# US 8,771,635 B2 · Hydrogen release from complex metal hydrides by solvation in ionic liquids

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- Number: US 8,771,635 B2
- Document ID: US8771635B2
- Status: Granted
- Kind: B2
- Application number: 13/094,464
- Filed: 2011-04-26
- Published: 2011-11-17
- Granted: 2014-07-08
- Earliest claimed: 2010-04-26
- Assignees: Toyota Motor Engineering & Manufacturing North America, Inc.
- Applicants: Rana F. Mohtadi; PremKumar Sivasubramanian
- Inventors: Rana F. Mohtadi; PremKumar Sivasubramanian
- Web page: https://patentgrep.com/patent/US8771635B2

## CPC

- C07D 233/54: having two double bonds between ring members or between ring members and non-ring members
- C01B 3/065: by reaction of inorganic compounds with hydrides
- Y02E 60/36: Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
- C07D: HETEROCYCLIC COMPOUNDS (macromolecular compounds C08)
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

A hydrogen release material includes a complex metal hydride and an ionic liquid wherein the hydrogen release material has a lower hydrogen release temperature in comparison to the complex metal hydride alone. Also disclosed is a process of releasing hydrogen from a storage material including the steps of: providing a complex metal hydride; combining the metal hydride with an ionic liquid in a desired amount forming a mixture; and heating the mixture to a temperature releasing hydrogen wherein the temperature is lower in comparison to the complex metal hydride alone.

## Claims

### Claim 1

A hydrogen release material comprising:
a complex metal hydride;
an ionic liquid wherein the hydrogen release material has a lower hydrogen release temperature in comparison to the complex metal hydride alone and
wherein the ionic liquid includes a member selected from the group consisting of N,N′ imidazolium, N-pyridinium, pyridinium or pipperidinium cations with an anion including at least one of AlCl4−, Al2Cl7−, PF6−, BF4−, Cl− or CF3SO3−, and combinations thereof.

### Claim 2 (depends on 1)

The hydrogen release material of claim 1 wherein the hydrogen release material has a faster hydrogen release rate in comparison to the complex metal hydride alone.

### Claim 3 (depends on 1)

The hydrogen release material of claim 1 wherein the hydrogen release material has a more mobile and less stable complex hydride anion which lowers an activation barrier for hydrogen release in comparison to the complex metal hydride alone.

### Claim 4 (depends on 1)

The hydrogen release material of claim 1 wherein the complex metal hydride has a formula of M(BH4)x where M is an alkali metal, an alkaline earth metal or a transition metal and 1≦x≦2.

### Claim 5 (depends on 1)

The hydrogen release material of claim 1 wherein the complex metal hydride has a formula of M(AlH4)x where 1≦x≦2 and where M is an alkali metal, an alkaline earth metal or a transition metal.

### Claim 6 (depends on 1)

The hydrogen release material of claim 1 wherein the complex metal hydride is selected from the group consisting of: magnesium borohydride, sodium borohydride, potassium borohydride, lithium borohydride and combinations thereof.

### Claim 7 (depends on 1)

The hydrogen release material of claim 1 wherein the complex metal hydride cation is selected from the group consisting of: magnesium, calcium, strontium, barium, and mixtures thereof.

### Claim 8 (depends on 1)

The hydrogen release material of claim 1 wherein the complex metal hydride has the formula M(AlH4)x, wherein M is an alkali metal, an alkaline earth metal or a transition metal and the complex metal hydride is selected from the group consisting of LiAlH4, NaAlH4, Mg(AlH4)2 and Ca(AlH4)2.

### Claim 9 (depends on 1)

The hydrogen release material of claim 1 wherein the complex metal hydride is solubilized in the ionic liquid forming cations and anions.

### Claim 10 (depends on 1)

The hydrogen release material of claim 1 wherein when a solid complex metal hydride when combined with a solid ionic liquid forms a paste or liquid at room temperature.

### Claim 11 (depends on 1)

The hydrogen release material of claim 1 wherein the hydrogen release material is capable of reversible storage and release of hydrogen.

### Claim 12 (depends on 1)

The hydrogen release material of claim 1 wherein the ionic liquid is present in an amount of 5 to 60 weight percent based on a total weight of a mixture.

### Claim 13 (depends on 1)

The hydrogen release material of claim 1 wherein the combined ionic liquid and metal hydride form a liquid or a paste at room temperature.

### Claim 14

A process of releasing hydrogen from a storage material including the steps of:
providing a complex metal hydride;
combining the complex metal hydride with an ionic liquid in a desired amount forming a mixture, wherein the ionic liquid includes a member selected from the group consisting of N,N′ imidazolium, N-pyridinium, pyridinium or pipperidinium cations with an anion including at least one of AlCl4−, Al2Cl7−, PF6−, BF4−, Cl− or CF3SO3−, and combinations thereof; and
heating the mixture to a temperature releasing hydrogen wherein the temperature is lower in comparison to the complex metal hydride alone.

### Claim 15 (depends on 14)

The process of releasing hydrogen from a storage material of claim 14 including grinding the complex metal hydride.

### Claim 16 (depends on 14)

The process of releasing hydrogen from a storage material of claim 14 wherein the combining step includes grinding the complex metal hydride and the ionic liquid.

### Claim 17 (depends on 16)

The process of releasing hydrogen from a storage material of claim 16 wherein the ionic liquid melts followed by hydrogen release.

### Claim 18 (depends on 14)

The process of releasing hydrogen from a storage material of claim 14 wherein the ionic liquid solubilizes the complex metal hydride lessening hydrogen reaction diffusion limitations of a solid complex metal hydride material.

### Claim 19 (depends on 14)

The process of releasing hydrogen from a storage material of claim 14 wherein when a solid complex metal hydride when combined with a solid ionic liquid forms a paste or liquid at room temperature.

### Claim 20 (depends on 14)

The process of releasing hydrogen from a storage material of claim 14 including a step of recharging the hydrogen release material with hydrogen after release.

### Claim 21 (depends on 20)

The process of releasing hydrogen from a storage material of claim 20 wherein the recharging step occurs at a temperature and pressure lower than the complex metal hydride alone.

### Claim 22 (depends on 20)

The process of releasing hydrogen from a storage material of claim 20 wherein the recharging step occurs faster in comparison to the complex metal hydride alone.

### Claim 23 (depends on 20)

The process of releasing hydrogen from a storage material of claim 20 wherein the recharging step has a reduced activation barrier for hydrogen in comparison to the complex metal hydride alone.

### Claim 24 (depends on 20)

The process of releasing hydrogen from a storage material of claim 20 including a step of drying the ionic liquid by removing water prior to combining with the metal hydride.

### Claim 25 (depends on 14)

The process of claim 14 wherein the combined ionic liquid and metal hydride form a liquid or a paste at room temperature.
