초록 ▼

In a process for converting methane to liquid hydrocarbons, a feed containing methane is contacted with 0 dehydrocyclization catalyst under conditions effective to convert said methane to aromatic hydrocarbons, including benzene and/or naphthalene, and produce a first effluent stream comprising hydr

In a process for converting methane to liquid hydrocarbons, a feed containing methane is contacted with 0 dehydrocyclization catalyst under conditions effective to convert said methane to aromatic hydrocarbons, including benzene and/or naphthalene, and produce a first effluent stream comprising hydrogen and 0t least 5 wt % m>35 aromatic hydrocarbons than said feed. At least part the aromatic hydrocarbons from the first effluent stream is then reacted with hydrogen to produce a second effluent stream having a reduced benzene and/or naphthalene content compared with said first effluent stream.

대표청구항 ▼

The invention claimed is: 1. A process for converting methane to higher 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 conditions effective to convert said methane to aromatic hydrocarbo

The invention claimed is: 1. A process for converting methane to higher 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 conditions effective to convert said methane to aromatic hydrocarbons, including benzene and naphthalene, 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; and (b) reacting at least part said aromatic hydrocarbons from said first effluent stream with hydrogen to produce a second effluent stream having a reduced benzene and/or naphthalene content compared with said first effluent stream, wherein said reacting hydrogenates and hydrocracks at least a portion of the naphthalene in said first effluent stream to produce alkylated single ring aromatic compounds. 2. The process of claim 1, wherein at least part of the hydrogen used in (b) is from said first effluent stream. 3. A process for converting methane to higher hydrocarbons and hydrogen, the process comprising: (a) contacting a feed containing methane with a dehydrocyclization catalyst under non-oxidizing conditions effective to convert said methane to aromatic hydrocarbons, including benzene and/or naphthalene, 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; (b) reacting at least part of said aromatic hydrocarbons from said first effluent stream with at least part of the hydrogen from said first effluent stream, said reacting being conducted at a first location and producing a second effluent stream having a reduced benzene and/or naphthalene content compared with said first effluent stream; (c) transporting at least part of said second effluent stream to a second location remote from said first location; and (d) dehydrogenating at least part of said second effluent stream at said second location to produce hydrogen and a third effluent stream having an enhanced benzene and/or naphthalene content compared with said second effluent stream. 4. The process of claim 3 further comprising reacting at least part of the hydrogen from said first effluent stream with an oxygen containing species to produce a further effluent stream comprising water and hydrocarbon; and recycling at least part of the hydrocarbon in said further effluent stream to said contacting (a). 5. The process of claim 4 wherein said oxygen-containing species comprises carbon monoxide and/or carbon dioxide. 6. The process of claim 5 wherein said oxygen-containing species comprises carbon dioxide introduced to the process as part of a natural gas stream. 7. The process of claim 6 wherein said natural gas stream also contains at least part of the methane in the feed in (a). 8. The process of claim 4 wherein said further effluent stream comprises water and methane, ethane or a mixture of methane and ethane. 9. The process of claim 5 wherein oxygen-containing species comprises carbon monoxide and said further effluent stream comprises one or more of C2 to C5 paraffins and olefins, single-ring aromatic hydrocarbons and C1 to C3 alcohols. 10. The process of claim 4 wherein said reacting at least part of the hydrogen from said first effluent stream with an oxygen containing species includes selective hydrogen combustion. 11. The process of claim 3 wherein said feed in (a) also contains at least one of H2, H2O, CO and CO2. 12. The process of claim 3 wherein said feed in (a) contains less than 5 wt % of C3+ hydrocarbons. 13. The process of claim 1 wherein said conditions in (a) are non-oxidizing conditions. 14. The process of claim 3 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. 15. The process of claim 3 wherein said dehydrocyclization catalyst in (a) 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. 16. The process of claim 1 wherein said reacting (b) hydrocracks at least a portion of the naphthalene or benzene in said first effluent stream to produce normal and isoparaffins. 17. The process of claim 3 and further comprising separating at least one aromatic hydrocarbon from said first effluent stream. 18. The process of claim 17 wherein part of said first effluent stream remaining after separation of at least one aromatic hydrocarbon is used as fuel to provide heat to said contacting (a). 19. The process of claim 3 and further comprising alkylating at least one aromatic hydrocarbon in said first effluent stream with an alkylating agent. 20. The process of claim 19 wherein said alkylating agent comprises ethylene produced in said contacting (a). 21. The process of claim 19 wherein said alkylating agent comprises carbon monoxide and hydrogen or a reaction product thereof. 22. The process of claim 1 further comprising reacting at least part of the hydrogen from said first effluent stream with an oxygen containing species to produce a further effluent stream comprising water and hydrocarbon; and recycling at least part of the hydrocarbon in said further effluent stream to said contacting (a). 23. The process of claim 22 wherein said oxygen-containing species comprises carbon monoxide and/or carbon dioxide. 24. The process of claim 23 wherein said oxygen-containing species comprises carbon dioxide introduced to the process as part of a natural gas stream. 25. The process of claim 24 wherein said natural gas stream also contains at least part of the methane in the feed in (a). 26. The process of claim 22 wherein said further effluent stream comprises water and methane, ethane or a mixture of methane and ethane. 27. The process of claim 22 wherein oxygen-containing species comprises carbon monoxide and said further effluent stream comprises one or more of C2 to C5 paraffins and olefins, single-ring aromatic hydrocarbons and C1 to C3 alcohols. 28. The process of claim 22 wherein said reacting at least part of the hydrogen from said first effluent stream with an oxygen containing species includes selective hydrogen combustion. 29. The process of claim 22 wherein said feed in (a) also contains at least one of H2, H2O, CO and CO2. 30. The process of claim 22 wherein said feed in (a) contains less than 5 wt % of C3+ hydrocarbons. 31. The process of claim 22 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. 32. The process of claim 22 wherein said dehydrocyclization catalyst in (a) 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. 33. The process of claim 22 and further comprising separating at least one aromatic hydrocarbon from said first effluent stream. 34. The process of claim 33 wherein part of said first effluent stream remaining after separation of at least one aromatic hydrocarbon is used as fuel to provide heat to said contacting (a). 35. The process of claim 22 and further comprising alkylating at least one aromatic hydrocarbon in said first effluent stream with an alkylating agent. 36. The process of claim 35 wherein said alkylating agent comprises ethylene produced in said contacting (a). 37. The process of claim 35 wherein said alkylating agent comprises carbon monoxide and hydrogen or a reaction product thereof. 38. A process for converting methane to higher hydrocarbons and hydrogen, the process comprising: (a) contacting a feed containing methane with a dehydrocyclization catalyst under non-oxidizing conditions effective to convert said methane to aromatic hydrocarbons, including benzene and/or naphthalene, 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; (b) reacting at least part of said aromatic hydrocarbons from said first effluent stream with at least part of the hydrogen from said first effluent stream, said reacting being conducted at a first location and producing a second effluent stream having a reduced benzene and/or naphthalene content compared with said first effluent stream; (c) transporting at least part of said second effluent stream to a second location remote from said first location; (d) dehydrogenating at least part of said second effluent stream at said second location to produce hydrogen and a third effluent stream having an enhanced benzene and/or naphthalene content compared with said second effluent stream; and (e) reacting at least part of the hydrogen from said first effluent stream with an oxygen containing species to produce a further effluent stream comprising water and hydrocarbon; and recycling at least part of the hydrocarbon in said further effluent stream to said contacting (a).