# US 12,000,054 B2 · Electrolysis methods that utilize carbon dioxide for making a macro-assembly of nanocarbon

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- Number: US 12,000,054 B2
- Document ID: US12000054B2
- Status: Granted
- Kind: B2
- Application number: 17/993,299
- Filed: 2022-11-23
- Published: 2023-05-25
- Granted: 2024-06-04
- Earliest claimed: 2021-11-24
- Assignees: C2Cnt LLC
- Applicants: C2Cnt LLC
- Inventors: Stuart Licht; Gad Licht
- Web page: https://patentgrep.com/patent/US12000054B2

## CPC

- C25B 1/135: Carbon
- C01B 32/05: Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30
- C01B 32/15: Nano-sized carbon materials
- C01B 32/154: Preparation
- C01B 32/158: Carbon nanotubes
- C01B 32/16: Preparation
- C01B 32/162: characterised by catalysts
- C01B 32/174: Derivatisation; Solubilisation; Dispersion in solvents
- C01B 32/18: Nanoonions; Nanoscrolls; Nanohorns; Nanocones; Nanowalls
- C01B 32/184: Preparation
- C25B 9/09: Fused bath cells
- C25B 11/02: characterised by shape or form
- C25B 11/042: Electrodes formed of a single material
- C25B 11/046: Alloys
- C25B 11/091: consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
- D01F 9/12: Carbon filaments; Apparatus specially adapted for the manufacture thereof
- B01D 61/027: {Nanofiltration}
- B01D 71/0212: {Carbon nanotubes}
- B82Y 30/00: Nanotechnology for materials or surface science, e.g. nanocomposites
- B82Y 40/00: Manufacture or treatment of nanostructures
- C01B 2202/08: Aligned nanotubes
- C01B 2202/20: Nanotubes characterized by their properties
- C01B 2202/22: Electronic properties
- C01B 2202/30: Purity
- C01B 2202/34: Length
- C01B 2204/04: Specific amount of layers or specific thickness
- C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram
- C01P 2002/78: by stacking-plane distances or stacking sequences
- C01P 2002/82: by IR- or Raman-data
- C01P 2002/88: by thermal analysis data, e.g. TGA, DTA, DSC
- C01P 2002/90: Other crystal-structural characteristics not specified above
- C01P 2004/03: obtained by SEM
- C01P 2004/04: obtained by TEM, STEM, STM or AFM
- C01P 2006/16: Pore diameter
- C01P 2006/80: Compositional purity
- H01B 1/04: mainly consisting of carbon-silicon compounds, carbon or silicon
- Y02E 60/10: Energy storage using batteries
- 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)
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- D01F: CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
- B01D: SEPARATION (separating solids from solids by wet methods B03B, B03D; by pneumatic jigs or tables B03B; by other dry methods B07; magnetic or electrostatic separation of solid materials from solid materials or fluids, separation by high-voltage electric fields B03C; centrifuges, vortex apparatus B04; presses per se for squeezing-out liquid from liquid-containing material B30B9/02; treatment of water C02F, e.g. softening by ion-exchange C02F1/42; {arrangements of air intake cleaners in gas turbine plants F02C7/05} ; arrangements or mounting of filters in air-conditioning, air-humidification or ventilation F24F13/28)
- B82Y: SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- H01B: CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES (selection for magnetic properties H01F1/00; waveguides H01P {; printed circuits H05K})
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

The embodiments of the present disclosure relate to a method and apparatus for producing a carbon nanomaterial product (CNM) product that may comprise carbon nanotubes and various other allotropes of nanocarbon. The method and apparatus employ a consumable carbon dioxide (CO2) and a renewable carbonate electrolyte as reactants in an electrolysis reaction in order to make CNTs. In some embodiments of the present disclosure, operational conditions of the electrolysis reaction may be varied in order to produce the CNM product with a greater incidence of a desired allotrope of nanocarbon or a desired combination of two or more allotropes.

## Claims

### Claim 1

A method for producing a macro-assembly product, the method comprising steps of:
a. heating an electrolyte media to obtain a molten electrolyte media;
b. positioning the molten electrolyte media between an anode and a cathode of an electrolytic cell;
c. introducing a source of carbon into the electrolytic cell;
d. applying an electrical current to the cathode and the anode in the electrolytic cell; and
e. collecting a CNM product from the cathode, wherein the CNM product comprises the macro-assembly product that comprises a minimum relative-amount of a nanosponge having a ID/IG ratio of between 0.6 to 0.8, densely packed, substantially parallel carbon nanotubes (CNTs) having a ID/IG ratio of between 0.4 and 0.6 or a nano-web of CNTs having a ID/IG ratio of between 0.2 and 0.4.

### Claim 2 (depends on 1)

The method of claim 1, wherein the anode and the cathode are each made of a high nickel-content material, wherein the CNM product comprises the nanosponge and wherein the minimum relative-amount is at least 70% of the total weight of the CNM product.

### Claim 3 (depends on 1)

The method of claim 1, wherein the electrical current is applied in a first stage of increasing current density and a second stage of a higher and substantially constant current density.

### Claim 4 (depends on 3)

The method of claim 3, wherein during the first stage, the current density increases between about 0.005 A/cm2 to about 0.07 A/cm2 over about twenty minutes.

### Claim 5 (depends on 3)

The method of claim 3, wherein the higher and substantially constant current density is between about 0.1 A/cm2 and 0.3 A/cm2.

### Claim 6 (depends on 2)

The method of claim 2, further comprising a step of adding a nickel-containing additive to the electrolyte media or the molten electrolyte media.

### Claim 7 (depends on 5)

The method of claim 5, wherein a nickel-containing additive is added in an amount of between about 0.5 wt % and about 0.2 wt %, relative to the amount of the electrolyte media or the molten electrolyte media.

### Claim 8 (depends on 2)

The method of claim 2, wherein the high nickel-content material is a Nichrome alloy.

### Claim 9 (depends on 1)

The method of claim 1, wherein the anode is made of a high nickel-content material, wherein the CNM product comprises the nano-web of CNTs.

### Claim 10 (depends on 8)

The method of claim 8, wherein the cathode comprises copper.

### Claim 11 (depends on 8)

The method of claim 8, further comprising a step of adding a nickel-containing additive to the electrolyte media or the molten electrolyte media.

### Claim 12 (depends on 10)

The method of claim 10, wherein a nickel-containing additive is added in an amount of between about 0.5 wt % and about 2 wt %, relative to the amount of the electrolyte media or the molten electrolyte media.

### Claim 13 (depends on 8)

The method of claim 8, wherein the electrical current is applied at a current density of between about 0.1 and 0.5 A/cm2.

### Claim 14 (depends on 13)

The method of claim 13, wherein the current density is 0.2 A/cm2.

### Claim 15 (depends on 1)

The method of claim 1, further comprising a step of adding an iron-containing additive to the molten electrolyte and wherein the anode is a composite anode.

### Claim 16 (depends on 15)

The method of claim 15, wherein the iron-containing additive is added in an amount of about 0.5 wt % to about 2 wt %, relative to the amount of the electrolyte media or the molten electrolyte media.

### Claim 17 (depends on 15)

The method of claim 15, wherein the composite anode comprises a first layer of a first Inconel alloy and at least a second layer of a second Inconel alloy, and wherein the CNM product comprises the densely packed, substantially parallel CNTs.

### Claim 18 (depends on 15)

The method of claim 15, wherein the composite anode comprises a first layer of a Nichrome alloy and at least a second layer of an Inconel alloy, wherein the desired allotrope is the CNT of a desired length, and wherein the CNM product comprises the densely packed, substantially parallel CNTs.

### Claim 19 (depends on 1)

The method of claim 1, further comprising a step of introducing a magnetic additive component into the electrolytic cell, wherein the magnetic additive component comprises a magnetic material addition component, a carbide-growth component or any combination thereof, and wherein the macro-assembly product is magnetic and moves when in a magnetic field.

### Claim 20 (depends on 1)

The method of claim 1, further comprising a step of introducing a doping additive component into the electrolytic cell, wherein the macro-assembly product is doped and atoms of the doping additive component are directly incorporated throughout the doped macro-assembly product to impart desired physical and/or chemical properties to the doped macro-assembly product that are different than an undoped macro-assembly product.