CN1464035A - Process for producing gasoline from low-carbon hydrocarbon containing olefin as raw material - Google Patents
Process for producing gasoline from low-carbon hydrocarbon containing olefin as raw material Download PDFInfo
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- CN1464035A CN1464035A CN 02122471 CN02122471A CN1464035A CN 1464035 A CN1464035 A CN 1464035A CN 02122471 CN02122471 CN 02122471 CN 02122471 A CN02122471 A CN 02122471A CN 1464035 A CN1464035 A CN 1464035A
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Abstract
In the technological process of producing gasoline with low-carbon hydrocarbon containing olefin, the low-carbon hydrocarbon material containing olefin is reacted in a reactor with solid acid catalyst and modified solid acid catalyst to produce high octane value gasoline and vehicular liquefied gas as side product with gasoline selectivity higher than 90 %, arene content in gasoline organic 5-40 %, alkane content 10-80 % and research octane number 70-120. The catalyst with degraded activity may be high temperature sweeping regenerated in air or mixed nitrogen-oxygen atmosphere.
Description
Technical field
The present invention relates to produce the technology of gasoline, a kind of technology by mixed light-hydrocarbon raw material production stop bracket gasoline and by-product motor liquified gas specifically is provided, and the renovation process of the solid acid catalyst that uses in this technology is provided.
Background technology
At present especially liquefied petroleum gas (LPG) is most of burns as household fuel from the mixed light-hydrocarbon of refinery, and along with the raising of environmental requirement, liquefied petroleum gas (LPG) more and more comes into one's own as clean fuel for vehicle, and directly contain a large amount of alkene in the liquefied petroleum gas (LPG) from the refinery, can not be directly as vehicle fuel.If the liquefied gas from the refinery is produced stop bracket gasoline through reaction, and the qualified motor liquified gas of coproduction, the utilization of liquefied gas is more economical.
Patent CN87103258 is a catalyzer with the ZSM-5 zeolite, and polymerization of low-carbon olefin is produced gasoline, at 980KPa, and 361 ℃ of temperature of reaction, air speed 1.80h
-1, oily yield is 52.7%, the research octane number (RON) of oil is 91.9.
Patent CN98116429 solid superacid as catalyst Trimethylmethane and butene alkylated production clean gasoline.CN94120022 uses solid heteropoly acid catalyzing iso-butane alkane and butene alkylated production clean gasoline among the CN94 120018.
Patent CN89105117 with the ZSM-5 zeolite be catalyzer under 500-600 ℃ to aromatization of low carbon hydrocarbon, the content of aromatic hydrocarbons in oil is greater than 60%.
To divide the ZSM-5 with Zn be catalyzer to patent CN98101358 to sneak into alkene local soil type, at 520-550 ℃ to mixed C
4Carry out aromizing, aromatics yield is greater than 40%.
Summary of the invention
The object of the present invention is to provide a kind of method of producing stop bracket gasoline, be rich in the light hydrocarbon feedstocks of alkene in this way by conversion, can obtain very high high-octane gasoline of liquid yield and the qualified motor liquified gas of by-product.
To achieve these goals, the mixed light-hydrocarbon raw material is through one section reactor that is filled with catalyzer, and reactions such as aromizing, alkylation, superimposed, hydrogen transference take place, and generates stop bracket gasoline and by-product motor liquified gas.
Contain alkene in the mixed light-hydrocarbon raw material of the present invention, it consists of: one or more in carbon three, carbon four or the carbon five are 5-99% comprising olefin(e) centent, and alkane content is 1-95%, can also contain other component of minute quantity.Raw material can directly enter reactor reaction, also can with enter reactor after gases such as nitrogen/hydrogen mix.
Employed catalyzer is the solid acid catalyst of solid acid catalyst and modification in the above-mentioned reactor, specifically is the modified catalyst of one or more and these molecular sieve in ZSM-5, ZSM-11, ZSM-12, ZSM-35, MCM-22, Y molecular sieve, the beta molecular sieve.
The reaction conditions of reactor is: temperature of reaction is 100-550 ℃, and pressure is 0.1-5.0MPa, and air speed is that every gram catalyzer per hour advances 0.1-20 gram oil, and weight space velocity is suitableeer with 1-5.
Contain the olefin light hydrocarbon feedstocks complicated aromizing/alkylation/superimposed/hydrogenation reaction takes place in reactor, generate stop bracket gasoline, the selectivity of gasoline is greater than 90%, and aromaticity content is 5-40% (benzene is less than 2.5%) in the gasoline, and alkane content is 10-80%.Study of Gasoline method octane is 70-120.
Be lower than 5% through olefin(e) centent in the reacted remaining light hydrocarbon feedstocks, can be used as motor liquified gas and use.
Carrying out regenerated technology through reacted catalyzer is: purge regeneration through reacted catalyzer high temperature in chlorine, nitrogen oxygen atmosphere or air, regeneration temperature 200-550 ℃, pressure is 0.1-5.0MPa, and the volume space velocity of air is 50-10000h
-1Described density of hydrogen is 10-100%, and oxygen concentration is 1-100% in the nitrogen oxygen atmosphere.
Embodiment
Below by example in detail the present invention is described in detail.
The mixing lower carbon number hydrocarbons raw material that example 1-10 is used composed as follows: (wt%)
Propylene: 0.23%, propane 1.23%, Trimethylmethane: 35.23%, 1-butylene: 12.32%, normal butane: 12.36%, anti-2-butylene: 25.53%, suitable 2-butylene: 11.96%, carbon five components: 0.14%.
Example 1
Adopt ZSM-5/ZSM-11 mixed crystal molecular sieve, wherein the ratio of ZSM-5/ZSM-11 is 0.1/0.9 (wt), and molecular sieve was through 450 ℃ of steam-treated two hours.On molecular sieve, soak ammonium molybdate solution, make that the weight content of molybdenum is 5%.Reaction conditions is: 270 ℃ of temperature of reaction, reaction pressure 0.2MPa, air speed 1.0h
-1The yield of splitting gas in the tail gas (C1+C2) is 0.1%, and the yield of oil is: 35.2%.The weight of oil consists of: alkane 36.5%, alkene 35.6%, cyclic hydrocarbon 13.2%, aromatic hydrocarbons 14.7% (benzene content is 0.2%).The research octane number (RON) of oil: 94.3.
Example 2
Adopt ZSM-5/ZSM-11 mixed crystal molecular sieve, wherein the ratio of ZSM-5/ZSM-11 is 0.3/0.7 (wt), and molecular sieve was through 520 ℃ of steam-treated two hours.On molecular sieve, soak lanthanum nitrate hexahydrate, make that the weight content of lanthanum is 1%.Reaction conditions is: 330 ℃ of temperature of reaction, reaction pressure 2.0MPa, air speed 2.0h
-1The yield of splitting gas in the tail gas (C1+C2) is 0.2%, and the yield of oil is: 55.2%.The weight of oil consists of: alkane 30.4%, alkene 16.4%, cyclic hydrocarbon 8.4%, aromatic hydrocarbons 44.8% (benzene content is 1.5%).The research octane number (RON) of oil: 98.2.
Example 3
Adopt ZSM-5/ZSM-11 mixed crystal molecular sieve, wherein the ratio of ZSM-5/ZSM-11 is 0.8/0.2 (wt), and molecular sieve was through 550 ℃ of steam-treated two hours.Reaction conditions is: 400 ℃ of temperature of reaction, reaction pressure 5.0MPa, air speed 10.0h
-1The yield of splitting gas in the tail gas (C1+C2) is 4.4%, and the yield of oil is: 56.7%.The weight of oil consists of: alkane 19.4%, alkene 45.6%, cyclic hydrocarbon 9.4%, aromatic hydrocarbons 25.6% (benzene content is 2.3%).The research octane number (RON) of oil: 99.3.
Example 4
Adopt the ZSM-35 molecular sieve, molecular sieve was through 550 ℃ of steam-treated two hours.Reaction conditions is: 500 ℃ of temperature of reaction, reaction pressure 2.0MPa, air speed 2.0h
-1The yield of splitting gas in the tail gas (C1+C2) is 5.2%, and the yield of oil is: 65.2%.The weight of oil consists of: alkane 16.5%, alkene 35.4%, cyclic hydrocarbon 12.4%, aromatic hydrocarbons 35.7% (benzene content is 1.8%).The research octane number (RON) of oil: 99.6.
Example 5
Adopt the MCM-22 molecular sieve, on molecular sieve, soak ammonium molybdate solution, make that the weight content of molybdenum is 5%.Reaction conditions is: 150 ℃ of temperature of reaction, reaction pressure 3.0MPa, air speed 0.3h
-1The yield of splitting gas in the tail gas (C1+C2) is 0.05%, and the yield of oil is: 25.2%.The weight of oil consists of: alkane 12.0%, alkene 77.8%, cyclic hydrocarbon 4.5%, aromatic hydrocarbons 5.7% (benzene content is 0.2%).The research octane number (RON) of oil: 93.5.
Example 6
Adopt the ZSM-5 molecular sieve, molecular sieve was through 520 ℃ of steam-treated two hours.Reaction conditions is: 380 ℃ of temperature of reaction, reaction pressure 3.0MPa, air speed 3.0h
-1The yield of splitting gas in the tail gas (C1+C2) is 3.5%, and the yield of oil is: 50.3%.The weight of oil consists of: alkane 42.4%, alkene 10.2%, cyclic hydrocarbon 9.8%, aromatic hydrocarbons 37.6% (benzene content is 1.3%).The research octane number (RON) of oil: 92.5.
Example 7
Adopt the ZSM-11 molecular sieve, molecular sieve was through 520 ℃ of steam-treated two hours.Reaction conditions is: 350 ℃ of temperature of reaction, reaction pressure 0.5MPa, air speed 3.0h
-1The yield of splitting gas in the tail gas (C1+C2) is 1.2%, and the yield of oil is: 54.9%.The weight of oil consists of: alkane 35.6%, alkene 22.9%, cyclic hydrocarbon 10.2%, aromatic hydrocarbons 31.3% (benzene content is 1.1%).The research octane number (RON) of oil: 93.7.
Example 8
Adopt the ZSM-12 molecular sieve, molecular sieve was through 520 ℃ of steam-treated two hours.Reaction conditions is: 315 ℃ of temperature of reaction, reaction pressure 1.0MPa, air speed 2.0h
-1The yield of splitting gas in the tail gas (C1+C2) is 0.5%, and the yield of oil is: 45.2%.The weight of oil consists of: alkane 33.8%, alkene 30.2%, cyclic hydrocarbon 9.6%, aromatic hydrocarbons 26.4% (benzene content is 0.8%).The research octane number (RON) of oil: 94.3.
Example 9
Adopt Y molecular sieve, molecular sieve was through 480 ℃ of steam-treated two hours.Reaction conditions is: 300 ℃ of temperature of reaction, reaction pressure 2.5MPa, air speed 2.5h
-1The yield of splitting gas in the tail gas (C1+C2) is 0.9%, and the yield of oil is: 53.9%.The weight of oil consists of: alkane 23.1%, alkene 41.3%, cyclic hydrocarbon 13.2%, aromatic hydrocarbons 22.4% (benzene content is 0.7%).The research octane number (RON) of oil: 93.3.
Example 10
Adopt the beta molecular sieve, molecular sieve was through 470 ℃ of steam-treated two hours.Reaction conditions is: 280 ℃ of temperature of reaction, reaction pressure 1.5MPa, air speed 1.5h
-1The yield of splitting gas in the tail gas (C1+C2) is 0.5%, and the yield of oil is: 52.1%.The weight of oil consists of: alkane 24.3%, alkene 51.4%, cyclic hydrocarbon 8.7%, aromatic hydrocarbons 15.6% (benzene content is 0.3%).The research octane number (RON) of oil: 89.4.
The used mixed light-hydrocarbon raw material of example 11-13 is composed as follows: (wt%)
Propane 0.036%, Trimethylmethane 32.90%, normal butane 8.51%, anti-butene-2 16.27%, butene-1 15.99%, iso-butylene 17.52%, maleic-2 8.52%, 1,3-butadiene 0.25%
Example 11
Adopt the ZSM-5 molecular sieve of La, Mo modification, through 520 ℃ of steam-treated 3h.Reaction conditions is: temperature of reaction is 350 ℃, and reaction pressure is 1.8MPa, and weight space velocity is 1.8h
-1, the yield of the splitting gas in the tail gas (C1+C2) is 1.1%, the yield of gasoline is 56.7%.The weight of gasoline consists of: alkane 35%, and naphthenic hydrocarbon 9.5%, alkene 7.5%, aromatic hydrocarbons 48% (benzene content 0.9%), the RON of gasoline is 98.5
Example 12
With the mixed type molecular sieve of ZSM-5 and ZSM-35 (weight ratio is 1: 1) at 500 ℃ of following steam treatment 3h.Reaction conditions is: temperature of reaction is 340 ℃, and reaction pressure is 2.0MPa, and weight space velocity is 2.0h
-1, the yield of splitting gas in the tail gas (C1+C2) is 0.85%, the yield of gasoline is 58%.The weight of gasoline consists of: alkane 36%, and naphthenic hydrocarbon 6%, alkene 9%, aromatic hydrocarbons 49%, gasoline RON are 98.6.
Example 13
With blended MCM-22 and ZSM-35 molecular sieve at 500 ℃ of following steam treatment 3h.Reaction conditions is: temperature of reaction is 315 ℃, and reaction pressure is 1.8MPa, and weight space velocity is 1.7h
-1, the yield of splitting gas in the tail gas (C1+C2) is 0.80%, the yield of gasoline is 56%.The weight of gasoline consists of: alkane 24%, and naphthenic hydrocarbon 4%, alkene 40%, aromatic hydrocarbons 32%, the RON of gasoline are 95.4.
Example 14
The ZSM-5 molecular sieve of the La modification of inactivation (contain weight percentage be 0.8% La) is regenerated in air, and air pressure is 1.8MPa, and volume space velocity is 5000h
-1, regeneration temperature is 540 ℃, and the recovery time is 1h, reacts under the condition identical with example 11 through the catalyzer after the regeneration, and the yield of the splitting gas in the tail gas (C1+C2) is 1.5%, and the yield of gasoline is 58.6%.The weight of gasoline consists of: alkane 36.5%, and naphthenic hydrocarbon 9.5%, alkene 9%, aromatic hydrocarbons 45% (benzene content 0.9%), the RON of gasoline is 97.5, the regeneration rear catalyst is active basic identical with live catalyst.
Example 15
The ZSM-5 molecular sieve of the La modification of inactivation (contain weight percentage be 0.8% La) heats up in nitrogen and causes 530 ℃ of constant temperature, switches then to cause to feed the nitrogen oxygen atmosphere that contains 1% oxygen, and pressure is 1.8MPa, and volume space velocity is 5000h
-1, the content of the carbonic acid gas in the detection tail gas.When the content of the carbonic acid gas in the tail gas was lower than 0.1%, switching caused and feeds the nitrogen oxygen atmosphere that contains 2% oxygen, detects the content of the carbonic acid gas in the tail gas.When the content of the carbonic acid gas in the tail gas was lower than 0.1%, switching caused and feeds the nitrogen oxygen atmosphere that contains 5% oxygen, detects the content of the carbonic acid gas in the tail gas.When the content of the carbonic acid gas in the tail gas was lower than 0.1%, switching caused and feeds the nitrogen oxygen atmosphere that contains 10% oxygen, detects the content of the carbonic acid gas in the tail gas.When the content of the carbonic acid gas in the tail gas was lower than 0.1%, switching caused bubbling air, continues constant temperature 3h then.
React under the condition identical with example 11 through the catalyzer after the regeneration, the yield of the splitting gas in the tail gas (C1+C2) is 1.7%, and the yield of gasoline is 55.3%.The weight of gasoline consists of: alkane 24.6%, and naphthenic hydrocarbon 10.3%, alkene 8.4%, aromatic hydrocarbons 56.7% (benzene content 1.2%), the RON of gasoline is 99.7, the regeneration rear catalyst is active basic identical with live catalyst.
The present invention is not limited only to above example.In a word, the lower carbon number hydrocarbons mixture that contains alkene is converted into the stop bracket gasoline that meets national requirements for environmental protection after by process of the present invention, and can the by-product motor liquified gas.
Claims (9)
1, a kind of technology of producing gasoline by the lower carbon number hydrocarbons that contains alkene, it is characterized in that: the lower carbon number hydrocarbons raw material that contains alkene enters the reactor that is filled with molecular sieve catalyst, the reaction conditions of reactor is: temperature of reaction is 100-500 ℃, pressure is 0.1-5.0MPa, weight space velocity is that every gram catalyzer per hour advances 0.1-20 gram oil, generates stop bracket gasoline.
2, by the described technology of claim 1, it is characterized in that described lower carbon number hydrocarbons raw material is carbon three, carbon four or/and carbon five, wherein olefin(e) centent is 5-99%, alkane content is 1-95% and a small amount of other components.
3, by claim 1 or 2 described technologies, it is characterized in that, described lower carbon number hydrocarbons raw material with enter reactor after nitrogen or hydrogen mix.
4, by the described technology of claim 1, it is characterized in that described molecular sieve catalyst is that ZSM-5, ZSM-11, ZSM-12, ZSM-35, MCM-22, Y molecular sieve are or/and the beta molecular sieve.
5, by claim 1 or 4 described technologies, it is characterized in that described molecular sieve catalyst is a modified catalyst.
6,, it is characterized in that it is preferable that described weight space velocity is that every gram catalyzer per hour advances 1-5 gram oil by the described technology of claim 1.
By claim 1,4 or 5 described technologies, it is characterized in that 7, described catalyzer high temperature in air atmosphere purges regeneration, regeneration temperature is 100-550 ℃, and pressure is 0.1-5.0MPa, and the volume space velocity of air is 50-10000h
-1
By claim 1,4 or 5 described technologies, it is characterized in that 8, described catalyzer high temperature in nitrogen oxygen atmosphere atmosphere purges regeneration, wherein oxygen concentration is 1-100%.
By claim 1,4 or 5 described technologies, it is characterized in that 9, described catalyzer high temperature in hydrogen atmosphere purges regeneration, wherein density of hydrogen is 10-100%.
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| CN 02122471 CN1464035A (en) | 2002-06-05 | 2002-06-05 | Process for producing gasoline from low-carbon hydrocarbon containing olefin as raw material |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US7476774B2 (en) | 2005-02-28 | 2009-01-13 | Exxonmobil Research And Engineering Company | Liquid phase aromatics alkylation process |
| US7498474B2 (en) | 2005-02-28 | 2009-03-03 | Exxonmobil Research And Engineering Company | Vapor phase aromatics alkylation process |
| US7525002B2 (en) | 2005-02-28 | 2009-04-28 | Exxonmobil Research And Engineering Company | Gasoline production by olefin polymerization with aromatics alkylation |
| US8395006B2 (en) | 2009-03-13 | 2013-03-12 | Exxonmobil Research And Engineering Company | Process for making high octane gasoline with reduced benzene content by benzene alkylation at high benzene conversion |
| CN103894220A (en) * | 2012-12-25 | 2014-07-02 | 中国科学院大连化学物理研究所 | Molecular sieve mercury-free catalyst for acetylene hydrochlorination reaction, and preparation method thereof |
| CN110756220A (en) * | 2018-07-25 | 2020-02-07 | 中国石油天然气股份有限公司 | Preparation method and application of ZSM-35/ZSM-5 eutectic molecular sieve catalyst |
-
2002
- 2002-06-05 CN CN 02122471 patent/CN1464035A/en active Pending
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US7476774B2 (en) | 2005-02-28 | 2009-01-13 | Exxonmobil Research And Engineering Company | Liquid phase aromatics alkylation process |
| US7498474B2 (en) | 2005-02-28 | 2009-03-03 | Exxonmobil Research And Engineering Company | Vapor phase aromatics alkylation process |
| US7525002B2 (en) | 2005-02-28 | 2009-04-28 | Exxonmobil Research And Engineering Company | Gasoline production by olefin polymerization with aromatics alkylation |
| US8395006B2 (en) | 2009-03-13 | 2013-03-12 | Exxonmobil Research And Engineering Company | Process for making high octane gasoline with reduced benzene content by benzene alkylation at high benzene conversion |
| CN103894220A (en) * | 2012-12-25 | 2014-07-02 | 中国科学院大连化学物理研究所 | Molecular sieve mercury-free catalyst for acetylene hydrochlorination reaction, and preparation method thereof |
| CN110756220A (en) * | 2018-07-25 | 2020-02-07 | 中国石油天然气股份有限公司 | Preparation method and application of ZSM-35/ZSM-5 eutectic molecular sieve catalyst |
| CN110756220B (en) * | 2018-07-25 | 2022-10-04 | 中国石油天然气股份有限公司 | Preparation method and application of ZSM-35/ZSM-5 eutectic molecular sieve catalyst |
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