CN106607075A - Fluid catalyst for preparing olefin and arene and application of fluid catalyst - Google Patents
Fluid catalyst for preparing olefin and arene and application of fluid catalyst Download PDFInfo
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- CN106607075A CN106607075A CN201510685830.7A CN201510685830A CN106607075A CN 106607075 A CN106607075 A CN 106607075A CN 201510685830 A CN201510685830 A CN 201510685830A CN 106607075 A CN106607075 A CN 106607075A
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- aromatic hydrocarbons
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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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
Abstract
The invention relates to a fluid catalyst for preparing olefin and arene, and mainly solves the technical problem of a current catalytic cracking fluid catalyst applying to a naphtha catalytic cracking process that the yields of ethylene, propylene and arene are low. The technical scheme of the invention is characterized in that the catalyst comprises the following components in parts by weight: 0.5-10 parts of P2O5, 0.5-5 parts of at least one of ZnO, Ga2O3, Cr2O3 or MoO3, 0-10 parts of at least one of rare-earth element oxides, Fe2O3 or Co2O3, 20.0-55.0 parts of at least one of ZSM-5 or ZSM-11 zeolites, 10.0-30.0 parts of silica-alumina composite oxides and 25.0-60.0 parts of kaolin, so that the above problem can be well solved, and the fluid catalyst can be applied to industrial production of preparing the ethylene, propylene and arene through catalytic cracking of petroleum hydrocarbon.
Description
Technical field
The present invention relates to a kind of prepare fluid catalyst of the alkene with aromatic hydrocarbons and application.
Technical background
Ethylene, propylene and aromatic hydrocarbons are very important three kinds of petrochemical materials, and at present whole world ethylene is main with propylene
It is to be produced by steam-cracking process.Because traditional steam cracking reaction temperature is up to 820～1000 DEG C, process energy
Consumption is very high, accounts for the 50% of whole ethylene industry energy consumption.The process is non-catalytic free radical thermal cracking mechanism,
Ethylene/propene is than relatively low (0.5～0.7) in its product.Currently, face country and the 11th Five-Year phase is proposed to petrochemical industry
Between energy-saving 20% requirement and the propylene demand that increasingly increases, traditional steam-cracking process is experienced by sternly
High test.Catalytic pyrolysiss are the processes for carrying out producing low-carbon olefins by cracking to Petroleum using catalyst.With steaming
Vapour cracking is compared, and catalytic pyrolysiss have reaction temperature low (600-780 DEG C), and energy consumption is significantly reduced and reacted
The advantage of product propylene/ethylene ratio height (0.6～1.3).This technology occurs, and is traditional steam cracking production
The innovation of ethylene, propylene process brings hope.
Russian organic synthesiss academy and catalytic cracking catalyst active component be mainly manganese, vanadium, niobium, stannum,
The variable valency metal compound such as ferrum, wherein catalytic performance it is optimum be vanadium with ceramic (andalusite-corundum) as carrier
Sour potassium (or sodium) fluid catalyst.Although the catalyst has heat-resist, low coking rate and high stability
Advantage, but its cracking reaction temperature still up to 770 DEG C when.[Picciotti M.[J].Oil Gas
J,1997,95(25):53～56.]
Japanese Toyo Engineering Corporation consists of CaO from THR-RC fluid catalysts, Exemplary chemical：Al2O3：
SiO2：Fe2O3MgO=51.46：47.74：0.06：0.185：0.25.The catalyst is with light gasoline
Raw material, still up to 750 DEG C of the reaction temperature of cracking.[Zhang Jian, etc. [J]. petrochemical industry dynamic, 1995,
(11):24～30,34.] Μ S4087350 disclose normal pressure and are catalyzed the fluid bed Mg of volume increase alkene with decompression residuum
Base catalyst, the catalyst reaction temperatures are up to 745, and ethylene, propylene yield also only has 28.6%.
The technique of existing petroleum hydrocarbon catalytic pyrolysis ethylene and propylene, main target is ethylene and propylene.By
There is provided in the activated petroleum zeolite molecular sieve component for using.Modification component introduced in catalyst, is also main
For improving the activity and hydrothermal stability of catalyst.Display, single zeolite component, although have are studied
Certain Aromatization Activity, but its Aromatization Activity is also than relatively limited.And in single silicon oxide or oxidation
Al composition is usually used in the binding agent of the catalyst.Simple silicon oxide and alumina material, its catalysis activity is very weak.
Therefore, the introducing of single silicon oxide or alumina material, although the intensity of catalyst can be improved, but can
Can be because itself catalysis activity be extremely weak, to causing catalyst lytic activity to reduce.
In sum, there is ethylene+propylene+aromatic hydrocarbons in existing stone brain hydrocarbon catalytic pyrolysis preparing ethylene and the process of propylene
The low technical problem of yield.
The content of the invention
Technology to be solved by this invention, prior art prepare catalytic cracking fluid bed catalyst exist ethylene+
The low technical problem of propylene+aromatics yield.For one of solve problem, the present invention provides a kind of new catalyst,
The catalyst has the advantages that ethylene+propylene+high with aromatics yield.The two of problem to be solved by this invention are
A kind of method that petroleum hydrocarbon catalytic pyrolysis alkene and aromatic hydrocarbons are provided.
To solve technical problem one, the technical solution used in the present invention is as follows：A kind of stream for preparing alkene and aromatic hydrocarbons
Change bed catalyst, in terms of parts by weight, comprising following components：
A) 0.5～10 part of P2O5；
B) 0.5～5 part is selected from ZnO, Ga2O3、Cr2O3Or MoO3In at least one；
C) 0～10 part is selected from rare earth oxide, Fe2O3Or Co2O3In at least one；
D) at least one in 20.0～55.0 parts of ZSM-5 or ZSM-11 zeolites；
E) 10.0～30.0 parts of sial composite oxides；
G) 25.0～60.0 parts of Kaolin.
In above technical scheme, preferred technical scheme is：Aluminium oxide is in Alumina gel or acidified alumina
At least one, the presoma of the oxide of P elements is selected from the mixture of phosphoric acid or ammonium phosphate salt and mineral acid extremely
Few one kind, rare earth oxide preferably is selected from La2O3Or CeO2In at least one；With the weight of catalyst
Percentages, selected from C) in component consumption be 1～5%；In terms of the parts by weight of catalyst, P2O5's
Consumption is 1～6 part；The silicon oxide of zeolite used is 10～800 with the mol ratio of aluminium oxide；With sial composite oxygen
The weight ratio meter of compound, selected from E) in silicon oxide weight content be 5%～95%；The oxidation of zeolite used
Silicon is 20～300 with the mol ratio of aluminium oxide.
In above-mentioned technical proposal, it is preferred that component B) it is Ga2O3、Cr2O3Or MoO3At least one of with
The mixed-metal oxides I of ZnO；Preferably, by weight percentage, ZnO is in mixed-metal oxides I
In content be 20%～90%；Preferably, by weight percentage, ZnO is in mixed-metal oxides I
Content be 35%～75%.
In above-mentioned technical proposal, it is preferred that component B) it is selected from ZnO and Ga2O3；It is furthermore preferred that ZnO and
Ga2O3Weight ratio be (1：1)～(5:1)；Most preferably, ZnO and Ga2O3Weight ratio be (3:2)～(2:1).
In above-mentioned technical proposal, it is preferred that SiO in sial composite oxides2Weight percentage it is preferred
Scope 15～80%.
For the two of solve problem, a kind of method for preparing alkene and aromatic hydrocarbons, with petroleum hydrocarbon as raw material, in reaction temperature
Spend for 600～750 DEG C, the weight space velocity of petroleum hydrocarbon is 0.1～10h-1, reaction pressure be 0～2.0MPa, oil
Hydrocarbon is that under 0.1～8.0 reaction condition, reaction raw materials contact with above-mentioned fluid catalyst with the weight ratio of water
Reaction obtains the logistics containing ethylene, propylene and aromatic hydrocarbons.
Above technical scheme, preferred technical scheme is：Petroleum hydrocarbon is hydrocarbon component of the carbon number between 2～20
In the mixture of one or several.
In above-mentioned technical proposal, it is preferred that petroleum hydrocarbon is light naphthar.
In above-mentioned technical proposal, it is preferred that reaction temperature is 650～700 DEG C.
In above-mentioned technical proposal, it is preferred that the weight space velocity of petroleum hydrocarbon is 0.3～1h-1。
In above-mentioned technical proposal, it is preferred that reaction pressure is 0.1～1.0MPa.
In above-mentioned technical proposal, it is preferred that petroleum hydrocarbon is 0.3～4.0 with the weight ratio of water.
Catalyst according to the present invention, its preparation procedure is comprised the following steps：
A. the desired amount of presoma, Kaolin, P selected from sial composite oxides is weighed2O5Presoma,
At least one zeolite in ZSM-5 or ZSM-11 is soluble in water, and addition accounts for solid gross mass 0.1～5.0%
Pore creating material after mixing make within 10～60 minutes catalyst spray and be dried serosity used, by gained serosity through spraying
20～200 μm of microsphere is made in drying, by microsphere in 500～650 DEG C of 2～8h of roasting；By infusion process in roasting
Load on microsphere after burning is selected from B) and C) oxide, 80～120 DEG C of 8～24h of drying of Jing, 500～750 DEG C
2～8h of roasting is obtained fluid catalyst.Wherein pore creating material is sesbania powder, polyacrylamide, Polyethylene Glycol etc.
Organic substance of the molecular weight more than 1000.
The present invention introduces the metal oxide component with dehydrogenation functionality by the composition of catalyst, while
The weaker oxygen of the acidity commonly used in existing catalyst preparation is replaced using the aluminium silicon composite material with stronger acids
SiClx or alumina material, so can not only effectively improve activity of conversion, the ethylene+propene yield of catalyst,
The aromatisation yield of the process can also be effectively improved.
The present invention relates to a kind of producing olefin hydrocarbon by catalytic pyrolysis and aromatic hydrocarbons fluid catalyst and application, by using introducing
Dehydrogenation component, using the composite catalyst of stronger acids, compared with existing catalyst, ethylene+propene yield
And the yield of aromatic hydrocarbons is significantly improved, preferable technique effect is achieved.
Below by embodiment, the present invention is further elaborated.But the present invention is not limited in these embodiments.
Specific embodiment
[embodiment 1]
Weigh 40 grams of Kaolin, 108 grams of ZSM-5 molecular sieves, 5 grams of Ludox (40%SiO2), 95.2 grams
Alumina gel (21.0%Al2O3), 160 grams of water, 32.5 grams of strong phosphoric acid (85%) and 10 grams of sesbania powders, use
45 minutes prepared spray slurries of colloid mill emulsifying.By gained spray slurry at 270 DEG C, it is spray-dried and is obtained
10～200 μm of microsphere, then obtains roasting microsphere in 600 DEG C of roasting 4h.
The microsphere of 100 grams of roastings is taken, is impregnated containing 36.7 grams of zinc nitrate solutions with 90 grams, in room temperature ageing
12 hours, then 120 DEG C of Jing dryings 10 hours, 600 DEG C obtain naphtha catalytic cracking alkene in 4 hours by burning
Hydrocarbon fluid catalyst a, the composition of catalyst is listed in table 1.
The appreciation condition of reaction is that the weight space velocity of Petroleum is 4h-1, pressure is 0.1MPa, water and stone brain
The weight ratio of oil is 1:1,650 DEG C of reaction temperature, using fluidized-bed reactor, reaction evaluating result is listed in table 2.
Table 1
| Catalyst | Catalyst weight number is constituted | Zeolite |
| a | 5ZnO：10P2O5：10Al2O3：1SiO2：20 Kaolin：54ZSM-5 | 10 |
| b | 2Ga2O3：3P2O5：10SiO2：20Al2O3：25 Kaolin：40ZSM-5 | 150 |
| c | 3Ga2O3：3P2O5：4Al2O3：10.0SiO2：30.0 Kaolin：50.0ZSM-11 | 200 |
| d | 5ZnO：3.0P2O5：5La2O3：10Al2O3：4SiO2：29.0 Kaolin：44ZSM-5 | 100 |
| e | 2Cr2O3：3P2O5：5CeO2：0.5Al2O3：10SiO2：30 Kaolin：49.5ZSM-5 | 600 |
| f | 0.5ZnO：1.5P2O5：3.0La2O3:2SiO2：8Al2O3：25 Kaolin：60ZSM-5 | 800 |
| g | 2MoO3：5.0P2O5：3.0MnO2：12Al2O3：3SiO2：30 Kaolin：45ZSM-11 | 50 |
| h | 0.1Ga2O3：0.4ZnO：1.5P2O5：3.0La2O3:2SiO2：8Al2O3：25 Kaolin：60ZSM-5 | 800 |
| i | 0.2Ga2O3：0.3ZnO：1.5P2O5：3.0La2O3:2SiO2：8Al2O3：25 Kaolin：60ZSM-5 | 800 |
| j | 0.5Ga2O3：1.5P2O5：3.0La2O3:2SiO2：8Al2O3：25 Kaolin：60ZSM-5 | 800 |
| x | 0.5ZnO:1.5P2O5：3.0La2O3:10SiO2：25.0 Kaolin：60ZSM-5 | 800 |
| y | 0.5ZnO:1.5P2O5：3.0La2O3:10Al2O3：25.0 Kaolin：60ZSM-5 | 800 |
| z | 1.5P2O5：3.0La2O3:2SiO2：8Al2O3：25.5 Kaolin：60ZSM-5 | 800 |
[embodiment 2-10]
Embodiment 2～10, according to method same as Example 1 catalyst b～j, the composition row of catalyst are prepared
In table 1.
[comparative example 1]
With SiO2Replace the sial composite oxides in embodiment 6, the content of remaining component is identical, according to
The identical program technic of embodiment 6 prepares catalyst x.The evaluation methodology of catalyst x is adopted and the phase of embodiment 6
Same method evaluation.
[comparative example 2]
With Al2O3Replace the sial composite oxides in embodiment 6, the content of remaining component is identical, according to
The identical program technic of embodiment 6 prepares catalyst y.The evaluation methodology of catalyst y is adopted and the phase of embodiment 6
Same method evaluation.
[comparative example 3]
Dehydrogenation component ZnO is not introduced, using P same as Example 62O5、La2O3、SiO2、Al2O3
And zeolite content, catalyst z is prepared using program technic same as Example 6.The evaluation of catalyst z
Method adopts method evaluation same as Example 1.
[embodiment 11～14]
Embodiment 11～14 is obtained using catalyst a, change process conditions and raw material, reaction result is listed in table 3.
Table 2
| Embodiment | Catalyst | Ethylene+propylene+aromatics yield/% |
| 1 | a | 70.2 |
| 2 | b | 60.4 |
| 3 | c | 57.8 |
| 4 | d | 62.9 |
| 5 | e | 53.0 |
| 6 | f | 48.4 |
| 7 | g | 66.3 |
| 8 | h | 50.0 |
| 9 | i | 51.8 |
| 10 | j | 46.4 |
| Comparative example | ||
| 1 | x | 40.5 |
| 2 | y | 41.2 |
| 3 | z | 39.6 |
Table 3
Claims (10)
1. a kind of fluid catalyst for preparing alkene and aromatic hydrocarbons, in terms of parts by weight, comprising following components：
A) 0.5～10 part of P2O5；
B) 0.5～5 part is selected from ZnO, Ga2O3、Cr2O3Or MoO3In at least one；
C) 0～10 part is selected from rare earth oxide, Fe2O3Or Co2O3In at least one；
D) at least one in 20.0～55.0 parts of ZSM-5 or ZSM-11 zeolites；
E) 10.0～30.0 parts of sial composite oxides；
G) 25.0～60.0 parts of Kaolin.
2. the fluid catalyst for preparing alkene and aromatic hydrocarbons according to claim 1, it is characterised in that oxygen
Change at least one of the aluminum in Alumina gel or acidified alumina, the presoma of the oxide of P elements is selected from phosphoric acid
At least one of or the mixture of ammonium phosphate salt and mineral acid, rare earth oxide is selected from La2O3Or CeO2
In at least one.
3. the fluid catalyst for preparing alkene and aromatic hydrocarbons according to claim 1, it is characterised in that with
The percentage by weight meter of catalyst, selected from C) in component consumption be 1～5%.
4. the fluid catalyst for preparing alkene and aromatic hydrocarbons according to claim 1, it is characterised in that
In terms of the parts by weight of catalyst, P2O5Consumption be 1～6 part.
5. the fluid catalyst for preparing alkene and aromatic hydrocarbons according to claim 1, it is characterised in that institute
It is 10～800 with the silicon oxide of zeolite and the mol ratio of aluminium oxide.
6. the fluid catalyst for preparing alkene and aromatic hydrocarbons according to claim 1, it is characterised in that
With the weight ratio meter of sial composite oxides, selected from E) in the weight ratio of silicon oxide and aluminium oxide be (20:1)
～(1:20).
7. the fluid catalyst for preparing alkene and aromatic hydrocarbons according to claim 1, it is characterised in that system
The standby product based on propylene, the silicon oxide of zeolite used is 20～300 with the mol ratio of aluminium oxide.
8. a kind of method for preparing alkene and aromatic hydrocarbons, is 600～750 DEG C in reaction temperature with petroleum hydrocarbon as raw material,
The weight space velocity of petroleum hydrocarbon is 0.1～10h-1, reaction pressure is the weight ratio of 0.1～2.0MPa, petroleum hydrocarbon and water
For the fluid catalyst under 0.1～8.0 reaction condition, described in reaction raw materials and any one of claim 1～7
The reaction that contacts obtains the logistics containing ethylene, propylene and aromatic hydrocarbons.
9. the method for preparing alkene and aromatic hydrocarbons according to claim 8, it is characterised in that petroleum hydrocarbon is
The mixture of one or several in hydrocarbon component of the carbon number between 2～20.
10. the method for preparing alkene and aromatic hydrocarbons according to claim 8, it is characterised in that reaction temperature
For 650～700 DEG C, the weight space velocity of petroleum hydrocarbon is 0.3～5h-1, reaction pressure be 0～1.0MPa, petroleum hydrocarbon with
The weight ratio of water is 0.3～4.0.
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Cited By (1)
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| CN109364987A (en) * | 2018-11-29 | 2019-02-22 | 北京惠尔三吉绿色化学科技有限公司 | A kind of preparation method and application of the catalyst for the low-temperature catalyzed reaction propylene co-production aromatic hydrocarbons processed of lighter hydrocarbons |
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