CN103772126A - Combined method for preparing ethylbenzene by using refinery dry gas as raw material - Google Patents
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- CN103772126A CN103772126A CN201210413453.8A CN201210413453A CN103772126A CN 103772126 A CN103772126 A CN 103772126A CN 201210413453 A CN201210413453 A CN 201210413453A CN 103772126 A CN103772126 A CN 103772126A
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- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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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
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- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Abstract
A combined method for preparing ethylbenzene by using a refinery dry gas as a raw material comprises the following steps: alkylation: allowing ethylene and benzene in the raw materials to react to generate ethylbenzene, and unreacted ethane and others to enter an alkylation exhaust; 2, pressure swing adsorption PSA: allowing the C2 component in the alkylation exhaust to enter into a PSA concentrated gas after being subjected to separating and desorbing of methane, hydrogen and the like; 3, ethane cracking: allowing the PSA concentrated gas to perform pyrolysis to generate ethylene, hydrogen and other components, allowing the pyrolysis gas to enter into an oil absorption device after passing through a waste heat boiler and a quenched water tower for temperature reduction; 4, absorbing down C3 and the component containing more C in the pyrolysis gas subjected to oil absorption, obtaining the concentrated gases of C2 at the top of an absorption tower, including methane, hydrogen, ethane, ethylene light components; 5, selective hydrogenization: feeding hydrogenised concentrated gases of C2 into a decarbonizing unit and a refinery dry gas in the step 1 for mixing, desorbing the acidic gas, and then feeding the obtained gas to an alkylation device for cyclic utilization. The method solves the problems that the raw material is single and low in utilization ratio in the prior art and is a new combined method for preparing the ethylbenzene.
Description
Technical field
The present invention relates to a kind of technical field take oil refinery dry gas as waste ethylbenzene, specifically, relate to a kind of benzene absorption process that adopts and reclaim ethene in oil refinery dry gas and ethane the combined method for the preparation of ethylbenzene.
Background technology
In oil refinery dry gas, contain ethene, ethane.Oil refinery dry gas is burnt mainly as fuel at present, and utility value is lower.Ethylene recovery in dry gas can be made to rare ethene, be sent to hydrocarbonylation device and make raw material, as Benzene Device is prepared ethylbenzene or preparation to methyl-ethyl benzene etc.
The method that reclaims at present ethene from oil refinery dry gas mainly contains separation by deep refrigeration, oil-absorption process, Separation by Complexation method, pressure swing adsorption process etc., and the whole bag of tricks differs from one another.Separation by deep refrigeration technical maturity, Recovery rate of ethylene is high, but investment is large, and higher for rare ethylene recovery energy consumption; Separation by Complexation method, Recovery rate of ethylene is higher, but the impurity in raw material is required strictly, and pre-treatment expense is higher, needs special complexes absorption; Pressure swing adsorption process energy consumption is lower, but product purity is low, and Recovery rate of ethylene is low, and floor space is large; Oil-absorption process has the features such as small scale, strong adaptability, investment cost be low.
Ethylbenzene is a kind of important industrial chemicals.Along with the development of petrochemical processing industry, the refinery exhaust that contains in a large number low-concentration ethane provides new raw material sources for producing ethylbenzene.
From the fifties end, developed several take rare ethene as raw material and benzene produce the method for ethylbenzene.
As patents such as U.S. Pat 2939890, US3691245, US3702886.CN90109803.5 discloses a kind of rare ethene and has reacted the technological process of producing ethylbenzene with benzene, and raw materials used is the plant catalytic cracking dry gas that contains low-concentration ethane, does not need to refine in advance and directly reacts and produce ethylbenzene with benzene.
It is raw material that CN1154957 discloses a kind of plant catalytic cracking dry gas containing low-concentration ethane, directly reacts with benzene and produces improving one's methods of ethylbenzene.
Because of in oil refinery dry gas only in catalysis drying gas ethylene content higher, so these patents are only applicable to rare ethene that raw material is catalysis drying gas, and have only utilized the ethylene component in rare ethene, do not add utilization for ethane.
There is the problem that raw material is single and utilization ratio is not high in the technique that existing rare ethene take oil refinery dry gas is produced ethylbenzene as raw material and benzene.
Summary of the invention
The present invention produces as raw material and benzene the problem that raw material is single and utilization ratio is not high that ethylbenzene process exists in order to solve existing rare ethene take oil refinery dry gas, proposes a kind of efficient employing oil refinery dry gas and produce the combination process of ethylbenzene.Present method has combined the technology such as ethane cracking, oily absorption, alkylation, pressure-variable adsorption, and the ethene in oil refinery dry gas, ethane component are used.
The combined method of producing ethylbenzene with oil refinery dry gas of the present invention is achieved in that
Method of the present invention comprises the following steps:
1. alkylation: oil refinery dry gas enters alkyl plant after decarburization unit removes sour gas, ethene wherein reacts with benzene and generates ethylbenzene, and the components such as unreacted ethane enter in hydrocarbonylation tail gas;
2. pressure-variable adsorption: the hydrocarbonylation tail gas from alkyl plant enters pressure-swing absorption apparatus, carbon two components in this hydrocarbonylation tail gas, after the components such as separation removal methane, hydrogen, enter in PSA concentrated gas, send into afterwards pyrolyzer;
3. ethane cracking: the PSA concentrated gas from pressure-swing absorption apparatus enters ethane cracking furnace, carries out cracking at this and generates the components such as ethene, hydrogen, and the splitting gas obtaining enters oily absorption unit after waste heat boiler and quenching water column cooling;
4. oil absorbs: splitting gas from quenching water column is compressed, enter oil-absorption tower after imurity-removal, and it is absorption agent that oil-absorption tower adopts benzene or gasoline; Carbon three and above component in splitting gas are absorbed, and obtain comprising the carbon two concentrate gas of methane, hydrogen, ethane, vinyl light constituent at absorption tower top;
5. select hydrogenation: the alkynes in carbon two concentrate gas reacts with hydrogen at this and is removed, carbon two concentrate gas after hydrogenation are admitted to the decarburization unit in described step 1), mix with oil refinery dry gas, remove sour gas wherein, then send into alkyl plant and carry out recycle.
Described oil refinery dry gas is selected from catalytic cracked dry gas, catalytic pyrolysis dry gas, often one or more mixing of reducing pressure in dry gas, coking dry gas, hydrocracking dry gas;
Alkyl plant in described step (1) is selected from the one in following alkylation reaction technique known in the state of the art: fixed-bed reactor, catalytic distillation tower technology; Preferred alkylation is the method for disclosed pure ethylene or dry gas and producing phenylethane from alkylation of benzene in CN200910057824.1.
Very count by weight,
Hydrocarbonylation tail gas in described step (1) comprises 0～20% hydrogen, 20～50% methane and 20～50% ethane, and the content sum of each component is no more than 100%.
In step (2), in described PSA concentrated gas, ethane content is 50～95%.
In step (3),
Described ethane cracking furnace is ethane cracking furnace well known in the prior art or light hydrocarbon cracking stove;
Described pyrolyzer temperature out is 500～700 ℃, pressure 0.05～0.15MPa.G;
In ethane cracking furnace, ethane in the PSA concentrated gas scission reaction that reacts obtains comprising the splitting gas of following component: the hydrogen of 0～10%wt, the methane of 0～20%wt, the ethene of 20～50%wt and the ethane of 0～20%wt, and the content sum of each component is no more than 100%;
Described splitting gas, after cooling and heat recovery and utilization, is sent into oily absorption unit.
In step 4),
Described oily absorption unit, comprises compressor, oil-absorption tower and desorption tower;
The absorption temperature of described oil-absorption tower is 10～40 ℃, and absorption pressure is 0.5～2.0MPa.G; Wherein the rate of recovery of ethene is not less than 90%.
In step 5),
Described selective hydrogenation catalyst is disclosed acetylene selective hydrogenation catalyst in CN200910082421.2, and wherein main active ingredient is selected from one or both of Pt, Pd, and content is 0.01 % by weight～1.0 % by weight; Help active ingredient to comprise VIII family element, at least one in ⅠⅠ B family element Bi, Sb, Pb, In, Cs, Rb, its content is 0～20 % by weight of carrier gross weight;
The operational condition of described hydrogenation reaction is: reactor inlet temperature is generally 20～150 ℃, and reaction pressure is generally 1.0～5.0MPa, and the mol ratio of hydrogen and alkynes is 0.8～4.0, and air speed is generally 5000～20000h
-1.
The combination process of producing ethylbenzene with oil refinery dry gas of the present invention has following characteristics:
(1) in combination process of the present invention, can multiple oil refinery dry gas be raw material, this technique limit the catalysis drying gas that raw material is refinery, and raw material is applied widely;
(2) in combination process of the present invention, in hydrocarbonylation device, in oil refinery dry gas, ethene and benzene react and produce ethylbenzene, ethane component in dry gas enters hydrocarbonylation tail gas,, pyrolyzer cracking concentrated through PSA technology generates ethene, oil absorbs after concentrate, still the raw material that can be used as hydrocarbonylation device continues to react and produce ethylbenzene with benzene, and in oil refinery dry gas, each component is fully used, and the utilization ratio of raw material is high;
(3) in combination process of the present invention, adopted oily absorption techniques and pressure swing adsorption to reclaim carbon two components in gas mixture, the rate of recovery is high, simple to operate.
Accompanying drawing explanation
Fig. 1 is the schematic flow sheet take oil refinery dry gas as waste ethylbenzene of the present invention.
Embodiment
Further explain the method take oil refinery dry gas as waste ethylbenzene of the present invention below with reference to Fig. 1, but be not limited to this.
Fig. 1 is the principle process schematic diagram take oil refinery dry gas as waste ethylbenzene of the present invention, can on this principle flow chart, modify, increase other technology.
Further explain the present invention in the mode of embodiment below.
Embodiment 1
With reference to accompanying drawing 1, flow process is described.
Raw material is coking dry gas and the catalysis drying gas of refinery, catalysis drying gas chief component is hydrogen 3.79%(wt, as follows), nitrogen 32.58%, methane 18.97%, ethane 15.61%, ethene 12.58%, coking dry gas chief component is hydrogen 2.11%, nitrogen 6.96%, methane 45.07%, ethane 36.82%, ethene 2.91%, send into respectively decarburization unit, by acid gas removals such as carbonic acid gas wherein, be sent to afterwards alkyl plant; Hydrocarbonylation device adopts fixed-bed reactor, adopt ZSM-5 molecular sieve catalyzer I and ZSM-5 molecular sieve catalyst II, preferably adopt the method for recommending in CN200910057824.1 to produce ethylbenzene product, the hydrocarbonylation tail gas chief component that hydrocarbonylation device produces is hydrogen 4.55%, methane 37.76%, ethane 24.77%, ethene 0.18%, is sent to PSA device; Carbon two components in hydrocarbonylation tail gas obtain concentrate in PSA device, and the PSA concentrated gas chief component obtaining is methane 13.25%, ethane 78.26%, ethene 0.61%; PSA concentrated gas is sent to ethane cracking furnace and carries out cracking, the splitting gas chief component obtaining is hydrogen 1.64%, methane 16.03%, ethane 7.02%, ethene 28.78%, carbon 3 11.5%, temperature is 850 ℃, is cooled to, after 40 ℃, be sent to oily absorption unit through waste heat boiler and quenching water column; Splitting gas is the compressed 1.5MPa.G that boosts to first, enter afterwards oil-absorption tower, it is absorption agent that oil-absorption tower adopts benzene, 20 ℃ of tower top temperatures, pressure 1.1MPa.G, carbon in gas mixture three and above component are absorbed and get off to enter desorption tower, obtain carbon two concentrate gas at absorption tower tower top, the rate of recovery of ethene is 90%; Carbon two concentrate gas are allocated into after a certain amount of hydrogen and are entered selective hydrogenation reaction device, and alkynes and hydrogen reaction in concentrate gas are removed, the catalyzer of employing take palladium as active ingredient, 120 ℃ of temperature of reaction, hydrogen alkynes than 2, air speed 15000h
-1; Hydrogenation products gas is sent into decarburization unit again, mixes and remove sour gas at this with oil refinery dry gas, carries out recycle.
Comparative example 1
Raw material is the coking dry gas of refinery, and catalysis drying gas chief component is hydrogen 3.79%, nitrogen 32.58%, methane 18.97%, ethane 15.61%, ethene 12.58%, sends into alkyl plant.Hydrocarbonylation device is made up of alkylation reaction device, dealkylation reaction device, rough segmentation tower, absorption tower, benzene tower, de-toluene tower, ethylbenzene tower, de-ethylbenzene tower, diethylbenzene tower etc., adopt molecular sieve catalyst, conversion of ethylene is 98%, ethane is not participated in reaction, directly enter into hydrocarbonylation tail gas and discharger, hydrocarbonylation tail gas consists of hydrogen 4.1%, nitrogen 37.78%, methane 22.00%, ethane 19.10%, ethene 0.8%.
Claims (8)
1. a combined method of producing ethylbenzene with oil refinery dry gas, is characterized in that, described method comprises the following steps:
(1) alkylation: oil refinery dry gas enters alkyl plant after decarburization unit removes sour gas, ethene wherein reacts with benzene and generates ethylbenzene, and the components such as unreacted ethane enter in hydrocarbonylation tail gas;
(2) pressure-variable adsorption: the hydrocarbonylation tail gas from alkyl plant enters pressure-swing absorption apparatus, carbon two components in this hydrocarbonylation tail gas, after the components such as separation removal methane, hydrogen, enter in PSA concentrated gas, send into afterwards pyrolyzer;
(3) ethane cracking: the PSA concentrated gas from pressure-swing absorption apparatus enters ethane cracking furnace, carries out cracking at this and generates the components such as ethene, hydrogen, and the splitting gas obtaining enters oily absorption unit after waste heat boiler and quenching water column cooling;
(4) oil absorbs: splitting gas from quenching water column is compressed, enter oil-absorption tower after imurity-removal, and it is absorption agent that oil-absorption tower adopts benzene or gasoline; Carbon three and above component in splitting gas are absorbed, and obtain comprising the carbon two concentrate gas of methane, hydrogen, ethane, vinyl light constituent at absorption tower top;
(5) select hydrogenation: the alkynes in carbon two concentrate gas reacts with hydrogen at this and is removed, carbon two concentrate gas after hydrogenation are admitted to the decarburization unit in described step 1), mix with oil refinery dry gas, remove sour gas wherein, then send into alkyl plant and carry out recycle.
2. the combined method of producing ethylbenzene with oil refinery dry gas as claimed in claim 1, is characterized in that:
Described oil refinery dry gas is selected from catalytic cracked dry gas, catalytic pyrolysis dry gas, often one or more mixing of reducing pressure in dry gas, coking dry gas, hydrocracking dry gas;
Alkyl plant in described step (1) is selected from the one in following alkylation reaction technique known in the state of the art: fixed-bed reactor, catalytic distillation tower technology;
Meter very by weight, the hydrocarbonylation tail gas in described step (1) comprises 0～20% hydrogen, 20～50% methane and 20～50% ethane, the content sum of each component is no more than 100%.
3. the combined method of producing ethylbenzene with oil refinery dry gas as claimed in claim 2, is characterized in that:
In step (1), described alkylation is the method for disclosed pure ethylene or dry gas and producing phenylethane from alkylation of benzene in CN200910057824.1.
4. the combined method of producing ethylbenzene with oil refinery dry gas as claimed in claim 2, is characterized in that:
In step (2), in described PSA concentrated gas, ethane content is 50～95%.
5. the combined method of producing ethylbenzene with oil refinery dry gas as claimed in claim 2, is characterized in that:
In step (3),
Described ethane cracking furnace is ethane cracking furnace well known in the prior art or light hydrocarbon cracking stove;
Described pyrolyzer temperature out is 500～700 ℃, pressure 0.05～0.15MPa.G;
In ethane cracking furnace, ethane in the PSA concentrated gas scission reaction that reacts obtains comprising the splitting gas of following component: the hydrogen of 0～10%wt, the methane of 0～20%wt, the ethene of 20～50%wt and the ethane of 0～20%wt, and the content sum of each component is no more than 100%;
Described splitting gas, after cooling and heat recovery and utilization, is sent into oily absorption unit.
6. the combined method of producing ethylbenzene with oil refinery dry gas as claimed in claim 2, is characterized in that:
In step 4),
Described oily absorption unit, comprises compressor, oil-absorption tower and desorption tower;
The absorption temperature of described oil-absorption tower is 10～40 ℃, and absorption pressure is 0.5～2.0MPa.G; Wherein the rate of recovery of ethene is not less than 90%.
7. the combined method of producing ethylbenzene with oil refinery dry gas as claimed in claim 2, is characterized in that:
In step 5),
Described selective hydrogenation catalyst is disclosed acetylene selective hydrogenation catalyst in CN200910082421.2, and wherein main active ingredient is selected from one or both of Pt, Pd, and content is 0.01 % by weight～1.0 % by weight; Help active ingredient to comprise VIII family element, at least one in ⅠⅠ B family element Bi, Sb, Pb, In, Cs, Rb, its content is 0～20 % by weight of carrier gross weight;
The operational condition of described hydrogenation reaction is: reactor inlet temperature is 20～150 ℃, and reaction pressure is 1.0～5.0MPa, and the mol ratio of hydrogen and alkynes is 0.8～4.0, and air speed is 5000～20000h
-1.
8. the combined method of producing ethylbenzene with oil refinery dry gas as claimed in claim 7, is characterized in that:
In step (1), described alkylation is the method for disclosed pure ethylene or dry gas and producing phenylethane from alkylation of benzene in CN200910057824.1;
In step (2), in described PSA concentrated gas, ethane content is 50～95%;
In step (3),
Described ethane cracking furnace is ethane cracking furnace well known in the prior art or light hydrocarbon cracking stove;
Described pyrolyzer temperature out is 500～700 ℃, pressure 0.05～0.15MPa.G;
In ethane cracking furnace, ethane in the PSA concentrated gas scission reaction that reacts obtains comprising the splitting gas of following component: the hydrogen of 0～10%wt, the methane of 0～20%wt, the ethene of 20～50%wt and the ethane of 0～20%wt, and the content sum of each component is no more than 100%;
Described splitting gas, after cooling and heat recovery and utilization, is sent into oily absorption unit;
In step 4),
Described oily absorption unit, comprises compressor, oil-absorption tower and desorption tower;
The absorption temperature of described oil-absorption tower is 10～40 ℃, and absorption pressure is 0.5～2.0MPa.G; Wherein the rate of recovery of ethene is not less than 90%.
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| CN107473925A (en) * | 2017-08-31 | 2017-12-15 | 北京和利凯石化技术有限公司 | A kind of method that ethylbenzene is prepared using low-carbon alkanes |
| CN108424345A (en) * | 2017-02-14 | 2018-08-21 | 中国石化工程建设有限公司 | A kind of ethylbenzene production plants and technique |
| CN111423301A (en) * | 2020-05-09 | 2020-07-17 | 中国石油化工股份有限公司 | Combined process for preparing ethylbenzene from refinery dry gas |
| CN111440043A (en) * | 2020-05-09 | 2020-07-24 | 中国石油化工股份有限公司 | Combined process for preparing ethylbenzene from refinery dry gas |
| CN113336619A (en) * | 2021-05-13 | 2021-09-03 | 华陆工程科技有限责任公司 | Method for preparing acetylene gas by using oxo-synthesis gas |
| CN114436746A (en) * | 2020-11-04 | 2022-05-06 | 中国石油化工股份有限公司 | Process and system for purifying an ethylene-containing feed gas |
| CN114436732A (en) * | 2020-11-04 | 2022-05-06 | 中国石油化工股份有限公司 | Method and system for preparing ethylbenzene and hydrogen by using refinery dry gas |
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Cited By (8)
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| CN108424345A (en) * | 2017-02-14 | 2018-08-21 | 中国石化工程建设有限公司 | A kind of ethylbenzene production plants and technique |
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| CN111423301A (en) * | 2020-05-09 | 2020-07-17 | 中国石油化工股份有限公司 | Combined process for preparing ethylbenzene from refinery dry gas |
| CN111440043A (en) * | 2020-05-09 | 2020-07-24 | 中国石油化工股份有限公司 | Combined process for preparing ethylbenzene from refinery dry gas |
| CN114436746A (en) * | 2020-11-04 | 2022-05-06 | 中国石油化工股份有限公司 | Process and system for purifying an ethylene-containing feed gas |
| CN114436732A (en) * | 2020-11-04 | 2022-05-06 | 中国石油化工股份有限公司 | Method and system for preparing ethylbenzene and hydrogen by using refinery dry gas |
| CN113336619A (en) * | 2021-05-13 | 2021-09-03 | 华陆工程科技有限责任公司 | Method for preparing acetylene gas by using oxo-synthesis gas |
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