# US 8,785,699 B2 · Methods of higher alcohol synthesis

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- Number: US 8,785,699 B2
- Document ID: US8785699B2
- Status: Granted
- Kind: B2
- Application number: 13/866,948
- Filed: 2013-04-19
- Published: 2013-09-12
- Granted: 2014-07-22
- Earliest claimed: 2008-07-17
- Assignees: Pioneer Energy, Inc.
- Applicants: Pioneer Energy, Inc.
- Inventors: Emily Bostwick White; Cherie Wilson; Mark Berggren; Robert M. Zubrin
- Web page: https://patentgrep.com/patent/US8785699B2

## CPC

- C10L 1/1824: {mono-hydroxy}
- B01J 21/18: Carbon
- B01J 23/34: Manganese
- B01J 23/72: Copper
- B01J 23/80: with zinc, cadmium or mercury
- B01J 23/8892: {Manganese}
- B82Y 30/00: Nanotechnology for materials or surface science, e.g. nanocomposites
- C07C 29/154: containing copper, silver, gold, or compounds thereof
- C07C 29/34: by condensation involving hydroxy groups or the mineral ester groups derived therefrom, e.g. Guerbet reaction
- C10G 2/33: {characterised by the catalyst used}
- B01J 21/185: {Carbon nanotubes (carbon nanotubes per se C01B32/15)}
- B01J 23/007: {Mixed salts}
- C07C 2523/04: Alkali metals
- Y02P 20/52: using catalysts, e.g. selective catalysts
- C10L: FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B82Y: SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C10G: CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION (cracking to hydrogen or synthesis gas C01B; cracking or pyrolysis of hydrocarbon gases to individual hydrocarbons or mixtures thereof of definite or specified constitution C07C; cracking to cokes C10B); RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

Systems, catalysts, and methods are provided for transforming carbon based material into synthetic mixed alcohol fuel.

## Claims

### Claim 1

A method of producing liquid fuel from synthesis gas, the method comprising reacting the gas at pressures between about 500 and about 3000 psi and temperatures between about 200° C. and about 400° C. over a catalyst, wherein the catalyst consists essentially of copper, zinc, and potassium on a substrate.

### Claim 2 (depends on 1)

The method of claim 1, wherein the catalyst further comprises cobalt, manganese, or both cobalt and manganese.

### Claim 3 (depends on 1)

The method of claim 1, wherein the substrate is selected from the group consisting of silica, carbon nanotubes, and aluminum oxide.

### Claim 4 (depends on 1)

The method of claim 1, wherein the liquid fuel produced comprises methanol, ethanol, propanol, butanol, hydrocarbons, and/or mixtures thereof.

### Claim 5 (depends on 4)

The method of claim 4, wherein the methanol component of the product is removed via distillation to increase the energy content of the remaining fuel.

### Claim 6 (depends on 1)

The method of claim 1, wherein the synthesis gas is produced by steam reforming of biomass, corn stover, lignin, hemicellulose, coal, natural gas, landfill gas, and/or trash.

### Claim 7 (depends on 1)

The method of claim 1, wherein the synthesis gas is produced using the reverse water gas shift to convert CO2 to CO.

### Claim 8 (depends on 1)

The method of claim 1, wherein waste CO2 and hydrogen are converted into CO using reverse water gas shift, and wherein the CO is used as synthesis gas.

### Claim 9

A method of producing butanol, the method comprising reacting methanol with ethanol, propanol, or mixtures thereof at pressures under 3000 psi and temperatures between about 200° C. and about 400° C. using a catalyst, wherein the catalyst consists essentially of copper on hydrotalcite.

### Claim 10 (depends on 9)

The method of claim 9, wherein the hydrotalcite is a strongly basic variety and has a MgO to Al2O3 ratio greater than 1:1.

### Claim 11 (depends on 9)

The method of claim 9, wherein the methanol is produced on site by reacting synthesis gas on a copper and zinc catalyst at pressures between about 100 psi and about 3000 psi and temperatures between about 200° C. and about 400° C.

### Claim 12 (depends on 9)

The method of claim 9, wherein the methanol, ethanol, and/or propanol is produced from synthesis gas derived from of biomass, corn stover, lignin, hemicellulose, coal, natural gas, landfill gas, and/or trash.

### Claim 13

A method of producing a mixture of butanol, higher alcohols, and hydrocarbons from synthesis gas, the method comprising:
(a) reacting the gas at pressures between about 500 and about 3000 psi and temperatures between about 200° C. and about 400° C. over a catalyst, wherein the catalyst consists essentially of copper, zinc, and potassium on a substrate, to yield a mixture of alcohols and hydrocarbons comprising methanol, ethanol, propanol and butanol, as well as other alcohols and hydrocarbons; and
(b) reacting the methanol with the ethanol and/or propanol to produce butanol at pressures under 3000 psi and temperatures between about 200° C. and about 400° C. using a catalyst comprising copper on hydrotalcite.

### Claim 14 (depends on 13)

The method of claim 13, wherein the catalyst of step (a) further comprises cobalt, manganese, or both cobalt and manganese.

### Claim 15 (depends on 13)

The method of claim 13, wherein the hydrotalcite catalyst employed in step (b) is a basic variety and has a MgO to Al2O3 ratio greater than 1:1.

### Claim 16 (depends on 13)

The method of claim 13, wherein the synthesis gas is produced by steam reformation of biomass, corn stover, lignin, hemicellulose, coal, natural gas, landfill gas, and/or trash.

### Claim 17 (depends on 13)

The method of claim 13, wherein the synthesis gas is produced using the reverse water gas shift to convert CO2 to CO.

### Claim 18

A catalyst consisting essentially of copper, zinc, and potassium deposited on a substrate.

### Claim 19

A catalyst consisting essentially of copper, zinc, and potassium and at least one of cobalt and/or manganese deposited on a substrate.

### Claim 20

A catalyst consisting essentially of copper on hydrotalcite, wherein the hydrotalcite is a strongly basic variety with a MgO to Al2O3 ratio greater than 1:1.

### Claim 21 (depends on 20)

The catalyst of claim 20, wherein the hydrotalcite comprises carbon nanotubes.

### Claim 22 (depends on 20)

The catalyst of claim 20, wherein the source for Al and/or Cu are nanomaterials.

### Claim 23 (depends on 20)

The catalyst of claim 20, wherein a molecular template for ethanol is created by evaporating ethanol from the catalyst suspension.

### Claim 24 (depends on 20)

The catalyst of claim 20, wherein the catalyst is calcined in flowing air or a mixture of gases containing oxygen for about 2 to about 10 hours at a temperature between about 200° C. and about 1000° C.