CN106190287A - A kind of production method of high-quality cleaning fuel - Google Patents
A kind of production method of high-quality cleaning fuel Download PDFInfo
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- CN106190287A CN106190287A CN201510221987.4A CN201510221987A CN106190287A CN 106190287 A CN106190287 A CN 106190287A CN 201510221987 A CN201510221987 A CN 201510221987A CN 106190287 A CN106190287 A CN 106190287A
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Abstract
The invention provides the production method of a kind of high-quality high-octane rating clean vehicle gasoline, it is characterized in that with toluene and rich olefins lower carbon number hydrocarbons and/or coal base, bio-based oxygenatedchemicals as raw material, rich olefins lower carbon number hydrocarbons and/or oxygenatedchemicals are divided into multichannel, enter each reaction bed of multistage fixed bed reactor, with occur on a catalyst after the toluene mixing entered from reactor head alkylation, be dehydrated, be polymerized, isomerization, aromatisation, hydrogen migration etc. are reacted；Product is through isolated hydro carbons liquid phase component and gaseous component；Wherein liquid phase component is fractionated into obtaining rich aromatic hydrocarbons high octane gasoline component and a small amount of light diesel fuel component, and gaseous component is separated into dry gas and automobile-used alkane liquid gas.This production method has that flow process is simple, energy consumption is low, operation scheme motility is strong, gasoline products yield and octane number is high, the not unazotized advantage of sulfur-bearing.
Description
Technical field
The invention belongs to fuel for cleaning vehicle production technical field, specifically, relate to a kind of by toluene
With rich olefins lower carbon number hydrocarbons or coal base, the bio-based oxygenatedchemicals production automobile-used cleaning of high-quality high-octane rating
The method of gasoline and application.
Background technology
Along with the fast development of China's economy, the demand for petroleum resources is increasing.2013,
China's oil import more than 2.8 hundred million tons, external dependence degree more than 55%, the shortage of petroleum resources and effectively
The low bottleneck having become the economy and society sustainable development of restriction China of utilization rate.And in coming few decades,
The shortest in oil downstream product is automobile-used transport fuel, predominantly gasoline and diesel oil (present age oil stone
Change, volume 17 o. 11th in 2009, China's oil refining and the Thought of Countermeasures of petrochemical industry sustainable development).
Along with the growing interest to environmental issue, in recent years, the quality standard of product oil is all carried by various countries
Go out higher requirement, particularly the restriction index of sulfur content has constantly been upgraded.And China's gasoline production
Present situation be nearly 80% gasoline carry out catalytic cracking, its olefin(e) centent and sulfur content are high (in gasoline product
> 95% sulfur from catalytically cracked gasoline), and arene content relatively low (～20%), for reaching state IV or state
V standard-required, needs further hydrodesulfurization to reduce sulfur in gasoline, olefin(e) centent, and this process faces
Greatest problem be during produce loss of octane number.And it is China's Reformed Gasoline, alkylate oil, different
The high-knock rating gasoline blend components such as structure carburetion are in short supply.
On the other hand, current China petrochemical industry annual by-product dry gas, Rich propylene, liquefied gas, carbon
Fourth class olefin-containing lower carbon number hydrocarbons resource more than 2,000 ten thousand tons/year, these lower carbon number hydrocarbons resources of Optimum utilization also produce me
State's high-quality high-knock rating gasoline blend component in short supply is significant.Meanwhile, rich for China
The energy resource structure present situation of coal oil starvation, development is with coal base, especially with reproducible biomass energy
Based on bio-based oxygenatedchemicals produce high-quality clean fuel for vehicle process route, for ensure
China's energy strategy safely, the replacement that realizes vehicle fuel there is important strategic importance.The present invention carries
Supply a kind of to utilize industry low value toluene and rich olefins lower carbon number hydrocarbons or coal base, bio-based oxygenatedchemicals anti-
The new method of high-quality high-octane rating clean vehicle gasoline should be produced, have that flow process is simple, energy consumption is low,
Operation scheme motility is strong, gasoline products octane number height, the not unazotized advantage of sulfur-bearing.
Summary of the invention
It is an object of the invention to provide a kind of utilize industry low value toluene and rich olefins lower carbon number hydrocarbons or coal base,
The reaction of bio-based oxygenatedchemicals produces the new method of high-quality high-octane rating clean vehicle gasoline, the party
Method solves toluene and rich olefins lower carbon number hydrocarbons or coal base, bio-based oxygenatedchemicals reacts production high-quality
The key technology difficult problem such as bed temperature rise, catalyst easy in inactivation during high-octane rating clean vehicle gasoline,
Have that flow process is simple, energy consumption is low, operation scheme motility is strong, gasoline products yield and octane number is high,
The not unazotized advantage of sulfur-bearing.
The invention provides a kind of toluene and rich olefins lower carbon number hydrocarbons or coal base, bio-based oxygenatedchemicals anti-
The method that should produce high-quality high-octane rating clean vehicle gasoline, it is characterised in that: by raw material rich olefins
Lower carbon number hydrocarbons and/or oxygenatedchemicals are divided into multichannel, enter each reaction of multistage fixed bed reactor after heat exchange
Bed, raw material toluene enters reactor from top, is urging after mixing with lower carbon number hydrocarbons and/or oxygenatedchemicals
Occur in agent alkylation, be dehydrated, be polymerized, isomerization, aromatisation, the reaction such as hydrogen migration；Reaction
Product is through isolated hydro carbons liquid phase component and gaseous component；Wherein liquid phase component is fractionated into obtaining richness
Aromatic hydrocarbons high octane gasoline component and a small amount of light diesel fuel component, gaseous component is separated into dry gas and automobile-used alkane
Hydrocarbon liquefied gas.
Described raw material toluene is petroleum toluene, coking hydrogenation toluene, mixes light aromatic hydrocarbons, is the richest in benzene and gently evaporates
One of part oil kind or multiple mixture.Wherein, when raw material is petroleum toluene, its correspondence is met
The certified products standard that national standard requires；Raw material is coking hydrogenation toluene, mixes light aromatic hydrocarbons or be the richest in benzene
During light fraction oil, it is desirable to its sulfur content < 10ppm, diene and alkynes total content < 100ppm, alkali nitrogen,
< 1ppm, the impurity content of other non-hydrocarbons is with reference to petroleum toluene GB for burnt matter and inorganic metal ion content
Requirement.
Described raw material rich olefins lower carbon number hydrocarbons is one of carbon four after dry gas, Rich propylene, liquefied gas, ether
Kind or multiple mixture, olefin(e) centent is not less than 10wt%.For meeting state of China IV, state's V gasoline
Standard-required and improve catalyst service life, this programme can be according to lower carbon number hydrocarbons raw material impurities content
Feedstock pre-processing system is set flexibly: 1. such as sulfur content in lower carbon number hydrocarbons raw material > 50ppm, it is preferably provided with former
Material desulphurization system, controls sulfur content < 10ppm after desulfurization of raw material；2. such as alkadienes and alkynes group in raw material
Divide total content > 100ppm, preferred feedstock first chosen property hydrogenation reactor reaction, control diene in raw material
And alkynes total content < 10ppm；3. such as sulfur content < 50ppm and alkadienes and alkynes in lower carbon number hydrocarbons raw material
< 100ppm, described lower carbon number hydrocarbons raw material can be directly entered alkylation reactor to component total content.
Described feedstock oxygenates is the coal base/methanol of bio-based, dimethyl ether, ethanol, glycerol, fourth
One of alcohol, isobutanol oxygenatedchemicals kind or multiple mixture；Rich olefins lower carbon number hydrocarbons and containing oxidation
Compound raw material can be mixed into reactor with arbitrary proportion.
Described multistage fixed bed catalytic reactor, its bed progression is 2～5 grades, and beds at different levels are filled
Filling out catalyst can be equal proportion filling or the filling of non-equal proportion；
Wherein, first order bed passes through rich olefins lower carbon number hydrocarbons and oxygenatedchemicals with toluene (containing fresh toluene
With circulation toluene) mixing control alkene and oxygenatedchemicals mass percent concentration, it is achieved to reaction
The control of bed temperature rise, in its charging, alkene/oxygenatedchemicals mass percent concentration computational methods are as follows:
(l × x+m × y) ÷ (l+m+n)=p, wherein l, m, n are respectively rich olefins lower carbon number hydrocarbons, oxygen-containing chemical combination
Thing and the inlet amount of toluene unit interval, x and y is respectively alkene mass percent in rich olefins lower carbon number hydrocarbons
Alkyl mass percentage content in concentration, oxygenatedchemicals；P is the mixed alkene of all chargings/contain
Oxygen compound mass percent concentration, in the range from 12～30%；Determine according to reaction bed pre-control temperature rise
After p value, inlet amount n of saturated hydrocarbons unit interval can be calculated according to above-mentioned formula；
The control of the 2nd～5 grade of beds temperature rise, by entering this grade of bed from previous stage bed
Rich olefins lower carbon number hydrocarbons that component and this grade of bed newly inject and the mixing of oxygenatedchemicals are to control alkene/contain
The concentration of oxygen compound, or add further certain proportion toluene and control alkene and oxygenatedchemicals
Concentration and temperature, thus realize effective control of temperature rise；Its 2～5 reaction beds at different levels charging in alkene/
The density calculating method of oxygenatedchemicals is as follows: (l × x+m × y) ÷ (l+m+n+h)=p, wherein l, m,
N is respectively the rich olefins lower carbon number hydrocarbons of this grade of bed, oxygenatedchemicals and the charging of cold toluene unit interval
Amount, x and y is respectively in rich olefins lower carbon number hydrocarbons alkyl in alkene mass percent concentration, oxygenatedchemicals
Mass percentage content；H is the amount of the unit time interior component entering this grade of bed from previous stage bed；
P is the mixed alkene of all chargings/oxygenatedchemicals mass percent concentration, in the range from 12-30%；
After determining p value according to reaction bed pre-control temperature rise, the charge proportion that l, m, n can be adjusted flexibly makes
Above-mentioned equation is set up, it may be assumed that each reaction bed can be adjusted flexibly rich olefins lower carbon number hydrocarbons, oxygenatedchemicals
And the charge proportion of saturated hydrocarbons controls alkene and oxygenatedchemicals mass percent concentration in charging,
Realize the control to reaction bed temperature rise.
The catalyst that course of reaction is used is that Dalian Inst of Chemicophysics, Chinese Academy of Sciences produces
DL0812, DL0822 or DL0805 commercial catalyst.
The reaction condition of course of reaction is: reaction temperature 160～450 DEG C, pressure 0.1～4.0MPa, fulvene
Hydrocarbon lower carbon number hydrocarbons and/or oxygenate feedstock air speed are 0.1～2.0h-1, toluene and rich olefins lower carbon number hydrocarbons and/
Or oxygenatedchemicals mol ratio is 1.2～4.0, single reaction bed temperature rise is 10～50 DEG C.Preferably react
Condition is: reaction temperature 180～420 DEG C, pressure 0.5～3.5MPa, rich olefins lower carbon number hydrocarbons and/or oxygen-containing
Compound feeding air speed is 0.2～1.0h-1, toluene and rich olefins lower carbon number hydrocarbons and/or oxygenatedchemicals mol ratio
1.5～3.5.
Toluene and rich olefins lower carbon number hydrocarbons that the present invention provides or coal base, bio-based oxygenatedchemicals react and give birth to
The method producing high-quality high-octane rating clean vehicle gasoline, raw material toluene and rich olefins lower carbon number hydrocarbons or coal base,
Bio-based oxygen-containing compound material occur on a catalyst alkylation, be dehydrated, be polymerized, isomerization, virtue
Structure, hydrogen migration etc. are reacted, and generate rich aromatic hydrocarbons high-quality high octane gasoline component, and it is in harmonious proportion octane
Value reaches more than 115, and is substantially free of sulfur, the most nitrogenous, is that the high-quality clean vehicle gasoline of high-quality is adjusted
And component.It is anti-that the present invention solves toluene and rich olefins lower carbon number hydrocarbons or coal base, bio-based oxygenatedchemicals
High-quality high-octane rating clean vehicle gasoline process bed temperature rise, catalyst easy in inactivation etc. should be produced close
A key technology difficult problem, has that flow process is simple, energy consumption is low, operation scheme motility is strong, clean vehicle gasoline
Product yield and the high advantage of octane number.
Detailed description of the invention
The present invention will be further described by following example, but not thereby limiting the invention.
Embodiment 1
The method using the present invention to provide, with catalytic cracked dry gas (composition is shown in Table 1) and petroleum toluene be
Raw material.DL0812 catalyst divides 4 grades of equal proportion fillings in the reactor.
Table 1 catalytic cracked dry gas forms
| H2 | O2 | N2 | COx | CH4 | C2H4 | C2H6 | C3H6 | C3H8 | C4 | Others | |
| Vol% | 15.21 | 0.43 | 22.37 | 2.98 | 25.93 | 19.52 | 11.62 | 1.29 | 0.43 | 0.12 | 0.1 |
Catalytic cracked dry gas is divided into 4 tunnels to enter after heat exchange respectively in reactor Catalyst packing at different levels ratio
Level beds entrance, wherein the first order reacts entrance catalytic cracked dry gas raw material with toluene (containing fresh
Toluene and circulation toluene) enter reactor after Hybrid Heating, react on a catalyst.Reaction condition
As follows: each section of reaction bed inlet temperature 350 DEG C, pressure 1.0MPa, toluene/olefin molar ratio 3.0,
Alkene air speed 0.5h-1。
Conversion of ethylene and total alkene conversion in dry gas > 99%, alkene generates C5+ selectivity > 99%.
After separated, toluene loops back reactor inlet, and hydro carbons liquid product is fractionated into obtaining high-octane rating vapour
Oily and a small amount of light diesel fuel component, gasoline products mediation RON octane number > 120, it is substantially free of sulfur the most nitrogenous,
It it is the high-quality clean vehicle gasoline blend component of high-quality.
Embodiment 2
Using the method that the present invention provides, to be the richest in the light aromatic hydrocarbons of benzene, (toluene level～75wt%, remaining is benzene
And aliphatic hydrocarbon), after ether carbon four (olefin(e) centent～47wt%) and oxygenatedchemicals (mass ratio is: methanol: two
Methyl ether: ethanol: isobutanol=4:3:2:1) it is raw material, wherein after ether, carbon four and oxygenatedchemicals mass ratio are
1:4.DL0822 catalyst divides 4 grades of section filling, reactor Catalyst packings at different levels such as not in the reactor
Ratio is 15:20:30:35.
After ether, carbon four enters the 1st grade of beds entrance, the 2nd～4 grading oxygen-containing chemical combination after heat exchange
Raw material.Wherein first order reaction entrance carbon four raw material and methylbenzene raw material (containing fresh toluene and circulation toluene)
Enter reactor after Hybrid Heating, DL0822 occurs alkylation, be dehydrated, be polymerized, isomerization,
Aromatisation, hydrogen migration etc. are reacted.Reaction condition is as follows: each section of reaction bed inlet temperature 420 DEG C, pressure
Power 0.2MPa, light virtue is 1.5 with the mol ratio of (carbon four and oxygenatedchemicals after ether), alkene and containing oxidation
Compound air speed 0.2h-1.Alkene and oxygenatedchemicals conversion ratio > 99%, clean fuel yield > 99%.Warp
After separation, toluene loops back reactor inlet, and hydro carbons liquid product is fractionated into obtaining high-knock rating gasoline
With a small amount of light diesel fuel component, a small amount of automobile-used alkane liquid gas of by-product and very small amount dry gas.Gasoline products is adjusted
With RON octane number > 115, it is substantially free of sulfur the most nitrogenous, can be in harmonious proportion as high-quality clean vehicle gasoline
Component.
Embodiment 3
Use the method that the present invention provides, with Rich propylene (its composition is shown in Table 2) and petroleum toluene as raw material,
DL0805 catalyst divides the section fillings such as 5 sections in the reactor.
Rich propylene is divided into 5 tunnels to enter at different levels urging after heat exchange in reactor Catalyst packing at different levels ratio
Agent bed inlet, wherein the first order reaction entrance Rich propylene raw material and toluene (containing fresh toluene with follow
Ring toluene) enter reactor after Hybrid Heating, react on a catalyst.Reaction condition is as follows: each
Section reaction bed inlet temperature 170 DEG C, pressure 3.0MPa, benzene alkene mol ratio 2.0, alkene air speed 1.0h-1。
Propylene and total alkene conversion are equal > 99%, alkene generates C5+ selectivity > 99%.Product is separated, first
Benzene loops back alkylation reactor, and alkylation liquid is fractionated into obtaining high-knock rating gasoline and a small amount of light diesel fuel group
Point, gasoline products mediation octane number > 120, it is substantially free of sulfur the most nitrogenous, can be automobile-used clearly as high-quality
Clean gasoline blend component.
Table 2 Rich propylene forms
| C3H6 | C3H8 | C2H4 | C2H6 | CH4 | C4H8 | C4H10 | |
| Vol% | 57.46 | 8.59 | 19.62 | 2.33 | 1.02 | 7.3 | 3.68 |
Above-described embodiment only for technology design and the feature of the present invention are described, its object is to allow and is familiar with this
The personage of item technology will appreciate that present disclosure and implements according to this, can not limit the present invention with this
Protection domain.All equivalence changes made according to spirit of the invention or modification, all should contain
Within protection scope of the present invention.
Claims (6)
1. the production method of a high-quality cleaning fuel, it is characterised in that use toluene and rich olefins
Lower carbon number hydrocarbons and/or coal base, bio-based oxygenatedchemicals reaction production high-quality high-octane rating automobile-used cleaning vapour
Oil, particularly as follows: raw material rich olefins lower carbon number hydrocarbons and/or oxygenatedchemicals are divided into multichannel, enters after heat exchange
Each reaction bed of multistage fixed bed reactor；Raw material toluene enters reactor from top, with lower carbon number hydrocarbons
And/or occur on a catalyst after oxygenatedchemicals mixing alkylation, be dehydrated, be polymerized, isomerization, virtue
Structure, hydrogen transfer reaction；Product is isolated to hydro carbons liquid phase component and gaseous component；Wherein
Liquid phase component is fractionated into obtaining rich aromatic hydrocarbons high octane gasoline component and light diesel fuel component, and gaseous component divides
From for dry gas and automobile-used alkane liquid gas；
Described multistage fixed bed catalytic reactor, its bed progression is 2～5 grades:
Its first order bed controls alkene by the mixing of rich olefins lower carbon number hydrocarbons and oxygenatedchemicals and toluene
Hydrocarbon and oxygenatedchemicals mass percent concentration, it is achieved the control to reaction bed temperature rise, in its charging
Alkene/oxygenatedchemicals mass percent concentration computational methods are as follows: (l × x+m × y) ÷ (l+m+n)=
P, wherein l, m, n are respectively rich olefins lower carbon number hydrocarbons, oxygenatedchemicals and the charging of toluene unit interval
Amount, x and y is respectively in rich olefins lower carbon number hydrocarbons alkyl in alkene mass percent concentration, oxygenatedchemicals
Mass percentage content；P is the mixed alkene of all chargings/oxygenatedchemicals mass percent concentration,
In the range from 12～30%；After determining p value according to reaction bed pre-control temperature rise, can be according to above-mentioned formula
Calculate inlet amount n of saturated hydrocarbons unit interval；
The control of the 2nd～5 grade of beds temperature rise, by entering this grade of bed from previous stage bed
Rich olefins lower carbon number hydrocarbons that component and this grade of bed newly inject and the mixing of oxygenatedchemicals are to control alkene/contain
The concentration of oxygen compound, or interpolation certain proportion cold toluene controls alkene and oxygenatedchemicals further
Concentration and temperature, thus realize effective control of temperature rise；Alkene in the charging of its 2～5 reaction beds at different levels
The density calculating method of hydrocarbon/oxygenatedchemicals is as follows: (l × x+m × y) ÷ (l+m+n+h)=p, wherein l,
M, n are respectively entering of the rich olefins lower carbon number hydrocarbons of this grade of bed, oxygenatedchemicals and cold toluene unit interval
Doses, x and y is respectively in rich olefins lower carbon number hydrocarbons hydrocarbon in alkene mass percent concentration, oxygenatedchemicals
Base mass percentage content；H is the unit time interior component entering this grade of bed from previous stage bed
Amount；P is the mixed alkene of all chargings/oxygenatedchemicals mass percent concentration, in the range from
12-30%；After determining p value according to reaction bed pre-control temperature rise, i.e. the charge ratio of adjustable l, m, n
Example makes above-mentioned equation set up, it is achieved the control to reaction bed temperature rise；
Described catalyst is DL0812, DL0822 that Dalian Inst of Chemicophysics, Chinese Academy of Sciences produces
Or DL0805 commercial catalyst；
The reaction condition of described course of reaction is: reaction temperature 160～450 DEG C, pressure 0.1～4.0MPa,
Rich olefins lower carbon number hydrocarbons and/or oxygenate feedstock air speed are 0.1～2.0h-1, toluene and rich olefins lower carbon number hydrocarbons
And/or oxygenatedchemicals mol ratio is 1.2～4.0, single reaction bed temperature rise is 10～50 DEG C.
2. according to the production method of high-quality cleaning fuel described in claim 1, it is characterised in that: institute
State raw material toluene to be petroleum toluene, coking hydrogenation toluene, mix light aromatic hydrocarbons, be the richest in benzene light fraction oil
The mixture of one or more.
3. according to the production method of high-quality cleaning fuel described in claim 1, it is characterised in that: institute
Stating raw material rich olefins lower carbon number hydrocarbons is that one of carbon four is planted or many after dry gas, Rich propylene, liquefied gas, ether
The mixture planted, olefin(e) centent is not less than 10wt%.
4. according to the production method of high-quality cleaning fuel described in claim 3, it is characterised in that institute
State in rich olefins lower carbon number hydrocarbons raw material:
Sulfur content>50ppm time, desulfurization of raw material system is set, controls sulfur content<10ppm after desulfurization of raw material；
Alkadienes and alkynes component total content > 100ppm time, raw material first chosen property hydrogenation reactor reaction,
Control diene and alkynes total content < 10ppm in raw material；Sulfur content < 50ppm and alkadienes and alkynes group
< during 100ppm, rich olefins lower carbon number hydrocarbons raw material is directly entered alkylation reactor to divide total content.
5. according to the production method of high-quality cleaning fuel described in claim 1, it is characterised in that: institute
Stating feedstock oxygenates is the coal base/methanol of bio-based, dimethyl ether, ethanol, glycerol, butanol, different
One of butanol oxygenatedchemicals kind or multiple mixture.
6. according to the production method of high-quality cleaning fuel described in claim 1, it is characterised in that: anti-
The condition is answered to be: temperature 180～420 DEG C, pressure 0.5～3.5MPa, rich olefins lower carbon number hydrocarbons and/or containing oxidation
Compound Feed space velocities is 0.2～1.0h-1, toluene and rich olefins lower carbon number hydrocarbons and/or oxygenatedchemicals mol ratio
1.5～3.5.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106770891A (en) * | 2016-12-30 | 2017-05-31 | 神华集团有限责任公司 | Catalyst test apparatus and evaluation method |
| CN107118800A (en) * | 2017-06-12 | 2017-09-01 | 煤炭科学技术研究院有限公司 | HC fuel and preparation method thereof |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104419441A (en) * | 2013-09-02 | 2015-03-18 | 中国科学院大连化学物理研究所 | Method of producing gasoline blending component with high octane value by light aromatic hydrocarbon and/or alcohol/ether compound |
-
2015
- 2015-05-04 CN CN201510221987.4A patent/CN106190287A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104419441A (en) * | 2013-09-02 | 2015-03-18 | 中国科学院大连化学物理研究所 | Method of producing gasoline blending component with high octane value by light aromatic hydrocarbon and/or alcohol/ether compound |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106770891A (en) * | 2016-12-30 | 2017-05-31 | 神华集团有限责任公司 | Catalyst test apparatus and evaluation method |
| CN107118800A (en) * | 2017-06-12 | 2017-09-01 | 煤炭科学技术研究院有限公司 | HC fuel and preparation method thereof |
| CN107118800B (en) * | 2017-06-12 | 2019-04-12 | 煤炭科学技术研究院有限公司 | HC fuel and preparation method thereof |
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