# US 12,191,079 B2 · Composite electrodes for supercapacitors, ternary materials with flower-like molybdenum disulfide structures, and related methods

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- Number: US 12,191,079 B2
- Document ID: US12191079B2
- Status: Granted
- Kind: B2
- Application number: 18/594,193
- Filed: 2024-03-04
- Published: 2024-09-05
- Granted: 2025-01-07
- Earliest claimed: 2023-03-04
- Assignees: Purdue Research Foundation
- Applicants: Purdue Research Foundation
- Inventors: Jong Hyun Choi; Jaehoon Ji
- Web page: https://patentgrep.com/patent/US12191079B2

## CPC

- H01G 11/36: Nanostructures, e.g. nanofibres, nanotubes or fullerenes
- H01G 11/24: characterised by structural features of the materials making up or comprised in the electrodes, e.g. form, surface area or porosity; characterised by the structural features of powders or particles used therefor
- H01G 11/26: characterised by their structure, e.g. multi-layered, porosity or surface features
- H01G 11/86: specially adapted for electrodes (carbonisation or activation of carbon for the manufacture of electrodes H01G11/34)
- Y02E 60/13: Energy storage using capacitors
- H01G: CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE (selection of specified materials as dielectric H01B3/00; capacitors having potential barriers H10D1/62, H10K10/10)
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

Composite electrodes, supercapacitors equipped therewith, ternary materials for composite electrodes, and related methods. Such a composite electrode has a composite CNT-ZIF structure formed of a conductive network of carbon nanotubes (CNT) and a zeolitic imidazole framework (ZIF) coating covering the conductive network. A layer of molybdenum disulfide (MoS2) structures having flower-like morphologies is disposed on the composite CNT-ZIF structure. The MoS2 structures have pores that provide diffusion paths for ions to and/or from the ZIF coating and/or the conductive network of CNT.

## Claims

### Claim 1

A composite electrode for a supercapacitor, the electrode comprising:
a composite CNT-ZIF structure comprising a conductive network of carbon nanotubes (CNT) and a zeolitic imidazole framework (ZIF) coating covering the conductive network, the ZIF coating providing high ion diffusivity; and
a layer of molybdenum disulfide (MoS2) structures disposed on the composite CNT-ZIF structure, the MoS2 structures comprising pores that provide diffusion paths for ions to and/or from the ZIF coating and/or the conductive network of CNT, wherein the MoS2 structures have a flower-like (fMoS2) morphology.

### Claim 2 (depends on 1)

The composite electrode of claim 1, wherein the electrode provides an energy density of at least about 78 Wh/kg.

### Claim 3 (depends on 1)

The composite electrode of claim 1, wherein the electrode provides a power density of about 3,000 W/kg.

### Claim 4 (depends on 1)

The composite electrode of claim 1, wherein the electrode provides about 90% of capacitance retention over 3,000 cycles.

### Claim 5 (depends on 1)

A supercapacitor comprising:
a composite electrode according to claim 1; and
an electrolyte configured to provide ions for adsorption and/or desorption on the composite electrode.

### Claim 6 (depends on 5)

The supercapacitor of claim 5, wherein the supercapacitor is a hybrid supercapacitor.

### Claim 7

A method of fabricating a ternary electrode material having a flower-like molybdenum disulfide (fMoS2) morphology for a composite electrode, the method comprising:
fabricating a MoS2 structure on a composite CNT-ZIF structure to form the ternary composite electrode material, the composite CNT-ZIF structure comprises a carbon nanotubes (CNT) core surrounding by a porous zeolitic imidazole framework (ZIF) shell, and during the fabricating step an architecture of the MoS2 structure is controlled by adjusting a molar ratio of Mo and S reagents so as to form edge-rich flower-like MoS2 structures with sulfur vacancies (fMoS2).

### Claim 8 (depends on 7)

The method of claim 7, wherein the step of forming the composite CNT-ZIF structure comprises growing porous ZIF on CNT network via a solvothermal process.

### Claim 9 (depends on 7)

The method of claim 7, wherein the step of fabricating the MoS2 structure comprises adjusting the molar ratio of Mo and S reagents to provide excessive supply of sulfur precursors to molybdenum molecules.

### Claim 10 (depends on 9)

The method of claim 9, wherein the step of fabricating the MoS2 structure comprises adjusting the molar ratio of Mo and S reagents to provide a supply of molybdenum molecules to sulfur precursors in a Mo:S ratio of approximately 1:8.

### Claim 11 (depends on 7)

The method of claim 7, wherein the step of fabricating the MoS2 structure comprises blending thiourea and ammonium heptamolybdate tetrahydrate in an aqueous solution containing CNT-ZIF to form sulfur(S) precursors and molybdenum (Mo) precursors.

### Claim 12 (depends on 7)

The method of claim 7, wherein the step of fabricating the MoS2 structure comprises fabricating a layer of a plurality of the MoS2 structures on the composite CNT-ZIF structure.

### Claim 13 (depends on 7)

The method of claim 7, further comprising forming the composite CNT-ZIF structure comprising a CNT core surrounded by a porous ZIF shell.

### Claim 14

A ternary material comprising:
a composite CNT-ZIF structure comprising a conductive network of carbon nanotubes (CNT) and a zeolitic imidazole framework (ZIF) coating covering the conductive network; and
a layer of molybdenum disulfide (MoS2) structures disposed on the composite CNT-ZIF structure, the MoS2 structures comprising pores that provide diffusion paths for ions to and/or from the ZIF coating and/or the conductive network of CNT, wherein the MoS2 structures have a flower-like (fMoS2) morphology.
