WO2010144191A2 - Procédé de craquage catalytique sur lit fluidisé comprenant un procédé de conversion des gaz de combustion - Google Patents

Procédé de craquage catalytique sur lit fluidisé comprenant un procédé de conversion des gaz de combustion Download PDF

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Publication number
WO2010144191A2
WO2010144191A2 PCT/US2010/033545 US2010033545W WO2010144191A2 WO 2010144191 A2 WO2010144191 A2 WO 2010144191A2 US 2010033545 W US2010033545 W US 2010033545W WO 2010144191 A2 WO2010144191 A2 WO 2010144191A2
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Prior art keywords
regenerator
catalytic cracking
fluid catalytic
recited
catalyst
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WO2010144191A3 (fr
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Frank J Elvin
Iraj Isaac Rahmim
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Co2 Solutions LLC
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Co2 Solutions LLC
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    • 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
    • C10G11/14—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts
    • C10G11/18—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts according to the "fluidised-bed" technique
    • C10G11/182—Regeneration
    • 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
    • C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
    • C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P30/00—Technologies relating to oil refining and petrochemical industry
    • Y02P30/40—Ethylene production

Definitions

  • the present invention relates to a fluid catalytic cracking process which takes advantage of a flue gas conversion plant including a Fischer-Tropsch process to reduce carbon dioxide emissions and increase the production of useful hydrocarbon products, such as diesel oil, jet fuel, and other products.
  • a fluid catalytic cracking unit typically includes a reactor, a catalyst regenerator, which burns off carbon from the catalyst used in the reactor, a flue gas treatment plant which treats the flue gas from the catalyst regenerator, and a fractionator, which separates the products from the reactor.
  • the present invention discloses modifications to a fluid catalytic cracking unit in order to improve its hydrocarbon yield and to substantially reduce its carbon dioxide (CO2) emissions. As explained in more detail below, this is accomplished by combining one or more of the following modifications to the process: - Send the flue gases from the fluid catalyst cracking unit to a flue gas conversion plant which includes a Fischer-Tropsch process to convert H 2 and CO into hydrocarbon products such as diesel fuel.
  • any low value refinery fuel or other hydrocarbon or carbon source product in addition to the coke present in the catalyst to be regenerated in order to increase the amount of carbon available for the production of CO (which is then utilized in the Fischer- Tropsch process to increase the hydrocarbon yield.
  • Particularly useful for this purpose is the injection into the regenerator of the low value slurry oil from the bottoms of the main fractionator(s) of the fluid catalytic cracking unit. This also helps re-establish heat-balance in the reactor.
  • the heat balance is negatively affected with the combustion of carbon to CO (only 4,000 BTU/lb of carbon) instead of its combustion to CO 2 (14,000 BTU/lb of carbon) when operating in partial burn.
  • the incorporation of these process modifications to the fluid catalytic cracking unit may include the physical modification of the facility beyond the addition of the flue gas conversion plant with Fischer-Tropsch process. These modifications may include the addition of nozzles and distribution grids to the catalyst regenerator, the addition or modification of nozzles to the main fractionator(s), as well as resizing of components such as the regenerator and the gas plant, especially if the flue gas conversion plant does not include its own fractionators and instead makes use of the main fractionator(s) of the fluid catalytic cracking unit.
  • the Fischer-Tropsch products may then be routed to the main fractionator of the fluid catalytic cracking unit or to a separate fractionator.
  • the hydrogen can also be extracted from the off-gas from the fluid catalytic cracking unit.
  • slurry oil is injected into the regenerator, and the control system may be programmed to control the slurry oil injection at between 1 % and 10% of fluid catalytic cracking unit feed (preferably 5%).
  • CO 2 can be recycled with the air being injected into the catalyst regenerator of the fluid catalytic cracking unit to recycle the CO 2 to extinction and produce more CO.
  • the controller maintains equilibrium while effectively recycling the CO 2 to extinction.
  • heat can be supplied from extra coke on the catalyst, derived from cracking heavier, higher carbon feeds, or by rerouting the fluid catalytic cracking unit fractionator bottoms (slurry oil) into the regenerator instead of routing it to heavy fuel oil storage.
  • the slurry oil is about 90% carbon, making it an ideal source of carbon to produce CO in the regenerator and provide heat to heat-balance the fluid catalytic cracking unit.
  • the CO is converted into hydrocarbon in the Fischer-Tropsch unit.
  • the use of heavier feeds in the reactor and/or the recycle of slurry oil to the regenerator provide good ways to heat-balance the fluid catalytic cracking unit.
  • the reduction in available heat caused by not burning the CO to CO 2 in the regenerator also can be compensated by burning any other low value refinery fuel or product in the catalyst regenerator of the fluid catalytic cracking unit - such as absorber off-gas from the fluid catalytic cracking unit gas plant, and even gasoline from the fluid catalytic cracking unit if the price of gasoline is below diesel price, most of which will provide CO for diesel production in the Fischer-Tropsch process.
  • any hydrocarbon or carbon source for example charcoal or coal or wood or biomass, can be burned to produce the heat balance, and the CO from combustion can go to the Fischer-Tropsch process to produce hydrocarbons such as diesel fuel.
  • Another source of heat for the reactor of the fluid catalytic cracking unit can be the excess heat from the Fischer-Tropsch process.
  • the heat from the Fischer-Tropsch process can be converted into electricity, which can be used to heat up the regenerator using microwaves or radiant heating coils.
  • electricity from any source could be used to balance the fluid catalytic cracking unit heat requirements.
  • the heat from the Fischer-Tropsch process can be used to drive the compressor for the flue gas treatment for the fluid catalytic cracking unit, either by generating steam to directly drive the compressor or by generating steam to produce electricity to drive the compressor.
  • one embodiment of the present invention injects slurry oil (or any other solid, liquid or gaseous source of carbon or hydrocarbon such as charcoal, coal, biomass, etc.) into the catalyst regenerator, converts it to CO in the regenerator, and converts this CO to hydrocarbon in the Fischer-Tropsch flue gas conversion plant.
  • Residue cracking (catalytic cracking of heavy, high carbon feedstocks, vacuum bottoms, and atmospheric bottoms, as well as gas oil cracking) may be included in the process that is carried out in the fluid catalytic cracking unit.
  • the fluid cracking catalyst preferably is a zeolite or non zeolite silica alumina catalyst. It preferably contains less than one part per million Pt or other oxidation promoters, oxidation catalysts or oxidation chemicals. It preferably has pore volumes of 0.3 to 0.8 cc/gram and a surface area of at least 50 m 2 /g. It preferably has at least 1 ppm Ni or similar reducing promoter and less than 5000 ppm of Ti.
  • the carbon on regenerated catalyst (CRC), regenerator temperature and the flue gas composition are preferably continuously monitored and the relative flows of combustion gas, slurry oil, and CO2 recycle streams adjusted to achieve maximum CO production at the lowest CO 2 recycle rate.
  • the diesel oil and other hydrocarbon products from the Fischer-Tropsch flue gas conversion plant may be processed in the fluid catalytic cracking unit main fractionator.
  • FIG 1 is a schematic of a standard prior art fluid catalytic cracking unit (FCCU);
  • Figure 2 is a schematic of a fluid catalytic cracking unit including one embodiment of the present invention
  • FIG 3 is a schematic showing the inputs and outputs for the Flue gas conversion unit, which is Section 6 in Figure 2;
  • Figure 4 is a schematic showing an alternative embodiment of the Flue gas conversion unit of Figure 3
  • Figure 5 is a schematic showing a second alternative embodiment of the Flue gas conversion unit of Figure 3;
  • FIG. 6 is a schematic showing another alternative embodiment of the Flue gas conversion unit
  • FIG. 7 is a schematic showing some of the modifications which may be made to the catalyst regenerator
  • Figure 8A is an enlarged view of the slurry oil injection nozzle of Figure 7;
  • Figure 8B is an end view of the nozzle of Figure 8A;
  • Figure 9 is a table showing the fuel oil yield for the base case of a prior art fluid catalytic cracking unit
  • Figure 10 is a table showing the fuel oil yield for a fluid catalytic cracking unit with two different embodiments of the present invention wherein the regenerator is operated in partial CO burn. In case 2a the CO2 is not recycled, while in case 2B the CO 2 is recycled to extinction (in both cases there is no slurry oil injected into the regenerator);
  • Figure 11 is a table showing the fuel oil yield for a fluid catalytic cracking unit with the same two embodiments of the present invention as in Figure 10, except slurry oil is injected into the regenerator in both of these cases;
  • Figure 12 is a table showing the fuel oil yield for a fluid catalytic cracking unit with the same two embodiments of the present invention as in Figure 10, except that a shift reactor is used to produce H 2, in one instance there is no CO 2 recycle while in the second case there is CO 2 recycle to extinction;
  • Figure 13 is a table showing the fuel oil yield for a fluid catalytic cracking unit with the same two embodiments of the present invention as in Figure 10, except with a different fresh feedstock.
  • a typical prior art fluid catalytic cracking unit 10' has five major sections as shown in Figure 1 :
  • - section 4 is the catalyst regenerator 18'; and - section 5 is the flue gas treatment plant 20'.
  • Fluid cracking catalyst (FCC) in the fluid bed reactor 12' facilitates a reaction which converts the heavy hydrocarbon feed 22 (long- chain hydrocarbon molecules) into high value transportation fuels 24, 26 and liquid petroleum gases (LPG) 28, 30.
  • the feed 22 is atomized with steam 34 on its way into the reactor.
  • the atomized heavy hydrocarbon feed 22 is mixed with very hot, powdered catalyst, causing the heavy hydrocarbon feed 22 to vaporize and crack into smaller molecules.
  • the cracked product vapors are then separated from the spent catalyst.
  • the spent catalyst is stripped with steam 36 in the reactor stripper 48' to remove entrained hydrocarbons and is sent to the regenerator 18', and the cracked hydrocarbon vapors are sent to the main fractionator(s) 14'.
  • feed 22 is not converted or is only partially converted, resulting in low value slurry oil 32, which comes out of the bottoms of the fractionator(s) 14'). Some of the feed 22 is converted to low value coke, which is deposited on the spent catalyst.
  • the reactor 12' operates between 85O 0 F and 1100 0 F, at pressures of between 2 psig and 60 psig and with catalyst to oil ratios of between 2:1 and 30:1.
  • the main fractionator 14' (Section 2) separates the diesel 26 and slurry oil 32 from the gas 38, LPG 28, 20 and gasoline 24 by distillation.
  • the feed atomizing steam 34 and catalyst stripping steam 36 are removed from the fractionator 14' overhead receiver as condensed water 40.
  • the gas plant 16' (Section 3) further separates the off-gas 38, LPG 28, 30 and gasoline 24 by distillation and absorption.
  • the coke is burned off the spent catalyst with a gas containing oxygen, usually air 42.
  • the flue gases 44 from the catalyst regenerator 18' are a mixture of CO, CO2, SO2, N 2 , NO x and catalyst fines.
  • the catalyst regenerator 18' operates at temperatures between 1100 0 F and 1600 0 F and similar pressures to the reactor 12'.
  • CO in the flue gas 44 if present, is converted to CO 2 in a waste heat boiler, and the SO2 and catalyst fines are removed in a wet gas scrubber.
  • the CO2 and N 2 exit the fuel gas treatment section 20' (Section 5) at the outlet 46.
  • Fluid cracking catalyst circulates continuously from the reactor 12' (Section 1 ) to the catalyst regenerator 18' (Section 4), flowing from the regenerator 18' to the reactor 12' along the path (X), and from the reactor 12' to the regenerator 18' along the path (Y).
  • the catalyst provides four important functions: cracking; coke removal; removal of heat from the regenerator 18' (Section 4); and supply of heat to the reactor 12' (Section 1 ).
  • the fluid catalytic cracking unit Reactor (Section 1): Hot catalyst from the catalyst regenerator 18' (Section 4), at the regenerator temperature (approximately 1400 0 F) flows into the reactor 12' (Section 1 ) along the path labeled (X).
  • the hot catalyst provides the endothermic heat of reaction, heat of vaporization, and the heat to heat the oil to its cracking temperature.
  • the catalyst circulation rate depends on the feed preheat temperature, regenerator temperature, and reactor temperature, and is usually a ratio of about 6:1 catalyst to oil. However, some designs operate as high as a 30:1 catalyst to oil ratio.
  • the reactor temperature is controlled at approximately 1000 0 F.
  • the feed 22 to the reactor 12' (Section 1 ) is atomized with steam 34.
  • the reactor 12' converts a heavy hydrocarbon feedstock 22, with an API gravity of between 10° and 35° and a Conradson Carbon content of between 0% and 10%, into C 5 + gasoline 24, diesel 26, slurry oil 32, absorber off-gas 38 (which may include H 2 , H 2 S, Ci s, C 2 S,), C 3 S LPG 28, C 4 S LPG 30, and coke. Most of the coke is produced in the cracking reaction where it is deposited onto the surface of the catalyst.
  • the coke contains traces of sulfur, and some coke results from a small quantity of hydrocarbons that are entrained and absorbed onto the catalyst as it leaves the reactor-stripper 48' and enters the regenerator 18'.
  • the vapor products may be separated from the spent catalyst in the reactor 12' by many known separation devices such as cyclones. This ensures the correct oil/catalyst residence time and ensures that no catalyst goes over into the main fractionators 14' (Section 2).
  • the catalyst is stripped with steam 36 in the reactor stripper 48' as it flows from the reactor 12' (Section 1 ) to the regenerator 18' (Section 4), and the stripped hydrocarbons and steam are returned to the reactor 12'.
  • the atomizing steam 34, stripping steam 36, and reactor products leave the reactor 12' as a vapor and flow into the fractionators 14' (Section 2) for separation.
  • the catalyst flows from the reactor 12' (Section 1 ) to the regenerator 18' (Section 4) where the coke is burned off and the catalyst is reheated.
  • a fluid catalytic cracking unit 10' that is processing a gas oil with low Conradson carbon ( ⁇ .05%) may only produce 5% coke.
  • a fluid catalytic cracking unit 10' processing a residue feedstock with up to 10% Conradson carbon may produce up to 12% coke.
  • the coke includes about 6% hydrogen, 94% carbon, and trace amounts of sulfur. It is burned off the catalyst with an oxygen bearing gas 42, such as air.
  • the regenerator temperature is approximately 1400 0 F, and in some residue feedstock processing units the temperature is controlled with steam coils and heat exchangers to remove any excess heat.
  • the flue gases 44 (which may include H 2 O, SO 2 , N 2 , CO and CO 2 .) flow from the regenerator 18' (Section 4) to the flue gas treatment plant 20' (section 5) where any CO is burned to CO 2, and the SO 2 and catalyst fines are removed.
  • the flue gases 44 before treating can have a varied composition. They may contain 0% to 50% CO; 25% to 100% CO 2 , 0% to 6% O2; and 0%-80% N 2 depending on how the fluid catalytic cracking unit is operated, and whether air, or oxygen, or oxygen in air, or O 2 with other gases are used for combustion in the regenerator 18'.
  • the flue gas treatment plant 20' may include a waste heat boiler which converts CO to CO2 and may have a NO x treatment reactor.
  • the fluid catalyst is the fluid catalyst
  • the fluid catalyst provides the surface area, catalytic acidity and activity in the reactor 12'. As it leaves the reactor 12', it removes the unwanted coke (a compound with about 6% hydrogen and 94% carbon) produced during the cracking reactions.
  • the catalyst regenerator 18' the catalyst absorbs most of the heat released when the coke is burned off the catalyst with an oxygen rich gas 42 (usually air).
  • the catalyst is usually made from alumina-silica micro-spheres with diameters of 2-200 microns and impregnated with zeolites (including HY, REY, USY, ZSM-5), additives, including bottom cracking additive (BCA) max diesel additive, metal traps, and oxidation additives and co-catalysts such as Pt.
  • BCA bottom cracking additive
  • Figure 2 shows the fluid catalyst cracking unit 10 that has been modified to incorporate a flue gas conversion plant 50 (Section 6) within the facility.
  • the flue gas conversion plant 50 (Section 6) has within it a number of individual process units, including a Fischer-Tropsch process Plant (also referred to as an F-T plant), which produces useful hydrocarbons from the CO in the flue gas of the regenerator 18.
  • a Fischer-Tropsch process Plant also referred to as an F-T plant
  • the Fischer-Tropsch reactor itself can be slurry-type or tubular fixed-bed or fluidized bed.
  • the Fischer-Tropsch catalyst might be cobalt-based or iron- based or some other, newer, alternative.
  • the flue gas conversion plant 50 may include the following elements (See Figure 6):
  • the schematic of Figure 2 involves several modifications to the standard, prior art fluid catalytic cracking unit 10' of Figure 1 , which may include the modification of the fluid catalytic cracking unit main fractionator 14', regenerator 18', and gas plant 16', as explained in more detail below. It also includes the addition of a flue gas conversion plant 50 (Section 6).
  • the flue gas conversion plant 50 may have a CO shift reactor (See Figure 5), or there may not be a CO shift reactor (See Figure 3). It may include a hydrogen plant (See Figure 4), or it may use imported hydrogen.
  • the fluid catalyst cracking unit 10 includes the full integration of the Flue gas conversion plant 50 (and associated equipment such as mild hydrocracker and additional hydrotreating facilities, shift reactor and hydrogen plant) with the fluid catalytic cracking unit regenerator 18, fractionator 14 and gas plant 16.
  • the fluid catalytic cracking unit regenerator 18, fractionator 14 and gas plant 16 16.
  • modifications to the main fractionator 14' and the gas plant 16' may not be necessary.
  • modifications to the main fractionator 14' and the gas plant 16' may not be made.
  • a new fluid catalytic cracking unit flue gas conversion plant 50 (Section 6) is added to the fluid catalytic cracking unit.
  • the main process unit in the flue gas conversion section 50 is a Fischer-Tropsch (FT) plant.
  • FIG 3 shows an example of a flue gas conversion plant 50 (Section 6 of Figure 2), without shift reactor, wherein H 2 is imported from outside the fluid catalytic cracking unit complex. In that case, only the Fischer-Tropsch process is needed to convert the CO to hydrocarbons such as diesel oil in the flue gas conversion plant 50 (Section 6).
  • FIG. 4 shows an example of a flue gas conversion plant 50 (Section 6 of Figure 2), wherein H 2 is generated in a hydrogen plant that is incorporated into the fluid catalytic cracking unit complex, using either natural gas or absorber off-gas 38 from the fluid catalytic cracking unit gas plant.
  • Figure 5 shows an example of a flue gas conversion plant 50 (Section 6 of Figure 2), wherein H 2 is generated in a hydrogen plant that is incorporated into the fluid catalytic cracking unit complex, using either natural gas or absorber off-gas 38 from the fluid catalytic cracking unit gas plant.
  • Figure 5 shows an example of a flue gas conversion plant 50 (Section 6 of Figure 2)
  • a new nozzle may be added either in the reactor vapor overhead line 52 or into the main fractionation tower itself 54. This allows the product from the flue gas conversion plant 50 (Section 6) to be introduced and processed in the fractionators 14 (Section 2).
  • the catalyst regenerator 18 also may be modified to improve the conversion of CO 2 to CO as shown in Figures 2 and 7, adding a spray nozzle and/or an additional combustion air grid.
  • the slurry oil 32 from the main fractionators is injected into the lower section of the regenerator 18 (Section 4) preferably about three feet above the combustion air grid 56, at a point in the regenerator where the carbon on the catalyst is lowest and the O 2 concentration is the highest.
  • a secondary oxygen source 42* is injected along with the slurry oil 32 to provide atomization and controlled stoichiometric combustion of the slurry oil 32 to CO and H 2 O.
  • the CO 2 recycle also can be injected through the combustion air grid 56 along with the oxygen rich combustion gas 42.
  • a nozzle 58 See Figures 7, 8A, and 8B
  • Nozzles 58 may be added to allow the injection of any hydrocarbon, crude oil, oil sand, tar sand, synthetic oil from coal, tar sands or oil sands, or bio-mass, natural gas, absorber fluid catalytic cracking unit gas plant off-gas 38 or fluid catalytic cracking unit fractionator bottoms (also referred to as slurry oil 32), without contacting water or water vapor, for the purpose of heat balancing the fluid catalytic cracking unit 10 when recycling CO 2 .
  • the slurry oil 32 can be injected into both catalyst beds but preferentially is injected into the low CRC area in the full CO burn vessel.
  • the CO 2 can be injected into both vessels, but preferentially into the high CRC area in the partial burn vessel.
  • the CO 2 recycle can be injected into the regenerator 18 through the combustion air grid 56 with the air or oxygen rich combustion gas, with the slurry oil 32 via the nozzle 58, with the secondary oxygen source 42* at the nozzle 58, and/or through its own CO 2 recycle grid 60.
  • the nozzle 58 includes a slurry oil delivery pipe 62 inside a slightly larger "sleeve" pipe 64 in an arrangement similar to that of a single tube, shell and tube heat exchanger.
  • the slurry oil travels in the "tube side” 62, while air or recycled CO242 * (or a mixture of these) travels along the "shell side” 64.
  • This sleeve arrangement provides an insulating effect on the pipe 62 to keep it relatively cool against the heat of the regenerator 18, to prevent unwanted coking of the slurry oil in the pipe 62.
  • the pipe 62 terminates inside the sleeve 64 at a perforated plate 66 which allows the air/recycled CO 2 42 * to flow around and along the pipe 62 to continually cool it, and then diffuse into the slurry oil 32 in an atomizing chamber 68. Finally, the mixture of the slurry oil 32 and the air/recycled CO 2 42 * are sprayed out into the regenerator 18 through a horizontally oriented slotted opening 70 to ensure that the slurry oil is sprayed substantially horizontally, away from the refractory-lined walls of the regenerator 18 and not directed toward the distributor grids 60, 56.
  • the nozzle 58 includes a flange 72 for mounting to the regenerator wall.
  • the nozzle 58 projects into the regenerator at least far enough to ensure that it clears the refractory material lining the wall of the regenerator 18.
  • the fluid catalytic cracking unit 10 operates in partial CO burn. This means that the CRC is controlled between 0.1 % and 1.2 % in the fluid catalytic cracking unit regenerator 18 (Several methods are known in the industry for determining and controlling the CRC in the regenerator. For instance, the catalyst may be sampled hourly and the level of CRC can then be visually established, or the temperature in the regenerator can be monitored to empirically determine and control the CRC level).
  • the treated flue gases 46 from the flue gas treatment 20 (Section 5) are routed to the new flue gas conversion plant 50 (Section 6) where the CO is converted to diesel fuel.
  • the process is enhanced if the excess CO 2 from the flue gas conversion plant 50 (section 6) is recycled to the catalyst bed of the fluid catalytic cracking unit regenerator 18 to boost CO production, and ultimately convert all coke to CO instead of CO 2 .
  • the CO and CO2 are in equilibrium at a ratio of about 1 :1. This ratio stays constant as the CO 2 is recycled, as it is defined by thermodynamic conditions. Therefore, as the CO 2 is recycled, more Carbon is converted to CO. Ultimately, there is no net CO2, only CO2 recycle. All the carbon on the catalyst is converted to CO.
  • the heat released in the regenerator 18 in this operation is less than that typically required to balance the requirements of the fluid catalytic cracking unit reactor 12 (an exception may occur when processing high residue feedstocks, particularly if oxygen is injected into the regenerator to burn off the coke, as explained in more detail later). Therefore, additional fuel is injected into the catalyst regenerator 18. This can come from any carbon or hydrocarbon source (in addition to the coke present in the catalyst to be regenerated), and will also be converted to CO (and eventually into diesel fuel in the flue gas conversion plant 50).
  • a readily available source of additional fuel is the slurry oil 32 from the bottoms of the main fractionators, as it has a low value and a high carbon content, although absorber off-gas 38 from the fluid catalytic cracking unit gas plant could be used instead or in addition to the slurry oil to add heat or an entirely different source of carbon could be used. Heat balances are shown in Figure 12.
  • the flue gas conversion plant 50 converts the CO from the flue gas of the catalyst regenerator 18, water, and external H 2 if needed by the Fischer-Tropsch (FT) plant to hydrocarbons.
  • the hydrocarbon product from the Fischer-Tropsch process is middle distillate or diesel fuel, which is then processed in the main fractionator 14 of the fluid catalytic cracking unit.
  • the CO for the Fischer- Tropsch process comes from the flue gas of the catalyst regenerator 18.
  • the hydrogen may come from a variety of sources. For example, it can be imported as shown in Figure 3. Alternatively, H 2 may be produced by an electrolytic process. Hydrogen also can be extracted from the fluid catalytic cracking unit absorber off-gas 38 by membrane separation or pressure swing absorption.
  • the H 2 can be generated from an onsite H 2 plant using natural gas or preferably fluid catalytic cracking unit off- gas 38 as a feed. (The H 2 also could be supplemented from an external source and/or from H 2 in the fluid catalytic cracking unit absorber off-gas 38.)
  • H 2 also could be supplemented from an external source and/or from H 2 in the fluid catalytic cracking unit absorber off-gas 38).
  • the CO 2 from either the hydrogen plant ( Figure 4) or the shift reactor ( Figure 5) is vented to atmosphere or, alternatively, can be recycled to the catalyst regenerator 18.
  • the shift reactor consumes 67% of the CO from the treated flue gases 46 but still results in significant diesel fuel production in the Fischer-Tropsch plant.
  • Heat See dotted line in Figure 2) from the flue gas conversion plant 50 (Section 6) is recycled from the flue gas conversion plant 50 in the form of hot CO 2 that is recycled to the catalyst regenerator 18 to heat-balance the catalyst regenerator 18 (Section 4).
  • FIGs 10 and 11 The calculated yields from the modified fluid catalytic cracking unit with the Fischer-Tropsch flue gas conversion plant 50 (Section 6) are shown in Figures 10 and 11.
  • the improved process results in increased diesel fuel yields, reduced slurry oil yields, and lower CO 2 emissions.
  • Figure 9 shows the base gas oil yields from the base fluid catalytic cracking unit 10' without the Fischer-Tropsch flue gas conversion. In this case, it can be seen that a feed of 36,930 barrels per day yields 6,377 barrels per day of diesel fuel. This partial CO burn operation is in heat balance.
  • Figure 10 shows the yields in two different cases in which the fluid catalytic cracking unit 10 is coupled with the Fischer-Tropsch flue gas conversion plant 50 without shift in accordance with Figures 2 and 4, with the flue gases 46 being fed to the flue gas conversion plant 50 (Section 6) but without the slurry oil 32 being injected into the regenerator 18 (Section 4).
  • Column 2a is for the case in which the CO2is not recycled
  • column 2b is for the case in which the CO2 is recycled to extinction.
  • FIG 11 shows yields for the same process as shown in Figure 10, except with the slurry oil 32 being injected into the regenerator 18 (Section 4).
  • the CO comes from the flue gases 46, from the carbon deposited on the catalyst in the fluid catalytic cracking unit reactor 12 (Section 1 ), and from the carbon in the slurry oil 32 injected into the regenerator 18 (Section 4).
  • the heat from burning the slurry oil 32 in the regenerator 18 once again heat-balances the operation.
  • the same feed produces 8,637 barrels per day of diesel fuel without CO 2 recycle and 9,332 barrels per day of diesel fuel with CO 2 recycle, as compared with 6,377 barrels per day in the base case.
  • Figure 12 shows the case in which the shift reaction is used as shown in Figure 5, and the flue gases 46 go to the flue gas conversion plant 50 (Section 6), but the slurry oil 32 does not go to the regenerator 18 (Section 4).
  • part of the CO is converted to H 2 in the shift reactor.
  • Carbon on the catalyst from the residue feedstock supplies the heat to once again heat- balance the operation.
  • the same feed produces 6,638 barrels per day of diesel fuel without CO 2 recycle and 6,898 barrels per day of diesel fuel with CO 2 recycle.
  • Figure 13 shows a different fresh feed, using the arrangement of Figures 2 and 4, with the slurry oil 32 not being fed to the regenerator 18 (Section 4) and with the flue gases 46 being fed to the flue gas conversion plant 50 (Section 6), both with and without CO 2 recycle.
  • the application of the processes disclosed in this specification also allows for the operation of fluid catalytic cracking units under some unique and particularly interesting conditions. Already discussed above are the capabilities to operate: - under partial burn in the regenerator 18 to increase the production of
  • air can be injected into the regenerator 18 to help burn the coke.
  • a better choice is to inject oxygen into the regenerator 18, but if the coke is being burned to CO2, the amount of heat generated in the regenerator 18, when injecting oxygen, may be too great. This is especially true when operating with high residue feedstocks (such as feedstock with up to 10% Conradson carbon which may produce up to 12% coke).
  • the amount of heat generated can be so high that it risks melting the regenerator 18, even when using steam coils to remove the excess heat. Even when high residue feedstocks are not involved, it may be necessary to dilute the air or oxygen with nitrogen to prevent this high heat load in the regenerator 18.
  • thermodynamic equilibrium is normally a 1 :1 ratio of CO:CO2. If the CO2 is recycled, then the coke in the catalyst in the regenerator 18 will burn to CO in order to maintain that thermodynamic equilibrium). This substantially reduces the heat load as the heat released when burning the carbon to CO is one third of the heat released when burning the carbon to CO 2 .
  • the fluid catalytic cracking unit can then operate using these high residue feedstocks with oxygen injection diluted with the CO 2 recycle, eliminating the need to dilute the oxygen with nitrogen. The reason is two- fold:
  • the CO2 recycle dilutes the oxygen without the need for nitrogen. This provides a distinct advantage in that there is no longer a need to contend with nitrogen coming off as part of the flue gases of the regenerator 18. The separation is much simpler if there are only CO and CO2 coming off of the regenerator 18 (because the recycled CO2 is acting as the diluent for the oxygen) instead of CO, CO2, and nitrogen (with the nitrogen acting as the diluent). If the nitrogen is not separated out of the flue gas stream before it is sent to the flue gas conversion plant 50, then this large volume of nitrogen must be pressurized from the operating pressure in the regenerator (up to 60 PSIG) to that of the Fischer-Tropsch process (about 300 PSIG), and this could be very expensive.

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

Abstract

La présente invention concerne un procédé permettant de réduire les émissions de dioxyde de carbone et d'augmenter la production d'hydrocarbures de plus grande valeur dans une unité de craquage catalytique sur lit fluidisé.
PCT/US2010/033545 2009-06-10 2010-05-04 Procédé de craquage catalytique sur lit fluidisé comprenant un procédé de conversion des gaz de combustion Ceased WO2010144191A2 (fr)

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US18568209P 2009-06-10 2009-06-10
US61/185,682 2009-06-10
US12/615,453 2009-11-10
US12/615,453 US20100314290A1 (en) 2009-06-10 2009-11-10 Fluid catalytic cracking process including flue gas conversion process

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