CN1292824C - Selective absorption method for reducing propylene in catalytic cracking dry gas - Google Patents

Selective absorption method for reducing propylene in catalytic cracking dry gas Download PDF

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Publication number
CN1292824C
CN1292824C CNB2004100374330A CN200410037433A CN1292824C CN 1292824 C CN1292824 C CN 1292824C CN B2004100374330 A CNB2004100374330 A CN B2004100374330A CN 200410037433 A CN200410037433 A CN 200410037433A CN 1292824 C CN1292824 C CN 1292824C
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absorbent
dry gas
gas
propylene
absorption
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CN1689688A (en
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王清遐
徐龙伢
刘盛林
李建保
张银龙
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Dalian Institute of Chemical Physics of CAS
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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

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Abstract

The present invention relates to a method for absorbing propene from a dry gas generated from a catalytic cracking device in an oil plant. In the method, the propene in the catalytic cracking dry gas without any purification and refining is removed by an absorption device which selectively absorbs alkene; a contact mode between the dry gas and absorbent is in the form of contra flow, and the absorbent comprises one type or the mixture of a plurality of types of benzene, ethylenzene, diethylbenzene, triethylbenzene, more than three of ethylenzene (multi-ethylenzene), a diesel oil, gasoline, etc. The absorbent has the absorption conditions for the propene in the dry gas that the operation temperature is from 10 DEG C below zero to 40 DEG C below zero, the pressure is from 0.1 to 3.5MPa, and the volume ratio (ml/L) to the absorbent/the dry gas is from 3 to 25. The absorbent after adsorbing the gas has the desorption conditions that the temperature is from 20 DEG C to 300 DEG C, the pressure is from 0.1 to 3.5MPa, the volume ratio to a sweeping gas/the absorbent is from 1 to 15, and the sweeping time is from 1 to 10 hours, wherein the sweeping gas comprises one type of or the mixture of a plurality of types of N2, H2, methane, ethane, etc. The absorbent after the desorption can be used in a circulation mode.

Description

A kind of method of selecting to absorb propylene in the reduction catalytic cracked dry gas
Technical field
The present invention relates to mixed gas separation and field of purification, particularly by selecting to absorb the method that reduces propylene in the catalytic cracked dry gas.
Background technology
China's ethylene industry development speed is very fast relatively over past ten years, has built up big-and-middle-sized ethylene producing device 18 covers so far.After 2000, begin a collection of ethylene unit is transformed and extended, can reach 8,400,000 tons to national ethylene production capacity in 2005.China compares with external ethylene industry and also has very big gap.All multifactor costs of ethene that makes are higher than external, thereby influence the development of domestic ethene.The many oil plants of industry China will contain the catalytic cracked dry gas of ethene 12%～25% (volume fraction) in a large number to be burnt as the combustion gas or the torch of setting fire, and causes the waste of resource and the pollution of environment.At present, China's catalytic cracking unit scale occupies the second place of the world, and dry gas output is 112MtPa～315MtPa, and the ethene quantity in the dry gas is considerable.If it can be reclaimed, can improve the competitiveness of oil refining enterprise, also will relax the disparities between supply and demand of domestic ethene.It is significant to extract ethene from catalytic cracked dry gas.
At present, the technology of extraction ethene separation of propylene mainly contains separation by deep refrigeration, absorption and separation method, hydrate partition method, membrane separation process and adsorption method of separation from gaseous mixtures such as catalytic cracked dry gas.Wherein the hydrate partition method is emerging separation method, and membrane separation process and adsorption method of separation are in laboratory research or commerical test stage, and separation by deep refrigeration, absorption and separation method are quite ripe, and has realized industrialization, has obtained good economic benefit.Separation by deep refrigeration can obtain the ethene of polymer grade, but because the ethylene concentration in the dry gas is low, the general situation that is fit to handle a large amount of dry gas is particularly suitable for the area of concentration, refinery.It is when if refinery's scale is smaller, then uneconomical.
The absorption and separation method mainly utilizes each component of catalytic cracked dry gas different solubility in absorbent to separate.Middle cold oil absorption technique generally is to utilize oil products such as C3, C4 and aromatic hydrocarbons to make absorbent, at first removes methane and hydrogen, with rectifying each component that absorbs is separated one by one then.Operating temperature is minimum to be-70 ℃, is generally-20-40 ℃, and ethene purity is about 90%, and yield is a 85%[Wu thatch duckweed, Sun Li. the separation of oil refinery dry gas is reclaimed and comprehensive utilization, modern chemical industry, 2001,21 (5): 20-23]..Mehra technology is developed by houston, u.s.a AET company.This process using Mehrsolr solvent can be separated into cracked gas gases such as Fu Qing, methane rich and ethene on the gas processing plant of routine, for carrying out conventional fractionation in the downstream.It is 90% hydrogen and methane fuel gas that this technology can obtain purity, and hydrogen can further purify in pressure-swing absorption apparatus and reach 99% purity.The Mehrsolr solvent generally is that ployalkylene glycol dialkyl ether, N-methyl adjoin the special mixture of coughing up ketone, dimethyl cresols amine, propene carbonate, sulfolane and ethylene glycol triacetate.In addition, C 8～C 10Aromatic compound also can be used as the solvent of this technology.Operating temperature is generally about-37 ℃, and pressure is 1.7MPa[1.Mehra Y R.Using Extraction to treat hydrocarbongases, Chem.Eng.1986,93 (20): 53-55; 2.Savage P., Brooks K., Refinery gases:a quick source of ethylene, Chem.Week, 1988,142 (19): 16].
In the catalytic cracked dry gas of refinery except that the ethene that contains 10-25%, also have a certain amount of propylene and butylene, its content depends on the catalytic cracking unit working condition, because the alkylation speed ratio ethene of propylene, butylene and benzene is fast, except generating ethylbenzene and diethylbenzene, also there is following side reaction: propylene+benzene=propyl benzene (1); Butylene+benzene=butylbenzene (2).Reaction (1) and (2) all need consume benzene, the benzene consumption rate of process is increased, influence the ethylbenzene production cost, for this reason, the far grade of Wang Qing [selects to transform the research of ethene in the purification catalytic cracked dry gas, Liaoning chemical industry, 1989,4:32] adopt the modified ZSM-5 zeolite catalyst, can make propylene in the catalytic cracked dry gas, butylene is converted into hydro carbons, and wherein 95% ethene is retained.
Summary of the invention
The objective of the invention is on the basis of above-mentioned prior art, to provide a kind of by selecting to absorb the method that reduces propylene in the catalytic cracked dry gas.When using method provided by the invention to be used for catalytic cracked dry gas system ethylbenzene, can obviously reduce the utilization rate of benzene consumption and raising ethene.
For achieving the above object, thereby the method that propylene in the catalytic cracked dry gas is absorbed ethene purity in the raising dry gas by absorbent provided by the invention, absorb propylene with absorbent, with purge gas the absorbent that is absorbed with propylene is carried out desorb then, use with the recirculation of the absorbent after the purge gas desorb.Wherein:
Absorbent is to the acceptance condition of propylene in the dry gas:
Dry gas feeds from the lower end of absorption plant, and absorbent is from last endfeed, and the way of contact in the absorption tower of filler is housed of dry gas and absorbent is to streamed;
Temperature is-10-40 ℃, and pressure is 0.1-3.5MPa, absorbent/dry gas volume ratio (ml/L): 3-25;
Absorbent comprises one or more the mixture in benzene, ethylbenzene, diethylbenzene, triethylbenzene (TEB), the ethylo benzene more than three (multi-ethyl phenenyl), diesel oil and the gasoline;
Absorbent desorption condition after the adsorbed gas is:
Temperature is 20-300 ℃, and pressure is 0.1-3.5MPa, and purge gas/absorbent volume is than being 1-15, and purge time is 1-10 hour;
Purge gas comprises N 2, H 2, one or more mixture in methane and the ethane.
Described dry gas is the dry gas that produces from refinery catalytic cracking unit, and more than the propylene 50ppm, remaining gas is hydrogen, methane, ethane, ethene, carbon monoxide and carbon dioxide in the dry gas.
When adopting the method for the invention to be used for selectivity absorption catalytic cracked dry gas propylene, the catalytic cracked dry gas raw material need not any purification and refining.
The specific embodiment
Below in conjunction with embodiment the present invention is further elaborated, but the present invention is not produced any restriction.
Embodiment 1-7
Absorbing tower height 110cm, adding the high about 90cm of inertia Φ 3 ball fillers on the internal diameter 32mm absorption plant, dry gas enters from the bottom, under the condition that absorbent enters from the top, obtains following embodiment 1-7 result.Can find out that from embodiment result adsorbent/dry gas volume ratio is big more, the propylene that absorbs in the dry gas of back is few more, and adsorption temp is high more, and the propylene that absorbs in the dry gas of back is many more.
Embodiment 1 benzene is 17 ℃ absorption result
Adsorbent/benzene Absorption pressure/0.8MPa Experimental result Absorptivity (%)
Temperature (℃) Adsorbent flow (ml/h) Dry gas flow (L/h) Volume ratio (ml/L) N2 CH4 CO2 C2＝ C2 C3＝ C3 C2 C2＝ C3＝
17 120 20 6 17.63 39.12 3.47 24.01 15.58 0.19 0.07 12.57 2.70 83.19
17 150 20 7.5 18.14 40.65 3.33 23.10 14.68 0.08 0.02 17.62 6.39 92.92
17 180 20 9 19.04 40.89 3.27 22.61 14.15 0.04 0 20.59 8.37 96.46
The catalytic cracked dry gas raw material is formed 16.32 36.16 3.65 24.68 17.82 1.13 0.22
Embodiment 2 reverse alkylation material (diethylbenzene 30w%, triethylbenzene (TEB) 30w%, many ethylbenzene 40w%) are 15 ℃ absorption results
Adsorbent/reverse alkylation material Absorption pressure/0.8MPa Experimental result Absorptivity (%)
Temperature (℃) Adsorbent flow (ml/h) Dry gas flow (L/h) Volume ratio (ml/L) N2 CH4 CO2 C2＝ C2 C3＝ C3 C2 C2＝ C3＝
15 200 20 10 18.89 40.92 3.79 22.64 13.72 0.03 0 20.37 10.27 97.41
15 250 20 12.5 18.97 42.11 3.83 22.11 12.98 0 0 24.67 12.37 100
The catalytic cracked dry gas raw material is formed 15.90 36.43 3.83 25.23 17.23 1.16 0.20
Embodiment 3 ethylbenzene are 17 ℃ absorption result
Adsorbent/ethylbenzene Absorption pressure/0.8MPa Experimental result Absorptivity (%)
Temperature (℃) Adsorbent flow (ml/h) Dry gas flow (L/h) Volume ratio (ml/L) N2 CH4 CO2 C2＝ C2 C3＝ C3 C2 C2＝ C3＝
17 150 20 7.5 18.04 40.06 3.72 23.38 14.63 0.13 0.03 10.25 3.43 88.07
17 200 20 10 18.22 40.21 3.72 23.20 14.59 0.05 0 10.49 4.17 95.41
17 250 20 12.5 18.88 41.42 3.60 22.44 13.64 0.03 0 16.32 7.31 97.25
The catalytic cracked dry gas raw material is formed 19.71 34.92 3.57 24.21 16.30 1.09 0.20
Embodiment 4 diesel oil are 17 ℃ absorption result
Adsorbent/diesel oil Absorption pressure/0.8MPa Experimental result Absorptivity (%)
Temperature (℃) Adsorbent flow (ml/h) Dry gas flow (L/h) Volume ratio (ml/L) N2 CH4 CO2 C2＝ C2 C3＝ C3 C2 C2＝ C3＝
17 150 20 7.5 18.05 40.29 3.67 23.85 14.04 0.10 0 17.19 5.07 91.30
17 200 20 10 18.65 40.89 3.96 23.19 13.28 0.04 0 21.68 7.70 96.52
17 250 20 12.5 21.55 45.14 3.88 21.07 8.34 0.02 0 50.81 16.14 98.26
The catalytic cracked dry gas raw material is formed 15.99 36.71 3.89 25.13 16.96 1.15 0.19
Table 5 ethylbenzene/reverse alkylation material (weight ratio 1/1) is 10 ℃ absorption result
Adsorbent/ethylbenzene/reverse alkylation material=1/1 (w/w) Absorption pressure/0.8MPa Experimental result Absorptivity (%)
Temperature (℃) Adsorbent flow (ml/h) Dry gas flow (L/h) Volume ratio (ml/L) N2 CH4 CO2 C2＝ C2 C3＝ C3 C2 C2＝ C3＝
10 100 20 5 17.43 40.39 3.93 23.78 14.22 0.21 0.04 9.60 5.30 75.58
10 142 19.5 7.3 18.27 40.91 3.93 23.21 13.58 0.10 0 13.67 7.57 88.37
10 190 20 9.5 18.68 42.20 3.89 22.43 12.75 0.04 0 18.94 10.67 95.35
10 230 20.4 11.3 19.08 42.72 3.90 22.01 12.29 0 0 21.87 12.35 100
The catalytic cracked dry gas raw material is formed 16.15 38.11 3.94 25.11 15.73 0.86 0.10
Embodiment 6 ethylbenzene/reverse alkylation material (weight ratio 1/1) are 20 ℃ absorption result
Adsorbent/ethylbenzene/reverse alkylation material=1/1 (w/w) Absorption pressure/0.8MPa Experimental result Absorptivity (%)
Temperature (℃) Adsorbent flow (ml/h) Dry gas flow (L/h) Volume ratio (ml/L) N2 CH4 CO2 C2＝ C2 C3＝ C3 C2 C2＝ C3＝
20 193 18.9 10.2 18.39 42.32 3.92 22.48 12.83 0.10 0 18.64 10.26 87.95
20 253 18 14.1 19.53 43.48 3.88 21.38 11.72 0.02 0 25.68 14.65 97.59
The catalytic cracked dry gas raw material is formed 15.91 38.26 4.06 25.05 15.77 0.83 0.12
Embodiment 7 ethylbenzene/reverse alkylation material (weight ratio 1/1) are 40 ℃ absorption result
Adsorbent/ethylbenzene/reverse alkylation material=1/1 (w/w) Absorption pressure/0.8Mpa Experimental result Absorptivity (%)
Temperature (℃) Adsorbent flow (ml/h) Dry gas flow (L/h) Volume ratio (ml/L) N2 CH4 CO2 C2＝ C2 C3＝ C3 C2 C2＝ C3＝
40 155 22 7.1 18.17 40.12 3.98 23.41 13.85 0.39 0.08 10.53 6.13 54.65
40 180 22 8.2 18.70 40.43 3.93 23.06 13.57 0.25 0.05 12.34 7.54 70.93
40 271 21.7 12.6 19.57 41.65 3.85 22.23 12.59 0.11 0 18.67 10.87 87.21
The catalytic cracked dry gas raw material is formed 16.63 37.98 3.96 24.94 15.48 0.86 0.17
Embodiment 8:
Absorbent ethylbenzene/reverse alkylation material (weight ratio 1/1) is at 10 ℃, 0.8MPa, and adsorbent/dry gas volume ratio (ml/L) is under 11.3 the condition catalytic cracked dry gas to be absorbed back (the results are shown in embodiment 5), uses N 2Sweep gas, at 30 ℃, 0.1MPa, purge gas/absorbent volume is than being purge time 3 hours continuously under 5 the condition, and analysis result shows and do not detect methane, ethane in the absorbent, ethene and propylene gas illustrate almost all desorbs of gas of absorbent absorption under this condition.Absorbent ethylbenzene/reverse alkylation material (weight ratio 1/1) after the desorb carries out the adsorption/desorption cycling continuous 10 times, and is functional.
Embodiment 9:
Absorbent ethylbenzene/reverse alkylation material (weight ratio 1/1) is at 10 ℃, 0.8MPa, and adsorbent/dry gas volume ratio (ml/L) is under 11.3 the condition catalytic cracked dry gas to be absorbed back (the results are shown in embodiment 5), uses H 2Sweep gas, at 150 ℃, 1.0MPa, purge gas/absorbent volume is than being purge time 1 hour continuously under 12 the condition, and analysis result shows and do not detect methane, ethane in the absorbent, ethene and propylene gas illustrate almost all desorbs of gas of absorbent absorption under this condition.Absorbent ethylbenzene/reverse alkylation material (weight ratio 1/1) after the desorb carries out the adsorption/desorption cycling continuous 10 times, and is functional.

Claims (3)

1. select to absorb the method that reduces propylene in the catalytic cracked dry gas for one kind, the propylene with in the absorbent absorption dry gas carries out desorb with purge gas to the absorbent that is absorbed with propylene then; Wherein:
Absorbent is to the acceptance condition of propylene in the dry gas:
Dry gas feeds from the lower end of absorption plant, and absorbent is from last endfeed, and the way of contact in the absorption tower of filler is housed of dry gas and absorbent is to streamed;
Temperature is-10-40 ℃, and pressure is 0.1-3.5MPa, absorbent/dry gas volume ratio 3-25ml/L;
Absorbent comprises one or more the mixture in benzene, ethylbenzene, diethylbenzene, triethylbenzene (TEB), the ethylo benzene more than three, diesel oil and the gasoline;
Absorbent desorption condition after the absorption is:
Temperature is 20-300 ℃, and pressure is 0.1-3.5MPa, and purge gas/absorbent volume is than being 1-15, and purge time is 1-10 hour;
Purge gas comprises N 2, H 2, one or more mixture in methane and the ethane.
2. the method for claim 1 is characterized in that, more than the propylene 50ppm, remaining gas is hydrogen, methane, ethane, ethene, carbon monoxide and carbon dioxide in the described dry gas.
3. the method for claim 1 is characterized in that, uses with the recirculation of the absorbent after the purge gas desorb.
CNB2004100374330A 2004-04-30 2004-04-30 Selective absorption method for reducing propylene in catalytic cracking dry gas Expired - Fee Related CN1292824C (en)

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CN101659589B (en) * 2009-09-15 2013-01-02 中国石油化工集团公司 Refining method of raw material gas containing ethene in process of preparing ethylbenzene from ethene
CN101665396B (en) * 2009-09-15 2013-01-02 中国石油化工集团公司 Refining method of virgin gas containing ethane used in process for preparing ethylbenzene by ethane
CN101665397B (en) * 2009-09-15 2013-07-10 中国石油化工集团公司 Refining method of propylene containing ethane used in process for preparing ethylbenzene by ethane
CN101659590A (en) * 2009-09-15 2010-03-03 中国石油化工集团公司 Refining method of raw material gas containing ethene in process of preparing ethylbenzene from ethene
CN102039080B (en) * 2009-10-21 2013-08-28 中国石油化工股份有限公司 Concentration homogenization method of hydrocarbon-containing waste gas
CN102778073B (en) * 2012-08-10 2015-03-25 中石化广州工程有限公司 Refrigerating device and process for recycling propylene by using waste heat and waste pressure in intensified gas fractionation device
EP3443052A1 (en) 2016-04-15 2019-02-20 SABIC Global Technologies B.V. Separation of off gases from c3 hydrocarbons in propane dehydrogenation process
CN114432843B (en) * 2020-11-04 2023-09-08 中国石油化工股份有限公司 Method and device for separating gaseous hydrocarbon material
CN114773137B (en) * 2022-03-10 2023-09-19 吉首大学 Method for preparing olefin from synthesis gas and reaction separation integrated reaction device

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