US 6,114,400 AGranted

Synthesis gas production by mixed conducting membranes with integrated conversion into liquid products

AssigneeAir Products and Chemicals, Inc.

InventorsShankar Nataraj, Steven Lee Russek, Paul Nigel Dyer

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Abstract

Natural gas or other methane-containing feed gas is converted to a C.sub.5 -C.sub.19 hydrocarbon liquid in an integrated system comprising an oxygenative synthesis gas generator, a non-oxygenative synthesis gas generator, and a hydrocarbon synthesis process such as the Fischer-Tropsch process. The oxygenative synthesis gas generator is a mixed conducting membrane reactor system and the non-oxygenative synthesis gas generator is preferably a heat exchange reformer wherein heat is provided by hot synthesis gas product from the mixed conducting membrane reactor system. Offgas and water from the Fischer-Tropsch process can be recycled to the synthesis gas generation system individually or in combination.

Claims25

Dependent claims

A method for making a hydrocarbon product which comprises:

(a) providing a mixed conducting membrane reaction zone having an oxidant side and a reactant side which are separated by a solid mixed conducting membrane;
(b) introducing a feed gas comprising at least methane into the reactant side of the mixed conducting membrane reaction zone;
(c) heating an oxygen-containing oxidant gas feed and introducing the resulting heated oxidant gas feed into the oxidant side of the mixed conducting membrane reaction zone;
(d) permeating oxygen from the oxidant side of the mixed conducting membrane reaction zone through the mixed conducting membrane to the reactant side of the mixed conducting membrane reactor and reacting the oxygen with the feed gas to form at least hydrogen and carbon monoxide;
(e) withdrawing a hot synthesis gas product comprising at least hydrogen and carbon monoxide from the reactant side of the mixed conducting membrane reaction zone;
(f) withdrawing a hot oxygen-depleted nonpermeate gas from the oxidant side of the mixed conducting membrane reaction zone;
(g) providing a hydrocarbon synthesis and processing zone and reacting at least a portion of the synthesis gas product therein;
(h) withdrawing from the hydrocarbon synthesis and processing zone streams comprising (1) a hydrocarbon product comprising components having greater than four carbon atoms, (2) an offgas comprising one or more components selected from the group consisting of hydrogen, carbon monoxide, carbon dioxide, methane, and hydrocarbons containing two or more carbon atoms, and (3) water;
and
(i) converting at least a portion of the offgas into a recycle gas and utilizing at least a portion of this recycle gas to provide a portion of the feed gas to the mixed conducting membrane reaction zone.

7 more elements

A method for making a hydrocarbon product which comprises:

(a) providing a first catalytic reforming reaction zone comprising at least one catalyst which promotes the steam reforming of hydrocarbons;
(b) heating a reactant gas feed comprising water and one or more hydrocarbons, introducing the resulting heated reactant gas feed into the first catalytic reforming reaction zone, and withdrawing therefrom a partially reformed intermediate gas comprising at least methane, hydrogen, and carbon oxides;
(c) providing a mixed conducting membrane reaction zone having an oxidant side and a reactant side which are separated by a solid mixed conducting membrane;
(d) heating an oxygen-containing oxidant gas feed and introducing the resulting heated oxidant gas feed into the oxidant side of the mixed conducting membrane reaction zone;
(e) introducing the partially reformed intermediate gas of (b) into the reactant side of the mixed conducting membrane reaction zone;
(f) permeating oxygen from the oxidant side of the mixed conducting membrane reactor through the mixed conducting membrane to the reactant side of the mixed conducting membrane reaction zone, and reacting the oxygen with the partially reformed intermediate gas to form additional hydrogen and carbon monoxide;
(g) withdrawing a hot synthesis gas product comprising at least hydrogen and carbon monoxide from the reactant side of the mixed conducting membrane reaction zone;
(h) withdrawing a hot oxygen-depleted nonpermeate gas from the oxidant side of the mixed conducting membrane reaction zone;
(i) reacting a hydrocarbon-containing recycle stream and water in a second catalytic reforming reaction zone to generate recycle gas comprising at least methane, hydrogen, and carbon oxides;
(j) providing a hydrocarbon synthesis and processing zone and reacting therein at least a portion of a combined stream comprising the synthesis gas product of (g) and the recycle gas of (i);
(k) withdrawing from the hydrocarbon synthesis reaction zone streams comprising (1) a hydrocarbon product comprising components having greater than four carbon atoms, (2) an offgas comprising components selected from the group consisting of hydrogen, carbon monoxide, carbon dioxide, methane, and hydrocarbons containing two or more carbon atoms, and (3) water;
and
(l) utilizing at least a portion of the offgas of (k) to provide the hydrocarbon-containing recycle stream of (i).

10 more elements

A method for making a hydrocarbon product which comprises:

(a) providing a catalytic reforming reaction zone comprising at least one catalyst which promotes the steam reforming of hydrocarbons;
(b) heating a reactant gas feed comprising water and one or more hydrocarbons, introducing the resulting heated reactant gas feed into the catalytic reforming reaction zone, and withdrawing therefrom a hot partially reformed intermediate gas comprising at least methane, hydrogen, and carbon oxides;
(c) providing a mixed conducting membrane reaction zone having an oxidant side and a reactant side which are separated by a solid mixed conducting membrane;
(d) heating an oxygen-containing oxidant gas feed and introducing the resulting heated oxidant gas feed into the oxidant side of the mixed conducting membrane reaction zone;
(e) introducing the partially reformed intermediate gas of (b) into the reactant side of the mixed conducting membrane reaction zone;
(f) permeating oxygen from the oxidant side of the mixed conducting membrane reactor through the mixed conducting membrane to the reactant side of the mixed conducting membrane reaction zone, and reacting the oxygen with the partially reformed intermediate gas to form additional hydrogen and carbon monoxide;
(g) withdrawing a hot synthesis gas product comprising at least hydrogen and carbon monoxide from the reactant side of the mixed conducting membrane reaction zone;
(h) providing a hydrocarbon synthesis and processing zone and reacting therein at least a portion of the hot synthesis gas product of (g);
(i) withdrawing from the hydrocarbon synthesis and processing zone streams comprising (1) a hydrocarbon product comprising components having greater than four carbon atoms, (2) an offgas comprising components selected from the group consisting of hydrogen, carbon monoxide, carbon dioxide, methane, and hydrocarbons containing two or more carbon atoms, and (3) water;
and
(j) utilizing a portion of the water from the hydrocarbon synthesis and processing zone of (i) to provide at least a portion of the water in the reactant gas feed of (b).

8 more elements

Dependencies are inferred from the claim text.

Facts

Application: 09/157,712Filed 21 Sep 1998
Granted: 5 Sep 2000
Term ends: Not estimatedThe source records don’t support an estimate.

Classification12 codes

C10G 2/30
Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon: from carbon monoxide with hydrogen
C01B 3/36
By reaction of hydrocarbons with gasifying agents: using oxygen; using mixtures containing oxygen as gasifying agents
C01B 3/382
Using catalysts: processes with two or more reaction steps, of which at least one is catalytic, e.g. steam reforming and partial oxidation
C01B 13/0251
Physical processing only: by making use of membranes