RU2011130432A - METHOD FOR IMPLEMENTING THE FISHER-TROPSH PROCESS AT LOW PRESSURE - Google Patents

METHOD FOR IMPLEMENTING THE FISHER-TROPSH PROCESS AT LOW PRESSURE Download PDF

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RU2011130432A
RU2011130432A RU2011130432/04A RU2011130432A RU2011130432A RU 2011130432 A RU2011130432 A RU 2011130432A RU 2011130432/04 A RU2011130432/04 A RU 2011130432/04A RU 2011130432 A RU2011130432 A RU 2011130432A RU 2011130432 A RU2011130432 A RU 2011130432A
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fischer
tropsch
cobalt
psi
abs
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RU2011130432/04A
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RU2487159C2 (en
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Конрад АЯССЕ
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Вм Гтл, Инк.
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Priority claimed from PCT/CA2008/002306 external-priority patent/WO2010071967A1/en
Priority claimed from US12/318,106 external-priority patent/US8053481B2/en
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Abstract

1. Способ осуществления процесса Фишера-Тропша для получения жидких углеводородов, содержащих в основном дизельное топливо или дизельную смесь, с получением жидкого углеводородного продукта, содержащего менее 10 мас.% воска (>С23) и более 65% дизельной фракции (С9-С23), включающий:работу при давлении ниже 200 фунт/кв. дюйм (абс) и использование кобальтового катализатора, включающего носитель катализатора Фишера-Тропша с кристаллитами металлического кобальта на нем, причем кристаллиты металлического кобальта имеют средний диаметр более 16 нм.2. Способ по п.1, в котором указанный носитель катализатора Фишера-Тропша выбирают из группы, состоящей из оксида алюминия, гамма-оксида алюминия, оксида циркония, оксида титана, оксида кремния и их смесей.3. Способ по п.1, в котором кобальтовый катализатор содержит металлический кобальт и содержание металлического кобальта в кобальтовом катализаторе составляет по меньшей мере 15 мас.%.4. Способ по п.1, в котором конверсия СО в подаваемом газе составляет по меньшей мере 60%.5. Способ по любому из пп.1-4, в котором используют промотор и указанные промотор выбирают из группы, состоящей из рутения, рения, родия, никеля, циркония, титана и их смесей.6. Способ по любому из пп.1-4, в котором проводят однократную дистилляцию для уменьшения крекинга легких углеводородов, имеющих более низкую температуру кипения, чем дизельная фракция.7. Способ по п.1, в котором используют реактор Фишера-Тропша без рецикла отходящего газа.8. Способ по любому из пп.1-4 или 7, в котором используют установку риформинга с воздухом в качестве источника кислорода.9. Способ по любому из пп.1-4 или 7, в котором используемый в указанном спо�1. A method for implementing the Fischer-Tropsch process for producing liquid hydrocarbons containing mainly diesel fuel or a diesel mixture, producing a liquid hydrocarbon product containing less than 10 wt.% wax (>C23) and more than 65% diesel fraction (C9-C23) including: operation at pressures below 200 psi. inch (abs) and the use of a cobalt catalyst comprising a Fischer-Tropsch catalyst support with cobalt metal crystallites thereon, wherein the cobalt metal crystallites have an average diameter greater than 16 nm.2. The method of claim 1, wherein said Fischer-Tropsch catalyst support is selected from the group consisting of alumina, gamma alumina, zirconium oxide, titanium oxide, silica and mixtures thereof. The method according to claim 1, wherein the cobalt catalyst contains metal cobalt and the content of metal cobalt in the cobalt catalyst is at least 15 wt%.4. The method according to claim 1, in which the conversion of CO in the supplied gas is at least 60%. 5. The method according to any one of claims 1 to 4, in which a promoter is used and said promoter is selected from the group consisting of ruthenium, rhenium, rhodium, nickel, zirconium, titanium and mixtures thereof. The method according to any one of claims 1-4, in which a single distillation is carried out to reduce the cracking of light hydrocarbons having a lower boiling point than the diesel fraction.7. The method according to claim 1, in which a Fischer-Tropsch reactor is used without waste gas recycle.8. The method according to any one of claims 1-4 or 7, in which a reformer with air is used as an oxygen source.9. The method according to any one of claims 1-4 or 7, in which it is used in the specified way

Claims (38)

1. Способ осуществления процесса Фишера-Тропша для получения жидких углеводородов, содержащих в основном дизельное топливо или дизельную смесь, с получением жидкого углеводородного продукта, содержащего менее 10 мас.% воска (>С23) и более 65% дизельной фракции (С9-С23), включающий:1. The method of implementation of the Fischer-Tropsch process for producing liquid hydrocarbons containing mainly diesel fuel or a diesel mixture, to obtain a liquid hydrocarbon product containing less than 10 wt.% Wax (> C23) and more than 65% of the diesel fraction (C9-C23) including: работу при давлении ниже 200 фунт/кв. дюйм (абс) и использование кобальтового катализатора, включающего носитель катализатора Фишера-Тропша с кристаллитами металлического кобальта на нем, причем кристаллиты металлического кобальта имеют средний диаметр более 16 нм.operation at pressures below 200 psi. inch (abs) and the use of a cobalt catalyst comprising a Fischer-Tropsch catalyst carrier with cobalt metal crystallites on it, the metal cobalt crystallites having an average diameter of more than 16 nm. 2. Способ по п.1, в котором указанный носитель катализатора Фишера-Тропша выбирают из группы, состоящей из оксида алюминия, гамма-оксида алюминия, оксида циркония, оксида титана, оксида кремния и их смесей.2. The method according to claim 1, wherein said Fischer-Tropsch catalyst carrier is selected from the group consisting of alumina, gamma alumina, zirconia, titanium oxide, silicon oxide, and mixtures thereof. 3. Способ по п.1, в котором кобальтовый катализатор содержит металлический кобальт и содержание металлического кобальта в кобальтовом катализаторе составляет по меньшей мере 15 мас.%.3. The method according to claim 1, in which the cobalt catalyst contains cobalt metal and the content of metallic cobalt in the cobalt catalyst is at least 15 wt.%. 4. Способ по п.1, в котором конверсия СО в подаваемом газе составляет по меньшей мере 60%.4. The method according to claim 1, in which the conversion of CO in the feed gas is at least 60%. 5. Способ по любому из пп.1-4, в котором используют промотор и указанные промотор выбирают из группы, состоящей из рутения, рения, родия, никеля, циркония, титана и их смесей.5. The method according to any one of claims 1 to 4, in which a promoter is used and said promoter is selected from the group consisting of ruthenium, rhenium, rhodium, nickel, zirconium, titanium and mixtures thereof. 6. Способ по любому из пп.1-4, в котором проводят однократную дистилляцию для уменьшения крекинга легких углеводородов, имеющих более низкую температуру кипения, чем дизельная фракция.6. The method according to any one of claims 1 to 4, in which a single distillation is carried out to reduce the cracking of light hydrocarbons having a lower boiling point than the diesel fraction. 7. Способ по п.1, в котором используют реактор Фишера-Тропша без рецикла отходящего газа.7. The method according to claim 1, wherein a Fischer-Tropsch reactor is used without off-gas recycle. 8. Способ по любому из пп.1-4 или 7, в котором используют установку риформинга с воздухом в качестве источника кислорода.8. The method according to any one of claims 1 to 4 or 7, which uses a reforming unit with air as an oxygen source. 9. Способ по любому из пп.1-4 или 7, в котором используемый в указанном способе реактор Фишера-Тропша представляет собой реактор Фишера-Тропша с неподвижным слоем или барботажный реактор Фишера-Тропша со взвешенным слоем катализатора.9. The method according to any one of claims 1 to 4 or 7, wherein the Fischer-Tropsch reactor used in the method is a fixed bed Fischer-Tropsch reactor or a suspended Fischer-Tropsch bubble reactor. 10. Способ осуществления процесса Фишера-Тропша, работающий при давлении ниже 200 фунт/кв. дюйм (абс), с использованием воздушной автотермальной установки риформинга при конверсии СО по меньшей мере 60% и выходе дизельной фракции более 65 мас.% в однопроходном реакторе Фишера-Тропша, включающий стадию:10. The method of implementation of the Fischer-Tropsch process, operating at a pressure below 200 psi. inch (abs), using an air reforming autothermal plant with a CO conversion of at least 60% and a diesel fraction of more than 65 wt.% in a Fischer-Tropsch single pass reactor, comprising the step of: использования кобальтового катализатора, содержащего металлический кобальт в количестве по меньшей мере 15 мас.% и рений в количестве менее 2 мас.%, причем указанный кобальтовый катализатор включает материал носителя катализатора, который выбирают из группы, состоящей из оксида алюминия, оксида циркония, оксида кремния и их смесей, и содержит кристаллиты металлического кобальта на нем со средним диаметром более 16 нм.the use of a cobalt catalyst containing metallic cobalt in an amount of at least 15 wt.% and rhenium in an amount of less than 2 wt.%, said cobalt catalyst comprising a catalyst support material selected from the group consisting of alumina, zirconium oxide, silicon oxide and mixtures thereof, and contains crystallites of metallic cobalt on it with an average diameter of more than 16 nm. 11. Способ по п.10, в котором носитель катализатора Фишера-Тропша представляет собой гамма-оксид алюминия.11. The method of claim 10, wherein the Fischer-Tropsch catalyst carrier is gamma alumina. 12. Способ по п.10, в котором для удаления водорода из исходного газа Фишера-Тропша применяют селективные мембраны или молекулярные сита.12. The method of claim 10, wherein selective membranes or molecular sieves are used to remove hydrogen from the Fischer-Tropsch feed gas. 13. Способ по п.10, в котором рабочее давление составляет по меньшей мере 40 фунт/кв. дюйм (абс), а температура в реакторе Фишера-Тропша равна по меньшей мере 190°С.13. The method of claim 10, wherein the operating pressure is at least 40 psi. inch (abs), and the temperature in the Fischer-Tropsch reactor is at least 190 ° C. 14. Способ по п.10, в котором рабочее давление составляет менее 100 фунт/кв. дюйм (абс).14. The method of claim 10, wherein the operating pressure is less than 100 psi. inch (abs). 15. Способ осуществления процесса Фишера-Тропша по п.10, в котором указанный кобальтовый катализатор дополнительно содержит промотор, который выбирают из группы, состоящей из рутения, рения и их смесей.15. The method of implementing the Fischer-Tropsch process of claim 10, wherein said cobalt catalyst further comprises a promoter that is selected from the group consisting of ruthenium, rhenium and mixtures thereof. 16. Способ осуществления процесса Фишера-Тропша с конверсией СО по меньшей мере 60% и выходом дизельной фракции более 65 мас.% в реакторе Фишера-Тропша, включающий:16. A method of implementing the Fischer-Tropsch process with a CO conversion of at least 60% and a diesel fraction of more than 65 wt.% In a Fischer-Tropsch reactor, comprising: работу при давлении ниже 200 фунт/кв. дюйм (абс);operation at pressures below 200 psi. inch (abs); использование воздушного автотермальной установки риформинга; иthe use of an air refinery reforming plant; and использование кобальтового катализатора с содержанием металлического кобальта по меньшей мере 15 мас.% и рения менее 2 мас.% на носителе катализатора Фишера-Тропша, который выбирают из группы, состоящей из оксида алюминия, оксида циркония, оксида кремния и их смесей, причем указанный кобальтовый катализатор находится в форме кристаллитов металлического кобальта со средним диаметром более 16 нм.the use of a cobalt catalyst with a metal cobalt content of at least 15 wt.% and rhenium less than 2 wt.% on a Fischer-Tropsch catalyst carrier, which is selected from the group consisting of alumina, zirconia, silicon oxide and mixtures thereof, said cobalt the catalyst is in the form of crystallites of metallic cobalt with an average diameter of more than 16 nm. 17. Способ по п.16, в котором носитель катализатора Фишера-Тропша представляет собой оксид алюминия.17. The method of claim 16, wherein the Fischer-Tropsch catalyst carrier is alumina. 18. Способ по п.16, в котором отходящие газы установки риформинга Фишера-Тропша частично возвращают на рецикл в установку риформинга.18. The method according to clause 16, in which the exhaust gases of the Fischer-Tropsch reforming unit is partially returned for recycling to the reforming unit. 19. Способ по п.16, в котором для удаления водорода из исходного газа, подаваемого в реактор Фишера-Тропша, применяют селективные мембраны или молекулярные сита.19. The method according to clause 16, in which selective membranes or molecular sieves are used to remove hydrogen from the source gas fed to the Fischer-Tropsch reactor. 20. Способ по п.16, в котором рабочее давление составляет по меньшей мере 40 фунт/кв. дюйм (абс), а температура в реакторе Фишера-Тропша равна по меньшей мере 190°С.20. The method according to clause 16, in which the operating pressure is at least 40 psi. inch (abs), and the temperature in the Fischer-Tropsch reactor is at least 190 ° C. 21. Способ по п.16, в котором рабочее давление составляет не более 100 фунт/кв. дюйм (абс).21. The method according to clause 16, in which the operating pressure is not more than 100 psi. inch (abs). 22. Способ осуществления процесса Фишера-Тропша по п.16, в котором указанный реактор дополнительно включает промотор, который выбирают из группы, состоящей из рутения, рения и их смесей.22. The method of implementing the Fischer-Tropsch process according to clause 16, in which the specified reactor further includes a promoter, which is selected from the group consisting of ruthenium, rhenium and mixtures thereof. 23. Способ осуществления процесса Фишера-Тропша в реакторе Фишера-Тропша, включающий:23. A method of implementing the Fischer-Tropsch process in a Fischer-Tropsch reactor, including: работу при давлениях ниже 200 фунт/кв. дюйм (абс);operation at pressures below 200 psi. inch (abs); использование установки кислородного парового риформинга;use of an oxygen steam reforming unit; обеспечение конверсии СО по меньшей мере 60% и выхода дизельной фракции более 65 мас.%; иproviding a CO conversion of at least 60% and a diesel fraction yield of more than 65 wt.%; and использование кобальтового металлического катализатора с содержанием металлического кобальта по меньшей мере 15 мас.% и рения менее 2 мас.% на носителе катализатора Фишера-Тропша, который выбирают из группы, состоящей из оксида алюминия, оксида циркония, оксида кремния и их смесей, причем указанный носитель содержит кристаллиты металлического кобальта со средним диаметром более 16 нм.the use of a cobalt metal catalyst with a content of cobalt metal of at least 15 wt.% and rhenium less than 2 wt.% on a Fischer-Tropsch catalyst carrier selected from the group consisting of alumina, zirconia, silicon oxide and mixtures thereof, said the carrier contains cobalt metal crystallites with an average diameter of more than 16 nm. 24. Способ по п.23, в котором носитель катализатора Фишера-Тропша представляет собой гамма-оксид алюминия.24. The method of claim 23, wherein the Fischer-Tropsch catalyst carrier is gamma alumina. 25. Способ по любому из пп.23, в котором для удаления водорода из подаваемого в реактор Фишера-Тропша исходного газа применяют селективные мембраны или молекулярные сита.25. The method according to any one of paragraphs.23 to which, selective membranes or molecular sieves are used to remove hydrogen from the feed gas to the Fischer-Tropsch reactor. 26. Способ по любому из пп.23-25, в котором отходящий газ установки риформинга частично или полностью сжигают для получения тепла для установки риформинга.26. The method according to any one of paragraphs.23-25, in which the exhaust gas of the reforming unit is partially or completely burned to produce heat for the reforming unit. 27. Способ по любому из пп.23-25, в котором рабочее давление составляет по меньшей мере 40 фунт/кв. дюйм (абс), а температура равна по меньшей мере 190°С.27. The method according to any one of paragraphs.23-25, in which the operating pressure is at least 40 psi. inch (abs) and the temperature is at least 190 ° C. 28. Способ по любому из пп.23-25, в котором рабочее давление составляет меньше 100 фунт/кв. дюйм (абс).28. The method according to any one of paragraphs.23-25, in which the operating pressure is less than 100 psi. inch (abs). 29. Способ осуществления процесса Фишера-Тропша по любому из пп.23-25, в котором указанный реактор дополнительно включает промотор, который выбирают из группы, состоящей из рутения, рения и их смесей.29. The method of implementing the Fischer-Tropsch process according to any one of paragraphs.23-25, wherein said reactor further comprises a promoter that is selected from the group consisting of ruthenium, rhenium and mixtures thereof. 30. Способ осуществления процесса Фишера-Тропша с конверсией СО более 60% и выходом дизельной фракции более 65 мас.%, включающий:30. A method of implementing the Fischer-Tropsch process with a CO conversion of more than 60% and a diesel fraction yield of more than 65 wt.%, Including: работу при давлении ниже 200 фунт/кв. дюйм (абс), использование установки риформинга с неполным окислением воздухом или кислородом; иoperation at pressures below 200 psi. inch (abs), use of a reformer with incomplete oxidation by air or oxygen; and использование реактора Фишера-Тропша с кобальтовым катализатором, содержащим металлический кобальт в количестве более 15 мас.% и рений в количестве менее 2 мас.% на носителе катализатора Фишера-Тропша, который выбирают из группы, состоящей из оксида алюминия, оксида циркония и оксида кремния и их смесей, причем указанный кобальтовый катализатор находится в виде кристаллитов металла со средним диаметром более 16 нм.the use of a Fischer-Tropsch reactor with a cobalt catalyst containing more than 15 wt.% cobalt metal and less than 2 wt.% rhenium on a Fischer-Tropsch catalyst support selected from the group consisting of alumina, zirconium oxide and silicon oxide and mixtures thereof, wherein said cobalt catalyst is in the form of metal crystallites with an average diameter of more than 16 nm. 31. Способ по п.30, в котором носитель катализатора Фишера-Тропша представляет собой оксид алюминия.31. The method of claim 30, wherein the Fischer-Tropsch catalyst carrier is alumina. 32. Способ по п.30 или 31, в котором для удаления водорода из исходного газа, подаваемого в реактор Фишера-Тропша, применяют селективные мембраны или молекулярные сита.32. The method of claim 30 or 31, wherein selective membranes or molecular sieves are used to remove hydrogen from the feed gas fed to the Fischer-Tropsch reactor. 33. Способ по п.30, в котором рабочее давление составляет по меньшей мере 40 фунт/кв. дюйм (абс) и температура равна по меньшей мере 190°С.33. The method of claim 30, wherein the operating pressure is at least 40 psi. inch (abs) and a temperature of at least 190 ° C. 34. Способ по п.30, в котором рабочее давление составляет менее 100 фунт/кв. дюйм (абс).34. The method of claim 30, wherein the operating pressure is less than 100 psi. inch (abs). 35. Способ осуществления процесса Фишера-Тропша по п.30, в котором указанный реактор дополнительно включает промотор, который выбирают из группы, состоящей из рутения, рения и их смесей.35. The method for implementing the Fischer-Tropsch process according to claim 30, wherein said reactor further comprises a promoter selected from the group consisting of ruthenium, rhenium and mixtures thereof. 36. Способ по любому из пп.1, 10, 16, 23 или 30, в котором температура в реакторе Фишера-Тропша составляет, по меньшей мере, 190°С.36. The method according to any one of claims 1, 10, 16, 23 or 30, in which the temperature in the Fischer-Tropsch reactor is at least 190 ° C. 37. Способ по любому из пп.1, 10, 16, 23 или 30, в котором температура в реакторе Фишера-Тропша составляет, по меньшей мере, 190°С, рабочее давление составляет по меньшей мере 40 фунт/кв. дюйм (абс), причем в способе используют промотор, который выбирают из группы, состоящей из рутения, рения, родия, никеля, циркония, титана и их смесей; и в котором конверсия СО превышает 65%.37. The method according to any one of claims 1, 10, 16, 23 or 30, in which the temperature in the Fischer-Tropsch reactor is at least 190 ° C, the operating pressure is at least 40 psi. inch (abs), wherein the method uses a promoter that is selected from the group consisting of ruthenium, rhenium, rhodium, nickel, zirconium, titanium, and mixtures thereof; and in which the conversion of CO exceeds 65%. 38. Способ по п.37, в котором конверсия СО превышает 65%. 38. The method according to clause 37, in which the conversion of CO exceeds 65%.
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