# US 9,437,899 B2 · Solid-state rechargeable magnesium battery

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- Number: US 9,437,899 B2
- Document ID: US9437899B2
- Status: Granted
- Kind: B2
- Application number: 14/177,115
- Filed: 2014-02-10
- Published: 2015-08-13
- Granted: 2016-09-06
- Earliest claimed: 2014-02-10
- Assignees: Battelle Memorial Institute
- Applicants: Battelle Memorial Institute
- Inventors: Yuyan Shao; Jun Liu; Tianbiao Liu; Guosheng Li
- Web page: https://patentgrep.com/patent/US9437899B2

## CPC

- H01M 10/054: Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
- H01M 4/38: of elements or alloys
- H01M 10/0565: Polymeric materials, e.g. gel-type or solid-type
- H01M 4/466: {Magnesium based}
- H01M 4/5815: {Sulfides}
- H01M 4/5825: {Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines}
- H01M 10/056: characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M 10/0566: Liquid materials
- H01M 10/0567: characterised by the additives
- H01M 10/0569: characterised by the solvents
- H01M 2300/0082: Organic polymers
- 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

Embodiments of a solid-state electrolyte comprising magnesium borohydride, polyethylene oxide, and optionally a Group IIA or transition metal oxide are disclosed. The solid-state electrolyte may be a thin film comprising a dispersion of magnesium borohydride and magnesium oxide nanoparticles in polyethylene oxide. Rechargeable magnesium batteries including the disclosed solid-state electrolyte may have a coulombic efficiency ≧95% and exhibit cycling stability for at least 50 cycles.

## Claims

### Claim 1

An electrolyte comprising:
an all solid-state composition comprising
Mg(BH4)2;
A metal oxide of MgO; and
polyethylene oxide.

### Claim 2 (depends on 1)

The electrolyte of claim 1, where the electrolyte is a solid dispersion of Mg(BH4)2 and the metal oxide in polyethylene oxide.

### Claim 3 (depends on 1)

The solid-state electrolyte of claim 1, where the solid-state electrolyte is a thin film having an average thickness from 15 μm to 400 μm.

### Claim 4 (depends on 1)

The electrolyte of claim 1, wherein the metal is a Group IIA metal, a transition metal, or a combination thereof.

### Claim 5 (depends on 1)

The electrolyte of claim 1, comprising:
3-30 wt % Mg(BH4)2, based on a total weight of the electrolyte;
55-92 wt % polyethylene oxide, based on the total weight of the electrolyte; and
5-15 wt % metal oxide, based on the total weight of the electrolyte.

### Claim 6 (depends on 1)

The electrolyte of claim 1, comprising:
5-15 wt % Mg(BH4)2, based on a total weight of the electrolyte;
73-88 wt % polyethylene oxide, based on the total weight of the electrolyte; and
7-12 wt % metal oxide, based on the total weight of the electrolyte.

### Claim 7 (depends on 1)

The electrolyte of claim 1, wherein the metal oxide further comprises TiO2, ZrO2, or a combination thereof.

### Claim 8 (depends on 1)

The electrolyte of claim 1, where the metal oxide comprises metal oxide nanoparticles having an average diameter ≦500 nm.

### Claim 9 (depends on 8)

The electrolyte of claim 8, where the electrolyte is a solid dispersion of Mg(BH4)2 and the metal oxide nanoparticles in polyethylene oxide.

### Claim 10 (depends on 1)

The electrolyte of claim 1, where the electrolyte consists essentially of Mg(BH4)2, polyethylene oxide, and metal oxide.

### Claim 11 (depends on 10)

The electrolyte of claim 10, consisting essentially of:
3-30 wt % Mg(BH4)2, based on a total weight of the electrolyte;
55-92 wt % polyethylene oxide, based on the total weight of the electrolyte; and
5-15 wt % MgO nanoparticles, based on the total weight of the electrolyte, having an average diameter ≦500 nm.

### Claim 12 (depends on 1)

A rechargeable battery, comprising:
an anode comprising magnesium;
a cathode; and
the electrolyte of claim 1.

### Claim 13 (depends on 12)

The rechargeable battery of claim 12, where the anode is magnesium metal.

### Claim 14 (depends on 12)

The rechargeable battery of claim 12, where the cathode comprises stainless steel, Mo6S8, Mg2Mo6S8, MoS2, Mo6S8-ySey where y=0, 1, or 2, MgxS3O4 where 0<x<1, MgCoSiO4, MgFeSiO4, MgMnSiO4, V2O5, WSe2, sulfur, poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl methacrylate)/graphene, MnO2/acetylene black, or carbyne polysulfide.

### Claim 15 (depends on 12)

The rechargeable battery of claim 12, where the anode has a capacity fade of less than 20% after 50 discharge/charge cycles.

### Claim 16 (depends on 12)

The rechargeable battery of claim 12, where the battery has a coulombic efficiency ≧95%.

### Claim 17 (depends on 1)

A method for making an all solid-state magnesium electrolyte of claim 1, comprising:
making an all solid-state magnesium electrolyte by
forming an electrolyte mixture comprising Mg(BH4)2, polyethylene oxide, and a metal oxide a Group IIA metal, a transition metal, or a combination thereof; and
forming a thin film of the electrolyte mixture.

### Claim 18 (depends on 17)

The method of claim 17, where the thin film consists essentially of:
3-30 wt % Mg(BH4)2, based on a total weight of the thin film;
55-92 wt % polyethylene oxide, based on the total weight of the thin film; and
5-15 wt % metal oxide, based on the total weight of the thin film.