# US 2020/0399737 A1 · Recycling li-ion batteries using green chemicals and processes

> Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt

- Number: US 2020/0399737 A1
- Document ID: US20200399737A1
- Status: Published application
- Kind: A1
- Application number: 16/909,560
- Filed: 2020-06-23
- Published: 2020-12-24
- Earliest claimed: 2019-06-24
- Assignees: William Marsh Rice University
- Applicants: William Marsh Rice University
- Inventors: Mai K. Tran; Marco-Tulio F. Rodrigues; Ganguli Babu; Hemtej Gullapalli; Pulickel M. Ajayan
- Web page: https://patentgrep.com/patent/US20200399737A1

## CPC

- C22B 26/12: Obtaining lithium
- C22B 3/1608: {Leaching with acyclic or carbocyclic agents}
- C22B 3/44: by chemical processes (treatment or purification of solutions by liquid-liquid extraction C22B3/26, by ion-exchange extraction C22B3/42)
- C22B 7/006: {Wet processes}
- C22B 7/007: {by acid leaching}
- H01M 10/54: Reclaiming serviceable parts of waste accumulators
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- Y02E 60/10: Energy storage using batteries
- Y02P 10/20: Recycling
- Y02W 30/84: Recycling of batteries or fuel cells
- C22B: PRODUCTION AND REFINING OF METALS (electrolytic C25); PRETREATMENT OF RAW MATERIALS
- 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
- Y02W: CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT

## Abstract

A process for extracting, recovering and recycling metals and materials from spent lithium ion batteries (LIB) that comprises the contacting battery waste products with a deep eutectic solvent, and leaching the metal from the battery waste product and extracting the metal into the deep eutectic solvent with heat and agitation. After the leaching and extracting, the process further includes recovering the dissolved metals ions from the deep eutectic solvent solution, followed by a step of regeneration of cathode materials.

## Claims

### Claim 1

A process for extracting, recovering and recycling metals and materials from spent lithium ion batteries (LIB) comprising the steps of:
contacting battery waste product comprising metals and/or metal alloys with a deep eutectic solvent, wherein the deep eutectic solvent comprises a hydrogen bond acceptor compound and a hydrogen bond donor compound;
leaching the metal from the battery waste product and extracting the metal into the deep eutectic solvent with heat and agitation;
recovering the dissolved metals ions from the deep eutectic solvent solution; and
regeneration of cathode materials from the recovered dissolved metal ions for new energy application.

### Claim 2 (depends on 1)

The process of claim 1, wherein the leaching and extracting is conducted at a temperature ranging from room temperature (25° C.) to 220° C.

### Claim 3 (depends on 1)

The process of claim 1, wherein the leaching and extracting is conducted for 8 to 72 hr.

### Claim 4 (depends on 1)

The process of claim 1, wherein the leaching and extracting is conducted with temperature ranging between 120° C. to 220° C. and pressure between 10 kPA to 10 MPa for 12 to 24 hours.

### Claim 5 (depends on 1)

The process of claim 1, wherein a molar ratio of the hydrogen bond acceptor to hydrogen bond donor of the deep eutectic solvent ranges from 1:1 to 1:3.

### Claim 6 (depends on 1)

The process of claim 1, wherein the hydrogen bond donor is selected from an alcohol, an amine, a urea, a thiourea, an imidazole and a carboxylic acid.

### Claim 7 (depends on 6)

The process of claim 6, wherein the hydrogen bond acceptor is selected from a carnitine or a salt thereof, a betaine or a salt thereof, choline chloride, ethylammonium chloride, or salts with a chloride.

### Claim 8 (depends on 7)

The process of claim 7, wherein the hydrogen bond donor is ethylene glycol and wherein the hydrogen bond acceptor choline chloride.

### Claim 9 (depends on 1)

The process of claim 1, wherein the deep eutectic solvent is capable of extracting at least 50 wt % of the metal contained in the spent lithium ion battery waste product.

### Claim 10 (depends on 1)

The process of claim 1, wherein the recovering of the dissolved metals is accomplished via chemical precipitation.

### Claim 11 (depends on 10)

The process of claim 10, wherein the chemical precipitation includes mixing the metal containing deep eutectic solvent with a carbonate/hydroxide rich solution comprising at least 15 wt % of an alkali metal carbonate or metal hydroxide.

### Claim 12 (depends on 1)

The process of claim 1, further comprising recovering the deep eutectic solvent following the metal recovery step and recycling the deep eutectic solvent to the contacting step.

### Claim 13 (depends on 1)

The process of claim 1, wherein the regeneration of the cathode materials is achieved via addition of metal hydroxides directly to the deep eutectic solvent.

### Claim 14

A system for recovering and recycling metals from spent lithium ion batteries (LIB) comprising:
a vessel for contacting battery waste product comprising metals and/or metal alloys with a deep eutectic solvent, wherein the deep eutectic solvent comprises a hydrogen bond acceptor compound and a hydrogen bond donor compound, thereby leaching the metal from the battery waste product and extracting the metal into the deep eutectic solvent with heat and agitation;
a vessel for precipitating the dissolved metals ions from the deep eutectic solvent solution or
a vessel for electrodeposition of the dissolved metals ions from the deep eutectic solvent solution.

### Claim 15 (depends on 14)

The system of claim 14, wherein the system also includes a vessel for calcination of recovered metal ions.

### Claim 16 (depends on 14)

The system of claim 14, wherein the hydrogen bond donor is selected from an alcohol, an amine, a urea, a thiourea, an imidazole and a carboxylic acid.

### Claim 17 (depends on 14)

The system of claim 14, wherein the hydrogen bond acceptor is selected from a carnitine or a salt thereof, a betaine or a salt thereof, choline chloride, ethylammonium chloride, or salts with a chloride.

### Claim 18 (depends on 14)

The system of claim 14, wherein a molar ratio of the hydrogen bond acceptor to hydrogen bond donor of the deep eutectic solvent ranges from 1:1 to 1:3.

### Claim 19 (depends on 14)

The system of claim 14, wherein the vessel for contacting the battery waste is configured to be at least one of heated, agitated, pressurized.

### Claim 20

A process for extracting, recovering and recycling metals and materials from spent lithium ion batteries (LIB) comprising the steps of:
contacting battery waste product comprising metals and/or metal alloys with a deep eutectic solvent, wherein the deep eutectic solvent (DES) comprises choline chloride and ethylene glycol in a molar ratio ranging from 1:1 to 1:3, wherein the DES is mixed with the battery waste product in a ratio ranging from 5 g/0.001 g to 5 g/0.1 g;
leaching the metal from the battery waste product and extracting the metal into the deep eutectic solvent, wherein the leaching and extracting is conducted for 8 to 72 hr at a temperature ranging from 25° C. to 220° C.;
recovering the dissolved metals ions from the deep eutectic solvent solution; and
regeneration of cathode materials from the recovered dissolved metal ions for new energy application.
