CN103725309B - A kind of catalyst regeneration process reducing Carbon emission - Google Patents

A kind of catalyst regeneration process reducing Carbon emission Download PDF

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Publication number
CN103725309B
CN103725309B CN201210387210.1A CN201210387210A CN103725309B CN 103725309 B CN103725309 B CN 103725309B CN 201210387210 A CN201210387210 A CN 201210387210A CN 103725309 B CN103725309 B CN 103725309B
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dense
bed
catalyzer
catalyst
phase bed
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CN103725309A (en
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许友好
王新
李首先
龚剑洪
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Sinopec Research Institute of Petroleum Processing
China Petroleum and Chemical Corp
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Sinopec Research Institute of Petroleum Processing
China Petroleum and Chemical Corp
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    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P30/00Technologies relating to oil refining and petrochemical industry
    • Y02P30/40Ethylene production

Abstract

A kind of catalyst regeneration process reducing Carbon emission, band Pd/carbon catalyst first in burning tank after pure oxygen partial regeneration, enter through dilute phase pipe in the dense-phase bed of regenerating unit and burn residual coke, dense-phase bed arranges heat collector to control the temperature of dense-phase bed, flue gas traps enter smoke energy recovering system, carbon dioxide separating system separating carbon dioxide successively after cyclonic separation after, and the direct Returning reactor of regenerated catalyst recycles.The method not only can make catalyzer holomorphosis, and catalyst activity is more evenly distributed, thus reduces catalytic cracking by-product coke and dry gas yied; And significantly can reduce carbon emission, even reach zero carbon emission.

Description

A kind of catalyst regeneration process reducing Carbon emission
Technical field
The present invention relates to the renovation process containing Pd/carbon catalyst in a kind of hydrocarbon processing process.More particularly, the present invention relates to the catalyst regeneration process realizing carbon dioxide discharge-reduction in mink cell focus catalytic cracking process.
Background technology
Now, lot of challenges that the development of whole world petroleum refining industry faces oil price volatility, the aggravation of crude oil in poor quality trend, oil quality specification improves, energy-saving and emission-reduction requirement becomes sternly, biofuel develops rapidly etc., minimizing Carbon emission, mitigation of climate change have become petroleum refining industry and to have transformed mode of economic growth, kept the only way of Sustainable development.In October, 2009, national publication controls the action target of greenhouse gas emission, namely arrives the year two thousand twenty nationwide units gross domestic product CO 2discharge declined 40% to 45% than 2005, and during clearly proposing " 12 ", per GDP Carbon emission reduces by 17%, and country is in the likely collection " carbon tax " in good time of " 12 " period simultaneously.Therefore effectively reduce carbon emission in refining of petroleum and chemical process to seem and be even more important, trap, seal up for safekeeping and manage CO 2the vital task in refinery's future will be become.Carbon emission in heavy oil upgrading process is the carbon emission of catalytic cracking burning, hydrogen production process and the energy consumption of technological process mainly.Catalytic cracking unit is the core production equipment of refinery, becomes CO because catalyzer burns 2one of main source of discharge.
US2011/0155642A1 discloses a kind of catalytic cracking process process reducing Carbon emission, adopt coke-burning riser series connection dense bed regenerating unit, pure oxygen and the regeneration techniques in coke-burning riser multiple spot delivery of supplemental oxygen, this technology Special attention will be given to adds a tank in regeneration and circuit to be generated respectively, wherein the tank employing nitrogen of regenerative circuit carries out degassed to regenerated catalyst, and the tank of circuit to be generated burns efficiency to improve the front temperature of reclaimable catalyst regeneration to improve by introducing reclaimable catalyst and regenerated catalyst mixing.But the introducing of regenerative circuit nitrogen finally inevitably makes nitrogen play a reversed role in flue gas by revivifier, obviously lose the advantage of pure oxygen regeneration, only burn efficiency and increase, but the recovery of carbonic acid gas adds difficulty.
US4542114 discloses a kind of integral process process reclaiming the flue gas compositions such as carbonic acid gas, can be implemented in burning process and go back hydrogen manufacturing and carbon dioxide product, eliminate sulphur, the aerial discharge of oxynitride completely, the pure oxygen mixed gas that it adopts carbonic acid gas to dilute carries out catalyzer and burns to produce rich carbonated flue gas simultaneously.But this technique not increasing interior heat collecting device for realizing in revivifier, emphasize the wherein preferred 30-24% of oxygen concentration 60-21% in mixed gas, thus part losing the advantage adopting purity oxygen regeneration, burns efficiency as increased substantially, reducing revivifier size etc.
US5565089 discloses a kind of catalytic cracking catalyst process of regenerating, first enter revivifier with air to carry out catalyzer and burn, then the carbonic acid gas in reclaiming flue gas, recycled carbon dioxide and be incorporated to oxygen-containing gas stream gradually until in revivifier temperature normal, finally only inject oxygen and carbonic acid gas carries out burning of catalyzer.This process of regenerating only pays close attention to the improvement of regenerative process inlet system aspect and the process of flue gas, does not consider the problem of regenerator configuration or the concrete aspect such as reclaiming process process and catalytic cracking catalyst circulation.
CN1600431A discloses a kind of incomplete regen-eration smoke combustion technology, adopt the way of supplementing air in the incomplete regen-eration stack gas between catalyst regenerator and flue gas turbine inlet, CO in incomplete regen-eration flue gas is burnt away, thus make flue-gas temperature be increased to 660-760 DEG C, flue gas turbine inlet temperature is finally made to reach 640-700 DEG C, improve cigarette machine organic efficiency, reduce plant energy consumption with recovered flue gas pressure energy to greatest extent.Adopt the present invention, the concentration according to unit scale and CO and/or entraining hydrocarbon supplements air capacity 20-300Nm3/min, effectively can improve flue-gas temperature 20-80 DEG C, improves cigarette engine efficiency.For single hop incomplete regen-eration, in flue, supplement air flue gas also can be made to carry hydro carbons Thorough combustion secretly, eliminate its impact on cigarette machine, but effectively can not reduce CO2 emissions.
Catalyzer coke burning regeneration method due to routine in fluidized-bed, passes into air or oxygen-containing gas regenerates, and air is primarily of O 2and N 2composition, containing a large amount of N in the regenerated flue gas therefore produced after catalyzer coke burning regeneration 2, CO 2with a small amount of O 2and CO.And the flue gas of this composition is due to CO 2concentration is low, therefore CO 2separating difficulty is large, cost is high, cannot be isolated collection, directly can only discharge, thus cause Greenhouse effect after entering energy-recuperation system.
In addition, from the development of regenerator, pursue the at utmost recovery realizing regenerated catalyst activity, to realize the maximum conversion ability of hydro carbons always.But the activity of catalyzer is the concept statement of a macroscopical transformation efficiency, does not embody the pursuit of object product selectivity.For example can realize regenerated catalyst activation recovering during regeneration the highest, but this regenerated catalyst may cause high coke and dry gas yied due to its high reactivity when participating in reaction, this does not wish to see.Therefore need a kind of homogeneity pursuing catalyst activity recovery during regeneration, realize one acid on regenerated catalyst in other words and be uniformly distributed, thus realize low coke and dry gas yied, high object product selectivity.Therefore, be necessary develop a kind of reduction Carbon emission and improve optionally catalyst regeneration process.
Summary of the invention
The object of the invention is to provide a kind of catalyst regeneration process reducing Carbon emission on the basis of existing technology.
The catalyst regeneration process of reduction Carbon emission provided by the invention adopts the regenerating unit pattern of burning tank, dilute phase pipe series connection dense bed, burning tank to be fast bed operation, and dense bed is bubbling bed operation, and the method comprises:
(1) the band Pd/carbon catalyst from catalytic cracking unit stripping stage first adopts pure oxygen gas to regenerate in burning tank, and coke combustion reactions occurs, and the ratio of burning in burning tank is 40-50%;
(2) from burning tank, catalyzer out and flue gas enter dense-phase bed through dilute phase pipe, pure oxygen gas is supplemented further bottom dense-phase bed, make that the catalyzer of incomplete regen-eration burns further in dense-phase bed, holomorphosis, the ratio of burning of dense-phase bed is 50-60%;
(3) dense-phase bed arranges heat collector and carries out heat-obtaining to catalyzer, is no more than 750 DEG C preferably more than 720 DEG C with the temperature controlling dense-phase bed;
(4) supplement or not replenishment cycles flue gas bottom burning tank, when replenishment cycles flue gas, keep being not less than 30% from the oxygen concentration revivifier cyclone separation system flue gas out and be preferably not less than 40%;
(5) flue gas enters smoke energy recovering system after cyclonic separator is separated, and enters carbon dioxide separating system subsequently, traps after separating carbon dioxide, recycles from the revivifier direct Returning reactor of regenerated catalyst out.
The operational condition of described burning tank is: temperature 550-720 DEG C, and catalyzer mean residence time is preferred 30.0-80.0 second 20.0-90.0 second, and the gas superficial linear velocity of burning tank is that 1.0-3.0m/s is preferably 1.2-2.0m/s.In burning tank, can interior heat collector be set, also can not arranges, depend on that whether the temperature of burning tank is more than 750 DEG C.
The operational condition of described dense-phase bed is: temperature 600 ~ 750 DEG C, and catalyzer mean residence time is 1.0-4.0 minute preferred 1.0-3.0 minute, and gas superficial linear velocity is that 0.4-0.8m/s is preferably 0.4-0.6m/s.Dense-phase bed arrange heat collector be interior heat collector or/and external warmer, heat collector is one or more.
Described catalyzer comprises zeolite, inorganic oxide and optional clay, and each component accounts for total catalyst weight respectively and is: the heavy % of the heavy %-70 of the heavy % of the heavy %-50 of zeolite 1, the heavy % of the heavy %-99 of inorganic oxide 5, clay 0.Its mesolite is active ingredient, be selected from mesopore zeolite and/or optional large pore zeolite, mesopore zeolite accounts for the heavy % of 10 heavy %-100 of zeolite gross weight, preferably the heavy % of 20 heavy %-80, large pore zeolite accounts for the heavy % of 0 heavy %-90 of zeolite gross weight, preferably the heavy % of 20 heavy %-80.Mesopore zeolite is selected from one or more mixtures in ZSM series zeolite and/or ZRP zeolite, also can carry out modification to transition metals such as the non-metallic elements such as above-mentioned mesopore zeolite phosphorus and/or iron, cobalt, nickel.One or more mixture in this group zeolite that large pore zeolite is selected from the super steady Y obtained by Rare Earth Y (REY), rare earth hydrogen Y (REHY), different methods, high silicon Y is formed.
Inorganic oxide, as support of the catalyst, is selected from silicon-dioxide and/or aluminium sesquioxide or both mixtures.
Clay, as caking agent, is selected from one or more in kaolin, polynite, diatomite, saponite, rectorite leng, sepiolite, hydrotalcite and wilkinite.
Compared with existing renovation process, major advantage of the present invention is following two aspects:
1, the method not only can make catalyzer holomorphosis, significantly can reduce carbon emission, even zero carbon emission simultaneously, reduces Greenhouse effect.
2, the method significantly can reduce device catalyst inventory especially revivifier reserve, greatly reduces the size of static equipment and dynamic equipment, reduces investment, reduces floor space.
3, because purity oxygen concentration in regeneration system rapidly is high, thus make to burn efficiency and increase substantially, the recovery time shortens, and reduces the fragmentation of catalyzer, wearing and tearing, improves the service efficiency of catalyzer.
4, the activity that the method can realize regenerated catalyst is uniformly distributed, thus coke and dry gas yied in the product of catalytic cracking are reduced.
Accompanying drawing explanation
Accompanying drawing is the catalyst regeneration process schematic flow sheet of reduction Carbon emission provided by the invention.
Embodiment
Further illustrate method provided by the present invention below in conjunction with accompanying drawing, but the present invention is not therefore subject to any restriction.
Accompanying drawing is the catalyst regeneration process schematic flow sheet of reduction Carbon emission provided by the invention.
In accompanying drawing, each numbering is described as follows:
1,10,11,12,13,18,20,21 all pipeline is represented; 2 is burning tank; 3 is dilute phase pipe; 4 is dense-phase bed; 5 is freeboard of fluidized bed; 6 is revivifier; 7 and 17 are cyclone separation system; 8 is smoke energy recovering system; 9 is carbon dioxide separating system; 14 is riser reactor; 15 is stripping stage; 16 is settling vessel; 19 is oil and gas separating system; 22 is external warmer.
As shown in drawings, reclaimable catalyst enters burning tank 2 through inclined tube 1 to be generated, pure oxygen gas enters burning tank 2 through pipeline 20, concurrent green coke charcoal combustion reactions, up is contacted with reclaimable catalyst, flue gas and incomplete regen-eration catalyzer enter the dense-phase bed 4 of revivifier 6 through dilute phase pipe 3, purity oxygen also enters the bottom of dense-phase bed 4 through pipeline 21, thus makes the catalyzer of incomplete regen-eration burn further, regenerate.For controlling the temperature of dense-phase bed, be provided with external warmer 22.The flue gas of dense-phase bed through revivifier freeboard of fluidized bed 5, cyclone separation system 7 leaves revivifier.Directly enter smoke energy recovering system 8 recovered energy from a revivifier flue gas part out, another part returns to the bottom of dense-phase bed 4 through pipeline 10 circulation, can realize the lifting of the carbon dioxide in flue gas concentration entering carbon dioxide separating system 9.Enter carbon dioxide separating system 9 from energy-recuperation system 8 flue gas out, realize the trapping of carbonic acid gas.Regenerated catalyst after regeneration enters bottom riser reactor 14 through regenerator sloped tube 11, pre-lift medium enters through pipeline 12 that to promote regenerated catalyst bottom riser reactor up, stock oil enters riser reactor through pipeline 13 and to contact with regenerated catalyst and to carry out catalytic cracking reaction, and reaction oil gas enters oil and gas separating system 19 through settling vessel 16, cyclone separation system 17 and gas pipeline 18 successively and obtains various product.Reclaimable catalyst enters inclined tube 1 to be generated and turns back to burning tank 2 and regenerate after stripping stage 15 stripping, thus realizes recycling.
The following examples will be further described the present invention, but not thereby limiting the invention.The stock oil used in embodiment and comparative example is vacuum residuum, and its character lists in table 1.Catalyzer is produced by catalyzer branch office of Sinopec Group Shandong catalyst plant, and goods number is MLC-500, and its character lists in table 2.
Embodiment
Embodiment is carried out on catalytic cracking demonstration unit, as shown in drawings.Demonstration unit does not have smoke energy recovering system and carbon dioxide separating system.The wherein internal diameter 20 centimetres of burning tank, the internal diameter of dense-phase bed is 50 centimetres.According to renovation process proposed by the invention, catalyzer is regenerated, pass into pure oxygen gas respectively at burning tank and dense-phase bed, return bottom dense-phase bed from revivifier cyclone separation system flue gas partial out simultaneously.The temperature of burning tank is 650 DEG C, and revivifier dense-phase bed temperature is 640 DEG C.Catalyzer is 60 seconds in the residence time of burning tank, is 2 minutes at the mean residence time of dense-phase bed.In burning tank, gas superficial linear velocity is 1.4m/s, and in dense-phase bed, gas superficial linear velocity is 0.6m/s.Catalyzer after regeneration enters reactor, contacts with the stock oil listed by table 1, carries out catalytic cracking reaction, and regeneration condition, reaction conditions, regenerated catalyst carbon content and flue gas composition all lists in table 3.
Comparative example
Comparative example is also carry out on the catalytic cracking demonstration unit of same structure, but burning tank is different with the internal diameter of dense bed, the internal diameter of burning tank 40 centimetres, and the internal diameter of dense-phase bed is 200 centimetres, and other scantlings of the structure is identical with embodiment.The renovation process pair reclaimable catalyst identical with embodiment routinely regenerates, and burning tank and dense-phase bed pass into air respectively, and the middle portion temperature of burning tank is 685 DEG C, and revivifier dense-phase bed temperature is 690 DEG C.Catalyzer is 3 minutes in the residence time of burning tank, is 8 minutes at the mean residence time of dense-phase bed.In burning tank, gas superficial linear velocity is 1.5m/s, and in dense-phase bed, gas superficial linear velocity is 0.5m/s.Catalyzer after regeneration enters reactor, contacts with the stock oil listed by table 1, carries out catalytic cracking reaction, and regeneration condition, reaction conditions, regenerated catalyst carbon content and flue gas composition all lists in table 3.
As can be seen from the Comparative result of operational condition and table 3, compared with comparative example, the present invention is in burning tank size and regeneration dense bed size significantly reduces, device general reserve significantly reduces, consume prerequisite that wind index obviously reduces under, adopt renovation process proposed by the invention, on regenerated catalyst, carbon content reduces more, in addition, CO and N is not contained in the flue gas that this catalyst regeneration process produces 2, gas concentration lwevel, up to 57%, is conducive to separation and the trapping of carbonic acid gas.
Table 1
Table 2
Table 3

Claims (9)

1. reduce a catalyst regeneration process for Carbon emission, it is characterized in that the method adopts the regenerating unit pattern of burning tank, dilute phase pipe series connection dense bed, burning tank is fast bed operation, and dense bed is bubbling bed operation, and the method comprises:
(1) the band Pd/carbon catalyst from catalytic cracking unit stripping stage first adopts pure oxygen gas to regenerate in burning tank, and coke combustion reactions occurs, and the ratio of burning in burning tank is 40-50%;
(2) from burning tank, catalyzer out and flue gas enter dense-phase bed through dilute phase pipe, pure oxygen gas is supplemented further bottom dense-phase bed, make that the catalyzer of incomplete regen-eration burns further in dense-phase bed, holomorphosis, the ratio of burning of dense-phase bed is 50-60%;
(3) dense-phase bed arranges heat collector and carries out heat-obtaining to catalyzer, is no more than 750 DEG C with the temperature controlling dense-phase bed;
(4) from replenishment cycles flue gas bottom burning tank, keep being not less than 30% from the oxygen concentration revivifier cyclone separation system flue gas out;
(5) flue gas enters smoke energy recovering system after cyclonic separator is separated, and enters carbon dioxide separating system subsequently, traps after separating carbon dioxide, recycles from the revivifier direct Returning reactor of regenerated catalyst out.
2., according to the method for claim 1, it is characterized in that the operational condition of described burning tank is: temperature 550-720 DEG C, catalyzer mean residence time is 20.0-90.0 second, and gas superficial linear velocity is 1.0-3.0m/s.
3., according to the method for claim 2, it is characterized in that the operational condition of described burning tank is: catalyzer mean residence time is 30.0-80.0 second, and gas superficial linear velocity is 1.2-2.0m/s.
4., according to the method for claim 1, it is characterized in that the operational condition of described dense-phase bed is: temperature 600 ~ 750 DEG C, catalyzer mean residence time is 1.0-4.0 minute, and gas superficial linear velocity is 0.4-0.8m/s.
5., according to the method for claim 4, it is characterized in that the operational condition of described dense-phase bed is: catalyzer mean residence time is 1.0-3.0 minute, and gas superficial linear velocity is 0.4-0.6m/s.
6. according to the method for claim 1, it is characterized in that step (3) described heat collector be interior heat collector or/and external warmer, heat collector is one or more.
7., according to the method for claim 1, it is characterized in that the temperature of step (3) control dense-phase bed is no more than 720 DEG C.
8., according to the method for claim 1, it is characterized in that the oxygen concentration in step (4) described flue gas is not less than 40%.
9. according to the method for claim 1, it is characterized in that described catalyzer comprises zeolite, inorganic oxide and optional clay, each component accounts for total catalyst weight respectively and is: the heavy % of the heavy %-70 of the heavy % of the heavy %-50 of zeolite 1, the heavy % of the heavy %-99 of inorganic oxide 5, clay 0.
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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3844973A (en) * 1972-05-30 1974-10-29 Universal Oil Prod Co Fluidized catalyst regeneration by oxidation in a dense phase bed and a dilute phase transport riser
CN101850274A (en) * 2009-03-31 2010-10-06 中国石油化工股份有限公司 Catalyst regeneration method for improving selectivity of catalyst
CN101850276A (en) * 2009-03-31 2010-10-06 中国石油化工股份有限公司 Catalyst regeneration method for improving selectivity of catalyst

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
BRPI0905257B1 (en) * 2009-12-28 2018-04-17 Petroleo Brasileiro S.A. - Petrobras FLOW CATALYTIC CRACKING PROCESS WITH REDUCED CARBON DIOXIDE EMISSION

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3844973A (en) * 1972-05-30 1974-10-29 Universal Oil Prod Co Fluidized catalyst regeneration by oxidation in a dense phase bed and a dilute phase transport riser
CN101850274A (en) * 2009-03-31 2010-10-06 中国石油化工股份有限公司 Catalyst regeneration method for improving selectivity of catalyst
CN101850276A (en) * 2009-03-31 2010-10-06 中国石油化工股份有限公司 Catalyst regeneration method for improving selectivity of catalyst

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