IPC분류정보
국가/구분 |
United States(US) Patent
등록
|
국제특허분류(IPC7판) |
|
출원번호 |
UP-0792359
(2005-12-02)
|
등록번호 |
US-7759535
(2010-08-09)
|
국제출원번호 |
PCT/US2005/044042
(2005-12-02)
|
§371/§102 date |
20070605
(20070605)
|
국제공개번호 |
WO06/068814
(2006-06-29)
|
발명자
/ 주소 |
- Iaccino, Larry L.
- Feng, Xiaobing
- Vincent, Matthew J.
- Stavens, Elizabeth L.
|
출원인 / 주소 |
- ExxonMobil Chemical Patents Inc.
|
대리인 / 주소 |
|
인용정보 |
피인용 횟수 :
4 인용 특허 :
11 |
초록
▼
In a process for converting methane to higher hydrocarbons including aromatic hydrocarbons, a feed containing methane is contacted with a dehydrocyclization catalyst under conditions effective to convert said methane to aromatic hydrocarbons and produce a first effluent stream comprising aromatic hy
In a process for converting methane to higher hydrocarbons including aromatic hydrocarbons, a feed containing methane is contacted with a dehydrocyclization catalyst under conditions effective to convert said methane to aromatic hydrocarbons and produce a first effluent stream comprising aromatic hydrocarbons and hydrogen, wherein said first effluent stream comprises at least 5 wt % more aromatic hydrocarbons than said feed. At least part of the hydrogen from said first effluent stream is then reacted with an oxygen-containing species, such as carbon dioxide, to produce a second effluent stream having a reduced hydrogen content compared with said first effluent stream.
대표청구항
▼
The invention claimed is: 1. A process for converting methane to higher hydrocarbons including aromatic hydrocarbons, the process comprising: (a) contacting a feed containing methane with a dehydrocyclization catalyst under conditions effective to convert said methane to aromatic hydrocarbons and p
The invention claimed is: 1. A process for converting methane to higher hydrocarbons including aromatic hydrocarbons, the process comprising: (a) contacting a feed containing methane with a dehydrocyclization catalyst under conditions effective to convert said methane to aromatic hydrocarbons and produce a first effluent stream comprising aromatic hydrocarbons and hydrogen, wherein said first effluent stream comprises at least 5 wt % more aromatic rings than said feed; and (b) reacting at least part of the hydrogen from said first effluent stream with an oxygen-containing species selected from carbon monoxide, carbon dioxide, and mixtures thereof under conditions effective to produce a second effluent stream having a reduced hydrogen content compared with said first effluent stream; wherein reacting (b) comprises: (i) reacting hydrogen to form hydrocarbons and water, (ii) removing at least a portion of the water from said second effluent stream, and (iii) recycling at least portion of the hydrocarbons from said second effluent stream to said contacting (a). 2. The process of claim 1 wherein said feed in (a) also contains at least one of H2, H2O, CO and CO2. 3. The process of claim 1 wherein said feed in (a) contains less than 5 wt % of C3+ hydrocarbons. 4. The process of claim 1 wherein said conditions in (a) are non-oxidizing conditions. 5. The process of claim 1 wherein said conditions in (a) include a temperature of about 400° C. to about 1200° C., a pressure of about 1 kPa to about 1000 kPa and a weight hourly space velocity of about 0.1 hr−1 to about 1000 hr−1. 6. The process of claim 1 wherein said dehydrocyclization catalyst comprises a metal or compound thereof on an inorganic support. 7. The process of claim 6 wherein said metal or compound thereof comprises at least one of calcium, magnesium, barium, yttrium, lanthanum, scandium, cerium, titanium, zirconium, hafnium, vanadium, niobium, tantalum, chromium, molybdenum, tungsten, manganese, rhenium, iron, ruthenium, cobalt, rhodium, iridium, nickel, palladium, copper, silver, gold, zinc, aluminum, gallium, germanium, indium, tin, lead, bismuth or a transuranium element. 8. The process of claim 6 wherein said inorganic support comprises a microporous or mesoporous material. 9. The process of claim 1 wherein said dehydrocyclization catalyst comprises at least one of molybdenum, tungsten, rhenium, a molybdenum compound, a tungsten compound, and a rhenium compound on ZSM-5, silica or an aluminum oxide. 10. The process of claim 1 wherein said carbon dioxide is introduced to the process as part of a natural gas stream. 11. The process of claim 10 wherein said natural gas stream also contains at least part of the methane in the feed in (a). 12. The process of claim 1 wherein said hydrocarbons in said second effluent stream produced by said reacting (b) comprises methane, ethane or a mixture of methane and ethane. 13. The process of claim 1 wherein said hydrocarbons in second effluent stream produced by said reacting (b) comprises one or more of C2 to C5 paraffins and olefins, single-ring aromatic hydrocarbons and C1 to C3 alcohols. 14. The process of claim 1 wherein part of said first effluent stream is used as fuel to provide heat to said contacting (a). 15. The process of claim 1 and further comprising recovering aromatic hydrocarbons from said first effluent stream. 16. The process of claim 15 and further comprising alkylating at least part of said aromatic hydrocarbons in said first effluent stream with an alkylating agent, before or after said recovering. 17. The process of claim 16 wherein said alkylating agent comprises ethylene. 18. The process of claim 16 wherein said alkylating agent comprises carbon monoxide and hydrogen or a reaction product thereof. 19. The process of claim 18 wherein at least part of said carbon monoxide is produced by said reacting carbon dioxide with hydrogen and/or methane. 20. The process of claim 16 wherein said alkylating agent comprises methanol and/or dimethyl ether. 21. The process of claim 15 and further comprising reacting at least a portion of the recovered aromatic hydrocarbons with hydrogen from said first effluent stream. 22. The process of claim 21 wherein said reacting with hydrogen produces at least one of cyclohexene, cyclohexane, dihydronaphthalene (benzylcyclohexene), tetrahydronaphthalene (tetralin), hexahydronaphthalene (dicyclohexene), octahydronaphthalene and decahydronaphthalene (decalin). 23. The process of claim 21 wherein said at least a portion of said recovered aromatic hydrocarbons comprises naphthalene and said reacting with hydrogen produces alkylated benzenes. 24. A process for converting methane to higher hydrocarbons including aromatic hydrocarbons, the process comprising: (a) contacting a feed containing methane and at least one of H2, H2O, CO and CO2 with a dehydrocyclization catalyst under non-oxidizing conditions effective to convert said methane to aromatic hydrocarbons and produce a first effluent stream comprising aromatic hydrocarbons and hydrogen, wherein said first effluent stream comprises at least 5 wt % more aromatic rings than said feed, wherein said feed in (a) contains less than 5 wt % of C3+ hydrocarbons; and (b) reacting at least part of the hydrogen from said first effluent stream with an oxygen-containing species selected from carbon dioxide or carbon monoxide under conditions effective to produce a second effluent stream having a reduced hydrogen content compared with said first effluent stream; wherein reacting (b) comprises: (i) reacting hydrogen to form hydrocarbons and water, (ii) removing at least a portion of the water from said second effluent stream, and (iii) recycling at least portion of the hydrocarbons from said second effluent stream to said contacting (a). 25. The process of claim 24 and further comprising recovering aromatic hydrocarbons from said first effluent stream. 26. The process of claim 25 and further comprising alkylating at least part of said aromatic hydrocarbons in said first effluent stream with an alkylating agent, before or after said recovering. 27. The process of claim 26 wherein said alkylating agent comprises ethylene, carbon monoxide and hydrogen, or a reaction product of carbon monoxide and hydrogen. 28. The process of claim 25 and further comprising reacting at least a portion of the recovered aromatic hydrocarbons with hydrogen from said first effluent stream. 29. A process for converting methane to higher hydrocarbons including aromatic hydrocarbons, the process comprising: (a) contacting a feed containing methane and at least one of H2, H2O, CO and CO2 with a dehydrocyclization catalyst under non-oxidizing conditions effective to convert said methane to aromatic hydrocarbons and produce a first effluent stream comprising aromatic hydrocarbons and hydrogen, wherein said first effluent stream comprises at least 5 wt % more aromatic rings than said feed, wherein said feed in (a) contains less than 5 wt % of C3+ hydrocarbons; and (b) reacting at least part of the hydrogen from said first effluent stream with an oxygen-containing species selected from carbon dioxide or carbon monoxide under conditions effective to produce a second effluent stream having a reduced hydrogen content compared with said first effluent stream; wherein reacting (b) comprises: (i) reacting hydrogen to form hydrocarbons and water, (ii) removing at least a portion of the water from said second effluent stream, and (iii) recycling at least portion of the hydrocarbons from said second effluent stream to said contacting (a), wherein part of said first effluent stream is used as fuel to provide heat to said contacting (a). 30. The process of claim 29 and further comprising recovering aromatic hydrocarbons from said first effluent stream. 31. The process of claim 30 and further comprising alkylating at least part of said aromatic hydrocarbons in said first effluent stream with an alkylating agent, before or after said recovering. 32. The process of claim 31 wherein said alkylating agent comprises ethylene, carbon monoxide and hydrogen, or a reaction product of carbon monoxide and hydrogen. 33. The process of claim 30 and further comprising reacting at least a portion of the recovered aromatic hydrocarbons with hydrogen from said first effluent stream.
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