.001 Barrer, for water of less than 0.001 Barrer and for dinitrogen less than 0.001 Barrer.

### Claim 9 (depends on 8)

The system of claim 8, further comprising a storage facility configured to store ammonia and/or a combustion configured to combust ammonia from the storage facility and to generate one or more of electricity and thermal energy.

### Claim 10 (depends on 1)

A system comprising the electrolytic cell of claim 1 and a pressure device configured to provide the dinitrogen gas to the electrolytic cell at a pressure above ambient pressure, and configured to retrieve liquid ammonia from the electrolytic cell.

### Claim 11

An electrolytic cell unit comprising a first electrode, a second electrode, and an electrolyte, wherein the electrolyte is configured to allow transport of protons, wherein the first electrode is permeable for hydrogen and non-permeable for O2 and H2O, wherein the first electrode is at first side in contact with the electrolyte, wherein the second electrode is permeable for protons, and wherein the second electrode is at first side also in contact with the electrolyte.

### Claim 12 (depends on 11)

The electrolytic cell unit of claim 11, wherein the first electrode comprises one or more of Ni and Fe and wherein the second electrode comprises nickel metal or an alloy of nickel.

### Claim 13 (depends on 12)

The electrolytic cell unit of claim 12, wherein the first electrode comprises a metal or an alloy of one or more of Ni and Fe.

### Claim 14 (depends on 11)

A process for the production of ammonia comprising feeding a dinitrogen comprising fluid to the first electrode of the electrolytic cell unit of claim 11 and a water and KOH comprising fluid to the second electrode the electrolytic cell unit while applying a voltage difference in the range of 1.16 V up to 3.6V.

### Claim 15 (depends on 14)

The process of claim 14, wherein the dinitrogen comprising fluid at the first electrode is maintained at a pressure of at least 5 bar, and wherein the dinitrogen comprising fluid comprises at least 75 vol. % N2.

### Claim 16 (depends on 14)

The process of claim 14, wherein the ammonia at the first electrode is maintained at a partial pressure of at least 10 bar and at a temperature between 20 and 85° C.

### Claim 17 (depends on 14)

The process of claim 14, wherein the process further comprises one or more of storing and combusting the thus obtained ammonia.

### Claim 18 (depends on 14)

The process of claim 14, further comprising maintaining an ammonia partial pressure above the vapor pressure of ammonia at the temperature of operation.

### Claim 19 (depends on 14)

The process of claim 14, further comprising feeding a dinitrogen and hydrogen comprising fluid.

### Claim 20 (depends on 14)

The process of claim 14, wherein the first electrode is at a first side in contact with the electrolyte and at the second side is in fluid contact with a supply of the dinitrogen comprising fluid, wherein the second electrode is at the first side also in contact with the electrolyte, and at the second side in fluid contact with a supply of the water comprising fluid, and wherein a first fluid pressure at the second side of the first electrode and a second fluid pressure at the second side of the second electrode are substantially equal.

### Claim 21 (depends on 14)

The process of claim 14, further comprising retrieving liquid ammonia from the electrolytic cell unit from a second side of the first electrode.