CN104045499B - A kind of utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas - Google Patents
A kind of utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas Download PDFInfo
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Abstract
The invention discloses and a kind of utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas.The steps include: that the oil refinery dry gas raw material containing ethylene through heat exchange and/or is heated to 150～350 DEG C of entrance fixed bed reactors and aromatized catalyst haptoreaction, 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 aromatic hydrocarbon products such as aromatics seperation tower isolated benzene,toluene,xylene and heavy aromatics, sets First Heat Exchanger between the beds of described fixed bed reactors.Using the present invention that technological process can be made to simplify, and have oil refinery dry gas raw material and anticipate without any, in dry gas, Recovery rate of ethylene is high, aromatic hydrocarbon product purity height, can the most separated after as the feature of aromatic hydrocarbon product.
Description
Technical field
The invention belongs to petrochemical industry, utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas particularly to a kind of,
More specifically, it is that one includes catalytic cracked dry gas, catalytic pyrolysis dry gas, coking dry gas and ethylene plant's tail by oil refinery dry gas
The method that in gas, ethylene produces aromatic hydrocarbons through aromatization process.
Background technology
Catalytic cracking is the topmost course of processing of China's light materialization of heavy oil, the great value of ethylene contained therein.
At present, one of main path that some Petrochemical Enterprises dry gas utilize is dry gas and benzene reaction production ethylbenzene, but a lot of refinery will
Catalysis drying gas is sent into gas pipe network and is used as fuel gas, and some is even put into torch and burns, and causes the waste of resource.Therefore, as
What utilizes the ethylene resource in dry gas to become one of oil refining enterprise's problem needing solution.
Light aromatics (benzene, toluene and dimethylbenzene) is important Organic Chemicals and high-knock rating gasoline blend component,
Yield and scale are inferior to ethylene and propylene, although the yield of China's light aromatics rises appreciably recently, but China remains generation
One of main in boundary light aromatics breach state.Therefore, utilize oil refinery dry gas to produce aromatic hydrocarbons through aromatization process, can be effectively sharp
By the ethylene resource in dry gas, the aromatic hydrocarbon product of high added value can be produced again, be a kind of effective to utilize oil refinery dry gas
Mode.
United States Patent (USP) USP4, discloses a kind of process being waste ethylbenzene with the ethylene of dilution in 107,224,
Its reaction condition is: 290～450 DEG C, 0.1～100 atmospheric pressure, the weight (hourly) space velocity (WHSV) 0.1～100h of charging-1, benzene and ethylene molar
Ratio 1～30.Used catalyst is the molecular sieve catalyst containing ZSM-5 etc. with shape-selective function.Dilute ethylene may be from refinery's dress
Put, such as the dry gas of catalytic cracking unit, but needed to remove sour gas H before as raw material2S、CO2And C2Above hydro carbons.
CN1051166A, CN1154957A disclose a kind of dilute ethylene and react the technical process producing ethylbenzene with benzene,
CN1103637A discloses a kind of dilute ethylene and reacts with toluene and produce the technical process to methyl-ethyl benzene, and this kind of patent feature is anti-
Answering temperature at 290～450 DEG C, reaction pressure is 0.1～2.5Mpa, and benzene (or ethylbenzene) is 3.0～12.0 with ethylene molecule ratio, second
Alkene weight space velocity 0.2～2.5h-1Process conditions under with benzene (or ethylbenzene) carry out reaction generate ethylbenzene (or to methyl-ethyl benzene), this
Class technique uses the refinery catalytic cracking dry gas containing low-concentration ethane to be raw material, and dilute ethylene raw need not refine in advance, second
Benzene (to methyl-ethyl benzene) selectivity high, but need through alkylation reaction, aromatic hydrocarbons (benzene) recovery, ethylbenzene (to methyl-ethyl benzene)
Steaming and take off several parts such as many ethylbenzene, technological process is complicated, needs to consume the aroamtic hydrocarbon raw material such as benzene or ethylbenzene.
Summary of the invention
It is an object of the invention to provide and a kind of utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas, main process is often
Under pressure or low-pressure state, ethylene in oil refinery dry gas is directly generated aromatic hydrocarbons through aromatization.Use the present invention can make technique stream
Journey is simplified, and has oil refinery dry gas raw material and anticipate without any, and in dry gas, Recovery rate of ethylene is high, aromatic hydrocarbon product purity
Height, can the most separated after as the feature of aromatic hydrocarbon product.
The present invention provides a kind of and utilizes the method for ethylene production aromatic hydrocarbons in oil refinery dry gas, it is characterised in that: containing ethylene
Oil refinery dry gas raw material is through heat exchange and/or is heated to 150～350 DEG C, after preferably 260～300 DEG C, enters fixed bed reactors and virtue
Structure catalyst haptoreaction, reacted oil gas enters knockout drum and carries out gas-liquid separation, and after gas-liquid separation, gaseous product enters
Entering gas pipeline network, product liquid enters the aromatic hydrocarbon products such as aromatics seperation tower isolated benzene,toluene,xylene and heavy aromatics, described
The beds of fixed bed reactors loads as n section from top to bottom, and n is 2～12, preferably 2～6；Front n-1 section bed operation temperature
Degree is between 240～550 DEG C, and between preferably 280～500 DEG C, weight (hourly) space velocity (WHSV) is 0.1～15.0h-1, preferably 2.0～10.0h-1；
N-th section of bed operating temperature is between 450～580 DEG C, and between preferably 480～550 DEG C, weight (hourly) space velocity (WHSV) is 0.1～4.0h-1, excellent
Select 0.25～1.0h-1；The ratio of first paragraph and n-th section of loaded catalyst is 150: 1～1: 1, preferably 40: 1～8: 1；Reaction
In device, pressure is between 0.1～1.0MPa, between preferably 0.1～0.4MPa；The beds of described fixed bed reactors it
Between set First Heat Exchanger, thus reach make full use of reaction heat and control the purpose of bed temperature.
The present invention is technically characterized in that the heat exchange of described raw material is further: first first between beds is changed
Carrying out in hot device, then carry out heat exchange with complete reacted oil gas in the second heat exchanger, reacted oil gas is in the second heat exchange
Gas-liquid separation is carried out with the laggard knockout drum of raw material heat exchange in device.
Aromatized catalyst used by aromatization of the present invention is mainly urged with metal-modified shape-selective molecular sieve
Agent.Molecular sieve is HZSM-5, HZSM-7, HZSM-8, HZSM-11, HZSM-12, HZSM-35 or HZSM-48 etc., preferably
HZSM-5, its content is 10～90 weight % accounting for total catalyst weight, and preferably 30～75 weight %, the silica alumina ratio of molecular sieve is
20～400, preferably 50～200；It is Zn-Al, Ga-Zn, Zn-Re, Al-Re or Zn-Al-Re for molecular sieve modified metal
Deng, its content (based on metallic state, account for total catalyst weight) is 0.5～15.0 weight %, preferably 2.0～10.0 weight %.Also
Other are can use to have the aromatized catalyst of aromatisation function.
The present invention compared with prior art has the effect that 1) in oil refinery dry gas the aromatization process of ethylene for putting
Thermal response, reactor batch temperature gradually rises from top to bottom, and the present invention uses and arranges the first heat exchange between reactor bed
Device, reaction raw materials carries out heat exchange in First Heat Exchanger, and can carry out heat exchange with reacted oil gas, makes temperature can reach former
Material preheating temperature requirement or have only to heat a little and i.e. can reach raw material preheating temperature requirement, makes reaction heat obtain abundant profit
With；2) catalyst segments in fixed bed reactors of the present invention loads, and is obtained by the difference of each section of loaded catalyst
Each section different heavy time reaction velocity, such that it is able to preferably control ethylene in dry gas in the reaction conversion ratio of each section and reaction
The degree of depth, and then effectively control reaction temperature rising.
Describe the present invention in detail by the drawings and specific embodiments 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 produces aromatic hydrocarbons.
Reference shown in figure is:
1-dry gas raw material, 2-First Heat Exchanger, 3-the second heat exchanger, 4-heating furnace, 5-aromatization reactor, 6-gas-liquid is divided
From tank, 7-gaseous product, 8-product liquid, 9-aromatics seperation tower, 10-benzene, 11-toluene, 12-dimethylbenzene, 13-heavy aromatics, 14-
First paragraph beds, 15-second segment beds.
Detailed description of the invention
As shown in Figure 1: wherein: in Fig. 1, beds is segmented into two sections.First oil refinery dry gas raw material 1 enters the first heat exchange
Device 2 and the second heat exchanger 3 carry out heat exchange, and the oil refinery dry gas raw material 1 after heat exchange enters heating furnace 4 again and carries out heating (or heated stove
By and heating furnace does not heats), be heated to 150～350 DEG C, after preferably 260～300 DEG C enter aromatization reactor 5 carry out virtue
Structureization is reacted, and aromatization reaction products, after the second heat exchanger 3 with oil refinery dry gas raw material 1 heat exchange, is carried out point through knockout drum 6
From, isolate gaseous product 7 and product liquid 8, gaseous product 7 goes out device and enters gas pipeline network, and product liquid 8 enters aromatic hydrocarbons and divides
Benzene 10, toluene 11, dimethylbenzene 12 and heavy aromatics (C is isolated from tower 99 +) 13 aromatic hydrocarbon products such as grade.
In described aromatization reactor 5, pressure is between 0.1～1.0MPa, between preferably 0.1～0.4MPa.
The bed operating temperature of described first paragraph beds 14 between 240～550 DEG C, preferably 280～500 DEG C it
Between, weight (hourly) space velocity (WHSV) is 0.1～15.0h-1, preferably 2.0～10.0h-1；The operation temperature of second segment beds 15 450～
Between 580 DEG C, between preferably 480～550 DEG C, weight (hourly) space velocity (WHSV) is 0.1～4.0h-1, preferably 0.25～1.0h-1；First paragraph is catalyzed
Between agent bed 14 and second segment beds 15, the ratio of loaded catalyst is 150: 1～1: 1, preferably 40: 1～8: 1.
Further illustrate the present invention below by embodiment, but and be not so limited the present invention.The present invention removes aromatisation list
Process conditions and the catalyst of other each operating units outside unit are conventional, specifically chosen can be according to the character of raw material, product
The requirements of product etc. are determined by the general knowledge of association area.
Embodiment 1
Take 737 grams of the HZSM-5 molecular sieve that commercially available silica alumina ratio is 60, add with containing 85 grams of Zn (NO3)2Solution 800ml in,
Quickly pulling an oar stirring, exchange 2.5 hours at 40 DEG C, filter serosity, filter cake is dried 3 hours after washing at 110 DEG C,
Roasting 3 hours at 500 DEG C, add containing 78 grams of Al after pulverizing2(SO4)3Solution 800ml in, stirring of quickly pulling an oar, at 40 DEG C
Exchanging 2.5 hours, filter serosity, filter cake is dried 3 hours after washing at 110 DEG C, with commercially available aluminium hydrate powder after pulverizing
483 grams of mix homogeneously, add HNO3Concentration is 8 weight % solution 500ml, be stirred, mediate after extruded moulding, at 110 DEG C
Under be dried 3 hours, at 500 DEG C, roasting obtains catalyst a in 6 hours.Calculating and Instrumental Analysis by butt, catalyst contains 70.0 weights
Amount %HZSM-5 molecular sieve, 2.8 weight %Zn and 1.2 weight %Al.
Embodiment 2～5
Embodiment 2～5 gives the example effects that a kind of catalytic cracked dry gas aromatisation produces aromatic hydrocarbons, wherein, fixed bed
In aromatization reactor, beds is divided into 4 sections；Aromatized catalyst used by embodiment 2～4 is catalysis prepared by laboratory
Agent a, aromatized catalyst used by embodiment 5 is commercially available aromatized catalyst m, and its main character is shown in Table 1.Catalytic cracked dry gas is former
The character of material is shown in Table 2, and aromatization condition and reaction result are shown in Table 3, and the composition distribution of aromatisation product liquid and character are shown in Table
4。
Embodiment 6～9
Embodiment 6～9 gives the example effects that a kind of catalytic cracked dry gas aromatisation produces aromatic hydrocarbons, wherein, fixed bed
In aromatization reactor, beds is divided into 2 sections；Aromatized catalyst used by embodiment 6～8 is catalysis prepared by laboratory
Agent a, aromatized catalyst used by embodiment 9 is certain commercially available aromatized catalyst m, and its main character is shown in Table 1.Catalytic cracked dry gas
The character of raw material is shown in Table 2, and aromatization condition and reaction result are shown in Table 5, and the composition distribution of aromatisation product liquid and character are shown 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/m2.g-1 | 285 | 305 |
| Pore volume/cm3.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, % |
| H2 | 1.91 | 20.22 |
| CH4 | 20.72 | 27.43 |
| C2H6 | 19.80 | 13.98 |
| C2H4 | 16.95 | 12.82 |
| C3 | 3.53 | 1.53 |
| C4 | 2.14 | 1.26 |
| C5 + | 0.46 | 0.13 |
| N2 | 21.44 | 16.22 |
| CO | 1.34 | 0.79 |
| CO2 | 11.71 | 5.62 |
Table 3 embodiment 2～5 aromatization condition and reaction result
The character of table 4 embodiment 2～5 liquid and composition distribution
Table 5 embodiment 6～9 aromatization condition and reaction result
The character of table 6 embodiment 6～9 liquid and composition distribution
Claims (6)
1. one kind utilizes the method for ethylene production aromatic hydrocarbons in oil refinery dry gas, it is characterised in that: the oil refinery dry gas raw material containing ethylene
Through heat exchange and/or be heated to 150～350 DEG C of entrance fixed bed reactors and aromatized catalyst haptoreaction, reacted oil
Gas enters knockout drum and carries out gas-liquid separation, and after gas-liquid separation, gaseous product enters gas pipeline network, and product liquid enters aromatics seperation
The aromatic hydrocarbon products such as tower isolated benzene,toluene,xylene and heavy aromatics, the beds of described fixed bed reactors to
Lower filling is n section, and n is 2～12；Front n-1 section bed operating temperature between 240～550 DEG C, weight (hourly) space velocity (WHSV) be 0.1～
15.0h-1；N-th section of bed operating temperature is between 450～580 DEG C, and weight (hourly) space velocity (WHSV) is 0.1～4.0h-1；First paragraph and n-th section
The ratio of loaded catalyst is 150: 1～1: 1；Reactor pressure is between 0.1～1.0MPa；Described fixed bed reactors
Beds between set First Heat Exchanger.
The most according to claim 1 utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas, it is characterised in that: described raw material
Heat exchange first First Heat Exchanger between beds in carry out, then carry out with reacted oil gas in the second heat exchanger
Heat exchange, reacted oil gas knockout drum laggard with raw material heat exchange in the second heat exchanger carries out gas-liquid separation.
The most according to claim 1 utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas, it is characterised in that: described contain
The oil refinery dry gas raw material of ethylene, after heat exchange and/or being heated to 260～300 DEG C, enters fixed bed reactors and Aromatizatian catalytic
Agent haptoreaction.
The most according to claim 1 and 2 utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas, it is characterised in that: described
Front n-1 section bed operating temperature is between 280～500 DEG C, and weight (hourly) space velocity (WHSV) is 2.0～10.0h-1；N-th section of bed operating temperature exists
Between 480～550 DEG C, weight (hourly) space velocity (WHSV) is 0.25～1.0h-1；The ratio of first paragraph and n-th section of loaded catalyst is 40: 1～8
∶1；Reactor pressure is between 0.1～0.4MPa.
The most according to claim 1 and 2 utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas, it is characterised in that: described
The beds of fixed bed reactors loads as n section from top to bottom, and n is 2～6.
The most according to claim 1 utilize the method for ethylene production aromatic hydrocarbons in oil refinery dry gas, it is characterised in that: described front n-
1 section of bed operating temperature is between 280～500 DEG C, and weight (hourly) space velocity (WHSV) is 2.0～10.0h-1；N-th section of bed operating temperature is 480
～between 550 DEG C, weight (hourly) space velocity (WHSV) is 0.25～1.0h-1；The ratio of first paragraph and n-th section of loaded catalyst is 40: 1～8: 1；
Reactor pressure is between 0.1～0.4MPa.
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Families Citing this family (5)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN105728017B (en) * | 2014-12-08 | 2018-07-10 | 中国科学院大连化学物理研究所 | A kind of preparation and application of 1 molecular sieve catalyst of binderless ZSM-11 |
| 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 |
| CN109321268B (en) * | 2018-11-15 | 2019-12-06 | 中国科学院山西煤炭化学研究所 | Method and device for preparing gasoline and aromatic hydrocarbon from Fischer-Tropsch synthesis tail gas |
| CN112831348B (en) * | 2020-12-30 | 2022-07-19 | 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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