Process for upgrading a carbonaceous material using microchannel process technology
원문보기
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
B09B-003/00
C01B-003/34
C10J-003/46
출원번호
US-0421007
(2009-04-09)
등록번호
US-8100996
(2012-01-24)
발명자
/ 주소
Simmons, Wayne W.
Litt, Robert Dwayne
Tonkovich, Anna Lee
Silva, Laura J.
Ryan, Daniel Francis
Stangeland, Bruce
Brophy, John
McDaniel, Jeffrey S.
출원인 / 주소
Velocys, Inc.
대리인 / 주소
Renner, Otto, Boisselle & Sklar, LLP
인용정보
피인용 횟수 :
3인용 특허 :
74
초록▼
This invention relates to a process for converting a carbonaceous material to a desired product comprising one or more hydrocarbons or one or more alcohols, the process comprising: (A) gasifying the carbonaceous material at a temperature in excess of about 700° C. to form synthesis gas; and (B) flow
This invention relates to a process for converting a carbonaceous material to a desired product comprising one or more hydrocarbons or one or more alcohols, the process comprising: (A) gasifying the carbonaceous material at a temperature in excess of about 700° C. to form synthesis gas; and (B) flowing the synthesis gas in a microchannel reactor in contact with a catalyst to convert the synthesis gas to the desired product.
대표청구항▼
1. A process for converting a carbonaceous material to a desired product comprising one or more hydrocarbons or one or more alcohols, the process comprising: (A) gasifying the carbonaceous material at a temperature of at least about 700° C. to form synthesis gas, the carbonaceous material comprising
1. A process for converting a carbonaceous material to a desired product comprising one or more hydrocarbons or one or more alcohols, the process comprising: (A) gasifying the carbonaceous material at a temperature of at least about 700° C. to form synthesis gas, the carbonaceous material comprising coal, oil, biomass, solid-waste, food resource, or a mixture of two or more thereof; and(B) flowing the synthesis gas in a microchannel reactor in contact with a catalyst to convert the synthesis gas to the desired product. 2. 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, landfill gas, biogas, natural gas, or a mixture of two or more thereof. 3. The process of claim 1 wherein the carbonaceous material is gasified in a counter-current fixed bed gasifier, co-current fixed bed gasifier, fluidized bed gasifier, entrained flow gasifier, a molten metal reactor, or a plasma based gasification system. 4. The process of claim 1 wherein the carbonaceous material is gasified in the presence of a gasification agent. 5. The process of claim 4 wherein the gasification agent comprises steam, oxygen, air, or a mixture of two or more thereof. 6. The process of claim 1 wherein the carbonaceous material contacts steam and molten metal in a molten metal reactor and reacts to form the synthesis gas. 7. The process of claim 1 wherein the synthesis gas comprises H2 and CO. 8. The process of claim 7 wherein the ratio of H2 to CO is in the range from about 0.5 to about 4. 9. The process of claim 1 wherein the synthesis gas produced in step (A) comprises H2 and CO, and prior to step (B), an additional amount of H2 is added to the synthesis gas. 10. The process of claim 1 wherein the synthesis gas produced in step (A) further comprises solid particulates, the solid particulates being removed from the synthesis gas prior to step (B). 11. The process of claim 1 wherein the synthesis gas produced in step (A) further comprises water, at least part of the water being removed from the synthesis gas prior to step (B). 12. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel in thermal contact with a heat exchanger, the catalyst being in the process microchannel. 13. The process of claim 1 wherein the microchannel reactor comprises a plurality of process microchannels and a plurality of heat exchange channels, the catalyst being in the process microchannels. 14. The process of claim 1 wherein the microchannel reactor comprises a plurality of process microchannels and a plurality of heat exchange channels, the catalyst being in the process microchannels, each heat exchange channel being in thermal contact with at least one process microchannel, 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 a plurality of the microchannel reactors are positioned in a vessel, each microchannel reactor comprising a plurality of process microchannels and a plurality of heat exchange channels, the catalyst being in the process microchannels, each heat exchange channel being in thermal contact with at least one process microchannel, the vessel being equipped with a manifold for flowing the synthesis gas to the process microchannels, a manifold for flowing the product from the process microchannels, a manifold for flowing a heat exchange fluid to the heat exchange channels, and a manifold for flowing the heat exchange fluid from the heat exchange channels. 16. The process of claim 15 wherein each microchannel reactor comprises from about 100 to about 50,000 process microchannels, and the vessel comprises from 1 to about 1000 microchannel reactors. 17. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel, the process microchannel having an internal dimension of width or height of up to about 10 mm. 18. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel, the process microchannel having a length of up to about 10 meters. 19. The process of claim 1 wherein the microchannel reactor comprises at leat one process microchannel and at least one heat exchange channel, the process microchannel and heat exchange channel being made of a material comprising: aluminum; titanium; nickel; copper; an alloy of any of the foregoing metals; steel; monel; inconel; brass; quartz; silicon; or a combination of two or more thereof. 20. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel, fluid flowing in the process microchannel contacting surface features in the process microchannel, the contacting of the surface features imparting a disruptive flow to the fluid. 21. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel and at least one heat exchange channel, the heat exchange channel comprising a microchannel. 22. The process of claim 1 wherein the catalyst used in step (B) is a Fischer-Tropsch catalyst, the reaction that is conducted in the microchannel reactor during step (B) is a Fischer-Tropsch reaction, and the desired product comprises one or more hydrocarbons. 23. The process of claim 22 wherein the Fischer-Tropsch catalyst comprises one or more of Co, Fe, Ni, Ru, Re, Os, and/or an oxide thereof, or a mixture of two or more thereof. 24. The process of claim 23 wherein the Fischer-Tropsch catalyst further comprises one or more metals from Group IA, IIA, IIIB or IIIB of the Periodic Table and/or an oxide thereof, a lanthanide metal and/or oxide thereof, an actinide metal and/or oxide thereof, or a mixture of two or more thereof. 25. The process of claim 23 wherein the Fischer-Tropsch catalyst further comprises one or more of Li, B, Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, La, Ac, Ti, Zr, Ce or Th, and/or an oxide thereof, or a mixture of two or more thereof. 26. The process of claim 23 wherein the Fischer-Tropsch catalyst further comprises a support, the support comprising one or more of alumina, zirconia, silica, aluminum fluoride, fluorided alumina, bentonite, ceria, zinc oxide, silica-alumina, silicon carbide, molecular sieve, or a mixture of two or more thereof. 27. The process of claim 22 wherein the Fischer-Tropsch catalyst comprises a composition represented by the formula CoM1aM2bOx wherein M1 is Fe, Ni, Ru, Re, Os, or a mixture of two or more thereof;M2 is Li, B, Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, La, Ac, Ti, Zr, Ce or Th, or a mixture of two or more thereof;a is a number in the range of zero to about 0.5;b is a number in the range of zero to about 0.5; andx is the number of oxygens needed to fulfill the valency requirements of the elements present. 28. The process of claim 22 wherein the Fischer-Tropsch catalyst comprises Co supported on alumina, the Co loading being at least about 5% by weight. 29. The process of claim 28 wherein the Fischer-Tropsch catalyst further comprises Re, Ru or a mixture thereof. 30. The process of claim 22 wherein the pressure in the microchannel reactor is in the range up to about 50 atmospheres. 31. The process of claim 22 wherein the temperature in the microchannel reactor is in the range from about 150 to about 300° C. 32. The process of claim 22 wherein the contact time within the microchannel reactor is up to about 2000 milliseconds. 33. The process of claim 22 wherein the conversion of CO in the microchannel reactor is in the range from about 10 to about 99%. 34. The process of claim 22 wherein the selectivity to methane in the desired product is up to about 25%. 35. The process of claim 22 wherein the desired product comprises one or more hydrocarbons boiling at a temperature of at least about 30° C. at atmospheric pressure. 36. The process of claim 22 wherein the desired product comprises one or more hydrocarbons boiling above a temperature of about 175° C. at atmospheric pressure. 37. The process of claim 22 wherein the desired product comprises one or more paraffins and/or one or more olefins of about 5 to about 100 carbon atoms. 38. The process of claim 22 wherein the desired product comprises one or more olefins, one or more normal paraffins, one or more isoparaffins, or a mixture of two or more thereof. 39. The process of claim 22 wherein the desired product is further processed using separation, fractionation, hydrocracking, hydroisomerizing, dewaxing, or a combination of two or more thereof. 40. The process of claim 22 wherein the desired product is further processed to form an oil of lubricating viscosity or a middle distillate fuel. 41. The process of claim 22 wherein the desired product is further processed to form a fuel. 42. The process of claim 1 wherein the catalyst used in step (B) is an alcohol-forming catalyst, the reaction that is conducted in the microchannel reactor during step (B) is an alcohol-forming reaction, and the desired product comprises one or more alcohols. 43. The process of claim 42 wherein the alcohol-forming catalyst comprises a catalyst metal of Nb, Ta, Mo, W, Tc, Re or a mixture of two or more thereof, in free form or combined form. 44. The process of claim 43 wherein the catalyst further comprises a cocatalyst metal of yttrium, a lanthanide series metal, an actinide series metal, or a combination of two or more thereof, in free form or combined form. 45. The process of claim 42 wherein the pressure in the microchannel reactor is in the range up to about 100 atmospheres. 46. The process of claim 42 wherein the temperature in the microchannel reactor is in the range from about 200 to about 500° C. 47. The process of claim 42 wherein the desired product comprises one or more alcohols having from 1 to about 10 carbon atoms. 48. The process of claim 42 wherein the desired product comprises methanol. 49. The process of claim 42 wherein the desired product comprises methanol, ethanol, 1-propanol, 2-propanol, 1-butanol, 2-butanol, 2-methyl-1-propanol, 2-methyl-2-propanol, 1-pentanol, 2-pentanol, or a mixture of two or more thereof. 50. The process of claim 1 wherein the catalyst is in the form of particulate solids. 51. The process of claim 1 wherein the microchannel reactor comprises one or more process microchannels, the catalyst being coated on interior walls of the process microchannels or grown on interior walls of the process microchannels. 52. The process of claim 1 wherein the catalyst is supported on a support having a flow-by configuration, a flow-through configuration, or a serpentine configuration. 53. The process of claim 1 wherein the catalyst is supported on a support having the configuration of a foam, felt, wad, fin, or a combination of two or more thereof. 54. The process of claim 1 wherein the catalyst is supported on a support in the form of a fin assembly comprising a plurality of parallel spaced fins. 55. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel, the process microchannel having at least one heat transfer wall and the heat flux for heat exchange within the microchannel reactor is in the range from about 0.01 to about 500 watts per square centimeter of surface area of the at least one heat transfer wall. 56. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel, the temperature at the entrance to the process microchannel being within about 80° C. of the temperature at the outlet of the process microchannel. 57. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel and at least one heat exchanger, the heat exchanger comprising at least one heat exchange channel in thermal contact with the at least one process microchannel, the process microchannel having fluid flowing in it in one direction, the heat exchange channel having fluid flow in a direction that is co-current or counter-current to the flow of fluid in the process microchannel. 58. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel and at least one heat exchanger, the heat exchanger comprising at least one heat exchange channel in thermal contact with the at least one process microchannel, the process microchannel having fluid flowing in it in one direction, the heat exchange channel having fluid flowing in it in a direction that is cross-current to the flow of fluid in the process microchannel. 59. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel and at least one heat exchanger, the at least one process microchannel being in thermal contact with at least one heat exchange channel, the length of the process microchannel and the length of the heat exchange channel being about the same. 60. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel and at least one heat exchanger, the heat exchanger comprising a heat exchange zone in thermal contact with the at least one process microchannel, the heat exchange zone comprising one or more heat exchange channels, the heat exchange channels extending lengthwise at right angles relative to the lengthwise direction of the process microchannel, the heat exchange zone extending lengthwise in the same direction as the process microchannel, the length of the heat exchange zone being shorter than the length of the process microchannel, the process microchannel having an entrance and an exit, the heat exchange zone being positioned at or near the process microchannel entrance. 61. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel and at least one heat exchanger, the heat exchanger comprising two heat exchange zones in thermal contact with the at least one process microchannel, each heat exchange zone comprising one or more heat exchange channels, the heat exchange channels extending lengthwise at right angles relative to the lengthwise direction of the process microchannel, the process microchannel having an entrance and an exit, the heat exchange zones extending lengthwise in the same direction as the process microchannel, the lengths of the heat exchange zones being shorter than the length of the process microchannel, the length of one of the heat exchange zones being shorter than the length of the other heat exchange zone, the heat exchange zones being positioned at or near the process microchannel entrance. 62. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel and at least one heat exchanger, a tailored heat exchange profile being provided along the length of the process microchannel, the local release of heat given off by the reaction conducted in the process microchannel being matched with cooling provided by the heat exchanger. 63. The process of claim 1 wherein the catalyst comprises a graded catalyst. 64. The process of claim 1 wherein the Quality Index Factor for the microchannel reactor is less than about 50%. 65. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel, the superficial velocity for fluid flowing in the process microchannel being at least about 0.01 m/s. 66. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel, the space velocity for fluid flowing in the process microchannel being at least about 1000 hr−1. 67. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel, the pressure drop for fluid flowing in the process microchannel being up to about 10 atmospheres per meter. 68. The process of claim 1 wherein the microchannel reactor comprises at least one process microchannel, the Reynolds number for the flow of fluid in the process microchannel being in the range from about 10 to about 4000. 69. The process of claim 1 wherein steam is used as a heat exchange fluid in the microchannel reactor during step (B) and the carbonaceous material is gasified in the presence of a gasification agent during step (A), the steam from step (B) being used as the gasification agent during step (A). 70. 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. 71. The process of claim 70 wherein the nitrogen is separated from the air in a microchannel separator using an ionic liquid as an absorbent liquid. 72. 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). 73. The process of claim 1 wherein during step (A) synthesis gas is formed in a gasifier and a Fischer-Tropsch tail gas is produced during step (B), the Fischer-Tropsch tail gas being converted to synthesis gas in a steam methane reforming microchannel reactor, the synthesis gas from the steam reforming microchannel reactor being combined with the synthesis gas from the gasifier. 74. The process of claim 73 wherein the synthesis gas formed during step (A) contains carbon dioxide, the carbon dioxide being separated from the synthesis gas and combined with the Fischer-Tropsch tail gas in the steam methane reforming microchannel reactor. 75. The process of claim 1 wherein the synthesis gas formed during step (A) contains carbon dioxide, the carbon dioxide being separated from the synthesis gas prior to step (B). 76. The process of claim 1 wherein the carbonaceous material comprises polyethylene or polyvinyl chloride, and the synthesis gas formed during step (A) comprises an ethylene-rich synthesis gas. 77. The process of claim 1 wherein the synthesis gas that is formed during step (A) is cooled in one or more heat exchangers prior to step (B). 78. The process of claim 77 wherein the one or more heat exchangers are microchannel heat exchangers. 79. The process of claim 1 wherein the synthesis gas contains contaminants and prior to step (B) the contaminants are separated from the synthesis gas using a microchannel separator containing an ionic liquid. 80. The process of claim 1 wherein the synthesis gas contains contaminants and prior to step (B) the contaminants are separated from the synthesis gas using a temperature swing adsorption or a pressure swing adsorption microchannel separator. 81. The process of claim 1 wherein the synthesis gas contains contaminants and prior to step (B) the contaminants are separated from the synthesis gas using a microchannel separator containing nanofibers or a nano-composite film. 82. The process of claim 1 wherein the synthesis gas contains contaminants and prior to step (B)(I) the contaminants are separated from the synthesis gas using a ZnO guardbed. 83. The process of claim 1 wherein the carbonaceous material comprises a non-food carbonaceous material. 84. The process of claim 1 wherein the carbonaceous material comprises a food resource. 85. The process of claim 1 wherein the microchannel reactor comprises a plurality of process microchannels, the process microchannels being formed by positioning a waveform between planar sheets. 86. The process of claim 85 wherein the microchannel reactor further comprises a plurality of heat exchange channels in thermal contact with the process microchannels, the heat exchange channels being formed by positioning a waveform between planar sheets. 87. The process of claim 1 wherein the catalyst used in step (B) is a Fischer-Tropsch catalyst, the catalyst comprising cobalt and a support, the cobalt concentration being in the range from about 35% to about 60% by weight of the catalyst. 88. The process of claim 1 wherein the catalyst used in step (B) is a Fischer-Tropsch catalyst, the catalyst being prepared by activating a catalyst precursor comprising a cobalt compound and a support with a gas comprising at least about 5 mol % of hydrocarbon. 89. The process of claim 1 wherein the catalyst used in step (B) is a Fischer-Tropsch catalyst, the catalyst being prepared by (a) preparing a liquid mixture of (i) at least one catalyst support or catalyst support precursor, (ii) at least one metal-containing compound, wherein said metal comprises V, Cr, Mn, Fe, Co, Ni, Cu, Mo and/or W, and (iii) at least one polar organic compound which acts as a solvent for the metal-containing compound, the liquid mixture comprising 0 to about 20 wt % of water based on the total weight of the mixture; (b) converting the mixture to a paste or solid residue; and (c) combusting the residue in an oxygen-containing atmosphere to at least partially convert the organic compound to carbon and to form the supported catalyst or catalyst precursor. 90. The process of claim 89 wherein the metal comprises Co. 91. The process of claim 1 wherein the desired product produced in step (B) is a Fischer-Tropsch product, the process further comprising hydrocracking at least part of the Fischer-Tropsch product in a microchannel reactor. 92. The process of claim 91 wherein the microchannel reactor used to conduct the hydrocracking is the same microchannel reactor used for forming the Fischer-Tropsch product. 93. The process of claim 1 wherein the catalyst used in step (B) comprises an alcohol forming catalyst and a dehydration catalyst, the desired product comprising one or more unsaturated hydrocarbons. 94. 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 microchannels within the microchannel reactor.
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