# US 9,752,245 B2 · Non-aqueous electrolyte for rechargeable magnesium ion cell

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- Number: US 9,752,245 B2
- Document ID: US9752245B2
- Status: Granted
- Kind: B2
- Application number: 14/309,132
- Filed: 2014-06-19
- Published: 2014-10-09
- Granted: 2017-09-05
- Earliest claimed: 2011-12-22
- Assignees: Pellion Technologies, Inc.
- Applicants: Pellion Technologies Inc.
- Inventors: Robert Ellis Doe; Ruoban Han; Yossef Gofer; Doron Aurbach; Nir Pour; Evgeny Sterenberg
- Web page: https://patentgrep.com/patent/US9752245B2

## CPC

- C25D 3/66: from melts
- C25D 3/42: of light metals
- C25D 3/665: {from ionic liquids}
- H01M 10/054: Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
- H01M 10/0568: characterised by the solutes
- H01M 10/0569: characterised by the solvents
- H01M 4/466: {Magnesium based}
- H01M 2300/0025: Organic electrolyte
- Y02E 60/10: Energy storage using batteries
- C25D: PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
- 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

A non-aqueous Magnesium electrolyte comprising: (a) at least one organic solvent; (b) at least one electrolytically active, soluble, inorganic Magnesium (Mg) salt complex represented by the formula: MgaZbXc wherein a, b, and c are selected to maintain neutral charge of the molecule, and Z and X are selected such that Z and X form a Lewis Acid, and 1≦a≦10, 1≦b≦5, and 2≦c≦30. Further Z is selected from a group consisting of aluminum, boron, phosphorus, titanium, iron, and antimony; X is selected from the group consisting of I, Br, Cl, F and mixtures thereof. Rechargeable, high energy density Magnesium cells containing an cathode, an Mg metal anode, and an electrolyte of the above-described type are also disclosed.

## Claims

### Claim 1

A non-aqueous electrolyte solution comprising:
(a) at least one organic solvent; and
(b) at least one electrolytically active, soluble, inorganic magnesium (Mg) salt complex represented by the formula MgaZbXc, and Z and X are selected such that Z and X forma Lewis Acid; and 1≦a≦10, 1≦b≦5, and 2≦c≦30,
wherein
Z is selected from the group consisting of aluminum, boron, phosphorus, titanium, iron, and antimony; and
X is selected from the group consisting of I, Br, Cl, F and mixtures thereof, and
wherein the Mg:Z ratio is greater than 1:2.

### Claim 2 (depends on 1)

The non-aqueous electrolyte solution of claim 1, wherein a, b, and c are selected to maintain neutral charge of the molecule.

### Claim 3 (depends on 1)

The non-aqueous electrolyte solution of claim 1, wherein 1≦a≦10, 1≦b≦2, and 3≦c≦30.

### Claim 4 (depends on 1)

The non-aqueous electrolyte solution of claim 1, wherein the magnesium (Mg) salt complex is represented by formula MgnZX3+(2*n), wherein n is from 1 to 5.

### Claim 5 (depends on 1)

A method of preparing a non-aqueous electrolyte solution of claim 1, comprising:
combining a source of magnesium, and a source of Z, in an electrolyte solvent.

### Claim 6 (depends on 1)

An electrochemical cell, comprising:
a non-aqueous electrolyte solution according to claim 1;
a magnesium-containing anode and
a cathode capable of reversible electrochemical reaction with magnesium.

### Claim 7 (depends on 6)

The electrochemical cell of claim 6, wherein the magnesium anode is selected from the group consisting of Mg, Mg alloys, electrodeposited Mg, anatase TiO2, rutile TiO2, Mo6S8, FeS2, TiS2, and MoS2.

### Claim 8 (depends on 6)

The electrochemical cell of claim 6, wherein the cathode is selected from the group consisting of Chevrel phase Mo6S8, MnO2, CuS, Cu2S, Ag2S, CrS2, VOPO4, layered TiS2, V2O5, MgVO3, MoS2, MgV2O5, MoO3, spinel CuCr2S4, MgCr2S4, MgMn2O4, MgNiMnO4, Mg2MnO4, NASICON MgFe2(PO4)3 and MgV2(PO4)3, olivine MgMnSiO4 and MgFe2(PO4)2, tavorite Mg0.5VPO4F, TiP2O7, VP2O7, MgMnF4, and FeF3.

### Claim 9 (depends on 1)

The non-aqueous electrolyte solution of claim 1, wherein the Mg molarity in the electrolyte solution is at least 0.1 M.

### Claim 10 (depends on 1)

The non-aqueous electrolyte solution of claim 1, wherein the at least one organic solvent is one or more solvent selected from the group consisting of ethers, organic carbonates, lactones, ketones, nitriles, ionic liquids, aliphatic and aromatic hydrocarbon solvents and organic nitro solvents.

### Claim 11 (depends on 1)

The non-aqueous electrolyte solution of claim 1, wherein the at least one organic solvent is one or more solvent selected from the group consisting of THF, 2-methyl THF, dimethoxyethane, diglyme, ethyl diglyme, butyl diglyme, triglyme, tetraglyme, diethoxyethane, diethylether, proglyme, dimethylsulfoxide, dimethyl sulfite, sulfolane, acetonitrile, hexane, toluene, nitromethane, 1-3 dioxalane, 1-4 dioxane, trimethyl phosphate, tri-ethyl phosphate, hexa-methyl-phosphoramide (HMPA), N,N-propyl-methyl-pyrrolidinium-bis(trifluoromethylsulfonyl)imide (P13-TFSI), N,N-propyl-methyl-pyrrolidinium-diacetamide (P13-DCA), propyl-methyl-pyrrolidinium-bis(fluorosulfonyl)imide (P13-FSI), ethyl-dimethyl-propyl-ammonium-bis(trifluoromethylsulfonyl)imide (PDEA-TFSI), 1-(methoxyethyl)-1-methylpiperidinium-bis(trifluoromethylsulfonyl)imide (MOEMPP-TFSI), and ionic liquids.

### Claim 12

A non-aqueous magnesium electrolyte solution comprising a complex of an inorganic magnesium halide, wherein the inorganic magnesium halide comprises magnesium chloride, and an inorganic compound more Lewis-acidic than the inorganic magnesium halide in at least one organic solvent.

### Claim 13 (depends on 12)

The non-aqueous magnesium electrolyte solution of claim 12, wherein the compound is a Lewis acid.

### Claim 14 (depends on 12)

The non-aqueous magnesium electrolyte solution of claim 12, wherein the molar ratio of inorganic magnesium halide to the compound is greater than 1.

### Claim 15 (depends on 12)

The non-aqueous electrolyte solution of claim 12, wherein the compound is selected from the group consisting of BI3, BBr3, BCl3, BF3, AlI3, AlBr3, AlCl3, AlF3, PI3, PBr3, PCl3, PF3, TiI4, TiBr4, TiCl3, TiCl4, TiF3, TiF4, FeI2, FeBr3, FeBr2, FeCl3, FeCl2, FeF3, FeF2, SbI3 SbBr3, SbCl3, and SbF3.

### Claim 16 (depends on 12)

The non-aqueous electrolyte solution of claim 12, wherein the complex comprises a reaction product of MgCl2 and AlCl3.

### Claim 17 (depends on 16)

The non-aqueous electrolyte solution of claim 16, wherein the Mg:Al ratio is in the range of greater than 0.5.

### Claim 18 (depends on 12)

The non-aqueous electrolyte solution of claim 12, wherein the Mg molarity in the electrolyte solution is at least 0.1 M.

### Claim 19 (depends on 12)

The non-aqueous electrolyte solution of claim 12, wherein the at least one organic solvent is one or more solvent selected from the group consisting of ethers, organic carbonates, lactones, ketones, nitriles, ionic liquids, aliphatic and aromatic hydrocarbon solvents and organic nitro solvents.

### Claim 20 (depends on 12)

The non-aqueous electrolyte solution of claim 12, wherein the at least one organic solvent is one or more solvent selected from the group consisting of THF, 2-methyl THF, dimethoxyethane, diglyme, ethyl diglyme, butyl diglyme, triglyme, tetraglyme, diethoxyethane, diethylether, proglyme, dimethylsulfoxide, dimethyl sulfite, sulfolane, acetonitrile, hexane, toluene, nitromethane, 1-3 dioxalane, 1-4 dioxane, trimethyl phosphate, tri-ethyl phosphate, hexa-methyl-phosphoramide (HMPA), N,N-propyl-methyl-pyrrolidinium-bis(trifluoromethylsulfonyl)imide (P13-TFSI), N,N-propyl-methyl-pyrrolidinium-diacetamide (P13-DCA), propyl-methyl-pyrrolidinium-bis(fluorosulfonyl)imide (P13-FSI), ethyl-dimethyl-propyl-ammonium-bis(trifluoromethylsulfonyl)imide (PDEA-TFSI), 1-(methoxyethyl)-1-methylpiperidinium-bis(trifluoromethylsulfonyl)imide (MOEMPP-TFSI), and ionic liquids.

### Claim 21 (depends on 12)

The non-aqueous electrolyte solution of claim 12, for use in a magnesium electrochemical cell.

### Claim 22 (depends on 12)

The non-aqueous electrolyte solution of claim 12, for use in a magnesium plating bath.