CN105018128B - Method and catalyst for preparing high-octane rating gasoline component - Google Patents
Method and catalyst for preparing high-octane rating gasoline component Download PDFInfo
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- CN105018128B CN105018128B CN201410168005.5A CN201410168005A CN105018128B CN 105018128 B CN105018128 B CN 105018128B CN 201410168005 A CN201410168005 A CN 201410168005A CN 105018128 B CN105018128 B CN 105018128B
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Abstract
The invention relates to a preparation method of a high-octane rating gasoline component as well as a catalyst for preparing the high-octane rating gasoline component. The method comprises the following steps: enabling benzene and methanol to contact and react with the catalyst under the conditions that the temperature ranges from 350 to 500 DEG C and the pressure ranges from 0.1 to 1 MPa, wherein the molar ratio of the benzene to methanol is (0.3-2):1, the catalyst comprises an IM-5 molecular sieve containing phosphorus and a selectable bonding agent, and the content of phosphorus in the IM-5 molecular sieve containing the phosphorus is 1 to 10 percent according to P2O5. By adopting the method, the benzene and methanol can react to produce the gasoline high-octane rating component.
Description
Technical field
It is the present invention relates to a kind of preparation method of high octane gasoline component and a kind of for preparing the high-octane rating vapour
The catalyst of oil ingredient.
Background technology
Require to improve constantly in China's gasoline standard and exhaust emissions, and the big back of the body that high sulfur bauxite amount continues to increase
Under scape, due to sulfur reduction, Olefin decrease, cause gasoline pool loss of octane number of the China based on catalytically cracked gasoline larger, need for this
Want substantial amounts of antiknock component to reconcile gasoline.
Methanol is directly used as vehicle fuel and has certain advantage, but while there is obvious defect, such as methanol is poisonous,
Combustion heat value is low, combustibility is bad, hygroscopicity is strong, corrode and wear and tear electromotor, swelling sealing member etc., it is therefore necessary to research and develop
Convert methanol into the new way of vehicle fuel.
High octane gasoline component can be produced using benzene and methanol alkylation.Existing benzene/methanol alkylation method master
, used as catalytic active component, these method generally existing benzene conversion ratios are low for ZSM-5 to be adopted or the molecular sieve with MWW structures
And/or the deficiency that methanol alkylation rate is not high.(synthesis of multi-stage porous ZSM-5 molecular sieve and catalysis benzene, the methanol alkylation such as Lu Lu
The research of reaction, petroleum journal, 2012,2：111-115) using the catalysis benzene/methanol alkyl of the ZSM-5 molecular sieve with multi-stage porous
Change reaction, compared with common ZSM-5 molecular sieve, benzene conversion ratio can be made to improve about 9%, but its benzene conversion ratio is still not high enough, only up to
To 55%.CN102600887A reports anti-with the MCM-22 molecular sieve catalytics benzene/methanol alkylation of supported alkaline earth, rare earth metal
Should, under conditions of benzene is 2 with methanol molar ratio, makes the alkyl rate of methanol reach 90% or so, but benzene conversion ratio only has
45%.
As methanol is directly used as the restriction of the defect of vehicle fuel and gasoline standard to benzene content, therefore utilizing benzene
When producing high octane gasoline component with methanol alkylation, needs isolate benzene and methanol from product stream as recycle
Material.If benzene conversion ratio is low and/or methanol alkylation rate is not high, more recycle stocks will be caused, increase the energy of technical process
Consumption.In addition, when high octane gasoline component being produced using benzene and methanol alkylation, need to avoid as far as possible to generate non-gasoline and evaporate
Low value C of journey5 -Fraction.
Existing document is disclosed using IM-5 molecular sieve catalytic toluene and methanol alkylated reactions, using HIM-5 molecular sieves
When, toluene conversion is up to 55% or so, if carrying out P Modification to the molecular sieve, toluene conversion is significantly reduced.For
For ZSM-5, P Modification also results in toluene conversion and significantly reduces.Related document has CN102205251A.
The content of the invention
An object of the present invention is to improve benzene conversion ratio and the methanol alkylation rate of benzene/methanol alkylation reaction.This
The two of bright purpose are the C for avoiding benzene/methanol alkylation from generating non-gasoline boiling range in reacting5 -Fraction.The third object of the present invention
It is the recyclability for improving benzene/methanol alkylation catalyst.
Such as it is not particularly illustrated, the percentage composition in the present invention is weight/mass percentage composition.
A kind of preparation method of high octane gasoline component, under conditions of 350 DEG C～500 DEG C, 0.1MPa～1MPa, will
Benzene and methanol are contacted with catalyst, are reacted, the mol ratio 0.3～2 of benzene and methanol：1, the catalyst includes phosphorous IM-5 point
Son sieve and optional binding agent, in the phosphorous IM-5 molecular sieves, with P2O5The phosphorus content of meter is 1%～10%.
In the phosphorous IM-5 molecular sieves, SiO2/Al2O3Mol ratio is 20～150, preferably 30～80.
In the phosphorous IM-5 molecular sieves, with P2O5The phosphorus content of meter preferably 2%～8%, more preferably 3%～
5%.
Those skilled in the art know the method for carrying out P Modification to IM-5 molecular sieves, such as, refer to
Method in CN102205251A.
Preferably, the catalyst includes 30%～90% phosphorous IM-5 molecular sieves and 10%～70% bonding
Agent；It is highly preferred that the catalyst includes 50%～90% phosphorous IM-5 molecular sieves and 10%～50% binding agent.This
Art personnel know the binding agent for preparing molecular sieve catalyst, and conventional binding agent has aluminium oxide or silicon oxide, glues
Knot agent precursor is usually hydrated alumina, such as boehmite or boehmite, or Ludox.
Reaction temperature is preferably 400 DEG C～450 DEG C, and reaction pressure is preferably 0.1MPa～0.6MPa, and benzene is rubbed with methanol
That ratio preferably 0.5～1.5：1, more preferably 0.6～1.2：1.
The reaction condition further optimized in continuous production is：Reaction raw materials mass space velocity is 0.5～15 hour-1, more
It is preferred that 1～12 hour-1；The mole of carrier gas is 0～20 with the ratio of the integral molar quantity of mixed material：1, more preferably 0～12：1.This
Art personnel know the function and species of inert carrier gas, typically carry reaction raw materials with nitrogen and enter beds,
Can be using water vapour as carrier gas.
In the phosphorous IM-5 molecular sieves, rare earth metal can also be contained, the oxide with rare earth metal as trivalent is counted,
Rare earth metal content can be 3%～15%, preferably 5%～15%.
The rare earth metal is preferably lanthanum (La), cerium (Ce), praseodymium (Pr), neodymium (Nd), promethium (Pm), samarium (Sm) and europium (Eu) etc.
In one or more.In the rare earth metal content scope of defined, to oxide of all rare earth metals with which as trivalent
Its content is counted, such as La is with La2O3Meter, Ce are with Ce2O3Meter, Pr are with Pr2O3Meter, Nd are with Nd2O3Meter, Pm are with Pm2O3Meter, Sm with
Sm2O3Meter and Eu are with Eu2O3Meter etc..
A kind of catalyst for preparing high octane gasoline component, IM-5 molecular sieves including phosphorous and rare earth metal and
Optional binding agent, in the IM-5 molecular sieves of described phosphorous and rare earth metal, with P2O5The phosphorus content of meter is 1%～10%；With dilute
Oxide meter of the earth metal for trivalent, rare earth metal content are 3%～15%.
In the IM-5 molecular sieves of described phosphorous and rare earth metal, the oxide with rare earth metal as trivalent is counted, rare earth metal
Content is preferably 5%～15%.
The rare earth metal is preferably lanthanum (La), cerium (Ce), praseodymium (Pr), neodymium (Nd), promethium (Pm), samarium (Sm) and europium (Eu) etc.
In one or more.In the rare earth metal content scope of defined, oxide of all rare earth metals with which as trivalent is counted
Its content, such as La is with La2O3Meter, Ce are with Ce2O3Meter, Pr are with Pr2O3Meter, Nd are with Nd2O3Meter, Pm are with Pm2O3Meter, Sm are with Sm2O3
Meter and Eu are with Eu2O3Meter etc..
Preferably, the catalyst include 30%～90% phosphorous and rare earth metal IM-5 molecular sieves and 10%～
70% binding agent；It is highly preferred that the catalyst include 50%～90% phosphorous and rare earth metal IM-5 molecular sieves and
10%～50% binding agent.Those skilled in the art know the binding agent for preparing molecular sieve catalyst, conventional bonding
Agent has aluminium oxide or a silicon oxide, and binding agent precursor is usually hydrated alumina, such as boehmite or boehmite, or
Ludox.
The invention provides a kind of method for preparing above-mentioned catalyst, including：
(1) ion exchange is carried out with the solution and H-IM-5 molecular sieves of phosphorus-containing compound, obtain P/IM-5 molecular sieves；
(2) impregnated with P/IM-5 molecular sieves with the solution containing rare earth metal.
Described phosphorus-containing compound is selected from phosphoric acid, ammonium phosphate, ammonium hydrogen phosphate, ammonium dihydrogen phosphate, triphenyl phosphorus and tricresyl phosphate
In methyl ester one or more.
In step (1), the mode of ion exchange preferably adopts infusion process.During dipping, the solution and H-IM- of phosphorus-containing compound
The liquid/solid ratio of 5 molecular sieves is 1ml/g～5ml/g, preferred 2ml/g～4ml/g；Dip time is 2 hours～5 hours, dipping temperature
Spend for 40 DEG C～85 DEG C.Solid after dipping obtains final product P/IM-5 molecules in 90 DEG C～120 DEG C dryings, 450 DEG C～550 DEG C roastings
Sieve.
In step (2), during dipping, the solution containing rare earth metal is 1ml/g～5ml/ with the liquid/solid ratio of P/IM-5 molecular sieves
G, preferably 2ml/g～4ml/g, dip time are 2 hours～5 hours, and dipping temperature is 40 DEG C～85 DEG C.Solid after dipping exists
90 DEG C～120 DEG C dryings, 450 DEG C～550 DEG C roastings, obtain final product P-La/IM-5 molecular sieves.
In this specification, when scope or multiple occurrences is given to amount, concentration or other values or parameter, it should be understood
For specifically disclosing by the institute for arbitrarily being formed with any range lower limit or occurrence to any range higher limit or occurrence
There is scope, whether separately disclose these numerical value pair.
The present invention is alkylated reaction using the extensive benzene of Commercial sources with cheap methanol, not only can provide
For the antiknock component that gasoline reconciles, but also vehicle fuel can be converted methanol into.Compared with prior art, this
It is bright while significantly improving benzene conversion ratio and methanol alkylation rate, it means that less circulated material quantity, significantly can subtract
The energy consumption of few process units；The present invention can also generate, even not generate the C of non-gasoline boiling range less5 -Fraction；Changed by rare earth
Property, invention also improves the recyclability of benzene/methanol alkylation catalyst.
Specific embodiment
In embodiment,
Benzene conversion ratio=[benzene mole number in (benzene mole number in benzene mole number product in reactant)/reactant] ×
100%,
Methanol alkylation rate=[(toluene molar number+C8Aromatic hydrocarbons molal quantity × 2+C9First in aromatic hydrocarbons molal quantity × 3)/reactant
Alcohol molal quantity] × 100%.
Example 1
Prepare P/IM-5 molecular sieves.
(1) H-IM-5 molecular sieves are prepared
By SiO2/Al2O3Mol ratio be 47 NaIM-5 molecular sieve concentration be the ammonium nitrate solution of 0.5mol/L in 80
DEG C carry out ion exchange 3 times, every time 2 hours.The molecular sieve of gained after exchange is washed with deionized, then at 90 DEG C of dryings 10
Hour, 500 DEG C of roastings 5 hours, H-IM-5 molecular sieve Z are obtained0, its Na2O content is less than 0.1 mass %.
(2) P/IM-5 molecular sieves are prepared
By ammonium dihydrogen phosphate that above-mentioned H-IM-5 molecular sieves concentration is 0.2mol/L with the liquid/solid ratio of 2.12ml/g
In 80 DEG C of stirring dippings two hours, 90 DEG C of dryings 10 hours, 500 DEG C of roastings 4 hours were obtained the P/IM-5 molecular sieves of P Modification
Z1, its P2O5Content is 3.0 mass %.
Example 2
P/IM-5 molecular sieves are prepared by the method for example 1, except for the difference that with the phosphoric acid hydrogen that concentration is 0.2mol/L in (2) step
Two ammonium salt solutions are with the liquid/solid of 3.52ml/g than dipping Z0Molecular sieve, is obtained P/IM-5 molecular sieve Z after drying, roasting2, its P2O5
Content is 5.0 mass %.
Example 3
P/IM-5 molecular sieves are prepared by the method for example 1, except for the difference that with the phosphoric acid hydrogen that concentration is 0.2mol/L in (2) step
Two ammonium salt solutions are obtained P/IM-5 molecular sieve Z with the liquid/solid of 5.63ml/g than dipping Z0 molecular sieves after drying, roasting3, its P2O5
Content is 8.0 mass %.
Example 4
P/IM-5 molecular sieves are prepared by the method for example 1, except for the difference that with the phosphoric acid hydrogen that concentration is 0.2mol/L in (2) step
Two ammonium salt solutions are with the liquid/solid of 1.41ml/g than dipping Z0Molecular sieve, is obtained P/IM-5 molecular sieve Z after drying, roasting4, its P2O5
Content is 2.0 mass %.
Example 5
P-IM-5 molecular sieves are prepared by the method for example 1, except for the difference that with the phosphoric acid hydrogen that concentration is 0.2mol/L in (2) step
Two ammonium salt solutions are with the liquid/solid of 6.35ml/g than dipping Z0Molecular sieve, is obtained P/IM-5 molecular sieve Z after drying, roasting5, its P2O5
Content is 9.0 mass %.
Example 6～12
Example 6～12 is used for evaluating catalytic performance of the IM-5 molecular sieves of P Modification in benzene/methanol alkylation reaction.
On fixed-bed reactor, 2.0g molecular sieves are loaded, N is used2For carrier gas, by the amount that benzyl alcohol mol ratio is 11
Benzene and methanol is passed through, in 450 DEG C, 0.28MPa, feedstock quality air speed 4.0 hours-1, carrier gas N2It is 10 with mixed material mol ratio
Under conditions of reacted, the results are shown in Table 1.
Table 1
As shown in Table 1, compared with HZSM-5 molecular sieves, the benzene conversion ratio of HIM-5 molecular sieves and methanol alkylation rate with
HZSM-5 molecular sieves are suitable；It has surprisingly been found that compared with HIM-5 molecular sieves, the benzene conversion ratio of P/IM-5 molecular sieves and first
Alcohol alkyl rate is significantly improved.
Example 13
Prepare the catalyst containing binding agent and P/IM-5 molecular sieves.
Take the Z of 50g1Molecular sieve, is sufficiently mixed uniformly with 18.5g boehmites (aluminium oxide containing 66.3 mass %),
Suitable quantity of water is added to mediate, extruded moulding, 90 DEG C of dryings 10 hours, 500 DEG C of roastings 4 hours, pelletizing is obtained catalyst C1, wherein contain
The Z of 80 mass %1The aluminium oxide of molecular sieve, 20 mass %.
Example 14
Catalyst is prepared by the method for example 13, except for the difference that with 41.7 Ludox (silicon dioxide containing 30 mass %) generation
For boehmite, roller forming, 90 DEG C of dryings 10 hours, 500 DEG C of roastings 4 hours are obtained catalyst C2, wherein containing 80 matter
The Z of amount %1The silicon oxide of molecular sieve, 20 mass %.
Example 15
Catalyst is prepared by the method for example 13, is except for the difference that replaced Z1 molecular sieves with Z2 molecular sieves, and is intended thin with 50.4g
Diaspore and Z2Molecular sieve extruded moulding, drying, roasting, pelletizing are obtained catalyst C3, the Z wherein containing 60 mass %2Molecule
Sieve, the aluminium oxide of 40 mass %.
Example 16～18
Example 16～18 is used for evaluating the performance of the alkylation catalyst containing binding agent.
On fixed-bed reactor, 2.0g catalyst is loaded, by benzene：Methanol molar ratio is 1：1 amount is passed through benzene and first
Alcohol, in 440 DEG C, 0.28MPa, feedstock quality air speed 4.0 hours-1, with water vapour as carrier gas, water is 4 with mixed material mol ratio
Under conditions of reacted, the results are shown in Table 2.
Table 2
Example 19
Prepare P-La/IM-5 molecular sieves.
By numbering Z in embodiment 10Molecular sieve concentration be the ammonium dihydrogen phosphate of 0.2mol/L with 2.12ml/g's
In 80 DEG C of stirring dippings two hours, 90 DEG C of dryings 10 hours, 500 DEG C of roastings 4 hours were obtained the P/IM-5 of P Modification to liquid/solid ratio
Molecular sieve, then the lanthanum nitrate hexahydrate that above-mentioned P/IM-5 molecular sieves concentration is 0.2mol/L is existed with the liquid/solid ratio of 3.07ml/g
80 DEG C of stirring dippings two hours, 90 DEG C of dryings 10 hours, 500 DEG C of roastings 4 hours are obtained the composite modified P-La/IM-5 of phosphorus lanthanum
Molecular sieve Z6, its P2O5Content be 3.0 mass %, La2O310 mass % of content.
Example 20
P-La/IM-5 molecular sieves are prepared by the method for example 19, except for the difference that with the phosphoric acid hydrogen two that concentration is 0.2mol/L
Ammonium salt solution is with the liquid/solid of 3.52ml/g than dipping Z0Molecular sieve, is obtained P/IM-5 molecular sieves after drying, roasting, then by P/IM-
5 molecular sieve concentration are that the lanthanum nitrate hexahydrate of 0.2mol/L stirs dipping two hours with the liquid/solid ratio of 4.60ml/g at 80 DEG C, 90
DEG C drying 10 hours, 500 DEG C of roastings 4 hours, is obtained the composite modified P-La/IM-5 molecular sieve Z of phosphorus lanthanum7, its P2O5Content is 5
Quality %, La2O315 mass % of content.
Example 21
P-La/IM-5 molecular sieves are prepared by the method for example 19, except for the difference that with the biphosphate that concentration is 0.2mol/L
Ammonium salt solution is with the liquid/solid of 3.52ml/g than dipping Z0Molecular sieve, is obtained P/IM-5 molecular sieves after drying, roasting, then by P/IM-
5 molecular sieve concentration are that the lanthanum nitrate hexahydrate of 0.2mol/L is less than impregnating two in 80 DEG C of stirrings together with the liquid/solid of 3.68ml/g
When, 90 DEG C of dryings 10 hours, 500 DEG C of roastings 4 hours are obtained the composite modified P-La/IM-5 molecular sieve Z of phosphorus lanthanum8, its P2O5Contain
Measure as 5 mass %, La2O312 mass % of content.
Example 22
P-La/IM-5 molecular sieves are prepared by the method for example 19, except for the difference that with the phosphoric acid hydrogen two that concentration is 0.2mol/L
Ammonium salt solution is with the liquid/solid of 5.68ml/g than dipping Z0Molecular sieve, is obtained P/IM-5 molecular sieves after drying, roasting, then by P/IM-
5 molecular sieve concentration are that the lanthanum nitrate hexahydrate of 0.2mol/L is impregnated two hours with the liquid/solid ratio of 1.54ml/g, and 90 DEG C of dryings 10 are little
When, 500 DEG C of roastings 4 hours are obtained the composite modified P-La/IM-5 molecular sieve Z of phosphorus lanthanum9, its P2O5Content be 8 mass %, La2O3
5 mass % of content.
Example 23
P-La/IM-5 molecular sieves are prepared by the method for example 22, SiO is except for the difference that first used2/Al2O3Mol ratio be 68
NaIM-5 molecular sieves, prepare H-IM-5 molecular sieves using the method for example 1 and then substitute Z with which0Molecular sieve, is obtained phosphorus lanthanum and is combined
Modified P-La/IM-5 molecular sieve Z10, its P2O5Content be 8 mass %, La2O35 mass % of content.
Example 24
Phosphorus-mischmetal (P-RE/IM-5) molecular sieve is prepared by the method for example 19, except for the difference that with concentration is
The ammonium dihydrogen phosphate of 0.2mol/L is with the liquid/solid of 3.52ml/g than dipping Z0Molecular sieve, is obtained P/ after drying, roasting
IM-5 molecular sieves, then the hydrochloric acid solution of the mischmetal that P/IM-5 molecular sieve concentration is 0.2mol/L (is consisted of into LaCl3：
CeCl3：YCl3：Other=27.8：70.1：1.9：0.2) with the liquid/solid of 3.68ml/g than little in 80 DEG C of stirring dippings two together
When, 90 DEG C of dryings 10 hours, 500 DEG C of roastings 4 hours are obtained the composite modified P-RE/IM-5 molecular sieve Z of phosphorus mischmetal11, its
P2O5Content be 5 mass %, RE2O312 mass % of content.
Example 25
Prepare the catalyst containing binding agent and P-La/IM-5 molecular sieves.
Take the Z of 50g7Molecular sieve, is sufficiently mixed uniformly with 41.7 Ludox (silicon dioxide containing 30 mass %), is added suitable
Amount water roller forming, 90 DEG C of dryings 10 hours, 500 DEG C of roastings 4 hours are obtained catalyst C4, the Z wherein containing 80 mass %7Molecule
Sieve, the silicon oxide of 20 mass %.
Example 26～33
Example 26～32 evaluates the performance of modified molecular screen and catalyst in benzyl alcohol alkylated reaction.
On fixed-bed reactor, 2.0g molecular sieves are loaded, N is used2For carrier gas, by the amount that benzyl alcohol mol ratio is 11
Benzene and methanol is passed through, in 430 DEG C, 0.28MPa, feedstock quality air speed 4.0 hours-1, carrier gas N2It is 4 with mixed material mol ratio
Under the conditions of reacted.Methanol alkylation rate in example 26～32 is all higher than 98%, and other the results are shown in Table 1.
Table 3
*Z2Reaction condition is shown in the condition of example 6～12
Implement 34～35
Implementing 34～35 is used for illustrating the recyclability of catalyst.
The regeneration condition of catalyst is：In air atmosphere, with the ramp of 2 DEG C/min to 540 DEG C, 540 DEG C of constant temperature 4 are little
When.
On fixed-bed reactor, 2.0g molecular sieves are loaded, N is used2For carrier gas, by the amount that benzyl alcohol mol ratio is 11
Benzene and methanol is passed through, in 440 DEG C, 0.28MPa, feedstock quality air speed 8.0 hours-1, carrier gas N2It is 10 with mixed material mol ratio
Under conditions of reacted, the results are shown in Table 4.
Table 4
Claims (7)
1. a kind of preparation method of high octane gasoline component, including：In 350 DEG C～500 DEG C, the condition of 0.1MPa～1MPa
Under, benzene and methanol are contacted with catalyst, reacted, the mol ratio 0.3～2 of benzene and methanol：1, the catalyst includes phosphorous
IM-5 molecular sieves and optional binding agent, in the phosphorous IM-5 molecular sieves, with P2O5The phosphorus content of meter is 1%～10%.
2. in accordance with the method for claim 1, it is characterised in that in the phosphorous IM-5 molecular sieves, SiO2/Al2O3Mole
Than for 30～80.
3. in accordance with the method for claim 1, it is characterised in that in the phosphorous IM-5 molecular sieves, with P2O5The phosphorus of meter contains
Measure as 3%～5%.
4. in accordance with the method for claim 1, it is characterised in that the catalyst includes 30%～90% phosphorous IM-5
Molecular sieve and 10%～70% binding agent.
5. in accordance with the method for claim 1, it is characterised in that reaction temperature is 400 DEG C～450 DEG C, reaction pressure is
0.1MPa～0.6MPa, benzene are 0.6～1.2 with the mol ratio of methanol：1.
6. in accordance with the method for claim 1, it is characterised in that in the phosphorous IM-5 molecular sieves, also containing rare earth gold
Category, the oxide with rare earth metal as trivalent are counted, and rare earth metal content is 3%～15%.
7. in accordance with the method for claim 6, it is characterised in that the rare earth metal is lanthanum, cerium, praseodymium, neodymium, promethium, samarium and europium
In one or more.
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| CN107151022B (en) * | 2016-03-02 | 2020-03-24 | 中国石油化工股份有限公司 | Mesoporous P-IM-5 molecular sieve, and preparation method and application thereof |
| CN107552086B (en) * | 2016-06-30 | 2021-01-08 | 中国石油化工股份有限公司 | Modified IM-5 molecular sieve, preparation method and application thereof, and toluene methanol alkylation reaction method |
| CN107971016B (en) * | 2016-10-21 | 2019-10-25 | 中国石油化工股份有限公司 | A kind of catalytic cracking catalyst and preparation method thereof containing phosphorous IMF structure molecular screen |
| CN115725320B (en) * | 2021-08-31 | 2024-10-11 | 中国石油化工股份有限公司 | Method for reducing benzene content in gasoline |
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