IPC분류정보
국가/구분 |
United States(US) Patent
등록
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국제특허분류(IPC7판) |
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출원번호 |
US-0576458
(2009-10-09)
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등록번호 |
US-8747656
(2014-06-10)
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발명자
/ 주소 |
- Tonkovich, Anna Lee
- Arora, Ravi
- Brophy, John
- Daly, Francis P.
- Deshmukh, Soumitra
- Fanelli, Maddalena
- Jarosch, Kai Tod Paul
- LaPlante, Timothy J.
- Long, Richard Q.
- Mazanec, Terry
- Ryan, Daniel Francis
- Silva, Laura J.
- Simmons, Wayne W.
- Stangeland, Bruce
- Wang, Yong
- Yuschak, Thomas
- Perry, Steven T.
- Marco, Jeffrey Dale
- Marchiando, Michael Alan
- Litt, Robert Dwayne
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출원인 / 주소 |
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대리인 / 주소 |
Renner, Otto, Boisselle & Sklar, LLP
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인용정보 |
피인용 횟수 :
4 인용 특허 :
74 |
초록
This invention relates to a process for conducting a hydrocracking or a hydrotreating process in a microchannel reactor. This invention also relates to a process and apparatus for flowing a vapor and liquid into a plurality of microchannels in a microchannel processing unit.
대표청구항
▼
1. A process, comprising: flowing reactants comprising a hydrocarbon reactant and hydrogen in a process microchannel in contact with a catalyst to form one or more products, the hydrocarbon reactant comprising a liquid; and removing the product from the process microchannel; wherein: (a) the hydroca
1. A process, comprising: flowing reactants comprising a hydrocarbon reactant and hydrogen in a process microchannel in contact with a catalyst to form one or more products, the hydrocarbon reactant comprising a liquid; and removing the product from the process microchannel; wherein: (a) the hydrocarbon reactant comprises a hydrocarbon with a first hydrocarbon chain length, the hydrocarbon reactant being converted to two or more hydrocarbon products, the hydrocarbon products having chain lengths that are shorter than the first hydrocarbon chain length; or(b) the hydrocarbon reactant comprises one or more heteroatoms bonded to the hydrocarbon reactant and at least one of the heteroatoms reacts with the hydrogen to form a heteroatom containing compound, the product comprising a hydrocarbon product characterized by the absence of heteroatoms or a reduced heteroatom content as compared to the hydrocarbon reactant;wherein the process is conducted in a microchannel reactor comprising a plurality of the process microchannels, the microchannel reactor further comprising a distribution apparatus for flowing the hydrocarbon reactant and hydrogen into the plurality of process microchannels, the distribution apparatus being positioned at the entrance to the process microchannels, the distribution apparatus comprising a separation plate and a redistribution plate, the separation plate overlying the redistribution plate, the hydrocarbon reactant and hydrogen contacting the separation plate and separating into a vapor phase and a liquid phase, the vapor phase and the liquid phase flowing to the redistribution plate; the redistribution plate comprising a plurality of openings, the openings in the redistribution plate being aligned with the entrances to the process microchannels, the vapor phase contacting the liquid phase in the openings in the redistribution plate and forming a vapor/liquid mixture, the vapor/liquid mixture flowing into the process microchannels. 2. The process of claim 1 wherein the heteroatoms comprise one or more of nitrogen, sulfur, oxygen, metal, or a combination of two or more thereof. 3. The process of claim 1 wherein the pressure in the process microchannel is in the range from about 0.2 to about 20 MPa. 4. The process of claim 1 wherein the temperature in the process microchannel is in the range from about 50° C. to about 500° C. 5. The process of claim 1 wherein the ratio of hydrogen to hydrocarbon reactant is in the range from about 10 to about 6000 standard cubic centimeters of hydrogen per cubic centimeter of hydrocarbon reactant. 6. The process of claim 1 wherein gas flows in the process microchannel and at a superficial velocity of at least about 0.01 meters per second. 7. The process of claim 1 wherein the product comprises a hydrocracked Fischer-Tropsch synthesis product. 8. The process of claim 1 wherein the hydrocarbon reactant and the hydrogen are mixed prior to entering the process microchannel. 9. The process of claim 1 wherein the process microchannel is in a microchannel reactor, the microchannel reactor further comprising a reactant stream channel adjacent to the process microchannel, the process microchannel and the reactant stream channel having a common wall, a plurality of openings being in the common wall, the process further comprising flowing the hydrocarbon reactant in the process microchannel and flowing the hydrogen from the reactant stream channel through the openings in the common wall into the process microchannel in contact with the hydrocarbon reactant. 10. The process of claim 1 wherein the process microchannel has a reaction zone, the hydrocarbon reactant and hydrogen contacting each other in the reaction zone. 11. The process of claim 1 wherein the process microchannel has a mixing zone and a reaction zone, the mixing zone being upstream of the reaction zone, the hydrocarbon reactant and hydrogen contacting each other in the mixing zone. 12. The process of claim 1 wherein the process microchannel has a mixing zone and a reaction zone, the mixing zone being upstream of the reaction zone, part of hydrogen contacting the hydrocarbon reactant in the mixing zone to form an intermediate reaction mixture, the intermediate reaction mixture flowing into the reaction zone, and part of the hydrogen contacting the intermediate reaction mixture in the reaction zone. 13. The process of claim 1 wherein the process microchannel is in a microchannel reactor, the microchannel reactor comprising a plurality of the process microchannels, the microchannel reactor comprising a manifold providing a flow passageway for the reactants to flow into the process microchannels. 14. The process of claim 1 wherein the process microchannel is in a microchannel reactor, the microchannel reactor comprising a plurality of the process microchannels, the microchannel reactor comprising a first manifold providing a flow passageway for the hydrocarbon reactant to flow into the process microchannels, and a second manifold providing a flow passageway for the hydrogen to flow into the process microchannels. 15. The process of claim 1 wherein the process microchannel is in a microchannel reactor, the microchannel reactor having an entrance and an exit, the product flowing out of the microchannel reactor through the exit, and at least part of the product flowing out of the microchannel reactor being recycled back into the microchannel reactor through the entrance. 16. The process of claim 1 wherein heat is transferred from the process microchannel to a heat exchanger. 17. The process of claim 1 wherein the process microchannel is in a microchannel reactor, the microchannel reactor comprising a plurality of the process microchannels, the microchannel reactor further comprising at least one heat exchange channel in thermal contact with the process microchannels, a heat exchange fluid being in the heat exchange channel, and heat is transferred from the process microchannel to the heat exchange fluid in the heat exchange channel. 18. The process of claim 17 wherein the heat exchange fluid undergoes a phase change in the heat exchange channel. 19. The process of claim 17 wherein the heat exchange fluid undergoes partial boiling in the heat exchange channel. 20. The process of claim 17 wherein an endothermic chemical reaction is conducted in the heat exchange channel. 21. The process of claim 20 wherein the endothermic chemical reaction comprises a steam reforming reaction or a dehydrogenation reaction. 22. The process of claim 17 wherein fluid flows in the process microchannel in a first direction, and the heat exchange fluid flows in the heat exchange channel in a second direction, the second direction being cross current, cocurrent and/or counter-current relative to the first direction. 23. The process of claim 17 wherein the heat exchange fluid comprises air, steam, liquid water, carbon monoxide, carbon dioxide, gaseous nitrogen, liquid nitrogen, gaseous hydrocarbon, liquid hydrocarbon, or a mixture of two or more thereof. 24. The process of claim 17 wherein the heat exchange fluid comprises the product and/or the hydrocarbon reactant. 25. The process of claim 17 where the total cross sectional area of the process microchannels in the reactor is greater than the total cross sectional area of the heat exchange channels in the reactor. 26. The process of claim 1 wherein a tailored heat exchange is provided along the length of the process microchannel to maintain a substantially isothermal temperature profile in the process microchannel. 27. The process of claim 1 wherein the catalyst comprises a graded catalyst. 28. The process of claim 1 wherein the catalyst comprises a flow-by structure or a flow-through structure. 29. The process of claim 1 wherein the process microchannel has an interior surface, the catalyst being coated or grown on the interior surface. 30. The process of claim 1 wherein the catalyst is in the form of particulate solids. 31. The process of claim 1 wherein the catalyst is supported by a structure which comprises a foam, felt, wad, honeycomb, one or more fins, or a combination of two or more thereof. 32. The process of claim 1 wherein the catalyst is in the form of a bed of particulate solids, and additional catalyst is washcoated and/or grown on one or more interior walls of the process microchannel. 33. The process of claim 1 wherein the catalyst comprises a zeolite. 34. The process of claim 33 wherein the catalyst further comprises a refractory inorganic oxide. 35. The process of claim 34 wherein the refractory inorganic oxide comprises alumina, magnesia, silica, titania, zirconia or silica-alumina. 36. The process of claim 33 wherein the catalyst comprises Y-zeolite, beta zeolite, omega zeolite, L-zeolite, or ZSM-5. 37. The process of claim 1 wherein the catalyst comprises a hydrogenation component. 38. The process of claim 37 wherein the hydrogenation component comprises a Group IVB metal, a Group VIII metal, or a compound of one or more thereof. 39. The process of claim 1 wherein the catalyst comprises one or more pillared clays, MCM-41, MCM-48, HMS, or a combination of two or more thereof. 40. The process of claim 1 wherein the catalyst comprises Pt, Pd, Ni, Co, Mo, W, or a combination of two or more thereof. 41. The process of claim 1 wherein the temperature of the reactants entering the process microchannel is within about 20° C. of the temperature of the product flowing out of the process microchannel. 42. The process of claim 1 wherein during part (b) the hydrocarbon reactant comprises atmospheric gas oil, vacuum gas oil, or a mixture thereof. 43. The process of claim 1 wherein during part (b) the hydrocarbon reactant comprises mineral oil, synthetic oil, or a mixture thereof. 44. The process of claim 1 wherein during part (b) the hydrocarbon reactant comprises straight run gas oil, vacuum gas oil, demetallized oil, deasphalted vacuum residue, coker distillate, cat cracker distillate, shale oil, tar sand oil, coal liquid, or a mixture of two or more thereof. 45. The process of claim 1 wherein the product comprises a middle distillate product boiling in the range from about 125° C. to about 375° C. 46. The process of claim 1 wherein the product comprises a C5 to 205° C. end point fraction. 47. The process of claim 1 wherein the product comprises gasoline, naphtha, diesel fuel, jet fuel and/or kerosene. 48. The process of claim 1 wherein the product comprises an isomerized product. 49. The process of claim 1 the weight hourly space velocity for the reactants with the catalyst is in the range from about 5 hr−1 to about 100 hr−1. 50. The process of claim 1 wherein the pressure drop for the flow of reactants and product in the process microchannel is up to about 0.08 MPa per centimeter of length of the process microchannel. 51. The process of claim 1 wherein subsequent to removing the product from the process microchannel a regenerating fluid flows through the process microchannel in contact with the catalyst, the residence time for the regenerating fluid in the process microchannel being from about 0.01 to about 1000 seconds. 52. The process of claim 1 wherein the microchannel Bond number is less than about 1. 53. The process of claim 1 wherein particulate solids are in the process microchannel, the process microchannel and the particulate solids have a Bond number that is less than about 1. 54. The process of claim 1 wherein a gas and a liquid are in the process microchannel, and mass transfer occurs between the gas and liquid, the particle or channel Bond number being less than about 1. 55. The process of claim 1 wherein the catalyst is regenerated in-situ in the process microchannel by oxidizing a carbonaceous material on the surface of the catalyst. 56. The process of claim 1 wherein the process is conducted in a plant facility, the plant facility comprising a plurality of the process microchannels, or one or more microchannel reactors containing the process microchannels or one or more reaction vessels containing one or more microchannel reactors, the catalyst in one or more of the process microchannels, microchannel reactors or reaction vessels being regenerated while the process is carried out in other process microchannels, microchannel reactors or reaction vessels in the plant facility. 57. The process of claim 1 wherein the process is conducted using a regenerated catalyst at a liquid hourly space velocity of about 5 hr−1 or above. 58. The process of claim 1 wherein the process is conducted under stable operating conditions using a regenerated catalyst for a period in excess of about 1200 hours. 59. The process of claim 1 wherein the hydrocarbon reactant comprises a mixture of hydrocarbons with an iso/normal mass fraction ratio that is less than about 0.2. 60. The process of claim 1 wherein the product comprises C5+ hydrocarbons with an iso/normal ratio that is greater than about 0.5; C20+ hydrocarbons with an iso/normal ratio that is greater than about 1; and/or C10+ hydrocarbons with an iso/normal ratio greater than about 1. 61. The process of claim 1 wherein the product has a cloud point that is less than about −10° C. 62. The process of claim 1 wherein the redistribution plate comprises: a first shim comprising a first planar surface and a plurality of first openings in the first planer surface;a second shim comprising a second planar surface, a plurality of second openings in the second planar surface, and a plurality of first through-holes in the second planar surface, the first shim overlying the second shim; anda third shim comprising a third planar surface and a plurality of second through-holes in the third planar surface, the second shim overlying the third shim, the second through-holes being aligned with the first through-holes, the third shim being adapted to overlie the entrances to the process microchannels, the second through-holes being aligned with the entrances to the process microchannels;the vapor flowing through the first openings into the first through-holes and from the first through-holes into the second through-holes; and the liquid flowing through the second openings onto the third planar surface and from the third planar surface into the second through-holes; the vapor and liquid mixing in this second through-holes, forming a vapor/liquid mixture and flowing into the process microchannels. 63. The process of claim 62 wherein the first openings in the first planar surface comprise a vapor manifold; and the second openings in the second planar surface comprise a liquid manifold. 64. The process of claim 1 wherein the redistribution plate comprises: a first shim comprising a first planar surface and a plurality of first openings in the first planer surface;a second shim comprising a second planar surface, a plurality of second openings in the second planar surface, and a plurality of first through-holes in the second planar surface, the first shim overlying the second shim;a third shim comprising a third planar surface and a plurality of second through-holes in the third planar surface, the second shim overlying the third shim, the second through-holes being aligned with the first through holes; anda fourth shim comprising a fourth planar surface and a plurality of third through-holes in the fourth planar surface, the third shim overlying the fourth shim, the third through-holes being aligned with the second through-holes, the fourth shim being adapted to overlie the entrances to the process microchannels, the third through-holes being adapted to be aligned with the entrances to the process microchannels;the liquid flowing through the first openings into the first through-holes, from the first through-holes into the second through-holes and from the second through-holes into the third-through holes; and the vapor flowing through the second openings into second through-holes and from the second through-holes into the third through-holes; the liquid and vapor mixing in the second and third through-holes, forming a vapor/liquid mixture and flowing into the process microchannels. 65. The process of claim 64 wherein the first openings in the first planar surface comprise a liquid manifold; and the second openings in the second planar surface comprise a vapor manifold. 66. The process of claim 1 wherein the redistribution plate comprises: a first shim comprising a first planar surface, a first opening in the first planer surface in a first side of the first planar surface, and a second opening in the first planar surface on a second side of the first planar surface, the first and second openings being in the form of open channels extending parallel to each other;a second shim comprising a second planar surface, a plurality of third openings in the second planar surface, and a plurality of fourth openings in the second planar surface, the third openings and the fourth openings being in the form of open channels extending parallel to each other, the first shim overlying the second shim, the third and fourth openings being aligned perpendicular to first and second openings, the first opening being aligned with part of the third openings, the second opening being aligned with part of the fourth openings; anda third shim comprising a third planar surface and a plurality of fifth openings in the third planar surface, the second shim overlying the third shim, the fifth openings being in the form of open channels extending parallel to each other and perpendicular to the third and fourth channels, the third shim being adapted to overlie the entrances to the process microchannels;the vapor flowing through the first openings into the third openings and from the third openings into the fifth openings; and the liquid flowing through the second openings into the fourth openings and from the fourth openings into the fifth openings; the vapor and liquid mixing in the fifth openings, forming a vapor/liquid mixture and flowing into the process microchannels. 67. The process of claim 66 wherein the first opening in the first planar surface comprises a vapor manifold; and the second opening in the first planar surface comprises a liquid manifold. 68. A process, comprising: flowing reactants comprising a hydrocarbon reactant and hydrogen in a process microchannel in contact with a catalyst to form one or more products, the hydrocarbon reactant comprising a liquid; and removing the product from the process microchannel; wherein: (a) the hydrocarbon reactant comprises a hydrocarbon with a first hydrocarbon chain length, the hydrocarbon reactant being converted to two or more hydrocarbon products, the hydrocarbon products having chain lengths that are shorter than the first hydrocarbon chain length; or(b) the hydrocarbon reactant comprises one or more heteroatoms bonded to the hydrocarbon reactant and at least one of the heteroatoms reacts with the hydrogen to form a heteroatom containing compound, the product comprising a hydrocarbon product characterized by the absence of heteroatoms or a reduced heteroatom content as compared to the hydrocarbon reactant;wherein the process is conducted in a microchannel reactor comprising a plurality of the process microchannels, the microchannel reactor further comprising a distribution apparatus for flowing the hydrocarbon reactant and hydrogen into the plurality of process microchannels, the hydrocarbon reactant comprising a first liquid and a second liquid, the distribution apparatus being positioned at the entrance to the process microchannels, the distribution apparatus comprisinga distributive plate, the distributive plate comprising:a first liquid manifold slot;a second liquid manifold slot;a vapor pathway;a first distribution channel extending from the first liquid manifold slot to the vapor pathway;a second distribution channel extending from the second liquid manifold slot to the vapor pathway;the hydrogen flowing through the vapor pathway, the first liquid flowing from the first liquid manifold slot through the first distribution channel into the vapor pathway in contact with the hydrogen flowing in the vapor pathway, and the second liquid flowing from the second liquid manifold slot through the second distribution channel into the vapor pathway in contact with the hydrogen flowing in the vapor pathway and the first liquid flowing in the vapor pathway. 69. The process of claim 68 wherein the distribution apparatus further comprises a first liquid feed plate for the first liquid, the first liquid feed plate being positioned on a first side of the distributive plate, the first liquid feed plate comprising a first liquid feed plate manifold slot, the first liquid feed entering the distribution apparatus through the first liquid feed plate manifold slot. 70. The process of claim 69 wherein the distribution apparatus further comprises a second liquid feed plate for the second liquid, the second liquid feed plate being positioned on a second side of the distributive plate, the second side of the distributive plate being opposite the first side of the distributive plate, the second liquid feed plate comprising a second liquid feed plate manifold slot, the second liquid entering the distribution apparatus through the second liquid feed plate manifold slot. 71. The process of claim 70 wherein a second distribution channel is positioned in the second liquid feed plate and is connected to the second liquid feed plate manifold slot. 72. The process of claim 69 wherein a first distribution channel is positioned in the first liquid feed plate and is connected to the first liquid feed plate manifold slot. 73. The process of claim 68 wherein a plurality of the first liquid manifold slots, second liquid manifold slots and vapor pathways are formed in the distributive plate. 74. The process of claim 68 wherein a plurality of the distributive plates are positioned in the distribution apparatus, the distributive plates being positioned side-by-side or stacked one above another. 75. The process of claim 68 wherein the first distribution channel and/or the second distribution channel are curved or constricted to increase pressure drop for fluid flowing in the first distribution channel and/or second distribution channel. 76. A process, comprising: flowing reactants comprising a hydrocarbon reactant and hydrogen in a process microchannel in contact with a catalyst to form one or more products, the hydrocarbon reactant comprising a liquid; and removing the product from the process microchannel; wherein: (a) the hydrocarbon reactant comprises a hydrocarbon with a first hydrocarbon chain length, the hydrocarbon reactant being converted to two or more hydrocarbon products, the hydrocarbon products having chain lengths that are shorter than the first hydrocarbon chain length; or(b) the hydrocarbon reactant comprises one or more heteroatoms bonded to the hydrocarbon reactant and at least one of the heteroatoms reacts with the hydrogen to form a heteroatom containing compound, the product comprising a hydrocarbon product characterized by the absence of heteroatoms or a reduced heteroatom content as compared to the hydrocarbon reactant;wherein the process is conducted in a microchannel reactor comprising a plurality of the process microchannels, the microchannel reactor further comprising a distribution apparatus for flowing the hydrocarbon reactant and hydrogen into the plurality of process microchannels, the hydrocarbon reactant comprising a first liquid and a second liquid, the distribution apparatus being positioned at the entrance to the process microchannels, the distribution apparatus comprising:a first distributive section;a second distributive section, the first distributive section overlying the second distributive section; anda third distributive section, the second distributive section overlying the third distributive section;the hydrogen flowing from the first distributive section through the second distributive section and the third distributive section into the microchannels, the first liquid flowing from the second distribution channel in contact with the vapor through the third distribution section into the microchannels, and the second liquid flowing from the third distribution section in contact with the vapor and the first liquid into the microchannels. 77. The process of claim 76 wherein the first distributive section comprises three plates stacked one above another, the three plates comprising: a manifold plate; a first distributive plate, the manifold plate overlying the first distributive plate; and a second distributive plate, the first distributive plate overlying the second distributive plate; the hydrogen flowing from the manifold plate to the first distributive plate, and through openings in the first distributive plate to the second distributive plate, and through openings in the second distributive plate to the second distributive section. 78. The process of claim 76 wherein the second distributive section comprises three plates stacked one above another, the three plates comprising: a manifold plate; a first distributive plate, the manifold plate overlying the first distributive plate; and a second distributive plate, the first distributive plate overlying the second distributive plate; the first liquid flowing from the manifold plate to the first distributive plate in contact with hydrogen from the first distributive section, and through openings in the first distributive plate to the second distributive plate, and through openings in the second distributive plate to the second distributive section. 79. The process of claim 76 wherein the third distributive section comprises three plates stacked one above another, the three plates comprising: a manifold plate; a first distributive plate, the manifold plate overlying the first distributive plate; and a second distributive plate, the first distributive plate overlying the second distributive plate; the second liquid flowing from the manifold plate to the first distributive plate in contact with hydrogen from the first distribution section and the first liquid from the second distribution section, and through openings in the first distributive plate to the second distributive plate, and through openings in the second distributive plate into the microchannels.
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