# US 12,224,432 B2 · Electroactive materials for metal-ion batteries

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- Number: US 12,224,432 B2
- Document ID: US12224432B2
- Status: Granted
- Kind: B2
- Application number: 18/214,304
- Filed: 2023-06-26
- Published: 2024-05-09
- Granted: 2025-02-11
- Earliest claimed: 2018-11-08
- Assignees: Nexeon Limited
- Applicants: Nexeon Limited
- Inventors: Charles Mason; Richard Taylor; James Farrell; William Macklin
- Web page: https://patentgrep.com/patent/US12224432B2

## CPC

- H01M 4/134: Electrodes based on metals, Si or alloys
- H01M 4/366: {as layered products}
- H01M 4/364: {as mixtures}
- H01M 4/386: {Silicon or alloys based on silicon}
- H01M 4/625: {Carbon or graphite}
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- H01M 2004/021: {Physical characteristics, e.g. porosity, surface area}
- H01M 2004/025: {with shapes other than plane or cylindrical}
- H01M 2004/027: {Negative electrodes}
- Y02E 60/10: Energy storage using batteries
- 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

## Abstract

This invention relates to particulate electroactive materials comprising a plurality of composite particles, wherein the composite particles comprise: (a) a porous carbon framework including micropores and optional mesopores having a total volume of at least 0.7 cm3/g and up to 2 cm3/g, wherein at least half of the total micropore and mesopore volume is in the form of pores having a diameter of no more than 1.5 nm; and (b) silicon located within the micropores and optional mesopores of the porous carbon framework in a defined amount relative to the total volume of the micropores and optional mesopores.

## Claims

### Claim 1

A particulate material comprising a plurality of composite particles, wherein the composite particles comprise:
(a) a porous carbon framework comprising micropores and optional mesopores,
wherein the micropores and optional mesopores have a total pore volume as measured by gas adsorption of P1 cm3/g, wherein P1 has a value of at least 0.7 and up to 1.3,
wherein the PD50 pore diameter as measured by gas adsorption is no more than 1.5 nm, and
wherein the PD90 pore diameter of the porous carbon framework is no more than 10 nm; and
(b) a plurality of elemental nanoscale silicon domains located at least within the micropores of the porous carbon framework;
wherein the weight ratio of silicon to the porous carbon framework in the composite particles is in the range from [0.7×P1 to 1.3×P1]:1, and
wherein at least 90 wt % of the silicon mass in the composite particles is located within the internal pore volume of the porous carbon framework.

### Claim 2 (depends on 1)

The particulate material according to claim 1, wherein P1 has a value of at least 0.75.

### Claim 3 (depends on 1)

The particulate material according to claim 1, wherein the PD50 pore diameter of the porous carbon framework is no more than 1.4 nm.

### Claim 4 (depends on 1)

The particulate material according to claim 1, wherein the PD60 pore diameter of the porous carbon framework is no more than 2 nm.

### Claim 5 (depends on 4)

The particulate material according to claim 4, wherein the PD70 pore diameter of the porous carbon framework is no more than 2.5 nm.

### Claim 6 (depends on 5)

The particulate material according to claim 5, wherein the PD80 pore diameter of the porous carbon framework is no more than 3 nm.

### Claim 7 (depends on 1)

The particulate material according to claim 1, wherein the PD90 pore diameter of the porous carbon framework is no more than 8 nm.

### Claim 8 (depends on 7)

The particulate material according to claim 7, wherein the PD95 pore diameter of the porous carbon framework is no more than 15 nm.

### Claim 9 (depends on 1)

The particulate material according to claim 1, wherein the porous carbon framework has a monomodal pore size distribution.

### Claim 10 (depends on 1)

The particulate material according to claim 1, wherein the porous carbon framework has a bimodal or multimodal pore size distribution.

### Claim 11 (depends on 10)

The particulate material according to claim 10, wherein the porous carbon framework has a bimodal or multimodal pore size distribution including at least one peak at less than 2 nm and at least one peak in the range from 5 to 50 nm.

### Claim 12 (depends on 1)

The particulate material according to claim 1, wherein the porous carbon framework further comprises macropores having a diameter in the range from greater than 50 nm to 100 nm having a total volume P2 cm3/g as measured by mercury porosimetry, wherein P2 is no more than 0.2×P1.

### Claim 13 (depends on 1)

The particulate material according to claim 1, wherein the weight ratio of silicon to the porous carbon framework is in the range from [0.7×P1 to 1.1×P1]:1.

### Claim 14 (depends on 1)

The particulate material according to claim 1, wherein at least a portion of the micropores comprise void space that is fully enclosed by the silicon.

### Claim 15 (depends on 1)

The particulate material according to claim 1, wherein the composite particles have a D50 particle diameter in the range of 0.5 to 50 μm.

### Claim 16 (depends on 15)

The particulate material according to claim 15, wherein the composite particles have a D50 particle diameter of at least 1 μm.

### Claim 17 (depends on 15)

The particulate material according to claim 15, wherein the composite particles have a D50 particle diameter of no more than 40 μm.

### Claim 18 (depends on 1)

The particulate material according to claim 1, wherein the composite particles have a D10 particle diameter of at least 0.2 μm.

### Claim 19 (depends on 1)

The particulate material according to claim 1, wherein the composite particles have a D90 particle diameter of no more than 80 μm.

### Claim 20 (depends on 1)

The particulate material according to claim 1, wherein the composite particles have a BET surface area of at least 0.1 m2/g and no more than 60 m2/g.

### Claim 21 (depends on 1)

The particulate material according to claim 1, wherein the volume of micropores and mesopores of the composite particles, as measured by nitrogen gas adsorption, is no more than 0.15×P1.

### Claim 22 (depends on 1)

The particulate material according to claim 1, having specific capacity on lithiation of 1200 to 2340 mAh/g.

### Claim 23 (depends on 1)

The particulate material according to claim 1, wherein
the PD50 pore diameter of the porous carbon framework is no more than 1.5 nm; and
the PD90 pore diameter of the porous carbon framework is no more than 6 nm.

### Claim 24 (depends on 1)

A composition comprising a particulate material as defined in claim 1 and at least one other component selected from: (i) a binder; (ii) a conductive additive; and (iii) an additional particulate electroactive material.

### Claim 25 (depends on 1)

An electrode comprising a particulate material as defined in claim 1 in electrical contact with a current collector.

### Claim 26 (depends on 25)

A rechargeable metal-ion battery comprising:
(i) an anode, wherein the anode comprises an electrode as described in claim 25;
(ii) a cathode comprising a cathode active material capable of releasing and reabsorbing metal ions; and
(iii) an electrolyte between the anode and the cathode.

### Claim 27

A particulate material comprising a plurality of composite particles, wherein the composite particles comprise:
(a) a porous carbon framework comprising micropores and optional mesopores,
wherein the micropores and optional mesopores have a total pore volume as measured by gas adsorption of P1 cm3/g, wherein P1 has a value of at least 0.7 and up to 1.3,
wherein the PD50 pore diameter as measured by gas adsorption is no more than 1.5 nm; and
(b) a plurality of elemental nanoscale silicon domains located at least within the micropores of the porous carbon framework;
wherein the weight ratio of silicon to the porous carbon framework in the composite particles is in the range from [0.7×P1 to 1.3×P1]:1,
wherein at least 90 wt % of the silicon mass in the composite particles is located within the internal pore volume of the porous carbon framework; and
wherein the composite particles have a D50 particle diameter of at least 2 μm.
