Process for converting hydrocarbon feedstocks with electrolytic recovery of halogen

a technology of electrolysis recovery and hydrocarbon feedstock, which is applied in the direction of solid-state devices, combustible gas purification/modification, non-metal raffination, etc., can solve the problems of difficult separation of intermediates, ineconomic value, and hbr electrolysis route to hydrogen, and achieves the effect of higher efficiency

Inactive Publication Date: 2008-12-25
REACTION 35 LLC
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Benefits of technology

[0015]The present invention combines the thermal (non-electrochemical) reactivity of halogens (preferably bromine) with hydrocarbons to produce hydrogen halide (preferably HBr) and reactive alkyl halides or other carbon-containing intermediates that may be converted to subsequent products, more readily than the original hydrocarbon, with the facile electrolysis of hydrogen halides or halide salts to create an overall process with significantly higher efficiency. The use of halogens prevents the total oxidation of the hydrocarbon to carbon dioxide and allows subsequent production of partial oxidation products.
[0023]In an important variation of the invention, an oxygen-depolarized electrode is used in the electrolyzer, and electrolysis of hydrogen halide yields molecular halogen and water, and electrolysis of alkaline halide yields molecular halogen and alkaline hydroxide, rather than hydrogen. This variation has the advantage of greatly reducing the power requirements of the electrolytic cell(s). An improved electrolytic cell, having an oxygen-depolarized electrode is also provided as yet another aspect of the invention.
[0025]The present conventional commercial process for utilizing methane, coal, and other hydrocarbons yields syngas (CO+H2), which can be converted to higher value products, such as methanol and linear alkanes. The intermediate syngas is extremely expensive to form, and the nearly fully oxidized carbon must be reduced to form useful products. When compared to the conventional syngas process, the present invention is superior in many respects and has at least the following advantages:
[0030]No fired reformer, and thus greater safety when used on offshore platforms.

Problems solved by technology

In principle, hydrocarbons can be directly oxidized electrochemically using oxygen (as in a solid oxide fuel cell) and / or water to produce hydrogen; however this typically leads to complex, difficult to separate intermediates and is not economically useful.
However, this process requires that bromine produced in electrolysis be converted back to HBr, and this conversion step is a major disadvantage of the HBr electrolysis route to hydrogen.

Method used

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  • Process for converting hydrocarbon feedstocks with electrolytic recovery of halogen
  • Process for converting hydrocarbon feedstocks with electrolytic recovery of halogen
  • Process for converting hydrocarbon feedstocks with electrolytic recovery of halogen

Examples

Experimental program
Comparison scheme
Effect test

example 1

Bromination of Methane

[0091]Methane (11 sccm, 1.0 atm) was combined with nitrogen (15 sccm, 1.0 atm) at room temperature via a mixing tee and passed through an 18° C. bubbler full of bromine. The CH4 / N2 / Br2 mixture was passed into a preheated glass tube (inside diameter 2.29 cm, length, 30.48 cm, filled with glass beads) at 500° C., where bromination of methane took place with a residence time of 60 seconds, producing primarily bromomethane, dibromomethane and HBr:

CH4+Br2→CH3Br+CH2Br2+HBr

[0092]As products left the reactor, they were collected by a series of traps containing 4M NaOH, which neutralized the HBr and hexadecane (containing octadecane as an internal standard) to dissolve as much of the hydrocarbon products as possible. Volatile components like methane were collected in a gas bag after the HBr / hydrocarbon traps.

[0093]After the bromination reaction, the coke or carbonaceous deposits were burned off in a flow of heated air (5 sccm) at 500° C. for 4 hours, and the CO2 was cap...

example 2

CH3Br Coupling to Light Olefins

[0094]2.27 g of a 5% Mg-doped ZSM-5 (CBV8014) zeolite was loaded in a tubular quartz reactor (1.0 cm ID), which was preheated to 400° C. before the reaction. CH3Br, diluted by N2, was pumped into the reactor at a flow rate of 24 μl / min for CH3Br, controlled by a micro liquid pump, and 93.3 ml / min for N2. The CH3Br coupling reaction took place over the catalyst bed with a residence time of 0.5 sec and a CH3Br partial pressure of 0.1 based on this flow rate setting.

[0095]After one hour of reaction, the products left the reactor and were collected by a series of traps containing 4M NaOH, which neutralized the HBr and hexadecane (containing octadecane as an internal standard) to dissolve as much of the hydrocarbon products as possible. Volatile components like methane and light olefins were collected in a gas bag after the HBr / hydrocarbon traps.

[0096]After the coupling reaction, the coke or carbonaceous deposits were burned off in a flow of heated air (5 s...

example 3

CH3Br Coupling to BTX

[0098]Pellets of Mn ion exchanged ZSM-5 zeolite (CBV3024, 6 cm in length) were loaded in a tubular quartz reactor (ID, 1.0 cm), which was preheated to 425° C. before the reaction. CH3Br, diluted by N2, was pumped into the reactor at a flow rate of 18 μl / min for CH3Br, controlled by a micro liquid pump, and 7.8 ml / min for N2. The CH3Br coupling reaction took place over the catalyst bed with a residence time of 5.0 sec and a CH3Br partial pressure of 0.5 based on this flow rate setting.

[0099]After one hour of reaction, the products left the reactor and were collected by a series of traps containing 4M NaOH, which neutralized the HBr and hexadecane (containing octadecane as an internal standard) to dissolve as much of the hydrocarbon products as possible. Volatile components like methane and light olefins were collected in a gas bag after the HBr / hydrocarbon traps.

[0100]After the coupling reaction, the coke or carbonaceous deposits were burned off in a flow of heat...

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Abstract

An improved continuous process for converting methane, natural gas, and other hydrocarbon feedstocks into one or more higher hydrocarbons, methanol, amines, or other products comprises continuously cycling through hydrocarbon halogenation, product formation, product separation, and electrolytic regeneration of halogen, optionally using an improved electrolytic cell equipped with an oxygen depolarized cathode.

Description

CROSS REFERENCE TO RELATED APPLICATION[0001]This application claims the benefit of priority to U.S. Provisional Application No. 60 / 930,220, filed May 14, 2007, the entire contents of which are incorporated by reference herein.FIELD OF THE INVENTION[0002]The present invention is directed to a process for converting natural gas and other hydrocarbon feedstocks into higher-value products, such as fuel-grade hydrocarbons, methanol, and aromatic compounds.BACKGROUND OF THE INVENTION[0003]U.S. patent application Ser. No. 11 / 703,358 (“the '358 application.”), entitled “Continuous Process for Converting Natural Gas to Liquid Hydrocarbons”, filed Feb. 5, 2007, based on U.S. Provisional Application No. 60 / 765,115, filed Feb. 3, 2006, describes a continuous process for reacting molecular halogen with a hydrocarbon feedstock to produce higher hydrocarbons. In one embodiment, the process includes the steps of alkane halogenation, “reproportionation” of polyhalogenated compounds to increase the a...

Claims

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Application Information

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Patent Type & Authority Applications(United States)
IPC IPC(8): C25B3/06C25B3/00
CPCC07C1/30C07C11/02C10B53/04C10B57/06C10G29/02C25B1/04C25B1/24Y02E60/366H01L2924/014C10G2300/1011C10G2300/1025C10G2400/30Y02P20/145Y02E60/36C07C1/26C07C29/124C07C209/08C07C17/06C07C31/04C07C11/04C07C11/06C07C211/03C07C19/075C10K3/00C25B3/27
Inventor GROSSO, PHILIPMCFARLAND, ERIC W.SHERMAN, JEFFREY H.
Owner REACTION 35 LLC
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