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Patent EP0112613A2 successfully refreshed from Google Patents.
EP0112613A2
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EP
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Process for producing hydrogen-rich gas from hydrocarbonaceous feeds
Assignee: BASF Catalysts LLC
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Filing: 1983-09-29
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Granted: —
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Expires: 2003-09-29
Abstract
Abstract Autothermal Reforming and Processes Utilizing the Same. The technical field of the invention concerns the production from hydrocarbonaceous feeds of hydrogen-rich gases and use of the same in various synthesis operations. An autothermal reforming process, as illustrated in Figure 2 of the drawings, comprises carrying out partial oxidation of a hydrocarbonaceous feed by introducing an oxidant gas (e.g., air), steam and hydrocarbonaceous feed (e.g., a hydrocarbon) into an apparatus (24), as illustrated in detail in Figure 3, which contains a catalytic partial oxidation section (24a). A monolithic catalyst (27) comprising palladium and platinum and, optionally, rhodium, distended upon a stabilized alumina wash-coat is contained within section (24a). At least one half by weight of the hydrocarbonaceous feed is catalytically oxidized in section (24a) at a high throughput rate to produce a heated effluent suitable for further processing, such as being passed through a steam reforming catalyst (31) contained in section (24b) of apparatus (24). The hydrogen-rich gas thus obtained may be used as is or further processed for use as a synthesis gas for methanol or ammonia synthesis, or for the synthesis of normally liquid hydrocarbons or synthetic natural gas.
Inventors
- 👤 Ronald M. Heck
- 👤 William T. Mcshea Iii
- 👤 William Buchanan
- 👤 Paul Flanagan
- 👤 Robert M. Yarrington
Bibliographic Details
Application Number
—
Jurisdiction
EP
Data Source
google_patents
Last Synchronized
2026-10-26 20:26
CPC Classifications
C; C01; C01B; C01B3/00; C01B3/02; C01B3/32; C01B3/34; C01B3/38; C01B3/382; B; B01; B01J; B01J19/00; B01J19/24; B01J19/248; B01J19/2485; B01J8/00; B01J8/02; B01J8/0242; B01J8/025; B01J8/0285; B01J2208/00; B01J2208/00008; B01J2208/00017; B01J2208/00477; B01J2208/00504; B01J2219/00; B01J2219/00049; B01J2219/00051; B01J2219/0015; B01J2219/00157; C01B2203/00; C01B2203/08; C01B2203/0805; C01B2203/0811; C01B2203/0827; C01B2203/14; C01B2203/142; C01B2203/146; C01B2203/147; C01B2203/148; C01B2203/80; C01B2203/82; Y; Y02; Y02E; Y02E20/00; Y02E20/16; Y02E20/18
Claims Analysis
Total Claims: 29
Claim 1
Independent Claim
292 words
A process for producing a hydrogen-rich gas by preheating an inlet stream comprising a hydrocarbonaceous feed, H 2 0 and an oxygen-containing oxidant gas to a preheat temperature at least sufficiently high to initiate catalytic oxidation of said hydrocarbonaceousfeed, and introducing the preheated inlet stream into a first catalyst zone (24a)to carry out catalytic partial oxidation therein, characterized in that: (a) the first catalyst zone (24a) comprises a monolithic body (27) having a plurality of gas flow passages extending therethrough and having a catalytically effective amount of palladium and platinum catalytic components dispersed therein, the amounts of hydrocarbonaceous feed, H 2 0 and oxygen introduced into said first catalyst zone (24a) being controlled to maintain in said inlet stream an H20 to C ratio of at least about 0.5, and an 0 2 to C ratio of at least about 0.2 but less than the stoichiometric amount of oxygen necessary to oxidize all the carbon of said feed to C0 2 ; (b) contacting the preheated inlet stream within said first catalyst zone (24a) with said palladium and platinum catalytic component on said monolith (27) to initiate and sustain therein catalytic oxidation of at least a sufficient quantity of said hydrocarbon feed to attain an elevated temperature within said first catalyst zone (24a) at least high enough to crack unoxidized C or heavier hydrocarbons, if any be present, to light hydrocarbons not heavier than C 4 hydrocarbons, the temperature of at least a portion of said monolithic body (27) being at least about 121°C higher than the ignition temperature of said inlet stream, whereby to produce a first catalyst zone effluent comprising, predominantly, hydrogen, carbon oxides and said light hydrocarbons; and (c) withdrawing the first catalyst zone effluent as a hydrogen-rich gas.
Claim 2
Dependent Claim
292 words
A process for producing a hydrogen-rich gas by preheating an inlet stream comprising a hydrocarbonaceous feed, H 2 0 and an oxygen-containing oxidant gas to a preheat temperature at least sufficiently high to initiate catalytic oxidation of said hydrocarbonaceousfeed, and introducing the preheated inlet stream into a first catalyst zone (24a)to carry out catalytic partial oxidation therein, characterized in that: (a) the first catalyst zone (24a) comprises a monolithic body (27) having a plurality of gas flow passages extending therethrough and having a catalytically effective amount of palladium and platinum catalytic components dispersed therein, the amounts of hydrocarbonaceous feed, H 2 0 and oxygen introduced into said first catalyst zone (24a) being controlled to maintain in said inlet stream an H20 to C ratio of at least about 0.5, and an 0 2 to C ratio of at least about 0.2 but less than the stoichiometric amount of oxygen necessary to oxidize all the carbon of said feed to C0 2 ; (b) contacting the preheated inlet stream within said first catalyst zone (24a) with said palladium and platinum catalytic component on said monolith (27) to initiate and sustain therein catalytic oxidation of at least a sufficient quantity of said hydrocarbon feed to attain an elevated temperature within said first catalyst zone (24a) at least high enough to crack unoxidized C or heavier hydrocarbons, if any be present, to light hydrocarbons not heavier than C 4 hydrocarbons, the temperature of at least a portion of said monolithic body (27) being at least about 121°C higher than the ignition temperature of said inlet stream, whereby to produce a first catalyst zone effluent comprising, predominantly, hydrogen, carbon oxides and said light hydrocarbons; and (c) withdrawing the first catalyst zone effluent as a hydrogen-rich gas.
Claim 3
Dependent Claim
46 words
The process of claim 1 further characterized in that the hydrocarbonaceous feed is a hydrocarbon feed and the elevated temperature attained in step (b) is high enough to catalytically steam reform hydrocarbons remaining in said first catalyst zone effluent without necessity of supplying external heat thereto.
Claim 4
Dependent Claim
37 words
The'process of claim 1 or claim 2 further characterized in that said first catalyst zone (24a) comprises palladium, platinum and, optionally, rhodium catalytic components distended upon a refractory metal oxide support layer carried on said monolithic body.
Claim 5
Dependent Claim
32 words
The process of claim 3 further characterized in that a volumetric hourly rate of at least 100,000 volumes of throughput per volume of catalyst is maintained in said first catalyst zone (24a).
Claim 6
Dependent Claim
59 words
The process of claim 1 or claim 2 further characterized in that the amounts of hydrocarbonaceous feed, H 2 0 and oxygen introduced into said first catalyst zone (24a) are controlled to provide therein an H 2 0 to C ratio of about 0.5 to 5 and an 0 2 to C ratio of from about 0.2 to 0.8.
Claim 7
Dependent Claim
30 words
The process of claim 1 or claim 2 further characterized in that the process is carried out at a pressure of about atmospheric pressure up to 142 kg/cm 2 .
Claim 8
Dependent Claim
97 words
The process of claim 1 or claim 2 further characterized in that the first catalyst zone effluent, while it is at an elevated temperature, is passed from said first catalyst zone (24a) to a second catalyst zone (24b) containing a platinum group metal steam reforming catalyst (31) therein and.is contacted in said second catalyst zone (24b) with said steam reforming catalyst (31) to react hydrocarbons in said first catalyst zone effluent with H 2 0 to produce hydrogen and carbon oxides therefrom, and the effluent of said second catalyst zone (24b) is withdrawn as a hydrogen-rich gas.
Claim 9
Dependent Claim
57 words
The process of claim 7 further characterized in that a volumetric hourly rate of at least 100,000 volumes of throughput per volume of catalyst is maintained in said first catalyst zone (24a) and a volumetric hourly rate of about 2,000 to 20,000 volumes of throughput per volume of catalyst is maintained in said second catalyst zone (24b).
Claim 10
Dependent Claim
28 words
The process of claim 8 further characterized in that the process is carried out at a pressure of about atmospheric pressure up to 142 kg/ cm 2 .
Claim 11
Dependent Claim
153 words
The process of claim 2 further characterized in that said oxidant gas comprises oxygen-enriched air and wherein the amounts of feed, H 2 0 and oxygen introduced into said first catalyst zone (24a) are controlled to maintain in said inlet stream an H 2 0 to C ratio of from about 0.5 to 5 and an 0 2 to C ratio of from about 0.35 to 0.65, and said effluent of said second catalyst zone (24b) comprises a synthesis gas which is cooled, the carbon monoxide in said cooled synthesis gas is reacted with H 2 0 to produce hydrogen; sulfur containing compounds and H 2 0 are removed from said synthesis gas; said synthesis gas is passed into an ammonia synthesis loop (286, 290,292, 298) to react the hydrogen with nitrogen thereof over an ammonia synthesis catalyst at ammonia synthesis conditions; and ammonia is withdrawn as product from said ammonia synthesis loop.
Claim 12
Dependent Claim
47 words
The process of claim 10 further characterized in that said-hydrocarbonaceous feed is a hydrocarbon feed, the air in the inlet stream (240) is enriched to at least about 33%, preferably about 33 to 50%, by volume oxygen and the preheat temperature is from about 427° to 760°C.
Claim 13
Dependent Claim
70 words
The process of claim 11 further characterized in that the amounts of feed, H 2 0, air and oxygen introduced into said first catalyst zone (24a) are controlled to maintain in.said inlet stream (240) an H 2 D to C ratio of from about 1 to 4, and an 0 2 to C ratio of from about 0.5 to 0.6, and the process is carried out at an elevated pressure.
Claim 14
Dependent Claim
44 words
The process of claim 11 further characterized in that said first catalyst zone (242a) is maintained at a temperature of from about 954° to 1316°C and the first catalyst zone effluent is introduced into said second catalyst zone (242b) at substantially the same temperature.
Claim 15
Dependent Claim
137 words
The process of claim 2 further characterized in that said oxidant gas comprises oxygen and the amounts of feed, H 2 0 and oxygen introduced into said first catalyst zone (142a) are controlled to maintain in said inlet stream (136) an H 2 0 to C ratio of from about 0.5 to 3 and an 0 2 to C ratio of from about 0.35 to 0.65, and said effluent of said second catalyst zone comprises a synthesis gas, the synthesis gas is cooled and sulfur-containing compounds and H 2 0 are removed therefrom; said synthesis gas is passed to a methanol synthesis loop (148, 150, 154, 156, 160, 166) to react the hydrogen with carbon oxides thereof over a methanol synthesis catalyst at methanol synthesis conditions; and methanol is withdrawn as product from said methanol synthesis loop.
Claim 16
Dependent Claim
26 words
The process of claim 14 further characterized in that said hydrocarbonaceous feed is a hydrocarbon feed and the preheat temperature is from about 472° to 760°C.
Claim 17
Dependent Claim
69 words
The process of claim 15 further characterized in that the'amounts of feed, H 2 0 and oxygen introduced into said first catalyst zone (142a) are controlled to maintain in said inlet stream (136) an H 2 0 to C ratio of from about 1 to 2.5 and an 0 2 to C ratio of from about 0.5 to 0.6, and the process is carried out at an elevated pressure.
Claim 18
Dependent Claim
41 words
The process of claim 15 further characterized in that said first catalyst zone is maintained at a temperature of from about 954° to 1316°C and the first zone effluent is introduced into said second catalyst zone at substantially the same temperature.
Claim 19
Dependent Claim
240 words
The process of claim 1 further characterized in that said hydrocarbonaceous feed comprises the liquid hydrocarbon by-product of a coal gasification process in which coal is reacted with steam and oxygen to produce (i) gasifier synthesis gas which is methanated to produce a synthesis natural gas and (ii) said liquid hydrocarbon by-product, and wherein said inlet stream is preheated to a temperature of less than about 649°C, and the temperature of at least a portion of said monolith (27) is at least about 139°C greater than the ignition temperature of said inlet stream, but not more than about 1,093°C, said oxidant gas comprises oxygen, and the amounts of liquid hydrocarbon by-product, H 2 0 and oxygen intro- ducted into said first catalyst zone are controlled to maintain in said inlet stream (378) an H 2 0 to C ratio of from about 0.5 to 5 and an 0 2 to C ratio of from about 0.15 to 0.4, whereby to produce a first catalyst zone effluent comprising primarily methane, hydrogen, carbon monoxide, carbon dioxide, H 2 0 and C 2 - C 4 hydrocarbons; wherein said effluent is passed to a treatment zone (384, 342) for the removal of carbon dioxide and water therefrom; the thus-treated first catalyst zone effluent is withdrawn as a secondary synthesis gas; and said gasifier synthesis gas and said secondary synthesis gas are methanated in a methanation zone (390) to provide synthetic natural gas therefrom.
Claim 20
Dependent Claim
95 words
The process of claim 18 further characterized in that said first catalyst zone effluent, while still at an elevated temperature, is passed from said first catalyst zone (380a) to a second catalyst zone (380b) containing a steam reforming catalyst therein, and the first catalyst zone effluent is contacted in said second catalyst zone (380b) with said steam reforming catalyst (31) to react hydrocarbons therein with H 2 0 to produce hydrogen and carbon oxides therefrom, and then the effluent of said second catalyst zone is passed as said effluent to said treatment zone (384, 342).
Claim 21
Dependent Claim
16 words
The process of claim 19 further characterized in that preheat temperature is about 427° to 649°C.
Claim 22
Dependent Claim
44 words
The process of claim 19 further characterized in that said first catalyst zone (380a) is maintained at a temperature of from about 760° to 1093°C and the first catalyst zone effluent is introduced into said second catalyst zone (380b) at substantially the same temperature.
Claim 23
Dependent Claim
166 words
The process of claim 2 further characterized in that said hydrocarbonaceous feed is a normally gaseous hydrocarbon feed, said oxidant gas comprises oxygen and the amounts of feed, H 2 0 and oxygen introduced into said first catalyst zone (442a) are controlled to maintain in said inlet stream an H 2 0 to C ratio of from about 0.5 to 5 and an 0 2 to C ratio of from about 0.4 to about 0.65, and wherein the effluent of said second catalyst zone (442b) comprises a gas mixture which includes hydrogen, carbon monoxide and carbon dioxide and is passed to a carbon dioxide removal zone (448) in which carbon dioxide is separated therefrom, the separated carbon dioxide is recycled to said inlet stream (440) in an amount sufficient so that said inlet stream comprises from about 5 to 20 mole percent carbon dioxide; and the carbon dioxide-depleted effluent of said second catalyst zone (442b) is obtained as a synthesis gas comprising hydrogen and carbon oxides.
Claim 24
Dependent Claim
89 words
The process of claim 22 further characterized in that normally liquid hydrocarbons are synthesized from said synthesis gas comprising hydrogen and carbon oxides by passing said synthesis gas to a hydrocarbon synthesis reactor (458) in which CO and H 2 are reacted to form hydrocarbons of different molecular weight, including normally liquid hydrocarbons, separating the resulting hydrocarbons into product and by-product streams, and recycling the resulting by-product stream of hydrocarbons to said inlet stream (440) as a part of said hydrocarbon feed and withdrawing the product stream of hydrocarbons.
Claim 25
Dependent Claim
28 words
The process of claim 23 further characterized in that the preheat temperature is from about 427° to 760°C and the process is carried out at an elevated pressure.
Claim 26
Dependent Claim
42 words
The process of claim 23 further characterized in that said first catalyst zone (442a) is maintained at a temperature from about 954° to 1316°C and the first zone effluent is introduced into said second catalyst (442b) zone at substantially the same temperature.
Claim 27
Dependent Claim
44 words
The process of claim 1 or claim 7 wherein the catalytically effective metals of the first catalyst zone comprise 10 to 90% by weight, preferably 25 to 75% by weight palladium, and 90 to 10% by weight, preferably 75 to 25% by weight platinum.,
Claim 28
Dependent Claim
41 words
The process of claim 26 wherein the catalytically effective metals of the second catalyst zone comprise 90 to 10% by weight, preferably 80 to 60% by weight platinum and 10 to 90% by weight, preferably 20 to 40% by weight rhodium.
Claim 29
Dependent Claim
29 words
The process of claim 26 wherein the catalytically effective metals of the first catalyst zone comprise 60 to 40% by weight palladium and 40 to 60% by weight platinum.
References Cited (Backward Citations)
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