CN107866254A - Catalyst for the equal acid anhydride of durol gaseous oxidation system - Google Patents
Catalyst for the equal acid anhydride of durol gaseous oxidation system Download PDFInfo
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- CN107866254A CN107866254A CN201610846430.4A CN201610846430A CN107866254A CN 107866254 A CN107866254 A CN 107866254A CN 201610846430 A CN201610846430 A CN 201610846430A CN 107866254 A CN107866254 A CN 107866254A
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- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
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- B01J27/22—Carbides
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- C07D493/00—Heterocyclic compounds containing oxygen atoms as the only ring hetero atoms in the condensed system
- C07D493/02—Heterocyclic compounds containing oxygen atoms as the only ring hetero atoms in the condensed system in which the condensed system contains two hetero rings
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Abstract
The present invention relates to a kind of catalyst for the equal acid anhydride of durol gaseous oxidation system, it is more mainly to solve the side reaction of durol gas phase oxidation in the prior art, the problem of causing equal acid anhydride yield low.The present invention uses oxide catalyst, and the catalyst uses α Al2O3, carborundum, ceramic ring or its mixture be carrier, active component includes v element, lanthanide series, and the technical scheme of at least one of nonmetalloid and alkali earth metal, preferably resolves the technical problem, side reaction when reducing equal acid anhydride synthesis occurs, and improves the yield of equal acid anhydride.
Description
Technical field
The present invention relates to a kind of catalyst for the equal acid anhydride of durol gaseous oxidation system and preparation method thereof, and equal acid anhydride
Synthetic method.
Technical background
With developing rapidly for the industry such as oil refining, chemical fibre and polyester, large-scale ethylene plant, catalytic reforming unit, virtue
Hydrocarbon device, disproportionation, isomerization process etc. are by the substantial amounts of C10 aromatic hydrocarbons of by-product.Therefore, how effectively using C10 aromatic hydrocarbon resources into
For a big important topic of petrochemical industry.As the important intermediate of high added value fine chemical product, have 4 symmetrical carboxyls special
Many, which can be made, in the pyromellitic acid anhydride (PMDA, equal acid anhydride) of different structure has superior heat resistance, electrical insulating property and chemically-resistant medicine
The product of moral character.It is primarily useful for producing monomer, medicine intermediate, the epoxy resin of the heat stable resins such as polyimides, polyimidazole
Curing agent etc., the sophisticated technology such as aviation, aerospace, electronics industry field is can be widely applied to its manufactured product.Therefore, will refine
Change by-product C10 aromatic hydrocarbons in content it is higher durol extraction after be further processed into high added value equal acid anhydride have it is extremely important
Research Significance and significant economic benefit.
At present, vapour phase oxidation process is used mostly to prepare equal acid anhydride using durol as raw material, because the process is one multiple
Miscellaneous heterogeneous catalysis process, a variety of side reactions be present, cause the yield of equal acid anhydride very low.Vapour phase oxidation process prepares equal acid anhydride catalyst master
If using vanadium system as active component, it is aided with a small amount of metallic element, the theoretical yield that equal acid anhydride is calculated by chemical equation should
This reaches 163%, but the catalyst activity that traditional preparation method is worth is relatively low, and the actual recovery highest of equal acid anhydride is only capable of
Reach the 56% of theoretical yield.Therefore, it is to the selectivity of equal acid anhydride to improve catalyst by changing the preparation method of catalyst
It is very necessary.
CN101037439A discloses a kind of carrier model polyoxometallate catalyst, can react at a lower temperature.
CN01105883.8 reports one kind with V2O5And TiO2For major catalyst, Nb2O5、Cs2O and P2O5For the catalytic body of co-catalyst
System.US6084109 discloses a kind of V2O5-WO3Catalyst, manganese, antimony, bismuth, phosphorus, the oxide system of copper or its mixture.It is above-mentioned
Method is made in durol oxidation and had made great progress in the preparation of equal acid anhydride catalyst, but still it is relatively low equal acid anhydride yield to be present
Problem.
The content of the invention
One of technical problems to be solved by the invention are the problem of equal acid anhydride yield are low in the prior art, there is provided one kind is used for
The catalyst of the equal acid anhydride of durol gaseous oxidation system, the catalyst have the characteristics of equal acid anhydride high income.
The two of the technical problems to be solved by the invention are to provide a kind of with solving one of technical problem corresponding catalysis
The preparation method of agent.
The three of the technical problems to be solved by the invention are to provide a kind of with solving that one of technical problem is corresponding to be used for
The method of the equal acid anhydride of durol gaseous oxidation system.
To solve one of above-mentioned technical problem, technical scheme disclosed in this invention is：One kind is used for durol gas phase
The catalyst of equal acid anhydride is made in oxidation, it is characterised in that the catalyst uses α-Al2O3, carborundum, ceramic ring or its mixture is carry
Body, active component include v element, lanthanide series, and at least one of nonmetalloid and alkali earth metal.It is preferred that institute
State active component while including v element, lanthanide series, at least one element selected from nonmetalloid and selected from alkaline-earth metal
At least one of element.Now have between nonmetalloid and the element of alkaline-earth metal in terms of equal acid anhydride yield is improved and cooperate with
Effect.
In above-mentioned technical proposal, the lanthanide series is selected from least one of La, Ce, Pr, Nd, Sm and Eu.More preferably
For La and Ce.
In above-mentioned technical proposal, the nonmetalloid is selected from least one of B, Si, As, Te and Se.More preferably
B、Te。
In above-mentioned technical proposal, the alkali earth metal is selected from least one of Be, Mg, Ca, Sr and Ba.
In above-mentioned technical proposal, as most preferred technical scheme, the active component is simultaneously including v element, group of the lanthanides member
Element, nonmetalloid and alkali earth metal；Such as the active constituent includes V, La, B and Mg, or V, La, Te, Mg, Ba,
Either V, La, B, Te, Mg, Ca or V, La, Ce, B, Te, Mg, Ca.
In above-mentioned technical proposal, the ratio of v element and lanthanide series is 1 in the catalyst:(1-10), more preferably
1:(3-8)；The ratio of v element and nonmetalloid and alkali earth metal summation is 1 in the catalyst：(0.01-1), more
Preferably 1：(0.02-0.5).
To solve the two of above-mentioned technical problem, technical solution of the present invention is as follows：The technical scheme of one of above-mentioned technical problem
Described in the preparation method for the equal acid anhydride catalyst of durol gaseous oxidation system, it includes several steps：
(1) vanadium source is added in oxalic acid solution, obtains mixed solution；By lanthanide series, nonmetalloid and alkaline earth gold
Belong to element compound and add reaction system, obtain presoma；
(2) presoma is sprayed on carrier, catalyst is obtained after roasting.
In above-mentioned technical proposal, step (1) the vanadium source preferably is selected from vanadium oxide, metavanadate, positive vanadate and vanadium chloride
At least one.Step (1) described lanthanide series preferably is selected from lanthana, lanthanum chloride, lanthanum nitrate, lanthanum sulfate, lanthanum acetate, oxidation
At least one of cerium, cerous nitrate, cerous sulfate and cerous acetate.The compound of step (1) described nonmetalloid preferably is selected from boric acid, five
At least one of ammonium borate, borate, telluric acid, tellurium oxide and tellurate.The compound of step (1) described alkali earth metal
It preferably is selected from least one of alkaline earth oxide, chloride, nitrate, sulfate and acetate.
In above-mentioned technical proposal, the described preparation method for being used to synthesize equal acid anhydride catalyst, it is characterised in that by catalyst
Presoma be fitted into flush coater, at 210-265 DEG C heat after uniformly spray on carrier.
In above-mentioned technical proposal, the described preparation method for being used for durol and preparing equal acid anhydride catalyst, it is characterised in that
The carrier of catalyst precursor will be coated with Muffle kiln roasting, sintering temperature is 490-570 DEG C of temperature, roasting time 2-
8h。
To solve the three of above-mentioned technical problem, technical scheme is as follows：The method that durol prepares equal acid anhydride, with
Durol, air are raw material, using fixed bed reactors, synthesize equal acid anhydride in the presence of a catalyst.
Reaction process condition is as follows in above-mentioned technical proposal：The mass concentration of durol is 34-52g/m3, it reacts work
Skill condition：Air speed is 4300~6400hr-1, reaction temperature be 280~530 DEG C, reaction pressure is normal pressure.
Compared with prior art, key of the invention is that the active component of catalyst includes a certain amount of v element, lanthanum
Series elements and selected from least one of nonmetalloid and alkaline-earth metal element, be advantageous to improve the active of catalyst and stably
Property, so as to improve the yield of equal acid anhydride.
Test result indicates that acid anhydride yield achieves preferable technique effect, especially up to 77.8% prepared by the present invention
In catalyst active component simultaneously including v element, lanthanide series, selected from least one of nonmetalloid metallic element and
During selected from least one of alkaline-earth metal metallic element, more prominent technique effect is achieved, can be used for the conjunction of equal acid anhydride
Cheng Zhong.Below by embodiment, the present invention is further elaborated.
Embodiment
【Embodiment 1】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
8 parts of lanthanum nitrates, 0.2 part of ammonium borate are added in solution, continue to obtain catalyst precursor after stirring.By complex catalyst precursor
After body filtration drying, it is fitted into flush coater, uniformly sprays on inert carrier carborundum.Catalyst precursor will be coated with
Inert carrier is in Muffle furnace, 530 DEG C of roastings, and catalyst is obtained after natural cooling.Catalyst is in 525 DEG C of reaction temperature, air speed
5150h-1Under, checked and rated in fixed bed reactors, it is 74.0% to measure equal acid anhydride yield, and its appraisal result refers to table 1.
【Embodiment 2】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
8 parts of lanthanum nitrates, 0.2 part of strontium nitrate are added in solution, continue to obtain catalyst precursor after stirring.By complex catalyst precursor
After body filtration drying, it is fitted into flush coater, uniformly sprays on inert carrier carborundum.Catalyst precursor will be coated with
Inert carrier is in Muffle furnace, 530 DEG C of roastings, and catalyst is obtained after natural cooling.Catalyst is in 525 DEG C of reaction temperature, air speed
5150h-1Under, checked and rated in fixed bed reactors, it is 73.9% to measure equal acid anhydride yield, and its appraisal result refers to table 1.
【Comparative example 1】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
8 parts of lanthanum nitrates are added in solution, continue to obtain catalyst precursor after stirring.By catalyst precursor filtration drying
Afterwards, it is fitted into flush coater, uniformly sprays on inert carrier carborundum.The inert carrier for being coated with catalyst precursor is existed
In Muffle furnace, 530 DEG C are calcined, and catalyst is obtained after natural cooling.Catalyst is in 525 DEG C of reaction temperature, air speed 5150h-1Under,
Checked and rated in fixed bed reactors, it is 69.4% to measure equal acid anhydride yield, and its appraisal result refers to table 1.
By compared with embodiment 1~2 as can be seen that the catalyst that uses of the present invention, using containing V, La and B activity simultaneously
Component while catalyst performance ratio containing V, La and Sr active component is more excellent containing only the performance of V, La active constituent catalyst,
The yield of equal acid anhydride is higher.
【Embodiment 3】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
8 parts of cerous nitrates, 0.2 part of ammonium tellurate are added in solution, continue to obtain catalyst precursor after stirring.By complex catalyst precursor
After body filtration drying, it is fitted into flush coater, uniformly sprays on inert carrier carborundum.Catalyst precursor will be coated with
Inert carrier is in Muffle furnace, 530 DEG C of roastings, and catalyst is obtained after natural cooling.Catalyst is in 525 DEG C of reaction temperature, air speed
5150h-1Under, checked and rated in fixed bed reactors, it is 74.2% to measure equal acid anhydride yield, and its appraisal result refers to table 1.
【Embodiment 4】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of ammonium metavanadate is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.By 8
Part cerous nitrate, 0.2 part of ammonium tellurate are added in solution, continue to obtain catalyst precursor after stirring.By catalyst precursor
After filtration drying, it is fitted into flush coater, uniformly sprays on inert carrier carborundum.The lazy of catalyst precursor will be coated with
Property carrier in Muffle furnace, 530 DEG C of roastings, obtain catalyst after natural cooling.Catalyst is in 525 DEG C of reaction temperature, air speed
5150h-1Under, checked and rated in fixed bed reactors, it is 74.4% to measure equal acid anhydride yield, and its appraisal result refers to table 1.
【Embodiment 5】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of ammonium metavanadate is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.By 8
Part lanthanum nitrate, 0.2 part of sodium chloride are added in solution, continue to obtain catalyst precursor after stirring.By catalyst precursor
After filtration drying, it is fitted into flush coater, uniformly sprays on inert carrier carborundum.The lazy of catalyst precursor will be coated with
Property carrier in Muffle furnace, 530 DEG C of roastings, obtain catalyst after natural cooling.Catalyst is in 525 DEG C of reaction temperature, air speed
5150h-1Under, checked and rated in fixed bed reactors, it is 74.3% to measure equal acid anhydride yield, and its appraisal result refers to table 1.
【Embodiment 6】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
8 parts of cerous nitrates, 0.2 part of rubidium sulfate are added in solution, continue to obtain catalyst precursor after stirring.By complex catalyst precursor
After body filtration drying, it is fitted into flush coater, uniformly sprays on inert carrier carborundum.Catalyst precursor will be coated with
Inert carrier is in Muffle furnace, 530 DEG C of roastings, and catalyst is obtained after natural cooling.Catalyst is in 525 DEG C of reaction temperature, air speed
5150h-1Under, checked and rated in fixed bed reactors, it is 74.5% to measure equal acid anhydride yield, and its appraisal result refers to table 1.
【Embodiment 7】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
8 parts of lanthanum nitrates, 0.1 part of ammonium borate and 0.1 part of strontium nitrate are added in solution, continue to obtain complex catalyst precursor after stirring
Body.After catalyst precursor filtration drying, it is fitted into flush coater, uniformly sprays on inert carrier carborundum.Will spraying
There is the inert carrier of catalyst precursor in Muffle furnace, 530 DEG C are calcined, and catalyst is obtained after natural cooling.Catalyst is anti-
Answer 525 DEG C of temperature, air speed 5150h-1Under, checked and rated in fixed bed reactors, it is 75.1% to measure equal acid anhydride yield, its appraisal result
Refer to table 1.
The present embodiment is compared with embodiment 1~2 as can be seen that nonmetallic B element and alkaline-earth metal Sr elements are improving
Acid anhydride yield has preferably synergy.
【Embodiment 8】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
8 parts of lanthanum nitrates, 0.05 part of ammonium borate, 0.05 part of ammonium tellurate and 0.1 part of strontium nitrate are added in solution, continue to obtain after stirring
To catalyst precursor.After catalyst precursor filtration drying, it is fitted into flush coater, uniformly sprays and be carbonized in inert carrier
On silicon.The inert carrier of catalyst precursor will be coated with Muffle furnace, 530 DEG C of roastings, obtain catalyst after natural cooling.
Catalyst is in 525 DEG C of reaction temperature, air speed 5150h-1Under, checked and rated in fixed bed reactors, it is 75.7% to measure equal acid anhydride yield,
Its appraisal result refers to table 1.
The present embodiment can be seen that nonmetallic B and Te elements and exists with the other active components of the present invention compared with Example 7
Improving equal acid anhydride yield has preferably synergy.
【Embodiment 9】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
8 parts of lanthanum nitrates, 0.1 part of ammonium tellurate, 0.05 part of strontium nitrate and 0.05 part of rubidium sulfate are added in solution, continue to obtain after stirring
To catalyst precursor.After catalyst precursor filtration drying, it is fitted into flush coater, uniformly sprays and be carbonized in inert carrier
On silicon.The inert carrier of catalyst precursor will be coated with Muffle furnace, 530 DEG C of roastings, obtain catalyst after natural cooling.
Catalyst is in 525 DEG C of reaction temperature, air speed 5150h-1Under, checked and rated in fixed bed reactors, it is 75.8% to measure equal acid anhydride yield,
Its appraisal result refers to table 1.
The present embodiment can be seen that alkaline-earth metal Sr and Rb element and the other activearms of the present invention compared with Example 7
Divide and improving equal acid anhydride yield with preferably synergy.
【Embodiment 10】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
8 parts of lanthanum nitrates, 0.05 part of ammonium borate, 0.05 part of ammonium tellurate, 0.05 part of strontium nitrate and 0.05 part of rubidium sulfate are added in solution, after
Continue and obtain catalyst precursor after stirring.After catalyst precursor filtration drying, it is fitted into flush coater, uniformly sprays
On inert carrier carborundum.The inert carrier of catalyst precursor will be coated with Muffle furnace, 530 DEG C of roastings are naturally cold
But catalyst is obtained afterwards.
Catalyst is in 525 DEG C of reaction temperature, air speed 5150h-1Under, checked and rated in fixed bed reactors, measure equal acid anhydride yield
For 76.4%, its appraisal result refers to table 1.
The present embodiment is compared with embodiment 8, embodiment 9 as can be seen that V, lanthanide series metal La, nonmetallic B and Te elements, alkali
Earth metal Sr and Rb has extraordinary synergy in the equal acid anhydride yield of raising.
【Embodiment 11】
95g oxalic acid and 380ml distilled water are weighed in flask, stirring is warming up to 85 DEG C, after oxalic acid all dissolving, is made into
Oxalic acid solution.1 part of vanadic anhydride is added in the oxalic acid solution prepared and continues to stir, obtains vanadyl oxalate ammonium salt solution.
4 parts of lanthanum nitrates, 4 parts of cerous nitrates, 0.05 part of ammonium borate, 0.05 part of ammonium tellurate, 0.05 part of strontium nitrate and 0.05 part of rubidium sulfate are added
Enter in solution, continue to obtain catalyst precursor after stirring.After catalyst precursor filtration drying, load flush coater
In, uniformly spray on inert carrier carborundum.The inert carrier of catalyst precursor will be coated with Muffle furnace, 530
DEG C roasting, obtains catalyst after natural cooling.Catalyst is in 525 DEG C of reaction temperature, air speed 5150h-1Under, in fixed bed reactors
Middle examination, it is 778% to measure equal acid anhydride yield, and its appraisal result refers to table 1.
The present embodiment can be seen that compared with Example 10 V, lanthanide series metal La and Ce element, nonmetallic B and Te elements,
Alkaline-earth metal Sr and Rb has extraordinary synergy in the equal acid anhydride yield of raising.
Table 1
Claims (10)
1. a kind of catalyst for the equal acid anhydride of durol gaseous oxidation system, it is characterised in that the catalyst uses α-Al2O3、
Carborundum, ceramic ring or its mixture are carrier, and active component includes v element, lanthanide series, and nonmetalloid and alkaline earth
At least one of metallic element.
2. catalyst as claimed in claim 1, it is characterised in that the lanthanide series in La, Ce, Pr, Nd, Sm, Eu extremely
Few one kind.
3. catalyst as claimed in claim 1, it is characterised in that the nonmetalloid in B, Si, As and Te at least one
Kind.
4. catalyst as claimed in claim 1, it is characterised in that the alkali earth metal is in Be, Mg, Ca, Sr and Ba
It is at least one.
5. catalyst as claimed in claim 1, it is characterised in that the ratio of v element and lanthanide series is 1 in catalyst：(1-
10)。
6. catalyst as claimed in claim 1, it is characterised in that v element and nonmetalloid and alkaline earth element are total in catalyst
The ratio of sum is 1：(0.01-1).
A kind of 7. preparation method for being used for durol and preparing equal acid anhydride catalyst described in claim 1, it is characterised in that including
Several steps：
(1) vanadium source is added in oxalic acid solution, obtains mixed solution；By lanthanide series, nonmetalloid and alkaline-earth metal member
Plain compound adds reaction system, obtains presoma；
(2) presoma is sprayed on carrier, catalyst is obtained after roasting.
8. the preparation method of equal acid anhydride catalyst is prepared for durol as claimed in claim 6, it is characterised in that will be catalyzed
The presoma of agent is fitted into flush coater, is uniformly sprayed after being heated at 210-265 DEG C on carrier.
9. the preparation method of equal acid anhydride catalyst is prepared for durol as claimed in claim 6, it is characterised in that will spray
There is the carrier of catalyst precursor in Muffle kiln roasting, sintering temperature is 490-570 DEG C of temperature, roasting time 2-8h.
10. a kind of method for preparing equal acid anhydride for durol, using durol, air as raw material, using fixed bed reactors,
The mass concentration of durol is 34-52g/m3, its reaction process condition：Air speed is 4300~6400hr-1, reaction temperature be
280~530 DEG C, reaction pressure is normal pressure, and equal acid anhydride is synthesized in the presence of any one catalyst described in Claims 1 to 5.
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| CN112536025A (en) * | 2019-09-20 | 2021-03-23 | 中国石油化工股份有限公司 | Catalyst for preparing pyromellitic anhydride by oxidizing durene and preparation method and application thereof |
| CN112536025B (en) * | 2019-09-20 | 2023-04-07 | 中国石油化工股份有限公司 | Catalyst for preparing pyromellitic anhydride by oxidization of durene and preparation method and application thereof |
| CN115228462A (en) * | 2021-04-23 | 2022-10-25 | 中国石油化工股份有限公司 | Supported catalyst for synthesizing pyromellitic dianhydride by gas phase oxidation, preparation method thereof and method for synthesizing pyromellitic dianhydride by oxidation of pyromellitic dianhydride |
| CN115228462B (en) * | 2021-04-23 | 2023-11-24 | 中国石油化工股份有限公司 | Supported catalyst for synthesizing maleic anhydride by gas phase oxidation, preparation method thereof and method for synthesizing maleic anhydride by durene oxidation |
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