CN102389753B - Double-fluidized-bed reactor for endothermic reactions and method for supplying heat for endothermic reactions - Google Patents
Double-fluidized-bed reactor for endothermic reactions and method for supplying heat for endothermic reactions Download PDFInfo
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Abstract
The invention discloses a double-fluidized-bed reactor for endothermic reactions and a method for supplying heat for endothermic reactions. The double-fluidized-bed reactor comprises: a bed body of a fluidized bed for endothermic reactions, which is closed and in which a first fluidized bed layer consisting of particles of catalyst for endothermic reactions or reactant particles, is arranged, wherein the bottom of the bed body is provided with a first gas distributor which is connected with a gas source of the first gas to supply the first gas to the first fluidized bed layer; and a bed body of a fluidized bed for supplying heat, which is closed and in which a second fluidized bed layer consisting of hot carrier particles is arranged, wherein the bottom of the bed body a second gas distributor which is connected with a gas source of a second gas for supplying the second gas to the second fluidized bed layer. The bed body of the fluidized bed for endothermic reactions and the bed body of the fluidized bed for supplying heat are embedded together. The double-fluidized-bed reactor for endothermic reactions, which is disclosed by the embodiment of the invention has the advantages of safety, stability, high heat conductivity and the like and is particularly suitable for supplying heat to medium/high temperature endothermic reactions at a temperature of above 400 DEG C.
Description
Technical field
The present invention relates to the chemical reaction equipment technical field, especially relate to the heat supply method of a kind of endothermic reaction with double-fluidized-bed reactor and the endothermic reaction.
Background technology
Chemical reaction process is followed certain fuel factor usually, known according to the chemical potential variation of material before and after reaction, some reactive absorption heat, and heat is emitted in some reaction.Correspondingly, the chemical reactor design need to arrange heat supply or move hot means according to reaction heat.Wherein, the stable and uniform of middle high temperature (referring to more than the 400 ℃) endothermic reaction is a difficult point in chemical industry for heat problem.
In industry, usually adopt the tube furnace reactor to implement the strong endothermic reaction under hot conditions.Particularly, in the endothermic reaction pipe thinner at diameter, carry out, pipe is outer rely on fuel (fuel oil or combustion gas) burning by temperature increase to thousands of degrees centigrade, by radiation, be the reaction tube heat supply.The tube furnace reactor belongs to external-burning for thermal reactor, can meet the heat request that supplies of the high temperature gas phase endothermic reaction.
And, for the hydrocarbon vapor reforming reaction that has solid-phase catalyst to participate in, a kind of compact endothermic reaction apparatus that uses dense arrangement metal reaction pipe is proposed in ZL94192942.6.This device, by special nozzle arrangements design, imports the long and thin flame of generation in combustion chamber by fuel and air, avoids the reaction tube hot-spot; And, by particular design, prevent reaction tube caused bending when bearing higher than the average tube temperature.This endothermic reaction apparatus is not only applicable to the endothermic reaction of High Temperature Gas phase, is applicable to the hydrocarbon vapor reforming reaction that solid-phase catalyst participates in yet.Although this external-burning design can meet the high-temperature heat supply requirement, and see that from reaction tube heatproof angle the uniformity of temperature increases, but due to the difference of diverse location flame temperature and the difference of reaction tube and flame relative position, temperature in whole reaction tube still is difficult to the strict guarantee homogeneous, so external-burning is not suitable for conversion ratio for thermal reactor and selectively to the highstrung endothermic reaction process of temperature.
With respect to this, fluidized-bed reactor is applicable to the chemical reaction process that solid phase reaction material or solid-phase catalyst participate in, have advantages of that production capacity is large, heat supply/move heat energy power strong and conduct heat evenly, solid phase components is easy to move into/shift out.Traditional fluidized-bed reactor is usually by arranging shift out/supply response of interior heat-obtaining/heating coil pipe heat.For exothermic reaction, usually in heat production coil pipe, pass into water or steam heat-obtaining; When getting thermal change when larger, also external warmer can be set, solid material is drawn and moved heat.For the endothermic reaction, can use steam heating when reaction temperature is low, in heating coil pipe, pass into steam; When desired reaction temperature is higher, can substitute steam as heating medium with conduction oil; When temperature, during higher than the decomposition temperature of conduction oil, need to adopt fused salt as heating medium.Although fused salt can reach higher heat supply temperature, to equipment, corrosiveness may be arranged, operation easier is large, is not suitable for continuous run in long period, therefore in industrial fluidized bed reactor, seldom is used.In addition, existing fluidized-bed reactor operates enhanced heat exchange by fluidization, but in can not directly solving, the strong endothermic chemical reaction under the high-temperature condition supplies heat problem.
Summary of the invention
The present invention is intended at least solve one of technical problem existed in prior art.
For this reason, one object of the present invention is to propose the double-fluidized-bed reactor of the endothermic reaction that a kind of strong endothermic reaction can be under middle hot conditions provides heat evenly, efficiently.
Another object of the present invention is to propose a kind of heat supply method of the endothermic reaction of first aspect present invention embodiment with the endothermic reaction of double-fluidized-bed reactor that utilize, and the described endothermic reaction is the non-oxide dehydrogenation of alkane or hydrocarbon vapor reforming or hydrocarbon cracking production CNT.
According to the double-fluidized-bed reactor of the endothermic reaction of the embodiment of the present invention, comprise: endothermic reaction fluidized bed body, the described endothermic reaction is the first fluidized bed bed consisted of with catalyst granules or reactant particle the endothermic reaction that is provided with sealing and inner with the fluidized bed body, the described endothermic reaction is provided with the first gas distributor with the bottom of fluidized bed body, and described the first gas distributor is connected with the first gas source of the gas in order to supply with the first gas to described first fluidized bed bed, and heat supply fluidized bed body, described heat supply is the second fluid bed bed consisted of the heat carrier particle that is provided with sealing and inner with the fluidized bed body, described heat supply is provided with the second gas distributor with the bottom in the fluidized bed body, described the second gas distributor is connected with the second gas source of the gas in order to supply with the second gas in described the second fluid bed bed, wherein, described the first gas is reacting gas or fluidized gas, described the second gas is fluidized gas, described fluidized gas comprises air, oxygen and combination thereof, the described endothermic reaction is arranged on described heat supply with in the fluidized bed body, the interior required heat of the endothermic reaction is provided with the fluidized bed body by described heat supply so that the described endothermic reaction is with the fluidized bed body with the fluidized bed body, and the described endothermic reaction further comprises with double-fluidized-bed reactor: heater, described heater has the heater body, the first conduit and the second conduit, described the first conduit and described the second conduit are connected to described heater body and described heat supply is used between the fluidized bed body, so that described heater and described heat supply are with form the peripheral passage of heat carrier particle between the fluidized bed body by described the first conduit and described the second conduit.
According to the double-fluidized-bed reactor of the endothermic reaction of the embodiment of the present invention, because the endothermic reaction is arranged on described heat supply with in the fluidized bed body and be that inside is provided with the second fluid bed bed consisted of the heat carrier particle in heat supply with the fluidized bed body with the fluidized bed body, therefore the reaction in-situ of the heat carrier particle by the second fluid bed bed or the heat that carries from other place can be for the endothermic reaction with providing the endothermic reaction needed heat in fluid bed.In addition, owing to being conducted heat by the heat carrier particle, therefore than the gas heat-transfer medium have that safety, stable, applicable temperature range are wider, heat transfer efficiency advantages of higher more.
In addition, the endothermic reaction according to the above embodiment of the present invention can also have following additional technical characterictic with double-fluidized-bed reactor:
According to one embodiment of present invention, described heat carrier particle is alumina particle, silica dioxide granule or the catalyst cracking particles that particle diameter is 60～120 microns.
According to some embodiments of the present invention, described heat supply is located at the described endothermic reaction with in the fluidized bed body with the fluidized bed body, the described endothermic reaction is provided with the first discharge port with the bottom of fluidized bed body and top is provided with the first charging aperture, described heat supply is provided with for spray into the fuel nozzle ports of fuel in described the second fluid bed bed with the bottom of fluidized bed body, described heat supply is provided with and extends to the described endothermic reaction second discharge port external by fluidized bed and top is provided with the second charging aperture with the bottom of fluidized bed body, and described the second charging aperture is connected with and extends to the conduit of described heat supply with the bottom of fluidized bed body.
Alternatively, described fuel comprises fuel oil, combustion gas and combination thereof.
Alternatively, be provided with fin on the outer wall of described heat supply with the fluidized bed body.
Further, described fin is multistage, and the orientation of adjacent two sections fins is staggered.
According to some embodiment more of the present invention, the described endothermic reaction is arranged on described heat supply with in the fluidized bed body with the fluidized bed body, and the described endothermic reaction further comprises with double-fluidized-bed reactor: heater, described heater has the heater body, the first conduit and the second conduit, wherein, described the first conduit and described the second conduit are connected to described heater body and described heat supply is used between the fluidized bed body, so that described heater and described heat supply are with form the peripheral passage of heat carrier particle between the fluidized bed body by described the first conduit and described the second conduit.
Alternatively, the described endothermic reaction is provided with the first gas-solid separating device for gas solid separation with the top of fluidized bed body, and described the first gas-solid separating device is cyclone separator or metallic filter or the combination of the two.
Further, described heat supply is provided with the second gas-solid separating device for gas solid separation with the top of fluidized bed body, and this second gas-solid separating device is cyclone separator or metallic filter or the combination of the two.
Further, in the described endothermic reaction is used the fluidized bed body with fluidized bed body and described heat supply, wherein be set in inner one and be provided with a plurality of.
Utilize the heat supply method of the described endothermic reaction of the arbitrary embodiment of first aspect present invention with the endothermic reaction of double-fluidized-bed reactor according to second aspect present invention embodiment, the described endothermic reaction is the non-oxide dehydrogenation of alkane or hydrocarbon vapor reforming or hydrocarbon cracking production CNT, and comprise the following steps: the endothermic reaction that is a) 60～100 microns by average grain diameter is introduced the described endothermic reaction with in the fluidized bed body with catalyst granules; B) pass into the described endothermic reaction using reacting gas as described the first gas with in the fluidized bed body, described reacting gas is pending alkane or the hydro carbons gaseous mixture for the treatment of reformer feed and water vapour or for the production of methane, ethene, propylene or its mixture of CNT; And c) described the second gas is passed into described heat supply with in the fluidized bed body so that described heat carrier wherein is grain fluidized, the second fluid bed bed original position produces heat or obtains heat in order to provide heat for endothermic reaction fluid bed by the heat carrier particles circulating from outer thermal source.
According to some embodiments of the present invention, wherein, at step c) in by described heat supply with spraying into fuel in the fluidized bed body and making it burn to make described the second fluid bed bed to produce heat, described fuel comprises fuel oil, combustion gas and combination thereof.In the situation that use fuel oil, preferably at bed temperature, under the condition higher than this fuel oil self-ignition point, spray into fuel oil.
According to other embodiment of the present invention, what described heat carrier particle was coking and deactivation treats regeneration catalyzing Cracking catalyst particle so that at step c) in by the described coke burning regeneration for the treatment of regeneration catalyzing Cracking catalyst particle, make described the second fluid bed bed produce heat.
According to some embodiment more of the present invention, wherein, described heater be catalytic cracking regenerator and described heat carrier particle for the regeneration catalyzing Cracking catalyst particle from described catalytic cracking regenerator so that at step c) in split by described catalysis the coke burning regeneration reaction occurred in regenerator and supplement described the second fluid bed bed heat.
According to some embodiments of the present invention, draw off continuously or off and on and contain the granule materials that catalyst and carbon phase product form from the discharge port of the bottom of described first fluidized bed bed, continuously or off and on from the charge door on the top of described first fluidized bed bed, fill into new catalyst granules simultaneously.
The accompanying drawing explanation
Above-mentioned and/or additional aspect of the present invention and advantage are from obviously and easily understanding becoming the description of embodiment in conjunction with following accompanying drawing, wherein:
Fig. 1 is the structural representation of the endothermic reaction according to an embodiment of the invention with double-fluidized-bed reactor;
Fig. 2 is the structural representation of the endothermic reaction of the variation according to the present invention with double-fluidized-bed reactor;
Fig. 3 is the structural representation of the endothermic reaction of another embodiment according to the present invention with double-fluidized-bed reactor;
Fig. 4 is the heat supply method of the endothermic reaction according to an embodiment of the invention with the endothermic reaction of double-fluidized-bed reactor.
The specific embodiment
Below describe embodiments of the invention in detail, the example of described embodiment is shown in the drawings, and wherein same or similar label means same or similar element or the element with identical or similar functions from start to finish.Be exemplary below by the embodiment be described with reference to the drawings, only for explaining the present invention, and can not be interpreted as limitation of the present invention.
In description of the invention, term " vertically ", " laterally ", " on ", orientation or the position relationship of the indications such as D score, 'fornt', 'back', " left side ", " right side ", " vertically ", " level ", " top ", " end " be based on orientation shown in the drawings or position relationship, be only the present invention for convenience of description rather than require the present invention with specific orientation structure and operation, therefore can not be interpreted as limitation of the present invention.
Describe the heat supply method with the endothermic reaction of double-fluidized-bed reactor and the non-oxide dehydrogenation of alkane or hydrocarbon vapor reforming or hydrocarbon cracking production CNT according to the endothermic reaction of the embodiment of the present invention in detail below with reference to accompanying drawing.
According to the double-fluidized-bed reactor of the endothermic reaction of the embodiment of the present invention, comprising: fluidized bed body 1 and heat supply fluidized bed body 2 for the endothermic reaction.
Particularly; the endothermic reaction is the first fluidized bed bed 11 consisted of with catalyst granules or reactant particle the endothermic reaction that is provided with sealing and inner with fluidized bed body 1; the endothermic reaction is provided with the first gas distributor 12 with the bottom in fluidized bed body 1, and described the first gas distributor 12 is connected in order to provide the first gas to first fluidized bed bed 11 with the first gas source of the gas (not shown).
Heat supply is the second fluid bed bed 21 consisted of the heat carrier particle that is provided with sealing and inner with fluidized bed body 2, heat supply is provided with the bottoms in fluidized bed body 2 that the second gas distributor 22, the second gas distributors 22 are connected with the second gas source of the gas (not shown) to interior supply the second gas of the second fluid bed bed 21.
Wherein, described the first gas is reacting gas or fluidized gas, described the second gas is fluidized gas, the fluidized gas of described the second gas comprises air, oxygen and combination thereof, and it is interior so that the endothermic reaction is provided with fluidized bed body 2 by heat supply with the required heat of the endothermic reaction in fluidized bed body 1 with fluidized bed body 2 that the endothermic reaction is arranged on heat supply with fluidized bed body 1.
As shown in Figure 3, according to the embodiment of the present invention, the endothermic reaction is arranged on heat supply with in fluidized bed body 2 with fluidized bed body 1, and the endothermic reaction further comprises heater 3 ' with double-fluidized-bed reactor.Heater 3 ' has heater body 31 ', the first conduit 32 ' and the second conduit 33 ', wherein, the first conduit 32 ' and the second conduit 33 ' are connected to heater body 31 ' and heat supply is used between fluidized bed body 2, so that heater 3 ' and heat supply are with form the peripheral passage of heat carrier particle between fluidized bed body 2 by the first conduit 32 ' and the second conduit 33 '.Thus, by heat supply is continuously removed in heater 3 ' and is heated by heater 3 ' by the first conduit 32 ' with the heat carrier particle in fluidized bed body 2, after this return to heat supply with in fluidized bed body 2 by the second conduit 33 ' again, thereby can be heated the heat carrier particle by heater 3 '.
It should be noted that, so-called " endothermic reaction is sealing with fluidized bed body 1 " and " heat supply is what seal with fluidized bed body 2 " are not to be intended to limit it seal to be isolated from the outside fully and refer to that heat supply is isolated with the particle in fluidized bed body 1 and gas fully with fluidized bed body 2 and the endothermic reaction in reactor, with regard to the endothermic reaction, use 1 heat supply of fluidized bed body with regard to fluidized bed body 2, it can pass through charging aperture, discharging opening etc. respectively and be connected with outside.
In addition, it should be noted that, in the endothermic reaction is used fluidized bed body 2 with fluidized bed body 1 and 1 heat supply, wherein be set in inner one and can be provided with as required a plurality of.
According to the double-fluidized-bed reactor of the endothermic reaction of the embodiment of the present invention, the first gas passes into the first gas distributor 12 of double-fluidized-bed bed body 1 bottom from the endothermic reaction, make particle in first fluidized bed bed 11 in fluidized state, endothermic chemical reaction occurs in fluidization solid particle, and with one in fluidized bed body 2, be set in another with fluidized bed body 1 and heat supply due to the endothermic reaction, thereby heat supply is high temperature fluidized bed with fluidized bed body 2() according to deriving from reaction in-situ or being that the endothermic reaction is the low temperature fluid bed with fluidized bed body 1(by the heat that outside offers solid particle) provide the endothermic reaction needed heat, that is to say that particle in high temperature fluidized bed is as heat carrier.In addition, owing to being conducted heat by the heat carrier particle, therefore than the gas heat-transfer medium have that safety, stable, applicable temperature range are wider, heat transfer efficiency advantages of higher more.
The heat carrier particle that forms the second fluid bed bed 21 does not have special restriction, but consider alumina particle, it is high that silica dioxide granule has heat endurance, mechanical strength is high, thermal capacitance is larger, the advantages such as heat conductivility is strong, with catalyst cracking particles, can use the reaction in-situ of fluidized bed body 2 interior generations to provide heat for the endothermic reaction with fluidized bed body 1 by heat supply in addition, in examples more of the present invention, described heat carrier particle (forming the particle of the second fluid bed bed 21) can adopt the alumina particle that particle diameter is 60～120 microns, silica dioxide granule or catalyst cracking particles.
In some embodiments of the invention, as shown in Figure 1, heat supply is located at the endothermic reaction with in fluidized bed body 1 with fluidized bed body 2.Wherein, the endothermic reaction is provided with the first discharge port 13 with the bottom of fluidized bed body 1 and top is provided with the first charging aperture 14, heat supply is provided with for spray into the fuel nozzle ports 23 of fuel in the second fluid bed bed 21 with the bottom of fluidized bed body 2, heat supply is provided with and extends to the endothermic reaction and be provided with the second charging aperture 25 with fluidized bed body 1 outer the second discharge port 24 and top with the bottom of fluidized bed body 2, and the second charging aperture 25 is connected with and extends to the conduit 26 of heat supply with the bottom of fluidized bed body 2.
, it should be noted that, term " ”He“ top, bottom " is comparatively speaking herein, and " bottom " comprises bottom.
The double-fluidized-bed reactor of the endothermic reaction according to the above embodiment of the present invention, can carry out the heat hot carrier granular by the burning of the fuel that sprayed into by fuel nozzle ports 23, and and then provide heat with the fluidized bed body for the endothermic reaction.In addition, because being connected with, the second charging aperture 25 extends to the conduit 26 of heat supply with the bottom of fluidized bed body 2, and can be so that the heat carrier particle drops down onto heat supply with the bottom of fluidized bed body 2 in order to form the second fluid bed bed 21 more swimmingly along conduit 26.In examples more of the present invention, described fuel comprises fuel oil, combustion gas and combination thereof.
In variation more of the present invention, as shown in Figure 2, heat supply is located at the endothermic reaction with in fluidized bed body 1 with fluidized bed body 2, and the described endothermic reaction further comprises heater 3 and riser 4 with double-fluidized-bed reactor.Wherein, heater 3 is connected with the top of fluidized bed body 2 with heat supply, riser 4 is arranged on heat supply with in fluidized bed body 2, the first end of riser 4 (being the upper end in Fig. 2) is connected with heater 3, the second end of riser 4 (being the lower end in Fig. 2) extends to the second fluid bed bed 21 inside and described the second end is connected with the lifting source of the gas (not shown) that promotes gas is provided, so that heater 3 and heat supply are with between fluidized bed body 2, by riser 4, forming Fluid Circulations.Thus, by in riser 4, passing into lifting gas, heat supply is continuously removed in heater 3 and is heated by heater 3 by riser 4 with the heat carrier particle in fluidized bed body 2, after this return to again heat supply with in fluidized bed body 2, thereby can be heated by 3 pairs of heat carrier particles of heater.
It about the kind that promotes gas, is not particularly limited, for example, as long as can, so that the heat carrier particle circulates between heater 3 and heat supply are with fluidized bed body 2,, can adopt air, oxygen, steam etc.
In the situation that heat supply is arranged on the endothermic reaction with in fluidized bed body 1 with fluidized bed body 2, in order to increase heat exchange area between high temperature and low temperature fluid bed to increase heat transfer efficiency, alternatively, be provided with fin (not shown) on the outer wall of heat supply with fluidized bed body 2.In addition, fin, except augmentation of heat transfer, can also play the effects such as bubble crushing, increase turbulence.Preferably, for fear of the axial long formation channel of fin or dead band, can adopt the multistage fin structure, the orientation of adjacent segment fin is staggered.Length, width and thickness about fin can design as required, and the adjacent segment fin width can be the same or different.
In above-mentioned arbitrary embodiment, alternatively, the first gas-solid separating device 15, the first gas-solid separating devices 15 that the endothermic reaction can be provided with for gas solid separation with the top of fluidized bed body 1 can be cyclone separator or metallic filter or the combination of the two.In addition, as shown in Figure 1, can also be provided with the second gas-solid separating device 27 for gas solid separation with the top of fluidized bed body 2 in heat supply, similarly, this second gas-solid separating device 27 can be cyclone separator, metallic filter or the combination of the two.
The described endothermic reaction according to the above-mentioned arbitrary embodiment of utilizing of the embodiment of the present invention is described below and carries out the heat supply method of the endothermic reaction with double-fluidized-bed reactor.
Carry out with double-fluidized-bed reactor the technique that CNT is produced in the non-oxide dehydrogenation of alkane or hydrocarbon vapor reforming or hydrocarbon cracking according to the described endothermic reaction of the above-mentioned any one embodiment of utilizing of the embodiment of the present invention, comprise the following steps:
At first, the endothermic reaction that is 60～100 microns by average grain diameter is introduced the endothermic reaction with in fluidized bed body 1 with catalyst granules.Wherein, the endothermic reaction is different because of concrete technology with catalyst granules, can be for example Pt-Sn/Al
2o
3, Ni/Al
2o
3, Fe-Mo/MgO etc.From guaranteeing that not remarkable broken this considered on the one hand fluid mapper process, advantageously, select to have the particle of some strength.
Then, pass into the endothermic reaction using reacting gas as described the first gas with in fluidized bed body 1, described reacting gas is that alkane or hydro carbons are treated the gaseous mixture of reformer feed (natural gas or naphtha) and water vapour or for the production of the hydrocarbon raw material gas (such as methane, ethene or propylene etc.) of CNT.
Finally, by described the second gas pass into heat supply with in the fluidized bed body 2 so that described heat carrier wherein is grain fluidized, the second fluid bed bed 21 original positions produce heats or obtain heat in order to provide heat for endothermic reaction fluidized bed body by the heat carrier particles circulating from outer thermal source.
In order to ensure the active of catalyst or shift out in time carbon phase product, according to some embodiments of the present invention, preferably, draw off continuously or off and on and contain the granule materials that catalyst and carbon phase product form from the discharge port of the bottom of described first fluidized bed bed, continuously or off and on from the charge door on the top of described first fluidized bed bed, fill into new catalyst granules simultaneously.
In some embodiments of the invention, at step c) in by heat supply with spraying into fuel in fluidized bed body 2 and making it burn to make the second fluid bed bed 21 to produce heat, described fuel comprises fuel oil, combustion gas and combination thereof.In the situation that use fuel oil, preferably at bed temperature, under the condition higher than this fuel oil self-ignition point, spray into fuel oil.
In other embodiment of the present invention, what described heat carrier particle was coking and deactivation treats regeneration catalyzing Cracking catalyst particle so that at step c) in by the described coke burning regeneration for the treatment of regeneration catalyzing Cracking catalyst particle, make the second fluid bed bed 21 produce heat.
In some embodiment more of the present invention, heater 3 or 3 ' be catalytic cracking regenerator and described heat carrier particle for the regeneration catalyzing Cracking catalyst particle from described catalytic cracking regenerator so that at step c) in by supplementary the second fluid bed bed 21 heats of coke burning regeneration reaction that occur in described catalytic cracking regenerator.
Describe technique and the heat supply method according to the embodiment of the present invention in detail below by specific embodiment and with reference to accompanying drawing 4.
Embodiment mono-
Adopt the endothermic reaction as shown in Figure 1 to carry out the reaction of propane nonoxidation catalytic dehydrogenation with double-fluidized-bed reactor.Dehydrogenating propane is strong endothermic reaction, 600 ℃ of reaction temperatures.
At first, heat supply is lighted with fluidized bed body 2 inner nozzles, a body is heated up.
Then, by the inertia Al of 60～200 microns of average particulate diameters
2o
3particle, as the heat carrier particle in fluidized bed body 2 for heat supply, passes into air and makes its fluidisation.Fuel gas buring makes the second fluid bed bed heat up.
Then, by the Pt-Sn/Al of 60～100 microns of average grain diameters
2o
3catalyst granules is introduced the endothermic reaction with in fluidized bed body 1, passes into nitrogen and makes its fluidisation.Treat that first fluidized bed bed temperature rises to reaction temperature, by the first gas distributor, in the first fluidized bed, pass into reacting gas (i.e. the first gas) propane maintenance catalyst granules fluidisation, gradually reduce the nitrogen intake until stop fully simultaneously.
For driving force of heat transfer is provided, the regulating gas amount makes the second fluid bed bed temperature maintain 700 ℃ of left and right.
Embodiment bis-
Adopt the endothermic reaction as shown in Figure 1 to carry out the hydrocarbon vapor reforming reaction with double-fluidized-bed reactor.The reaction temperature of this reaction is 550 ℃.
Wherein, reaction gas is natural gas and water vapour, and gas product is synthesis gas.Catalyst granules Ni/Al in fluidized bed body 1 for the endothermic reaction
2o
3under the effect of reaction gas in bubbling or turbulence fluidized state.
As different from Example 1, in order to make the second fluid bed bed 21, produce heat, at first inwardly in fluid bed, pass into hot-air (for example, by the auxiliary combustion chamber heating), heat supply is heated up with fluid bed bed 21.Treat that temperature rises to 380 ℃, spray into light diesel fuel by fuel nozzle ports 23 and make it burn to heat heat supply with fluid bed bed 21 in order to provide heat for hydrocarbon vapor reforming.Wherein, the inertia Al that heat supply is 60～200 microns of average particulate diameters with the heat carrier particle in fluidized bed body 2
2o
3particle.
In addition, the straying quatity that can regulate light diesel fuel is controlled at 650 ℃ so that driving force of heat transfer to be provided by heat supply by the temperature of fluid bed bed.
Embodiment tri-
Adopt the endothermic reaction as shown in Figure 2 to carry out the reaction of butane nonoxidation catalytic dehydrogenation with double-fluidized-bed reactor.Butane dehydrogenation is strong endothermic process, and reaction temperature is 450 ℃.
Reaction gas is butane, and catalyst is with embodiment mono-.
The inertia Al that heat supply is 60～150 microns of average diameters with the heat carrier particle in fluidized bed body 2
2o
3, it circulates between with double-fluidized-bed reactor 3 with fluidized bed body 2 and the heating endothermic reaction in heat supply by riser, and heating the endothermic reaction can be the external-burning tube furnace with double-fluidized-bed reactor 3.The external-burning tube furnace relies on fuel combustion to obtain heat, thereby the mobile heat carrier particle in tube furnace can be heated to more than 550 ℃.
Embodiment tetra-
Adopt the endothermic reaction as shown in Figure 3 to carry out the reaction of same embodiment tri-with double-fluidized-bed reactor.Be that with the difference of embodiment tri-heat supply is set in the outside of the endothermic reaction with the fluidized bed body with the fluidized bed body, and the butane nonoxidation catalytic dehydrogenation reacts in the inboard endothermic reaction with carrying out in the fluidized bed body.The gas solid separation system that gas product is in series through cyclone separator and metallic filter carries out from the endothermic reaction, with fluidized bed body top, drawing after gas solid separation.
Embodiment five
Adopt the endothermic reaction as shown in Figure 2 to carry out with double-fluidized-bed reactor the endothermic reaction process that the propylene catalytic pyrolysis is produced CNT.550 ℃ of catalyst of reaction temperature are the Fe-Mo/MgO particle, and reaction raw materials is propylene.Using catalytic cracking catalyst as the heat carrier particle in the second fluid bed, using catalytic cracking regenerator as heater 3.That is to say, relying on catalytic cracking catalyst is the heat supply of propylene cracking reaction at catalytic cracking regenerator and heat supply with the circulation between the fluidized bed body.The CNT that the product of this process is solid phase, mixed in together with catalyst granules.Can draw off catalyst and carbon nanotube product from the discharge port intermittence of first fluidized bed bottom, intermittently fill into new catalyst from the charge door on first fluidized bed top simultaneously; Also can draw off continuously catalyst and carbon nanotube product, fill into continuously new catalyst simultaneously.
Embodiment six
Adopt the endothermic reaction as shown in Figure 3 to carry out the non-oxide dehydrogenation reaction process of propane of same embodiment five with double-fluidized-bed reactor, wherein, using catalyst cracker as heater 3.That is to say, heat supply is used as to catalytic cracking regenerator with fluid bed, using air as fluidized gas.
Directly enter heat supply with in the fluidized bed body from the spent agent of catalyst cracker, when completing catalytic cracking catalyst and burning, for the inboard endothermic reaction, with the reaction of the dehydrogenating propane in fluid bed, provide the heat that reacts required.
Be understandable that, heat supply can also be used as to the catalytic cracking Second reactivator with the fluidized bed body.Spent agent from catalytic cracking regenerator enters heat supply fluidized bed body, and under the air or oxygen effect, further abundant coke burning regeneration is emitted heat, and the regenerative agent after burning directly returns to catalyst cracker.Thus, the temperature in the catalytic cracking regenerator that can make by parameter adjustment is 680 ℃, and heat supply is 700 ℃ by the temperature of fluidized bed body, and 600 ℃ of the temperature of fluidized bed body for the endothermic reaction.
In the description of this specification, the description of reference term " embodiment ", " some embodiment ", " example ", " concrete example " or " some examples " etc. means to be contained at least one embodiment of the present invention or example in conjunction with specific features, structure, material or the characteristics of this embodiment or example description.In this manual, the schematic statement of above-mentioned term not necessarily referred to identical embodiment or example.And the specific features of description, structure, material or characteristics can be with suitable mode combinations in any one or more embodiment or example.
Although illustrated and described embodiments of the invention, those having ordinary skill in the art will appreciate that: in the situation that do not break away from principle of the present invention and aim can be carried out multiple variation, modification, replacement and modification to these embodiment, scope of the present invention is limited by claim and equivalent thereof.
Claims (14)
1. the double-fluidized-bed reactor of the endothermic reaction, is characterized in that, comprising:
Endothermic reaction fluidized bed body, the described endothermic reaction is the first fluidized bed bed consisted of with catalyst granules or reactant particle the endothermic reaction that is provided with sealing and inner with the fluidized bed body, the described endothermic reaction is provided with the first gas distributor with the bottom in the fluidized bed body, and described the first gas distributor is connected with the first gas source of the gas in order to supply with the first gas to described first fluidized bed bed; And
Heat supply fluidized bed body, described heat supply is the second fluid bed bed consisted of the heat carrier particle that is provided with sealing and inner with the fluidized bed body, described heat supply is provided with the second gas distributor with the bottom in the fluidized bed body, described the second gas distributor is connected with the second gas source of the gas in order to supply with the second gas in described the second fluid bed bed
Wherein, described the first gas is reacting gas or fluidized gas, and described the second gas is fluidized gas, and described fluidized gas comprises air, oxygen and combination thereof,
The described endothermic reaction is arranged on described heat supply with in the fluidized bed body, the interior required heat of the endothermic reaction is provided with the fluidized bed body by described heat supply so that the described endothermic reaction is with the fluidized bed body with the fluidized bed body,
And the described endothermic reaction further comprises with double-fluidized-bed reactor:
Heater, described heater has heater body, the first conduit and the second conduit,
Described the first conduit and described the second conduit are connected to described heater body and described heat supply is used between the fluidized bed body, so that described heater and described heat supply are with form the peripheral passage of heat carrier particle between the fluidized bed body by described the first conduit and described the second conduit.
2. the double-fluidized-bed reactor of the endothermic reaction according to claim 1, is characterized in that, described heat carrier particle is alumina particle, silica dioxide granule or the catalyst cracking particles that particle diameter is 60～120 microns.
3. the double-fluidized-bed reactor of the endothermic reaction according to claim 1, is characterized in that, described heat supply is located at the described endothermic reaction with in the fluidized bed body with the fluidized bed body,
The described endothermic reaction is provided with the first discharge port with the bottom of fluidized bed body and top is provided with the first charging aperture,
Described heat supply is provided with for spray into the fuel nozzle ports of fuel in described the second fluid bed bed with the bottom of fluidized bed body, described heat supply is provided with and extends to the described endothermic reaction second discharge port external by fluidized bed and top is provided with the second charging aperture with the bottom of fluidized bed body, and described the second charging aperture is connected with and extends to the conduit of described heat supply with the bottom of fluidized bed body.
4. the double-fluidized-bed reactor of the endothermic reaction according to claim 3, is characterized in that, described fuel comprises fuel oil, combustion gas and combination thereof.
5. according to claim 3-or the double-fluidized-bed reactor of the 4 described endothermic reaction, it is characterized in that, on the outer wall of described heat supply with the fluidized bed body, be provided with fin.
6. the double-fluidized-bed reactor of the endothermic reaction according to claim 5, is characterized in that, described fin is multistage, and the orientation of adjacent two sections fins is staggered.
7. the double-fluidized-bed reactor of the endothermic reaction according to claim 1, is characterized in that,
The described endothermic reaction is provided with the first gas-solid separating device for gas solid separation with the top of fluidized bed body, the combination that described the first gas-solid separating device is cyclone separator or metallic filter or cyclone separator and metallic filter.
8. the double-fluidized-bed reactor of the endothermic reaction according to claim 7, it is characterized in that, described heat supply is provided with the second gas-solid separating device for gas solid separation with the top of fluidized bed body, and described the second gas-solid separating device is cyclone separator or metallic filter or the two combination.
9. the double-fluidized-bed reactor of the endothermic reaction according to claim 1, is characterized in that, in the described endothermic reaction is used the fluidized bed body with fluidized bed body and described heat supply, wherein is set in inner one and is provided with a plurality of.
10. one kind is utilized in claim 1～9 heat supply method of the endothermic reaction of double-fluidized-bed reactor for the described endothermic reaction of any one, the described endothermic reaction is the non-oxide dehydrogenation of alkane or hydrocarbon vapor reforming or hydrocarbon cracking production CNT, it is characterized in that, comprise the following steps:
A) endothermic reaction that is 60～100 microns by average grain diameter is introduced the described endothermic reaction with in the fluidized bed body with catalyst granules;
B) pass into the described endothermic reaction using reacting gas as described the first gas with in the fluidized bed body, described reacting gas is pending alkane or the hydro carbons gaseous mixture for the treatment of reformer feed and water vapour or for the production of methane, ethene, propylene or its mixture of CNT; And
C) described the second gas is passed into described heat supply with in the fluidized bed body so that described heat carrier wherein is grain fluidized, make described the second fluid bed bed original position produce heat or obtain heat in order to provide heat for endothermic reaction fluidized bed body by the heat carrier particles circulating from outer thermal source.
11. the heat supply method of the endothermic reaction according to claim 10, it is characterized in that, utilize the double-fluidized-bed reactor of the described endothermic reaction of claim 3 or 4, wherein, at step c) in by described heat supply with spraying into fuel in the fluidized bed body and making it burn to make described the second fluid bed bed to produce heat, described fuel comprises fuel oil, combustion gas and combination thereof.
12. the heat supply method of the endothermic reaction according to claim 10, it is characterized in that, utilize the double-fluidized-bed reactor of the described endothermic reaction of claim 3 or 4, what wherein, described heat carrier particle was coking and deactivation treats regeneration catalyzing Cracking catalyst particle so that at step c) in by the described coke burning regeneration for the treatment of regeneration catalyzing Cracking catalyst particle, make described the second fluid bed bed produce heat.
13. the heat supply method of the endothermic reaction according to claim 10, it is characterized in that, wherein, described heater be catalytic cracking regenerator and described heat carrier particle for the regeneration catalyzing Cracking catalyst particle from described catalytic cracking regenerator so that at step c) in by the heat of supplementary described the second fluid bed bed of coke burning regeneration reaction that occurs in described catalytic cracking regenerator.
14. the heat supply method of the endothermic reaction according to claim 10, it is characterized in that, draw off continuously or off and on and contain the granule materials that catalyst and carbon phase product form from the discharge port of the bottom of described first fluidized bed bed, continuously or off and on from the charge door on the top of described first fluidized bed bed, fill into new catalyst granules simultaneously.
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| US10526707B2 (en) * | 2012-08-29 | 2020-01-07 | The University Of Tokyo | Heat exchanger type reaction tube |
| WO2014167473A1 (en) * | 2013-04-08 | 2014-10-16 | Saudi Basic Industries Corporation | Reactor and process for paraffin dehydrogenation to olefins |
| AU2016220415B2 (en) * | 2015-02-18 | 2018-05-31 | Exxonmobil Research And Engineering Company | Upgrading paraffins to distillates and lube basestocks |
| CN105709710A (en) * | 2016-03-03 | 2016-06-29 | 北京清新环境技术股份有限公司 | Multilayer fluidized bed parsing device for conducting pneumatic material return through row tube type heat exchange and coupling of molten salt |
| CN112675790A (en) * | 2020-12-04 | 2021-04-20 | 厦门大学 | Reactor and method for self-heat storage co-production of carbon nanotubes |
| CN113441092A (en) * | 2021-08-12 | 2021-09-28 | 成都市润和盛建石化工程技术有限公司 | Propane dehydrogenation method and system adopting tube array type fixed bed molten salt heating reactor |
| CN113797980B (en) * | 2021-10-14 | 2023-07-18 | 中国石油化工股份有限公司 | Double-particle catalyst coupling catalysis method and reaction system |
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