CN102397783B - Complete combustion heating and heat exchanging method used in flue gas adsorbent regeneration process - Google Patents
Complete combustion heating and heat exchanging method used in flue gas adsorbent regeneration process Download PDFInfo
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Abstract
The invention discloses a complete combustion heating and heat exchanging method used in a flue gas adsorbent regeneration process. The method comprises the following steps of: introducing an absorbent to be regenerated which adsorbs sulfide and/or nitride into an adsorbent regenerator; and combusting reducing gas and stoichiometric oxygen-containing material flow in a combustor for generating heat, making mixed gas and another portion of reducing gas enter the adsorbent regenerator together, directly heating the adsorbent to be regenerated and desorbing and regenerating at the high temperature, cooling all or a part of the desorbed and regenerated adsorbent, and returning to a flue gas adsorber for using, wherein the adsorbent is a catalytic cracking catalyst or a solid chemical agent compatible with a catalytic cracking device. In the method provided by the invention, heat generated by partial combustion of regenerated gas is directly used and is taken as the heat source for regenerating the adsorbent to be regenerated, so that the utilization rate of fuel heat is increased, and the operation flexibility of the catalytic cracking device is not influenced simultaneously.
Description
Technical field
The invention relates to a kind of catalyst cracking method of hydrocarbon ils, more particularly, is absorption and the regeneration method about regeneration flue gas desulfurization denitrification adsorbent in a kind of catalytic cracking unit.
Background technology
Catalytic cracking catalyst circulates between reactor and regenerator, usually when leaving reactor, contains approximately 3～10wt% of coke on catalyst, and the coke that must deposit with airborne oxygen burning-off in regenerator is to recover catalytic activity.The coke that deposits on catalyst is mainly reaction condensate, and main component is carbon and hydrogen, when cracked stock sulfur-bearing and nitrogen, also contains sulphur and nitrogen in coke.Catalyst warp and the oxygen of carbon deposit carry out regenerative response, generate CO
2, CO and H
2O also contains SOx (SO in regenerated flue gas
2, SO
3) and NOx (NO, NO
2).Regenerative response is exothermic reaction, and fuel factor is quite large, and the heat that provides this device thermal balance required is provided.
To processing the pollution problem of industrial smoke sulphur oxide and nitrogen oxide, the people such as Asit K.Das disclose a kind of method that removes simultaneously sulfur and nitrogen oxides, SO
2-NO
xAdsorption process, namely the SNAP method is (referring to " Simultaneous Adsorption of SO
2-NOx from Flue Gases in a Riser Configuration ", the people such as Asit K.Das, AIChE Journal, Vol.47, No.12, December 2001, P2831-2844).The method makes flue gas and the Na/ γ-Al that contains sulfur and nitrogen oxides
2O
3The adsorbent contact, this adsorbent can adsorb sulfur and nitrogen oxides, thereby reaches the purpose of purifying smoke.Described contact can be carried out in gas suspension absorber (GSA), and the temperature of contact is that 100～150 ℃, time of contact are 5 seconds.After contact was completed, absorption had the absorbent particles of sulfur and nitrogen oxides to collect with filter bag.Na/ γ-Al after the SNAP method is used
2O
3Adsorbent can be regenerated.Na/ γ-Al
2O
3The regenerative process of adsorbent is divided two stages: the adsorbent after (1) will use in the fluidized bed type regenerator is heated to 500 ℃, discharges NO
xPass into subsequently natural gas with NO
xBe reduced to N
2And O
2Discharging; (2) will remove NO in (1)
xAdsorbent again through natural gas and steam treatment with SO
xBe converted into H
2S reclaims.
CN101209391A discloses a kind of method and cracking method for hydrocarbon oil that removes sulfureous in flue gas oxide and/or nitrogen oxide, adopt catalytic cracking catalyst as the adsorbent that removes catalytic cracking catalyst regenerated flue gas sulphur oxide and nitrogen oxide in the method, its adsorption effect is suitable with existing Special adsorbent, and be not easy saturated, the condition of adsorbent reactivation is (such as being heated to 500 ℃, release NOx) condition that is compared to catalytic cracking catalyst regeneration relaxes, therefore as the structure not impact of adsorbent reactivation on catalytic cracking catalyst, in addition, process the used catalyst of adsorbent as regeneration fume from catalytic cracking, still can use in catalytic cracking process, its activity as catalytic cracking catalyst is not only unaffected, and slightly be improved.
Utilize adsorbent sulfur and nitrogen oxides in the adsorbing and removing regenerated flue gas before flue gas emptying, adsorption temp (being flue-gas temperature) is generally 200 ℃ of left and right.The processing of can regenerating of adsorbent to be generated after absorption, during regeneration, temperature is 500～600 ℃; Adsorbent after regeneration can turn back in the flue gas adsorptive reactor and reuse.When implementing adsorption operations, adsorption temp is flue-gas temperature, depends on the efficient of upstream smoke energy recovering system, and energy reclaims more thoroughly, and flue-gas temperature is lower, and adsorption efficiency is higher.When implementing the adsorbent reactivation operation, relatively harsh to the requirement of temperature, do not reach sufficiently high temperature, regeneration effect is difficult to guarantee.
The external warmer that CN101592449A discloses adsorbent reactivation device and catalytic cracking catalyst regenerator unites two into one, the method for adsorbent to be generated and catalytic cracking catalyst indirect heat exchange to be generated.
Normally, can adopt Electric heating (as electrically heated rod or electric furnace) to come heat reduction gas and spent agent; Also can adopt fuel heating furnace to come heat reduction gas and spent agent to improve the adsorbent reactivation temperature.The former directly consumes electric energy, and heating load is limited in a way; The latter need to make fuel combustion in heating furnace, then with the heated medium indirect heat exchange, the thermal efficiency is limited, thereby increases device and operating cost.
Summary of the invention
The technical problem to be solved in the present invention is to provide a kind of method of utilizing the burning reducing gas to obtain the direct heating of heat and regeneration flue gas desulfurization denitrification adsorbent.
Complete combustion heating and heat-exchange method in flue gas adsorbent regenerative process provided by the invention, comprise adsorbent is introduced in the flue gas absorber, contact with the regenerated flue gas of sulfur-bearing, nitride, sulphur in the adsorbing and removing flue gas, nitride are introduced the adsorbent to be generated that has adsorbed sulfide and/or nitride in the adsorbent reactivation device; Heat is given birth in reducing gas and the burning in burner of stoichiometric oxygenate stream, mist and another strand reducing gas together enter in the adsorbent reactivation device afterwards, directly heat adsorbent to be generated and carry out desorption and regeneration at high temperature, all or part of the returning after cooling in the flue gas absorber of the adsorbent after desorption and regeneration used.
The beneficial effect of method provided by the invention is:
The heat that utilizes reducing gas completing combustion to produce, direct another strand of Hybrid Heating regeneration gas and adsorbent to be generated, and regenerate simultaneously, improved the utilization rate of fuel thermal energy, do not affect the operating flexibility of catalytic cracking unit simultaneously.
Description of drawings
Accompanying drawing is complete combustion heating and the heat-exchange method schematic flow sheet in flue gas adsorbent regenerative process provided by the invention.
Description of reference numerals:
A-flue gas absorber; B-adsorbent reactivation device; C-regenerative agent heat exchanger; The D-burner; E-regeneration gas heat exchanger; The 1-smoke inlet; The outlet of 2-desulfurization removing nitric purifying smoke; 3-sorbent circulation pipe; 4,16-inclined tube; 5,15-unloads the agent pipeline; 6-reducing gas entrance; 7-promotes the gas entrance; 9,11,13-pipeline; 10-oxygen-containing gas entrance; The outlet of 12-regeneration tail gas; The 14-spent agent promotes standpipe; The 17-adsorbent adds the agent mouth.
The specific embodiment
Complete combustion heating in flue gas adsorbent regenerative process provided by the invention and heat-exchange method are so concrete enforcement:
Flue gas desulfuration and denitrification adsorbent (hereafter adsorbent) being introduced in the flue gas absorber, contacted with regenerated flue gas from the catalytic cracking catalyst regenerator, is 50 ℃～400 ℃, preferred 100～300 ℃ in temperature; Pressure is sulphur, the nitride in the adsorbing and removing regenerated flue gas under the condition of 0.001～0.20MPa, preferred 0.005～0.15MPa, the adsorbent to be generated that has adsorbed sulfide and/or nitride is introduced in the adsorbent reactivation device after heat exchange heats up, and carries out desorption and regeneration under the higher temperature of 450～650 ℃.
In method provided by the invention, described flue gas absorber is fluidized-bed reactor, and wherein, the filling density of adsorbent is 0.01～200kg/m
3, preferred 0.5～120kg/m
3
In method provided by the invention, the thermal source of described adsorbent reactivation device comes the heat that in comfortable burner, reducing gas completing combustion produces.After oxygen-containing gas and stoichiometric reducing gas heat up through the hot logistics heat exchange with the outlet of adsorbent reactivation device, enter the heat release of burning in burner, when oxygen-containing gas be air, when reducing gas is lighter hydrocarbons, by looking for stoichiometry to calculate the volume ratio of reducing gas and air, be about (1.5～1.1): 1.Another strand of high-temperature gas mixture body reducing gas after burning enters in the adsorbent reactivation device and contacts with adsorbent to be generated, in the time of heating adsorbent to be generated, with the oxysulfide that adsorbs on adsorbent to be generated, nitrogen oxide generation reduction reaction, generates H
2S, N
2, CO, CO
2And H
2O realizes the regeneration of adsorbent.
In the time of the heating spent agent, reduction reaction occuring, realizes the regeneration of adsorbent.Regeneration tail gas goes out device after routine is taken off dirt processing, heat exchange cooling, all or part of the returning after cooling in the flue gas absorber of the adsorbent after desorption and regeneration used, and also can turn back in the catalytic cracking catalyst regenerator or in catalyst cracker by promoting gas.
In method provided by the invention, temperature after described reducing gas and oxygen-containing gas and adsorbent reactivation device outlet logistics heat exchange is 150～250 ℃, the place mixes and lights at burner inlet, reducing gas completing combustion wherein, temperature reaches 700～800 ℃, and the cold reducing gas of burning afterproduct and another strand mixes, and temperature is 600～750 ℃, mist together enters the adsorbent reactivation device afterwards, directly heats and the adsorbent to be generated of regenerating; Mist after burning is not only as the thermal source carrier but also serve as the lift gas of adsorbent logistics to be generated, together enter the adsorbent reactivation device, as regeneration gas, and the oxysulfide that adsorbs on adsorbent to be generated, reaction of nitrogen oxides, make adsorbent recover adsorption activity.
Heated adsorbent to be generated is 300～400 ℃ through the inlet temperature that enters the adsorbent reactivation device after the preheating in early stage, and the temperature of adsorbent to be generated in regenerator of high-temperature gas mixture body and preheating is 500～650 ℃.
In method provided by the invention, preferred scheme is that the adsorbent to be generated of 50～400 ℃ is by after drawing in the flue gas absorber with having adsorbed oxysulfide and/or nitrogen oxide, temperature, before entering the adsorbent reactivation device, introduce in the regeneration gas heat exchanger as cooling medium and carry out preheating; Cooling medium rises through heat exchanger by promoting air lift, reaches 300～400 ℃ after heat exchange.The heat carrier of described heat exchanger is the regeneration tail gas of drawing in the adsorbent reactivation device, and its temperature is 450～600 ℃.
In method provided by the invention, preferred scheme is that reduction air-flow and air enter preheating in the reproducing adsorbent heat exchanger, and cold logistics is reduction air-flow and air, and hot logistics is that the temperature of drawing in the adsorbent reactivation device is the reproducing adsorbent of 500～650 ℃.After heat exchange, reduction air-flow and air themperature can reach 150～250 ℃, and hot logistics is cooled to 200～300 ℃.
Described regeneration gas heat exchanger can be contained all or part of pipeline of carrying spent agent.Described spent agent preheater can be the heating bath form, becomes the extension of adsorbent reactivation device heating bath.
Described regeneration gas heat exchanger is the heat-exchanger rig that contains tube side and shell side, and tube side can be single tube, also can be shell and tube.Cooling medium can select heat carrier to walk tube side with the operation of fluidisation attitude, and cooling medium is walked shell side, also can select heat carrier to walk shell side, and cooling medium is walked tube side.Preferred heat carrier is walked shell side, and cooling medium is walked tube side.
Described regenerative agent heat exchanger is the heat-exchanger rig that contains tube side and shell side, and tube side can be single tube, also can be shell and tube.Heat carrier can select heat carrier to walk tube side with the operation of fluidisation attitude, and cooling medium is walked shell side, also can select heat carrier to walk shell side, and cooling medium is walked tube side.Preferred heat carrier is walked tube side, and cooling medium is walked shell side.
Preferred embodiments of the present invention arrange heat exchanger, have further optimized the heat exchange process of flue gas desulfuration and denitrification processing section, have improved heat exchange efficiency.
Described cooling medium lift gas is reducing gas and/or inert gas.Described reducing gas is selected from hydrogen, carbon monoxide and contains one or more mixture in the hydro carbons of 1-5 carbon atom.One or more in preferred hydrogen, carbon monoxide, methane, ethane, propane, butane and pentane and various isomers thereof.Described inert gas is selected from one or more in zero group gas, nitrogen, carbon dioxide and water vapour in the periodic table of elements.
Described regeneration gas heat exchanger also can be for containing the heat-exchanger rig of tube side and shell side, and tube side can be single tube, also can be shell and tube.Cooling medium can select heat carrier to walk tube side with the operation of fluidisation attitude, and cooling medium is walked shell side, also can select heat carrier to walk shell side, and cooling medium is walked tube side.Preferred heat carrier is walked shell side, and cooling medium is walked tube side.
In method provided by the invention, reducing gas and oxygen-containing gas in entering the reproducing adsorbent heat exchanger before preferred preheating scheme be, cold logistics is reducing gas and oxygen-containing gas, and hot logistics is that the temperature of drawing in the adsorbent reactivation device is the reproducing adsorbent of 500～650 ℃.After heat exchange, reducing gas and oxygen-containing gas temperature can reach 150～250 ℃, and hot logistics is cooled to 200～300 ℃.
In method provided by the invention, the regeneration gas of introducing in the adsorbent reactivation device is the mixture of reducing gas and combustion product, contains unreacted reducing gas, carbon dioxide and water vapour in the mist after described burning, can also contain inert gas.
Described reducing gas is flammable reducing gas, contains or do not contain inert gas.Flammable reducing gas is selected from hydrogen, carbon monoxide and contains one or more mixture in the hydro carbons of 1-5 carbon atom, preferably the mixture of one or more in hydrogen, carbon monoxide, methane, ethane, propane, butane and pentane.Described inert gas preferred nitrogen.Wherein the adding proportion of inert gas is this area ratio commonly used, as long as enough gas flows are provided as the lifting medium time.Described reducing gas more preferably uses the dry gas in oil plant, is selected from one or more the mixture in catalytic cracking tail gas, catalytic reforming tail gas, hydrocracking tail gas and delayed coking tail gas.
In method provided by the invention, described flue gas adsorbent is the inorganic oxide with absorption oxysulfide, nitrogen oxide ability, can use disclosed any adsorbent in prior art, and the present invention is not limited in this respect, such as aluminium oxide etc.Preferred catalytic Cracking catalyst wherein.
In method provided by the invention, the saturated adsorbent of at least part of absorption is introduced to return in the flue gas absorber after the adsorbent reactivation device is regenerated and is used.When adsorbent is catalytic cracking catalyst, all or part of heat exchange of adsorbent can be returned after cooling in the flue gas absorber and used after regeneration, also can turn back in the catalytic cracking catalyst regenerator or in catalyst cracker by promoting gas.
In method provided by the invention, described catalytic cracking catalyst can be one or more in the constituent of fresh catalytic cracking catalyst, catalytic cracking catalyst to be generated, regeneration catalyzing Cracking catalyst and above-mentioned catalyst.
Described fresh catalyst refers to newly to prepare does not pass through any processing, not yet used catalytic cracking catalyst, or through the aging catalyst of steam, described fresh catalyst does not contain carbon deposit.
Described reclaimable catalyst refers in catalyst cracker, with inactivation or part inactivation after the hydrocarbon ils reaction, needs the catalyst of regeneration, and the carbon deposit content of reclaimable catalyst is generally 0.8～1.2wt%.
Described regenerated catalyst refers to regenerate by catalyst regeneration process and recovers the catalyst of catalytic activity, and the carbon deposit content of regenerated catalyst is generally below 0.8wt%, is preferably 0.01～0.2wt%.Described catalyst regeneration process is in regenerator, the carbon deposit that deposits in course of reaction on catalyst to be burnt, and makes reclaimable catalyst recover catalytic activity, and the heat that produces is supplied with catalyst cracker.
The constituent of described catalytic cracking catalyst refers to fresh or through one-component or several component in finished catalyst, they belong to the compatible chemical agent of catalytic cracking unit.
The preferred fresh catalyst that uses uses as adsorbent, because the fresh catalyst after using as adsorbent can directly join in conventional petroleum catalytic cracking industrial production flow process.
Described catalytic cracking catalyst as adsorbent can and/or contain the catalytic cracking catalyst of molecular sieve for silica-alumina catalyst, and these catalytic cracking catalysts are conventionally known to one of skill in the art.
In preferred situation, described adsorbent is the catalytic cracking catalyst that contains molecular sieve.
In general, the catalytic cracking catalyst that contains molecular sieve contains molecular sieve, heat-resistant inorganic oxide matrix, contains or argillaceous not; Take the adsorbent total amount as benchmark, the content of described molecular sieve is 1-90wt%, and the content of heat-resistant inorganic oxide matrix is 10-99wt%, and the content of clay is 0-80wt%.Described adsorbent is preferably take the adsorbent total amount as benchmark, and the content of described molecular sieve is 10-60wt%, and the content of heat-resistant inorganic oxide matrix is 40-90wt%, and the content of clay is 20-70wt%.
Molecular sieve as active component of cracking catalyst is conventionally known to one of skill in the art, and for example, described molecular sieve can be selected from faujasite, has the zeolite of MFI structure, one or more in Beta zeolite, modenite and phosphate aluminium molecular sieve; Preferred one or more in y-type zeolite, overstable gamma zeolite, ZSM-5 zeolite, ZRP zeolite and Beta zeolite of molecular screening.
Heat-resistant inorganic oxide matrix as the Cracking catalyst component is conventionally known to one of skill in the art, for example, described heat-resistant inorganic oxide matrix can be selected from one or more in aluminium oxide, silica, amorphous silicon aluminium, zirconia, titanium oxide, boron oxide, alkaline earth oxide; Be preferably described heat-resistant inorganic oxide matrix and be selected from one or more in aluminium oxide, silica, amorphous silicon aluminium.
Clay as the Cracking catalyst component is conventionally known to one of skill in the art, for example, described clay can be selected from one or more in kaolin, halloysite, imvite, diatomite, galapectite, saponite, rectorite, sepiolite, attapulgite, hydrotalcite, bentonite.
Preferred embodiments of the present invention arrange heat exchanger, comprise that high temperature regeneration tail gas is the facilities such as the spent agent preheater of thermal source, reducing gases that the high temperature regeneration agent is thermal source, air preheater, regenerator heating bath formula muff, further optimize the heat exchange process of flue gas desulfuration and denitrification processing section, improved heat exchange efficiency.
Illustrate with reference to the accompanying drawings the specific embodiment of method provided by the invention, but therefore the present invention is not restricted:
As shown in drawings, adsorbent is packed in flue gas absorber A by adding agent mouth 17, pending flue gas is passed in flue gas absorber A by entrance 1, adsorbent contacts with regenerated flue gas, oxysulfide in the adsorbing and removing flue gas and/or nitrogen oxide, the tail gas after purification take off dirt from purifying smoke outlet 2 through routine and discharge the flue gas absorber.Adsorbent to be generated after use is by inclined tube 4 output flue gas absorbers, and the adsorbent after a part is used still has certain adsorption capacity, can return in flue gas absorber A by sorbent circulation pipe 3 to reuse.
Be input to adsorbent to be generated in regenerated flue gas heat exchanger E through inclined tube 4, nationality promotes standpipe 14 by the castering action that promotes gas entrance 7 and introduce gases through spent agent and enters heat exchanger E, enters adsorbent reactivation device B after promoting temperature with the regeneration tail gas heat exchange.
Adsorbent can be drawn adsorption system through unloading agent mouth 5.
Reducing gases enters regenerative agent heat exchanger C and regenerative agent logistics heat exchange from adsorbent reactivation device B through reducing gases entrance 6, air through oxygen-containing gas entrance 10, and the part of reducing gas is mixed into through entrance 9 and hot-air the heat release of burning in burner D afterwards; Combustion product in burner the porch of burner afterbody or adsorbent reactivation device B with together enter regenerator B after the reducing gas of another burst preheating mixes, complete regenerative response when further heating spent agent.High temperature regeneration tail gas goes out device through heat exchanger E by regeneration tail gas outlet 12 after routine is taken off dirt; One of flow direction of high temperature regeneration adsorbent is all or part of reactor of introducing catalytic cracking regenerator or catalytic cracking unit through unloading agent mouth 15; Two of the flow direction of reproducing adsorbent mixture, be through inclined tube 16 through regenerative agent heat exchanger C and cold reducing gases logistics and cold air logistics heat exchange, return afterwards in absorber A.The adsorbent that replenishes adds entrance 17 through adsorbent and joins in absorber A.
Claims (6)
1. complete combustion heating and the heat-exchange method in a flue gas adsorbent regenerative process, it is characterized in that adsorbent is introduced in the flue gas absorber, contact with the catalytic cracking catalyst regenerated flue gas, sulphur in the adsorbing and removing flue gas, nitride are introduced the adsorbent to be generated that has adsorbed sulfide and/or nitride in the adsorbent reactivation device; Reducing gas and the completing combustion in burner of stoichiometric oxygenate stream, mist and another strand reducing gas together enter in the adsorbent reactivation device afterwards, directly heating adsorbent to be generated also at high temperature carries out desorption and regeneration, and all or part of the returning after cooling in the flue gas absorber of the adsorbent after desorption and regeneration used.
2. according to the method for claim 1, it is characterized in that described reducing gas and air mix and light, burn in burner, temperature reaches 700～900 ℃.
3. according to the method for claim 1, the inlet temperature that it is characterized in that the regeneration air stream of described adsorbent reactivation device heat is 600～800 ℃, and the inlet temperature of adsorbent to be generated is 300～400 ℃, and after two bursts of logistics mix, outlet temperature is 450～650 ℃.
4. according to the method for claim 1, it is characterized in that described reducing gas is selected from hydrogen, carbon monoxide and contains one or more in the hydro carbons of 1-5 carbon atom, contains or do not contain inert gas.
5. according to the method for claim 1, it is characterized in that described adsorbent to be generated is by after drawing in the flue gas absorber, before introducing adsorbent reactivation device, introduce in the regeneration tail gas heat exchanger as cooling medium, carry out heat exchange with the regeneration tail gas of being drawn by the adsorbent reactivation device.
6. according to the method for claim 1, after it is characterized in that described reproducing adsorbent is drawn by the adsorbent reactivation device, before returning to the flue gas absorber, also introduce the regenerative agent heat exchanger, enter air and the Restore All gas of burner in this preheating.
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101209391A (en) * | 2006-12-30 | 2008-07-02 | 中国石油化工股份有限公司 | Method for removing oxysulfide and/or nitrogen oxide from flue gas and hydrocarbon oil cracking method |
| CN101592449A (en) * | 2008-05-29 | 2009-12-02 | 中国石油化工股份有限公司 | Heat-exchange method in a kind of reactivation process of flue gas desulfuration and denitrification adsorbent |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101209391A (en) * | 2006-12-30 | 2008-07-02 | 中国石油化工股份有限公司 | Method for removing oxysulfide and/or nitrogen oxide from flue gas and hydrocarbon oil cracking method |
| CN101592449A (en) * | 2008-05-29 | 2009-12-02 | 中国石油化工股份有限公司 | Heat-exchange method in a kind of reactivation process of flue gas desulfuration and denitrification adsorbent |
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