CN104045499A - Method for producing aromatic hydrocarbons by utilization of ethene in refinery dry gas - Google Patents
Method for producing aromatic hydrocarbons by utilization of ethene in refinery dry gas Download PDFInfo
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- CN104045499A CN104045499A CN201310088416.9A CN201310088416A CN104045499A CN 104045499 A CN104045499 A CN 104045499A CN 201310088416 A CN201310088416 A CN 201310088416A CN 104045499 A CN104045499 A CN 104045499A
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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 discloses a method for producing aromatic hydrocarbons by the utilization of ethene in refinery dry gas. The method comprises the following steps: a refinery dry gas raw material containing ethene undergoes heat exchanged and/or is heated to 150-350 DEGC and enters a fixed bed reactor to contact and react with an aromatization catalyst; oil gas after the reaction enters a gas-liquid separation tank for gas-liquid separation; and gaseous products after gas-liquid separation enter a gas pipe network and liquid products enter an aromatic hydrocarbon separation tank for separation so as to obtain benzene, methylbenzene, dimethylbenzene and aromatic hydrocarbon products such as heavy aromatics and the like. A first heat exchanger is arranged between catalyst beds of the fixed bed reactor. By the method, technological process can be simplified; the refinery dry gas raw material requires no preliminary treatment; recovery rate of ethene in the dry gas is high; purity of aromatic hydrocarbons products is high; and aromatic hydrocarbons can be directly used as aromatic hydrocarbons products after separation.
Description
Technical field
The invention belongs to petrochemical industry, be particularly related to a kind of method of utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas, more particularly, be a kind ofly by oil refinery dry gas, to comprise that ethene in catalytic cracked dry gas, catalytic pyrolysis dry gas, coking dry gas and ethylene plant's tail gas produces the method for aromatic hydrocarbons through aromatization process.
Background technology
Catalytic cracking is the topmost course of processing of China's light materialization of heavy oil, and wherein contained ethene has utility value.At present, one of main path of some Petrochemical Enterprises dry gas utilizations is that ethylbenzene is produced in the reaction of dry gas and benzene, but a lot of refinery will catalysis drying gas sends into gas pipe network, is used as fuel gas, and some is even put into torch and burns, and has caused the waste of resource.Therefore, how to utilize ethene resource in dry gas to become one of problem that oil refining enterprise need to solve.
Light aromatics (benzene, toluene and dimethylbenzene) is important Organic Chemicals and stop bracket gasoline blend component, output and scale are inferior to ethene and propylene, although the output of China's light aromatics rises appreciably recently, China remains in the world one of main light aromatics breach state.Therefore, utilize oil refinery dry gas to produce aromatic hydrocarbons through aromatization process, can effectively utilize the ethene resource in dry gas, aromatic hydrocarbon product that again can production high added value, is a kind of effective mode of utilizing oil refinery dry gas.
US Patent No. P4, discloses the processing method that a kind of ethene of take dilution is waste ethylbenzene in 107,224, and its reaction conditions is: 290～450 ℃, and the weight hourly space velocity 0.1～100h of 0.1～100 normal atmosphere, charging
-1, benzene and ethylene molar ratio 1～30.Used catalyst is to contain ZSM-5 etc. to have the molecular sieve catalyst of selecting shape function.Rare ethene can, from refinery's device, as the dry gas of catalytic cracking unit, but need to remove sour gas H as before raw material
2s, CO
2and C
2above hydro carbons.
CN1051166A, CN1154957A disclose a kind of rare ethene and have reacted the technological process of producing ethylbenzene with benzene, CN1103637A discloses a kind of rare ethene and has reacted the technological process of producing methyl-ethyl benzene with toluene, this class patent feature is that temperature of reaction is at 290～450 ℃, reaction pressure is 0.1～2.5Mpa, benzene (or ethylbenzene) is 3.0～12.0 with ethylene molecule ratio, weight ethylene air speed 0.2～2.5h
-1processing condition under react with benzene (or ethylbenzene) and generate ethylbenzene (or to methyl-ethyl benzene), the plant catalytic cracking dry gas that this class process using contains low-concentration ethane is raw material, rare ethylene raw does not need to refine in advance, ethylbenzene (to methyl-ethyl benzene) selectivity high, but need to pass through, alkylation reaction, aromatic hydrocarbons (benzene) reclaim, ethylbenzene (to methyl-ethyl benzene) steams and take off several parts such as many ethylbenzene, technical process is complicated, need to consume the aroamtic hydrocarbon raw materials such as benzene or ethylbenzene.
Summary of the invention
The object of this invention is to provide a kind of method of utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas, main process is, under normal pressure or low-pressure state, ethene in oil refinery dry gas is directly generated to aromatic hydrocarbons through aromatization.Use the present invention can make technical process simplify, and have oil refinery dry gas raw material and anticipate without any, in dry gas, Recovery rate of ethylene is high, and aromatic hydrocarbon product purity is high, can be directly after separation as the feature of aromatic hydrocarbon product.
The invention provides a kind of method of utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas, it is characterized in that: the oil refinery dry gas raw material that contains ethene is through heat exchange and/or be heated to 150～350 ℃, preferably after 260～300 ℃, enter fixed-bed reactor and aromatized catalyst contact reacts, reacted oil gas enters knockout drum and carries out gas-liquid separation, after gas-liquid separation, gaseous product enters gas pipeline network, product liquid enters the separation of aromatic hydrocarbons knockout tower and obtains benzene, toluene, the aromatic hydrocarbon product such as dimethylbenzene and heavy aromatics, the beds of described fixed-bed reactor is loaded the section into n from top to bottom, n is 2～12, preferably 2～6, front n-1 section bed service temperature is between 240～550 ℃, and preferably, between 280～500 ℃, weight hourly space velocity is 0.1～15.0h
-1, preferred 2.0～10.0h
-1, n section bed service temperature is between 450～580 ℃, and preferably, between 480～550 ℃, weight hourly space velocity is 0.1～4.0h
-1, preferred 0.25～1.0h
-1, the ratio of first paragraph and n section loaded catalyst is 150: 1～1: 1, preferably 40: 1～8: 1, reactor pressure is between 0.1～1.0MPa, preferably between 0.1～0.4MPa, between the beds of described fixed-bed reactor, establish First Heat Exchanger, thereby reach the object that makes full use of reaction heat and control bed temperature.
The further technical characterictic of the present invention is: the heat exchange of described raw material is: first in the First Heat Exchanger between beds, carry out, again in the second interchanger with complete reaction after oil gas carry out heat exchange, reacted oil gas carries out gas-liquid separation with the laggard knockout drum of raw material heat exchange in the second interchanger.
Aromatization of the present invention aromatized catalyst used is mainly with metal-modified shape-selective molecular sieve catalyzer.Molecular sieve is HZSM-5, HZSM-7, HZSM-8, HZSM-11, HZSM-12, HZSM-35 or HZSM-48 etc., preferred HZSM-5, its content is 10～90 % by weight that account for total catalyst weight, preferably 30～75 % by weight, the silica alumina ratio of molecular sieve is 20～400, preferably 50～200; For molecular sieve modified metal, be Zn-Al, Ga-Zn, Zn-Re, Al-Re or Zn-Al-Re etc., its content (by metallic state, accounting for total catalyst weight) is 0.5～15.0 % by weight, preferably 2.0～10.0 % by weight.Also available other have the aromatized catalyst of aromizing function.
The effect that the present invention compared with prior art has is: 1) in oil refinery dry gas, the aromatization process of ethene is thermopositive reaction, reactor batch temperature raises from top to bottom gradually, the present invention adopts First Heat Exchanger is set between reactor bed, reaction raw materials carries out heat exchange in First Heat Exchanger, and can carry out heat exchange with reacted oil gas, make temperature can reach raw material preheating temperature requirement or only need a little heating can reach raw material preheating temperature requirement, reaction heat is fully used; 2) catalyst segments in fixed-bed reactor of the present invention is loaded, difference by each section of loaded catalyst has obtained each section of different reaction velocity when heavy, thereby can better control in dry gas ethene at reaction conversion ratio and the reaction depth of each section, and then effectively control reaction temperature rising.
By the drawings and specific embodiments, describe the present invention in detail below, but do not limit the scope of the invention.
Accompanying drawing explanation
Fig. 1 is the simple flow chart that a kind of oil refinery dry gas of the present invention is produced aromatic hydrocarbons.
Reference numeral shown in figure is:
1-dry gas raw material, 2-First Heat Exchanger, 3-the second interchanger, 4-process furnace, 5-aromatization reactor, 6-knockout drum, 7-gaseous product, 8-product liquid, 9-aromatic hydrocarbons knockout tower, 10-benzene, 11-toluene, 12-dimethylbenzene, 13-heavy aromatics, 14-first paragraph beds, 15-second segment beds.
Embodiment
As shown in Figure 1: wherein: in Fig. 1, beds is segmented into two sections.Oil refinery dry gas raw material 1 first enters First Heat Exchanger 2 and the second interchanger 3 carries out heat exchange, oil refinery dry gas raw material 1 after heat exchange enter again process furnace 4 heat (or through process furnace by and process furnace do not heat), be heated to 150～350 ℃, preferably enter aromatization reactor 5 after 260～300 ℃ and carry out aromatization, aromatization reaction products is after the second interchanger 3 and 1 heat exchange of oil refinery dry gas raw material, through knockout drum 6, carry out separation, isolate gaseous product 7 and product liquid 8, gaseous product 7 goes out device and enters gas pipeline network, product liquid 8 enters aromatic hydrocarbons knockout tower 9 and isolates benzene 10, toluene 11, dimethylbenzene 12 and heavy aromatics (C
9 +) 13 aromatic hydrocarbon products such as grade.
Described aromatization reactor 5 internal pressures are between 0.1～1.0MPa, preferably between 0.1～0.4MPa.
The bed service temperature of described first paragraph beds 14 is between 240～550 ℃, and preferably, between 280～500 ℃, weight hourly space velocity is 0.1～15.0h
-1, preferred 2.0～10.0h
-1; The service temperature of second segment beds 15 is between 450～580 ℃, and preferably, between 480～550 ℃, weight hourly space velocity is 0.1～4.0h
-1, preferred 0.25～1.0h
-1; Between first paragraph beds 14 and second segment beds 15, the ratio of loaded catalyst is 150: 1～1: 1, preferably 40: 1～8: 1.
Below by embodiment, further illustrate the present invention, but therefore do not limit the present invention.Processing condition and the catalyzer of other each operating units of the present invention except aromizing unit are conventional, and concrete selection can be determined by the general knowledge of association area according to the requirement of the character of raw material, product etc.
Embodiment 1
Get commercially available silica alumina ratio and be 737 grams, 60 HZSM-5 molecular sieve, add with containing 85 grams of Zn (NO
3)
2solution 800ml in, fast making beating is stirred, and exchanges 2.5 hours at 40 ℃, filters slurries, filter cake after washing at 110 ℃ dry 3 hours, at 500 ℃, roasting is 3 hours, adds containing 78 grams of Al after pulverizing
2(SO
4)
3solution 800ml in, fast making beating is stirred, and exchanges 2.5 hours at 40 ℃, filters slurries, filter cake after washing at 110 ℃ dry 3 hours, after pulverizing and 483 grams of commercially available aluminium hydrate powders mix, add HNO
3concentration is 8 % by weight solution 500ml, stirs, mediates rear extruded moulding, at 110 ℃, is dried 3 hours, and at 500 ℃, roasting obtains catalyzer a for 6 hours.Press butt and calculate and instrumental analysis, catalyzer is containing 70.0 % by weight HZSM-5 molecular sieves, 2.8 % by weight Zn and 1.2 % by weight Al.
Embodiment 2～5
Embodiment 2～5 has provided the effect example that a kind of catalytic cracked dry gas aromizing is produced aromatic hydrocarbons, and wherein, in fixed bed aromatization reactor, beds is divided into 4 sections; Embodiment 2～4 aromatized catalyst used is catalyzer a prepared by laboratory, and embodiment 5 aromatized catalyst used is commercially available aromatized catalyst m, and its main character is in Table 1.The character of catalytic cracked dry gas raw material is in Table 2, and aromatization condition and reaction result are in Table 3, and the distribution of aromizing product liquid composition and character are in Table 4.
Embodiment 6～9
Embodiment 6～9 has provided the effect example that a kind of catalytic cracked dry gas aromizing is produced aromatic hydrocarbons, and wherein, in fixed bed aromatization reactor, beds is divided into 2 sections; Embodiment 6～8 aromatized catalyst used is catalyzer a prepared by laboratory, and embodiment 9 aromatized catalyst used is certain commercially available aromatized catalyst m, and its main character is in Table 1.The character of catalytic cracked dry gas raw material is in Table 2, and aromatization condition and reaction result are in Table 5, and the distribution of aromizing product liquid composition and character are in Table 6.
Table 1 aromatized catalyst main character
| Project | Embodiment 1～3 | Embodiment 4 |
| Catalyst shape | White strip | White strip |
| Bulk density/kg.m -3 | 690 | 820 |
| Specific surface area/m 2.g -1 | 285 | 305 |
| Pore volume/cm 3.g -1 | 0.22 | 0.28 |
| Crushing strength/N.cm -1 | 103 | 83 |
Table 2 catalytic cracked dry gas feedstock property
| FCC dry gas forms | Weight fraction, % | Molar fraction, % |
| H 2 | 1.91 | 20.22 |
| CH 4 | 20.72 | 27.43 |
| C 2H 6 | 19.80 | 13.98 |
| C 2H 4 | 16.95 | 12.82 |
| C 3 | 3.53 | 1.53 |
| C 4 | 2.14 | 1.26 |
| C 5 + | 0.46 | 0.13 |
| N 2 | 21.44 | 16.22 |
| CO | 1.34 | 0.79 |
| CO 2 | 11.71 | 5.62 |
Table 3 embodiment 2～5 aromatization condition and reaction results
The character of table 4 embodiment 2～5 liquid and composition distribute
Table 5 embodiment 6～9 aromatization condition and reaction results
The character of table 6 embodiment 6～9 liquid and composition distribute
Claims (7)
1. a method of utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas, it is characterized in that: the oil refinery dry gas raw material that contains ethene is through heat exchange and/or be heated to 150～350 ℃ and enter fixed-bed reactor and aromatized catalyst contact reacts, reacted oil gas enters knockout drum and carries out gas-liquid separation, after gas-liquid separation, gaseous product enters gas pipeline network, product liquid enters the separation of aromatic hydrocarbons knockout tower and obtains the aromatic hydrocarbon products such as benzene,toluene,xylene and heavy aromatics, the beds of described fixed-bed reactor is loaded the section into n from top to bottom, and n is 2～12; Front n-1 section bed service temperature is between 240～550 ℃, and weight hourly space velocity is 0.1～15.0h
-1; N section bed service temperature is between 450～580 ℃, and weight hourly space velocity is 0.1～4.0h
-1; The ratio of first paragraph and n section loaded catalyst is 150: 1～1: 1; Reactor pressure is between 0.1～1.0MPa; Between the beds of described fixed-bed reactor, establish First Heat Exchanger.
2. the method for utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas according to claim 1, it is characterized in that: the heat exchange of described raw material is first carried out in the First Heat Exchanger between beds, in the second interchanger, carry out heat exchange with reacted oil gas again, reacted oil gas carries out gas-liquid separation with the laggard knockout drum of raw material heat exchange in the second interchanger.
3. the method for utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas according to claim 1, it is characterized in that: described in contain ethene oil refinery dry gas raw material through heat exchange and/or be heated to after 260～300 ℃, enter fixed-bed reactor and aromatized catalyst contact reacts.
4. the method for utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas according to claim 1 and 2, is characterized in that: described front n-1 section bed service temperature is between 280～500 ℃, and weight hourly space velocity is 2.0～10.0h
-1; N section bed service temperature is between 480～550 ℃, and weight hourly space velocity is 0.25～1.0h
-1; The ratio of first paragraph and n section loaded catalyst is 40: 1～8: 1; Reactor pressure is between 0.1～0.4MPa.
5. the method for utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas according to claim 1 and 2, is characterized in that: the beds of described fixed-bed reactor is loaded the section into n from top to bottom, and n is 2～6.
6. the method for utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas according to claim 5, is characterized in that: described front n-1 section bed service temperature is between 240～550 ℃, and weight hourly space velocity is 0.1～15.0h
-1; N section bed service temperature is between 450～580 ℃, and weight hourly space velocity is 0.1～4.0h
-1; The ratio of first paragraph and n section loaded catalyst is 150: 1～1: 1; Reactor pressure is between 0.1～1.0MPa.
7. the method for utilizing ethylene production aromatic hydrocarbons in oil refinery dry gas according to claim 6, is characterized in that: described front n-1 section bed service temperature is between 280～500 ℃, and weight hourly space velocity is 2.0～10.0h
-1; N section bed service temperature is between 480～550 ℃, and weight hourly space velocity is 0.25～1.0h
-1; The ratio of first paragraph and n section loaded catalyst is 40: 1～8: 1; Reactor pressure is between 0.1～0.4MPa.
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Cited By (5)
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| CN105728017A (en) * | 2014-12-08 | 2016-07-06 | 中国科学院大连化学物理研究所 | Preparation method and use of binder-free ZSM11 molecular sieve catalyst |
| CN106117003A (en) * | 2016-06-14 | 2016-11-16 | 中国石油大学(华东) | A kind of method that ethylene in oil refinery dry gas is converted into aromatic hydrocarbons |
| CN106190272A (en) * | 2016-08-24 | 2016-12-07 | 北京惠尔三吉绿色化学科技有限公司 | A kind of catalysis drying gas aromatisation gasoline shell and tube reactor |
| CN109321268A (en) * | 2018-11-15 | 2019-02-12 | 中国科学院山西煤炭化学研究所 | A kind of Fischer-Tropsch process exhaust prepares the method and device thereof of gasoline and aromatic hydrocarbons |
| CN112831348A (en) * | 2020-12-30 | 2021-05-25 | 宁夏宝利科技设计研究院有限公司 | Mixed light hydrocarbon modification process method and system |
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| Publication number | Priority date | Publication date | Assignee | Title |
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