Process for converting a carbonaceous material to methane, methanol and/or dimethyl ether using microchannel process technology
원문보기
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
B01J-019/00
C01B-003/22
C01B-003/32
C01B-003/50
C01B-003/52
C01B-003/56
C07C-001/04
C07C-001/20
C07C-002/84
C07C-009/06
C07C-011/04
C07C-029/152
C10J-003/00
출원번호
US-0420942
(2009-04-09)
등록번호
US-9908093
(2018-03-06)
발명자
/ 주소
Simmons, Wayne W.
Litt, Robert Dwayne
Mazanec, Terry
Tonkovich, Anna Lee
출원인 / 주소
Velocys, Inc.
대리인 / 주소
Renner, Otto, Boisselle & Sklar, LLP
인용정보
피인용 횟수 :
0인용 특허 :
76
초록▼
This invention relates to a process for converting a carbonaceous material to a desired product comprising methane, methanol and/or dimethyl ether, the process comprising: gasifying the carbonaceous material at a temperature in excess of about 700° C. to form synthesis gas; and flowing the synthesis
This invention relates to a process for converting a carbonaceous material to a desired product comprising methane, methanol and/or dimethyl ether, the process comprising: gasifying the carbonaceous material at a temperature in excess of about 700° C. to form synthesis gas; and flowing the synthesis gas through two or more reaction zones in a microchannel reactor to convert the synthesis gas to the desired product.
대표청구항▼
1. A process for converting a carbonaceous material to a desired product comprising methane, methanol or dimethyl ether, the carbonaceous material being selected from biomass and waste material, the process comprising: (A) gasifying the carbonaceous material in the presence of a gasification agent a
1. A process for converting a carbonaceous material to a desired product comprising methane, methanol or dimethyl ether, the carbonaceous material being selected from biomass and waste material, the process comprising: (A) gasifying the carbonaceous material in the presence of a gasification agent at a temperature of at least about 700° C. in a gasifier to form synthesis gas, the synthesis gas comprising H2 and CO, water, particulate solids, and contaminants, the contaminants being selected from sulfur, halogen, selenium, phosphorus and arsenic; andflowing the synthesis gas out of the gasifier and reducing the temperature of the synthesis gas flowing out of the gasifier;flowing the synthesis gas through one or more gas-liquid sorption devices, temperature swing adsorption devices, pressure swing adsorption devices, microchannel devices containing layers of nanofibers or nano-composite films, cyclones and/or condensers to reduce the level of water, particulate solids and contaminants in the synthesis gas;adding H2 to the synthesis gas to form an upgraded synthesis gas with a molar ratio of H2 to CO in the range from about 1.5 to about 4;converting the upgraded synthesis gas to the desired product in a microchannel reactor, the microchannel reactor including a first reaction zone and another reaction zone and comprising a plurality of process microchannels and a plurality of heat exchange channels, the process microchannels having lengths in the range from about 0.2 to about 3 meters;the upgraded synthesis gas being converted to the desired product using the following exothermic equilibrium limited reaction process steps (B)(I) and (B)(II); whereinstep (B)(I) comprises flowing the upgraded synthesis gas through a first reaction zone in the microchannel reactor at a first reaction temperature in contact with a first catalyst to form an intermediate product composition, the first catalyst being in the form of a fixed bed of particulate solids, the particulate solids of the first catalyst having a median particle diameter in the range from about 1 to about 1000 microns, the intermediate product composition comprising H2, CO and the desired product, the approach to equilibrium for conversion of the CO in the first reaction zone being at least about 5%; andstep (B)(II) comprises flowing the intermediate product composition from the previous step through another reaction zone in the microchannel reactor at another reaction temperature in contact with another catalyst to form the desired product, the another catalyst being in the form of a fixed bed of particulate solids, the particulate solids of the another catalyst having a median particle diameter in the range from about 1 to about 1000 microns, the approach to equilibrium for conversion of the CO in the another reaction zone being at least about 5%, the another reaction temperature being at least about 5° C. less than the first reaction temperature; andflowing a heat exchange fluid in the heat exchange channels during steps (B)(I) and (B)(II), and transferring heat from the process microchannels to the heat exchange channels, wherein the heat exchange fluid used in the heat exchange channels during steps (B)(I) and (B)(II) comprises steam, liquid water and/or air, and at least part of the steam, liquid water and/or air used in the heat exchange channels during steps (B)(I) and (B)(II) flows from the heat exchange channels to the gasifier and is used as the gasification agent during step (A). 2. The process of claim 1 wherein nitrogen is separated from air in a nitrogen separator prior to step (A) to provide an oxygen enriched air or purified oxygen, and the carbonaceous material is gasified during step (A) in the presence of the oxygen enriched air or purified oxygen. 3. The process of claim 2 wherein the nitrogen is separated from the air in a microchannel separator using an ionic liquid as an absorbent liquid. 4. The process of claim 1 wherein the carbonaceous material is pyrolyzed prior to step (A) resulting in the formation of a pyrolytic oil, the pyrolytic oil being gasified during step (A). 5. The process of claim 1 wherein the level of sulfur contaminants in the synthesis gas is reduced using a ZnO guardbed. 6. The process of claim 1 wherein the carbonaceous material comprises municipal solid waste, hazardous waste, refuse derived fuel, tires, trash, sewage sludge, animal waste, petroleum coke, trash, garbage, agricultural waste, corn stover, switch grass, wood cuttings, timber, grass clippings, construction demolition materials, plastic material, cotton gin waste, or a mixture of two or more thereof. 7. The process of claim 1 wherein the ratio of H2 to CO for the upgraded synthesis gas is in the range from about 1.5 to about 2.5. 8. The process of claim 1 wherein subsequent to step (B)(I) but prior to step (B)(II) the intermediate product composition formed in step (B)(I) flows through an additional reaction zone in the microchannel reactor at an additional reaction temperature in contact with an additional catalyst to form another intermediate product composition, the additional catalyst being in the form of a fixed bed of particulate solids, the particulate solids of the additional catalyst having a median particle diameter in the range from about 1 to about 1000 microns, the another intermediate product composition comprising synthesis gas and the desired product, the approach to equilibrium for the conversion of the synthesis gas in the additional reaction zone being at least about 5%. 9. The process of claim 1 wherein the conversion of CO in the first reaction zone is in the range from about 5% to about 95%, and the conversion of CO in the another reaction zone is in the range from about 5% to about 99%. 10. The process of claim 1 wherein the first catalyst in step (B)(I) has the same composition as the another catalyst in step (B)(II). 11. The process of claim 8 wherein the additional catalyst has the same composition as the first catalyst in step (B)(I), the another catalyst in step (B)(II), or both the first catalyst in step (B)(I) and the another catalyst in step (B)(II). 12. The process of claim 1 wherein the first catalyst in step (B)(I) has a different composition than the another catalyst in step (B)(II). 13. The process of claim 8 wherein the additional catalyst has a different composition than the first catalyst in step (B)(I), the another catalyst in step (B)(II), or both the first catalyst in step (B)(I) and the another catalyst in step (B)(II). 14. The process of claim 1 wherein the microchannel reactor comprises at least one manifold for flowing synthesis gas into the process microchannels, at least one manifold for flowing product out of the process microchannels, at least one manifold for flowing a heat exchange fluid into the heat exchange channels, and at least one manifold for flowing the heat exchange fluid out of the heat exchange channels. 15. The process of claim 1 wherein one or more microchannel reactors are used to form the desired product, the one or more microchannel reactors being positioned in a vessel. 16. The process of claim 15 wherein each microchannel reactor comprises from about 100 to about 50,000 process microchannels, and the vessel contains from 1 to about 1000 microchannel reactors. 17. The process of claim 15 wherein the vessel is a pressurized vessel. 18. The process of claim 1 wherein the process microchannels have an internal height of up to about 10 mm. 19. The process of claim 1 wherein the process microchannels and heat exchange channels are made of a material comprising: steel; aluminum; titanium; nickel; copper; an alloy of any of the foregoing metals; monel; inconel; brass; quartz; silicon; or a combination of two or more thereof. 20. The process of claim 1 wherein fluid flowing in the process microchannels contacts surface features in the process microchannels, the contacting of the surface features imparting a disruptive flow to the fluid. 21. The process of claim 1 wherein the heat exchange channels comprises microchannels. 22. The process of claim 1 wherein the process microchannels and the heat exchange channels have rectangular cross sections. 23. The process of claim 1 wherein the first catalyst and/or the another catalyst comprises a copper oxide, zinc oxide and/or an aluminum oxide. 24. The process of claim 23 wherein the first catalyst and/or the another catalyst further comprise an oxide of one or more rare earth elements, zirconium, yttrium, chromium, silver, gallium, vanadium, molybdenum, tungsten, titanium, or a mixture of two or more thereof. 25. The process of claim 1 wherein the first catalyst and/or the another catalyst comprise nickel, iron, cobalt, ruthenium, molybdenum, vanadium, titanium, an oxide of any of the foregoing metals, or a mixture of two or more of the foregoing metals and/or oxides. 26. The process of claim 1 wherein the first catalyst and/or another catalyst comprise vanadium and/or molybdenum in the form of a free metal, hydroxide, oxide and/or sulfide in combination with one or more salts, hydroxides, oxides or sulfides of one or more metals belonging to Group IA, IIA or IIIB from the Periodic Table. 27. The process of claim 1 wherein the process microchannels have at least one heat transfer wall, the heat flux for heat exchange within the microchannel reactor being in the range from about 0.01 to about 500 watts per square centimeter of surface area of the heat transfer wall. 28. The process of claim 1 wherein the pressure in the first reaction zone and/or the another reaction zone is in the range up to about 50 atmospheres. 29. The process of claim 1 wherein the average temperature in the first reaction zone is in the range from about 150 to about 400° C. 30. The process of claim 1 wherein the average temperature in the first reaction zone is in the range from about 250 to about 850° C. 31. The process of claim 1 wherein the contact time within the first reaction zone and/or the second reaction zone is up to about 2000 milliseconds. 32. The process of claim 1 wherein the process microchannels have fluid flowing in them in one direction, and the heat exchange channels have fluid flow in a direction that is co-current or counter-current to the flow of fluid in the process microchannels. 33. The process of claim 1 wherein the process microchannels have fluid flowing in them in one direction, and the heat exchange channels have fluid flowing in them in a direction that is cross-current to the flow of fluid in the process microchannels. 34. The process of claim 1 wherein the length of the process microchannels and the length of the heat exchange channels are about the same. 35. The process of claim 1 wherein the first catalyst and/or another catalyst comprise a graded catalyst. 36. The process of claim 1 wherein the Quality Index Factor for the microchannel reactor is less than about 50%. 37. The process of claim 1 wherein the superficial velocity for fluid flowing in the process microchannels is at least about 0.01 m/s. 38. The process of claim 1 wherein the space velocity for fluid flowing in the process microchannels is at least about 1000 hr−1. 39. The process of claim 1 wherein the pressure drop for fluid flowing in the process microchannels is up to about 10 atmospheres per meter. 40. The process of claim 1 wherein the Reynolds number for the flow of fluid in the process microchannels is in the range from about 10 to about 4000. 41. The process of claim 1 wherein the process microchannels are formed by positioning a waveform between planar sheets. 42. The process of claim 1 wherein the heat exchange channels are formed by positioning a waveform between planar sheets. 43. The process of claim 1 wherein the desired product comprises methanol, and the methanol is converted to one or more olefins. 44. The process of claim 43 wherein the methanol is converted to one or more olefins in a microchannel reactor. 45. The process of claim 43 wherein the methanol is converted to one or more olefins in the presence of a silico-alumino-phosphate catalyst. 46. The process of claim 1 wherein the desired product comprises methane, and the methane is converted to ethane, ethylene, or a mixture thereof. 47. The process of claim 46 wherein the methane is converted to ethane, ethylene, or a mixture thereof, in a microchannel reactor. 48. The process of claim 46 wherein the methane is converted to ethane, ethylene, or a mixture thereof, in the presence of an oxidative coupling catalyst. 49. The process of claim 1 wherein the product comprises dimethyl ether and CO2, the process further comprising reacting the CO2 with methane to form a mixture of CO and H2. 50. The process of claim 49 wherein the reaction of CO2 with methane is conducted in a microchannel reactor. 51. The process of claim 1 wherein the microchannel reactor is constructed of stainless steel with one or more copper or aluminum waveforms being used for forming the process microchannels. 52. The process of claim 1 wherein at least part of the desired product is separated from the intermediate product composition subsequent to or during step (B)(I) but prior to step (B)(II). 53. The process of claim 1, wherein the carbonaceous material is gasified in a counter-current fixed bed gasifier to form the synthesis gas. 54. The process of claim 1, wherein the carbonaceous material is gasified in a co-current fixed bed gasifier to form the synthesis gas. 55. The process of claim 1, wherein the carbonaceous material is gasified in a plasma based gasification system to form the synthesis gas. 56. The process of claim 4, wherein liquid hydrocarbons are separated from the synthesis gas prior to step (B)(I) and are combined with the carbonaceous material prior to being pyrolyzed. 57. The process of claim 1, wherein the carbonaceous material is gasified in a fluidized bed gasifier. 58. The process of claim 1, wherein the carbonaceous material is gasified in an entrained flow gasifier. 59. The process of claim 1 wherein the particulate solids are separated from the synthesis gas by flowing the synthesis gas through a cyclone.
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