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CN1066134C - New process for synthetising m-nitrobenzoic - Google Patents

New process for synthetising m-nitrobenzoic Download PDF

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Publication number
CN1066134C
CN1066134C CN98114154A CN98114154A CN1066134C CN 1066134 C CN1066134 C CN 1066134C CN 98114154 A CN98114154 A CN 98114154A CN 98114154 A CN98114154 A CN 98114154A CN 1066134 C CN1066134 C CN 1066134C
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China
Prior art keywords
acid
methyl
methyl benzoate
nitrobenzoate
temperature
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CN98114154A
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CN1203905A (en
Inventor
鲍亚华
叶伟
郭纯仁
王大春
汪锡茂
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JINHAI CHEMICAL PLANT LIAOHE PETROLEUM FIELD
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JINHAI CHEMICAL PLANT LIAOHE PETROLEUM FIELD
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C201/00Preparation of esters of nitric or nitrous acid or of compounds containing nitro or nitroso groups bound to a carbon skeleton
    • C07C201/06Preparation of nitro compounds
    • C07C201/08Preparation of nitro compounds by substitution of hydrogen atoms by nitro groups
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C201/00Preparation of esters of nitric or nitrous acid or of compounds containing nitro or nitroso groups bound to a carbon skeleton
    • C07C201/06Preparation of nitro compounds
    • C07C201/12Preparation of nitro compounds by reactions not involving the formation of nitro groups

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

The present invention relates to a novel synthetic method for preparing m-nitrobenzoic acid which is an important intermediate body in the chemical field of synthetic dye, medicines, etc. The method comprises: coarse methyl benzoate as a byproduct in the production process of dimethyl terephthalate as a polyester raw material is treated by sulfuric acid, is purified through crude distillation and then is nitrified by mixed acid of concentrated nitric acid and concentrated sulfuric acid, nitrified products are cooled, washed and separated to obtain methyl-m-nitrobenzoate, and then, the methyl-m-nitrobenzoate is hydrolyzed and neutralized by diluted alkali to obtain m-nitrobenzoic acid. With coarse methyl benzoate as raw material, the synthetic method has the characteristics of low cost, high yield, good product quality, etc. and is suitable for popularization.

Description

The M-NITROBENZOIC ACID synthetic method
The present invention relates to a kind of synthetic method that is used to produce chemical field important intermediate M-NITROBENZOIC ACIDs such as synthetic dyestuff, medicine.
M-NITROBENZOIC ACID (m-NBA) is the important intermediate of Chemicals such as synthetic dyestuff, medicine, and its source is many to be oxidized to p-nitrobenzoic acid with para-nitrotoluene and to pay product and purify and produce m-NBA, and this kind method raw material sources are limited, the trouble of purifying, and cost is higher.English Patent 1519617 (1974) and 4288615 (1980) propose with the nitrated method of producing m-NBA of phenylformic acid, and its shortcoming is that acid consumption is big, and raw material is expensive, and transformation efficiency is on the low side.The disclosed nitrated method of producing methyl-m-nitrobenzoate (m-NBAE) and m-NBA of methyl benzoate (BME) of utilizing of China's Chemicals catalogues (1980J0124171 organic synthesis topical reference book), the working condition gentleness, yield is higher, but because of the source of BME producing after with methanol esterification from phenylformic acid, cost is also higher, so only can small serial production reagent.In addition, the method for producing m-NBA such as meta-nitrotoluene air oxidation process etc. also all is subjected to effects limit such as raw material, cost, can not apply.
The object of the present invention is to provide that a kind of cost is low, yield is high, the M-NITROBENZOIC ACID synthetic method of good product quality.
The present invention realizes like this.This kind synthetic method is utilized the by product crude methyl benzoate of polyester (PET) raw material dimethyl terephthalate (DMT) (DMT) production process, after vitriolization and rectification and purification, use concentrated nitric acid and vitriol oil mixed acid nitrification again, itrated compound is isolated methyl-m-nitrobenzoate through cooling, washing, make M-NITROBENZOIC ACID with diluted alkaline hydrolysis, neutralization again.
This synthetic method is implemented according to the following steps:
1, thick BME vitriolization.Adopt sulfuric acid or the oleum of concentration 80-98% (98% the best), under normal temperature to 60 ℃ temperature, thick BME is carried out acidifying.The sulfuric acid consumption is 2-30% (weight percent), decides according to foreign matter content, and mixing time can be 30 minutes one 24 hours.Extremely neutral with the frozen water washing then.
2, rectifying.BME after the acid treatment is placed in the rectifying tower, excision lower boiling p-Xylol (PX), water and high boiling material, the wherein positive fraction (197-201 ℃, normal pressure) of intercepting, BME purity can reach 95-99.5%.Rectifying can be operated under vacuum or normal pressure;
3, nitration reaction.With BME concentrated nitric acid and the vitriol oil mixed acid nitrification after purifying.Concentration of nitric acid is 65-99% (with 95% an above optimum) in the nitration mixture, sulfuric acid concentration 85-98% (98% the best) or oleum, and BME and nitration mixture proportioning (mol ratio) are: BME: HNO 3: H 2SO 4=1: 1: 0.5-1: 1.4: 2, nitrated temperature is-10-+30 ℃, nitrated time 1-4 hour.Nitrated mode: available a part of sulfuric acid bottoming, in reactor, add BME, drip nitration mixture again, also can adopt the mode that BME is dripped in nitration mixture:
4, cooling, washing, separation obtain thick m-NBAE.Nitration reaction liquid is poured into trash ice liquid or added temperature is in the water at low temperature of 0-15 ℃ (2-5 ℃ of the best), and m-NBAE is fully separated out.Isolate about 40% sulfuric acid and micro-nitric acid, filter cake cold water thorough washing obtains the wet product of thick m-NBAE;
5, with diluted alkaline hydrolysis, neutralization, make m-NBA.Adopt diluted alkaline (NaOH, KOH, the NH of concentration 5-20% (with 8% the best) 3), the m-NBAE crude product hydrolysis salify under 90-110 ℃ of (95-98 ℃ of the best) temperature with moisture 10-30% decolours with small amount of activated in case of necessity; Use (H again 2SO 4, HNO 3, HCL) to be neutralized to pH value in 20-70 ℃ of temperature range be 2-3; Filter the m-NBA solid, remove things such as inorganic salt with 30 ℃ of water washings, filter cake obtains flaxen m-NBA powder crystallization in vacuum, 60 ℃ of following dryings.
By product crude methyl benzoate during M-NITROBENZOIC ACID synthetic method provided by the invention is produced with the polyester raw material dimethyl terephthalate (DMT) is a raw material, has characteristics such as cost is low, yield is high, good product quality, is suitable for and applies.
Embodiment 1:
To specification is the sulfuric acid that adds 198 gram concentration 98% in the four-necked bottle stirred reactor of 1L earlier, under 15-16 ℃ of temperature, add 136 BMEs of gram through purifying, then, dropping restrains the nitric acid of concentration 95% and the nitration mixture that 67.5 sulfuric acid that restrain concentration 98% mix by 76.5, adds afterreaction 1 hour; Add 0-5 ℃ of cold water 250mL in reaction solution, the separate sulfur sour water is used 500L water washing filter cake more then, washes out a small amount of yellow oil; Filter cake is carried out dry 146 gram m-NBAE, 76 ℃ of its fusing points, content 96.5%, the yield 78.74% of getting under vacuum; Get 73 gram m-NBAE, to wherein adding 22 gram solid NaOH and 400mL water, at 98 ℃ of following alkaline hydrolysis; After oil reservoir disappears, add 3% gac and boiled 10 minutes, filter and obtain sodium salt liquid, use 30%H 2SO 4Being neutralized to pH value is 2, gets the m-NBA white precipitate; After the filtration, dry under vacuum and 66 ℃ of temperature with 300mL35 ℃ of water washing filter cake, m-NBA solid 56 grams, 140 ℃ of its fusing points, content 98.5%, m-NBA is 67.02% to the BME yield.
Embodiment 2:
Press embodiment 1 appointed condition, the sulfuric acid mixing back with 176 gram concentration 95% nitric acid and 418 gram concentration 98% adds in the reactor earlier, under agitation drips 340 gram BME then, nitration reaction under 10-15 ℃ of temperature; Handle by example 1, get 430 gram m-NBAE after the drying; Get 92 gram m-NBAE, adding 21 gram NaOH, 400mL water are handled by example 1 and are produced m-NBA, get 58.5 gram dry products after the drying.141 ℃ of its fusing points, content 98.0%, yield 71.02%.
Embodiment 3:
Make reflux with the 1L there-necked flask, get one-level industrial goods concentration and be 96% phenylformic acid 122 grams, add the sulfuric acid of 256 gram methyl alcohol and 2 gram concentration 98%, under 72-85 ℃ of temperature, refluxed 5 hours, remove methyl alcohol and water; NaHCO with concentration 5% 3In the aqueous solution and carboxylate to pH value be 7, tell and slightly heat up in a steamer BME and carry out rectifying, intercept 198-201 ℃ 126 restrain purification BME; Produce m-NBAE and m-NBA with this BME by example 1 method, obtain the m-NBA white powder at last.141.5 ℃ of its fusing points, yield 70.67%.

Claims (1)

1, a kind of M-NITROBENZOIC ACID synthetic method, it is characterized in that: this method is after utilizing the by product crude methyl benzoate process vitriolization and rectification and purification of polyester raw material dimethyl terephthalate (DMT) production process, use concentrated nitric acid and vitriol oil mixed acid nitrification again, itrated compound is isolated methyl-m-nitrobenzoate through cooling, washing, make a nitre phenyl formic acid with diluted alkaline hydrolysis, neutralization again; The implementation step of this synthetic method is as follows: A, crude methyl benzoate vitriolization adopt sulfuric acid or the oleum of concentration 80-98%, under normal temperature to 60 ℃ temperature, crude methyl benzoate is carried out acidifying, the sulfuric acid consumption is 2-30%, decide according to foreign matter content, mixing time is 30 minutes-24 hours, and is extremely neutral with the frozen water washing then; B, the rectifying methyl benzoate after with acid treatment places in the rectifying tower, excision lower boiling p-Xylol, water and high boiling material, and the wherein positive fraction of intercepting, rectifying is operated under vacuum or normal pressure; Methyl benzoate after C, nitration reaction will be purified concentrated nitric acid and vitriol oil mixed acid nitrification, concentration of nitric acid is 65-99% in the nitration mixture, and sulfuric acid concentration is 85-98% or oleum, and methyl benzoate and nitration mixture proportioning are methyl benzoate: HNO 3: H 2SO 4=1: 1: 0.5-1: 1.4: 2, nitrated temperature is-10-+30 ℃, nitrated time 1-4 hour, nitrated mode can add methyl benzoate with a part of sulfuric acid bottoming in reactor, drip nitration mixture again, also methyl benzoate can be dripped in nitration mixture; D, cooling, washing, separation, obtain thick methyl-m-nitrobenzoate, pouring nitration reaction liquid into trash ice liquid or adding temperature is in 0-15 ℃ the water, methyl-m-nitrobenzoate is fully separated out, isolate about 40% sulfuric acid and micro-nitric acid, filter cake cold water thorough washing obtains the wet product of thick methyl-m-nitrobenzoate; E, the hydrolysis of usefulness diluted alkaline, neutralization, make the diluted alkaline that a nitre phenyl formic acid adopts concentration 5-20%, methyl-m-nitrobenzoate crude product hydrolysis salify under 90-110 ℃ of temperature with moisture 10-30%, with the small amount of activated decolouring, being neutralized to pH value with acid under 20-70 ℃ of temperature again is 2-3, nitre phenyl formic acid solid between filtration in case of necessity, with 30 ℃ of water washings, remove inorganic salt, filter cake obtains a nitre phenyl formic acid powder crystallization in vacuum, 60 ℃ of following dryings.
CN98114154A 1998-07-14 1998-07-14 New process for synthetising m-nitrobenzoic Expired - Fee Related CN1066134C (en)

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Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN105859581A (en) * 2016-04-21 2016-08-17 河间瀛州化工有限责任公司 New nitration technology used in production of 2-cyano-4-nitro chlorobenzene
CN110143879B (en) * 2019-04-29 2022-07-12 南京师范大学 Device and method for recycling by-products generated in preparation of p-nitroacetophenone
CN113105323B (en) * 2021-03-24 2022-07-19 江苏永安化工有限公司 Green preparation process of 2-methyl-3-methoxybenzoyl chloride

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3978118A (en) * 1975-07-11 1976-08-31 Gulf Research & Development Company Process for converting styrene or polystyrene to nitrobenzoic acids
GB1519602A (en) * 1974-10-03 1978-08-02 Bofors Ab Preparing meta-nitrobenzoic acid

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1519602A (en) * 1974-10-03 1978-08-02 Bofors Ab Preparing meta-nitrobenzoic acid
US3978118A (en) * 1975-07-11 1976-08-31 Gulf Research & Development Company Process for converting styrene or polystyrene to nitrobenzoic acids

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