RU2010104993A - COMPREHENSIVE METHOD OF CRACKING WITH PSEUDO-LIQUID CATALYST FOR PRODUCING MIXTURES OF HYDROCARBONS HAVING HIGH FUEL QUALITY - Google Patents

COMPREHENSIVE METHOD OF CRACKING WITH PSEUDO-LIQUID CATALYST FOR PRODUCING MIXTURES OF HYDROCARBONS HAVING HIGH FUEL QUALITY Download PDF

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RU2010104993A
RU2010104993A RU2010104993/04A RU2010104993A RU2010104993A RU 2010104993 A RU2010104993 A RU 2010104993A RU 2010104993/04 A RU2010104993/04 A RU 2010104993/04A RU 2010104993 A RU2010104993 A RU 2010104993A RU 2010104993 A RU2010104993 A RU 2010104993A
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cracking
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fraction
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Джакомо РИСПОЛИ (IT)
Джакомо Рисполи
Альберто МОДЖИ (IT)
Альберто МОДЖИ
Джованни ФАРАЧИ (IT)
Джованни ФАРАЧИ
Паоло ПОЛЛЕЗЕЛЬ (IT)
Паоло Поллезель
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Эни С.П.А. (It)
Эни С.П.А.
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
    • B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
    • B01J29/74—Noble metals
    • B01J29/7469—MTW-type, e.g. ZSM-12, NU-13, TPZ-12 or Theta-3
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
    • B01J21/12—Silica and alumina
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
    • B01J29/78—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J29/7869—MTW-type, e.g. ZSM-12, NU-13, TPZ-12 or Theta-3
    • B01J35/617—
    • B01J35/647—
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G11/02—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils characterised by the catalyst used
    • C10G11/04—Oxides
    • C10G11/05—Crystalline alumino-silicates, e.g. molecular sieves
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G45/00—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds
    • C10G45/58—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to change the structural skeleton of some of the hydrocarbon content without cracking the other hydrocarbons present, e.g. lowering pour point; Selective hydrocracking of normal paraffins
    • C10G45/60—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to change the structural skeleton of some of the hydrocarbon content without cracking the other hydrocarbons present, e.g. lowering pour point; Selective hydrocracking of normal paraffins characterised by the catalyst used
    • C10G45/62—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to change the structural skeleton of some of the hydrocarbon content without cracking the other hydrocarbons present, e.g. lowering pour point; Selective hydrocracking of normal paraffins characterised by the catalyst used containing platinum group metals or compounds thereof
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G69/00—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process
    • C10G69/02—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process plural serial stages only
    • C10G69/04—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process plural serial stages only including at least one step of catalytic cracking in the absence of hydrogen
    • B01J35/633—
    • B01J35/635—
    • B01J35/638—

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Materials Engineering (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Catalysts (AREA)

Abstract

1. Комплексный способ превращения углеводородных фракций, происходящих из нефти, в смеси углеводородов, обладающие высоким топливным качеством, который включает следующие стадии: ! 1) проведение крекинга с псевдоожиженным катализатором (КПК) углеводородной фракции с получением смеси, содержащей ЛРГ (легкий рецикловый газойль); ! 2) разделения смеси, полученной на предшествующей стадии КПК, с целью выделения по меньшей мере одной фракции ЛРГ и фракции ТРГ (тяжелого рециклового газойля); ! 3) возможно, повторную подачу по меньшей мере части фракции ТРГ на стадию КПК; ! 4) проведение гидроочистки фракции ЛРГ; ! 5) проведение реакции продукта, полученного на стадии (4), с водородом, в присутствии каталитической системы, включающей: ! a) один или более металлов, выбранных из Pt, Pd, Ir, Ru, Rh и Re; ! b) алюмосиликат кислой природы, выбранный из цеолита, принадлежащего к семейству MTW, и полностью аморфного микро-мезопористого алюмосиликата, имеющего мольное соотношение SiO2/Al2O3 в диапазоне от 30 до 500, площадь поверхности более чем 500 м2/г, объем пор в диапазоне от 0,3 до 1,3 мл/г, средний диаметр пор менее 40 Å, при этом стадию крекинга с псевдоожиженным катализатором проводят при температуре в диапазоне от 490 до 530°C; и на стадии крекинга с псевдоожиженным катализатором температура предварительного нагрева питающего потока находится в диапазоне от 240 до 350°C. ! 2. Способ по п.1, в котором происходящие из нефти углеводородные фракции, обработанные на первой стадии комплексного способа, представляют собой газойль, вакуумный газойль, мазут, продукты термического крекинга и остатки гидрокрекинга. ! 3. Способ по п.1 или 2, в котором стадию крекинга с псевдо 1. An integrated method for converting hydrocarbon fractions derived from oil into mixtures of hydrocarbons of high fuel quality, which includes the following steps: ! 1) carrying out cracking with a fluidized catalyst (FCC) of the hydrocarbon fraction to obtain a mixture containing LRG (light cycle oil); ! 2) separating the mixture obtained in the preceding FCC step to isolate at least one LRG fraction and a TRG (heavy cycle oil) fraction; ! 3) possibly re-feeding at least a portion of the TRG fraction to the CPC stage; ! 4) hydrotreatment of the LRG fraction; ! 5) carrying out the reaction of the product obtained in step (4) with hydrogen in the presence of a catalytic system comprising: ! a) one or more metals selected from Pt, Pd, Ir, Ru, Rh and Re; ! b) an acidic aluminosilicate selected from a zeolite belonging to the MTW family and a fully amorphous micro-mesoporous aluminosilicate having a SiO2/Al2O3 mole ratio in the range of 30 to 500, a surface area of more than 500 m2/g, a pore volume in the range of 0.3 to 1.3 ml/g, average pore diameter less than 40 Å, while the stage of cracking with a fluid catalyst is carried out at a temperature in the range from 490 to 530°C; and in the fluid catalyzed cracking stage, the preheating temperature of the feed stream is in the range of 240 to 350°C. ! 2. Process according to claim 1, wherein the oil-derived hydrocarbon fractions treated in the first stage of the integrated process are gas oil, vacuum gas oil, fuel oil, thermal cracking products and hydrocracking residues. ! 3. The method according to claim 1 or 2, in which the stage of cracking with pseudo

Claims (21)

1. Комплексный способ превращения углеводородных фракций, происходящих из нефти, в смеси углеводородов, обладающие высоким топливным качеством, который включает следующие стадии:1. An integrated method for converting hydrocarbon fractions originating from oil into a mixture of hydrocarbons having high fuel quality, which includes the following stages: 1) проведение крекинга с псевдоожиженным катализатором (КПК) углеводородной фракции с получением смеси, содержащей ЛРГ (легкий рецикловый газойль);1) carrying out cracking with a fluidized catalyst (CCP) of the hydrocarbon fraction to obtain a mixture containing LHR (light recycle gas oil); 2) разделения смеси, полученной на предшествующей стадии КПК, с целью выделения по меньшей мере одной фракции ЛРГ и фракции ТРГ (тяжелого рециклового газойля);2) separation of the mixture obtained in the previous stage of the CPC, in order to isolate at least one fraction of LHR and the fraction of TEG (heavy recycle gas oil); 3) возможно, повторную подачу по меньшей мере части фракции ТРГ на стадию КПК;3) it is possible to re-supply at least a portion of the TEG fraction to the CPC stage; 4) проведение гидроочистки фракции ЛРГ;4) hydrotreating the LHR fraction; 5) проведение реакции продукта, полученного на стадии (4), с водородом, в присутствии каталитической системы, включающей:5) the reaction of the product obtained in stage (4), with hydrogen, in the presence of a catalytic system, including: a) один или более металлов, выбранных из Pt, Pd, Ir, Ru, Rh и Re;a) one or more metals selected from Pt, Pd, Ir, Ru, Rh and Re; b) алюмосиликат кислой природы, выбранный из цеолита, принадлежащего к семейству MTW, и полностью аморфного микро-мезопористого алюмосиликата, имеющего мольное соотношение SiO2/Al2O3 в диапазоне от 30 до 500, площадь поверхности более чем 500 м2/г, объем пор в диапазоне от 0,3 до 1,3 мл/г, средний диаметр пор менее 40 Å, при этом стадию крекинга с псевдоожиженным катализатором проводят при температуре в диапазоне от 490 до 530°C; и на стадии крекинга с псевдоожиженным катализатором температура предварительного нагрева питающего потока находится в диапазоне от 240 до 350°C.b) an acidic aluminosilicate selected from a zeolite belonging to the MTW family and a fully amorphous micro-mesoporous aluminosilicate having a SiO 2 / Al 2 O 3 molar ratio in the range of 30 to 500, a surface area of more than 500 m 2 / g, the pore volume in the range from 0.3 to 1.3 ml / g, the average pore diameter of less than 40 Å, while the cracking stage with a fluidized catalyst is carried out at a temperature in the range from 490 to 530 ° C; and at the stage of cracking with a fluidized catalyst, the temperature of the pre-heating of the feed stream is in the range from 240 to 350 ° C. 2. Способ по п.1, в котором происходящие из нефти углеводородные фракции, обработанные на первой стадии комплексного способа, представляют собой газойль, вакуумный газойль, мазут, продукты термического крекинга и остатки гидрокрекинга.2. The method according to claim 1, in which the hydrocarbon fractions derived from oil processed in the first stage of the complex method are gas oil, vacuum gas oil, fuel oil, thermal cracking products and hydrocracking residues. 3. Способ по п.1 или 2, в котором стадию крекинга с псевдоожиженным катализатором проводят при температуре в диапазоне от 450 до 650°C, давлении в реакционной зоне в диапазоне от 0,13 до 0,44 МПа (от 1,3 до 4,5 кг/см2), соотношении катализатор/нефтепродукт от 1 до 10 кг/кг и времени пребывания паров в реакционной зоне от 0,5 до 10 с.3. The method according to claim 1 or 2, in which the cracking stage with a fluidized catalyst is carried out at a temperature in the range from 450 to 650 ° C, pressure in the reaction zone in the range from 0.13 to 0.44 MPa (from 1.3 to 4.5 kg / cm 2 ), the ratio of catalyst / oil from 1 to 10 kg / kg and the residence time of the vapor in the reaction zone from 0.5 to 10 s. 4. Способ по п.1, в котором фракцию ТРГ, полученную при разделении, по меньшей мере частично повторно направляют на стадию КПК.4. The method according to claim 1, in which the fraction of the TWG obtained by separation, at least partially re-sent to the stage of the CPC. 5. Способ по п.1, в котором гидроочистку проводят в присутствии катализатора на основе соединений металлов группы VI и/или группы VIII, нанесенных на носитель.5. The method according to claim 1, in which the hydrotreating is carried out in the presence of a catalyst based on metal compounds of group VI and / or group VIII, supported on a carrier. 6. Способ по п.1, в котором гидроочистку проводят при температуре в диапазоне от 200 до 400°C.6. The method according to claim 1, in which the hydrotreating is carried out at a temperature in the range from 200 to 400 ° C. 7. Способ по п.6, в котором температура находится в диапазоне от 330 до 380°C.7. The method according to claim 6, in which the temperature is in the range from 330 to 380 ° C. 8. Способ по п.1, в котором давление на стадии гидроочистки находится в диапазоне от 2 до 10 МПа (от 20 до 100 бар).8. The method according to claim 1, in which the pressure at the stage of hydrotreating is in the range from 2 to 10 MPa (from 20 to 100 bar). 9. Способ по п.8, в котором давление находится в диапазоне от 4 до 8 МПа (от 40 до 80 бар).9. The method of claim 8, in which the pressure is in the range from 4 to 8 MPa (40 to 80 bar). 10. Способ по п.1, в котором компонент (b) кислой природы представляет собой алюмосиликат, имеющий мольное соотношение SiO2/Al2O3 в диапазоне от 50 до 300.10. The method according to claim 1, in which the component (b) of an acidic nature is an aluminosilicate having a molar ratio of SiO 2 / Al 2 O 3 in the range from 50 to 300. 11. Способ по п.1, в котором компонент (b) кислой природы представляет собой алюмосиликат, имеющий пористость в диапазоне от 0,4 до 0,5 мл/г.11. The method according to claim 1, in which component (b) of an acidic nature is an aluminosilicate having a porosity in the range from 0.4 to 0.5 ml / g. 12. Способ по п.1, в котором компонент (b) кислой природы представляет собой микропористый алюмосиликат, имеющий порошковый рентгеновский спектр, который не свидетельствует о кристаллической структуре, и не имеет пиков.12. The method according to claim 1, in which the component (b) of an acidic nature is a microporous aluminosilicate having a powder x-ray spectrum, which does not indicate a crystalline structure, and has no peaks. 13. Способ по п.1, в котором металл компонента (а) выбирают из платины, иридия или их смеси.13. The method according to claim 1, in which the metal of component (a) is selected from platinum, iridium, or mixtures thereof. 14. Способ по п.1, в котором металл, или смесь металлов, компонента (а) находится в количестве в диапазоне от 0,1 до 5 мас.%, в расчете на общую массу каталитической композиции, при этом массовое процентное содержание металла, или металлов, относится к содержанию металла в виде элементарного металла.14. The method according to claim 1, in which the metal, or a mixture of metals, component (a) is in an amount in the range from 0.1 to 5 wt.%, Calculated on the total weight of the catalytic composition, while the mass percentage of the metal, or metals, refers to the metal content in the form of elemental metal. 15. Способ по п.14, в котором металл находится в количестве в диапазоне от 0,3 до 1,5%.15. The method according to 14, in which the metal is in an amount in the range from 0.3 to 1.5%. 16. Способ по п.1, в котором реакцию гидроочищенного легкого рециклового газойля с водородом проводят в присутствии каталитической системы, включающей:16. The method according to claim 1, in which the reaction of the hydrotreated light recycle gas oil with hydrogen is carried out in the presence of a catalytic system, including: a) один или более металлов, выбранных из Pt, Pd, Ir, Ru, Rh и Re;a) one or more metals selected from Pt, Pd, Ir, Ru, Rh and Re; b) алюмосиликат кислой природы, выбранный из цеолита, принадлежащего к семейству MTW, и полностью аморфного микропористого алюмосиликата, имеющего мольное соотношение SiO2/Al2O3 в диапазоне от 30 до 500, площадь поверхности более чем 500 м2/г, объем пор от 0,3 до 1,3 мл/г, средний диаметр пор менее 40 Å, при температуре в диапазоне от 240 до 380°C, при давлении в диапазоне от 1 до 10,1 МПа (от 10 до 100 атм), при объемной скорости в диапазоне от 0,5 до 5 ч-1 и соотношении водорода и питающего потока (Н2/HC) от 400 до 2000 л (н.у.)/кг.b) an acidic aluminosilicate selected from a zeolite belonging to the MTW family and a fully amorphous microporous aluminosilicate having a SiO 2 / Al 2 O 3 molar ratio in the range of 30 to 500, a surface area of more than 500 m 2 / g, pore volume from 0.3 to 1.3 ml / g, average pore diameter less than 40 Å, at a temperature in the range from 240 to 380 ° C, at a pressure in the range from 1 to 10.1 MPa (from 10 to 100 atm), at space velocity in the range from 0.5 to 5 h -1 and the ratio of hydrogen and the feed stream (N 2 / HC) from 400 to 2000 l (NU) / kg 17. Способ по п.16, в котором кислотный компонент (b) представляет собой цеолит MTW; давление составляет выше 2 МПа (20 атм) и ниже или равно 8 МПа (80 атм), и температура находится в диапазоне от 250 до 330°C.17. The method according to clause 16, in which the acid component (b) is an MTW zeolite; the pressure is above 2 MPa (20 atm) and lower than or equal to 8 MPa (80 atm), and the temperature is in the range from 250 to 330 ° C. 18. Способ по п.16, в котором кислотный компонент (b) представляет собой алюмосиликат, давление составляет выше 2 МПа (20 атм) и ниже или равно 8 МПа (80 атм), и температура находится в диапазоне от 300 до 380°C.18. The method according to clause 16, in which the acid component (b) is an aluminosilicate, the pressure is above 2 MPa (20 atm) and less than or equal to 8 MPa (80 atm), and the temperature is in the range from 300 to 380 ° C . 19. Способ по п.1, в котором гидроочистку проводят при часовой объемной скорости в диапазоне от 0,3 до 3 ч-1.19. The method according to claim 1, in which the hydrotreating is carried out at an hourly space velocity in the range from 0.3 to 3 h -1 . 20. Способ по п.1, в котором на стадии гидроочистки применяют соотношение Н2/питающий поток в диапазоне от 200 до 2000 л (н.у.)/л.20. The method according to claim 1, in which at the stage of hydrotreating apply the ratio of N 2 / feed stream in the range from 200 to 2000 l (NU) / L. 21. Способ крекинга с псевдоожиженным катализатором (КПК) для превращения происходящих из нефти углеводородных фракций в смеси, содержащие легкий рецикловый газойль (ЛРГ), в котором температура предварительного нагрева составляет в диапазоне от 240 до 350°C, а процесс проводят при температуре в диапазоне от 490 до 530°C. 21. The method of cracking with a fluidized catalyst (CPC) for converting oil-derived hydrocarbon fractions into mixtures containing light recycle gas oil (LHG), in which the preheating temperature is in the range from 240 to 350 ° C, and the process is carried out at a temperature in the range from 490 to 530 ° C.
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