CN103725310B - A kind of catalyst regeneration process reducing Carbon emission - Google Patents
A kind of catalyst regeneration process reducing Carbon emission Download PDFInfo
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- CN103725310B CN103725310B CN201210387279.4A CN201210387279A CN103725310B CN 103725310 B CN103725310 B CN 103725310B CN 201210387279 A CN201210387279 A CN 201210387279A CN 103725310 B CN103725310 B CN 103725310B
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- 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
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- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Abstract
A kind of catalyst regeneration process reducing Carbon emission, band Pd/carbon catalyst first in the first revivifier after pure oxygen partial regeneration, enter in Second reactivator through U type transfer line and burn residual coke through pure oxygen, be divided into three parts from the first revivifier flue gas out, wherein first part's flue gas recirculation is supplemented to bottom Second reactivator; Semi regeneration catalyzer is delivered to Second reactivator from the first revivifier by second section; Part III enters smoke energy recovering system; Enter carbon dioxide separating system from Second reactivator flue gas out with after the flue gas of smoke energy recovering system the first revivifier out converges, trap after separating carbon dioxide, 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
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 20-300Nm
3/ 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 block form two device regenerating unit pattern, first revivifier, Second reactivator are arranged in juxtaposition, connected by U-shaped catalyst transport between first revivifier, Second reactivator, first revivifier is turbulent bed operation, Second reactivator 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 the first revivifier, and coke combustion reactions occurs, and the ratio of burning of the first revivifier is 55-65%;
(2) from the first revivifier bottom, semi regeneration catalyzer out enters Second reactivator through U-shaped catalyst transport, pure oxygen gas is supplemented further bottom Second reactivator, make that the catalyzer of incomplete regen-eration burns further in dense-phase bed, holomorphosis, the ratio of burning of Second reactivator is 35-45%;
(3) be divided into three parts from the first revivifier flue gas out, wherein first part's flue gas recirculation is supplemented to bottom Second reactivator; Semi regeneration catalyzer is delivered to Second reactivator from the first revivifier as delivery medium by second section; Part III enters smoke energy recovering system, and flue gas recirculation needs to keep the oxygen concentration in Second reactivator to be not less than 30% and is preferably not less than 40%;
(4) enter carbon dioxide separating system in the lump from Second reactivator flue gas out with after the flue gas of smoke energy recovering system the first revivifier out converges, trap after separating carbon dioxide;
(5) the direct Returning reactor of regenerated catalyst recycles.
The operational condition of described first revivifier is: temperature 550-700 DEG C, and catalyzer mean residence time is 1.0-4.0 minute preferred 1.0-3.0 minute, and the gas superficial linear velocity of the first revivifier is that 0.6-1.0m/s is preferably 0.7-0.9m/s.In first revivifier, 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 Second reactivator is: temperature 580-700 DEG C, and catalyzer mean residence time is 1.0-5.0 minute preferred 1.0-4.0 minute, and gas superficial linear velocity is that 0.4-0.8m/s is preferably 0.4-0.6m/s.Second reactivator arranges heat collector, is no more than 750 DEG C preferably more than 720 DEG C with the temperature controlling Second reactivator dense-phase bed.Second reactivator 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.
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:
1,3,4,7,8,9,10,11,12,17,18,23 all pipeline is represented; 2 is the first revivifier; 16 is Second reactivator; 6 is U-shaped catalyst transport; 13,14 and 22 cyclone separation system is; 15 is smoke energy recovering system; 26 is carbon dioxide separating system; 19 is riser reactor; 20 is stripping stage; 21 is settling vessel; 24 is oil and gas separating system; 25 is external warmer.
As shown in drawings, reclaimable catalyst enters the first revivifier 2 through inclined tube 1 to be generated, and pure oxygen gas also enters the first revivifier 2 through pipeline 3, contacts the combustion reactions of concurrent green coke charcoal with reclaimable catalyst.Incomplete regen-eration catalyzer is from the bottom of the first revivifier 2 through U-shaped catalyst transport 6, be promoted to Second reactivator 16 by through pipeline 12 from the circulating flue gas of the first revivifier.The flue gas of the first revivifier through cyclone separation system 13, pipeline 7 out after, smoke energy recovering system 15 recovered energy is entered at least partially through pipeline 9, another part is divided into two-way, one tunnel goes pipeline 12 as lifting medium, another road enters through pipeline 4 that Second reactivator 16 is auxiliary to be burnt, and can realize the lifting of the carbon dioxide in flue gas concentration entering carbon dioxide separating system 26 simultaneously.Pure oxygen gas also enters bottom Second reactivator 16 through pipeline 8 and burns further.Second reactivator arranges external warmer 25 to control Second reactivator temperature.The flue gas of Second reactivator 16 leaves Second reactivator through cyclone separation system 14 and enters carbon dioxide separating system 26 through pipeline 10 with after smoke energy recovering system 15 the first revivifier flue gas out out converges, and realizes the separation and collection of carbonic acid gas.Enter bottom riser reactor 19 from Second reactivator 16 regenerated catalyst out through regenerator sloped tube 11, pre-lift medium enters through pipeline 17 that to promote regenerated catalyst bottom riser reactor up, stock oil enters riser reactor through pipeline 18 and to contact with regenerated catalyst and to carry out catalytic cracking reaction, and reaction oil gas enters oil and gas separating system 24 through settling vessel 21, cyclone separation system 22 and gas pipeline 23 successively and obtains various product.Reclaimable catalyst enters inclined tube 1 to be generated and turns back to the first revivifier 2 and regenerate after stripping stage 20 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 50 centimetres of the first revivifier dense-phase bed, the internal diameter of Second reactivator dense-phase bed is 40 centimetres.According to renovation process proposed by the invention, catalyzer is regenerated, pure oxygen gas is passed into respectively at the first revivifier and Second reactivator dense-phase bed, simultaneously return bottom Second reactivator dense-phase bed from the first revivifier cyclone separation system flue gas part out, another part as lifting medium transport incomplete regen-eration catalyzer to Second reactivator, last part and go out demonstration unit after Second reactivator flue gas out converges.The bed temperature of the first revivifier is 660 DEG C, and Second reactivator dense-phase bed temperature is 670 DEG C.Catalyzer is 2 minutes in the residence time of the first revivifier dense-phase bed, is 3 minutes at the mean residence time of Second reactivator dense-phase bed.The gas superficial linear velocity of the first revivifier is 0.82m/s, and Second reactivator gas superficial linear velocity is 0.54m/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.In table 3 flue gas consist of the first revivifier and Second reactivator flue gas converge after composition.
Comparative example
Comparative example is also carry out on the catalytic cracking demonstration unit of same structure, but the first revivifier is different with embodiment with the internal diameter of Second reactivator dense-phase bed, the internal diameter of the first revivifier dense-phase bed 200 centimetres, the internal diameter of Second reactivator dense-phase bed is 160 centimetres, and other scantlings of the structure is identical with embodiment.The renovation process pair reclaimable catalyst identical with embodiment routinely regenerates, and the first revivifier and Second reactivator dense-phase bed pass into air respectively, and the bed temperature of the first revivifier is 670 DEG C, and Second reactivator dense-phase bed temperature is 710 DEG C.Catalyzer is 9 minutes in the residence time of the first revivifier dense-phase bed, is 12 minutes at the mean residence time of Second reactivator dense-phase bed.The gas superficial linear velocity of the first revivifier is 0.8m/s, and Second reactivator 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.In table 3 flue gas consist of the first revivifier and Second reactivator flue gas converge after composition.
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 56.2%, is conducive to separation and the trapping of carbonic acid gas.
Table 1
Table 2
Table 3
Claims (10)
1. one kind is reduced the catalyst regeneration process of Carbon emission, it is characterized in that the method adopts block form two device regenerating unit pattern, first revivifier, Second reactivator are arranged in juxtaposition, connected by U-shaped catalyst transport between first revivifier, Second reactivator, first revivifier is turbulent bed operation, Second reactivator 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 the first revivifier, and coke combustion reactions occurs, and the ratio of burning of the first revivifier is 55-65%;
(2) from the first revivifier bottom, semi regeneration catalyzer out enters Second reactivator through U-shaped catalyst transport, pure oxygen gas is supplemented further bottom Second reactivator, make that the catalyzer of incomplete regen-eration burns further in dense-phase bed, holomorphosis, the ratio of burning of Second reactivator is 35-45%, Second reactivator arranges heat collector, is no more than 750 DEG C with the temperature controlling Second reactivator dense-phase bed;
(3) be divided into three parts from the first revivifier flue gas out, wherein first part's flue gas recirculation is supplemented to bottom Second reactivator; Semi regeneration catalyzer is delivered to Second reactivator from the first revivifier as delivery medium by second section; Part III enters smoke energy recovering system, and flue gas recirculation needs to keep the oxygen concentration in Second reactivator to be not less than 30%;
(4) enter carbon dioxide separating system in the lump from Second reactivator flue gas out with after the flue gas of smoke energy recovering system the first revivifier out converges, trap after separating carbon dioxide;
(5) the direct Returning reactor of regenerated catalyst recycles.
2., according to the method for claim 1, it is characterized in that the operational condition of described first revivifier is: temperature 550-700 DEG C, catalyzer mean residence time is 1.0-4.0 minute, and gas superficial linear velocity is 0.6-1.0m/s.
3., according to the method for claim 2, it is characterized in that the operational condition of described first revivifier is: catalyzer mean residence time is 1.0-3.0 minute, and gas superficial linear velocity is 0.7-0.9m/s.
4., according to the method for claim 1, it is characterized in that the operational condition of described Second reactivator is: temperature 580-700 DEG C, catalyzer mean residence time is 1.0-5.0 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 Second reactivator is: catalyzer mean residence time is 1.0-4.0 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 described heat collector be interior heat collector or/and external warmer, heat collector is one or more.
7., according to the method for claim 6, it is characterized in that the temperature controlling Second reactivator 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 (3) 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.
10., according to the method for claim 1, it is characterized in that step (3) flue gas recirculation needs to keep the oxygen concentration in Second reactivator to be not less than 40%.
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Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4332674A (en) * | 1980-07-15 | 1982-06-01 | Dean Robert R | Method and apparatus for cracking residual oils |
| 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 |
| 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 |
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| BRPI0905257B1 (en) * | 2009-12-28 | 2018-04-17 | Petroleo Brasileiro S.A. - Petrobras | FLOW CATALYTIC CRACKING PROCESS WITH REDUCED CARBON DIOXIDE EMISSION |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4332674A (en) * | 1980-07-15 | 1982-06-01 | Dean Robert R | Method and apparatus for cracking residual oils |
| 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 |
| 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 |
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