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CN105565566A - Method for performing Fenton treatment on 6-nitro-1-diazo-2-naphthol-4-sulfonic acid wastewater and coproducing sodium sulfate - Google Patents

Method for performing Fenton treatment on 6-nitro-1-diazo-2-naphthol-4-sulfonic acid wastewater and coproducing sodium sulfate Download PDF

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CN105565566A
CN105565566A CN201510940078.6A CN201510940078A CN105565566A CN 105565566 A CN105565566 A CN 105565566A CN 201510940078 A CN201510940078 A CN 201510940078A CN 105565566 A CN105565566 A CN 105565566A
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nitro
waste water
sodium sulfate
sulfonic acid
fenton process
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CN105565566B (en
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陈伟东
李茂�
赵益明
夏骏钢
章文刚
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Zhejiang Run Tu Research Institute Co Ltd
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    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F9/00Multistage treatment of water, waste water or sewage
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01DCOMPOUNDS OF ALKALI METALS, i.e. LITHIUM, SODIUM, POTASSIUM, RUBIDIUM, CAESIUM, OR FRANCIUM
    • C01D5/00Sulfates or sulfites of sodium, potassium or alkali metals in general
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01DCOMPOUNDS OF ALKALI METALS, i.e. LITHIUM, SODIUM, POTASSIUM, RUBIDIUM, CAESIUM, OR FRANCIUM
    • C01D5/00Sulfates or sulfites of sodium, potassium or alkali metals in general
    • C01D5/16Purification
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/001Processes for the treatment of water whereby the filtration technique is of importance
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/02Treatment of water, waste water, or sewage by heating
    • C02F1/04Treatment of water, waste water, or sewage by heating by distillation or evaporation
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/02Treatment of water, waste water, or sewage by heating
    • C02F1/04Treatment of water, waste water, or sewage by heating by distillation or evaporation
    • C02F1/048Purification of waste water by evaporation
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/28Treatment of water, waste water, or sewage by sorption
    • C02F1/283Treatment of water, waste water, or sewage by sorption using coal, charred products, or inorganic mixtures containing them
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/52Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/52Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities
    • C02F1/5236Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities using inorganic agents
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/66Treatment of water, waste water, or sewage by neutralisation; pH adjustment
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/72Treatment of water, waste water, or sewage by oxidation
    • C02F1/722Oxidation by peroxides
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/34Nature of the water, waste water, sewage or sludge to be treated from industrial activities not provided for in groups C02F2103/12 - C02F2103/32
    • C02F2103/36Nature of the water, waste water, sewage or sludge to be treated from industrial activities not provided for in groups C02F2103/12 - C02F2103/32 from the manufacture of organic compounds
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2301/00General aspects of water treatment
    • C02F2301/08Multistage treatments, e.g. repetition of the same process step under different conditions
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2305/00Use of specific compounds during water treatment
    • C02F2305/02Specific form of oxidant
    • C02F2305/026Fenton's reagent

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Abstract

The invention discloses a method for performing Fenton treatment on 6-nitro-1-diazo-2-naphthol-4-sulfonic acid wastewater and coproducing sodium sulfate, which comprises the following steps: (1) adding alkali into 6-nitro-1-diazo-2-naphthol-4-sulfonic acid wastewater, and regulating the pH value to 2.0-3.0; (2) under stirring conditions, adding activated carbon, FeSO4 and H2O2 into the wastewater subjected to pH value regulation to perform oxidation reaction; (3) adding alkali into the oxidated wastewater to regulate the pH value to 9-10; (4) adding an Al2(SO4)3 solution into the wastewater treated by the step (3) until the pH value of the reaction system reaches 6-7, sufficiently standing and settling to obtain a turbid solution, and filtering the turbid solution to obtain a filtrate; (5) if the filtrate obtained in the step (4) satisfies the treatment requirements, concentrating by evaporation and drying to obtain the industrial-grade sodium sulfate; and if the filtrate obtained in the step (4) does not satisfy the treatment requirements, repeating the steps (2)-(4) until the filtrate satisfies the treatment requirements. The treatment method has the advantages of simple technique and no environment pollution, and can coproduce sodium sulfate in the treatment process, thereby maximally utilizing the resources.

Description

A kind of method of Fenton process 6-nitro-1,2,4-sulfonic acid waste water co-production sodium sulfate
Technical field
The invention belongs to Industrial Wastewater Treatment and the reuse technology field of environment protection, be specifically related to the waste water comprehensive treating process produced in 6-nitro-1,2,4-sulfonic acid production process, co-producing sodium sulfate, belongs to cleaner production category simultaneously.
Background technology
6-nitro-1,2,4-sulfonic acid, No. CAS is 5366-84-7, and structure is as shown in formula I, and Chinese another name is 6-nitro-DNSA, a kind of important dyestuff intermediate, mainly for the manufacture of matching stain and metallized dye.
The production method of 6-nitro-1,2,4-sulfonic acid take ethyl naphthol as main raw material, prepares through nitrosification, sulfonation, reduction transposition, diazotization, acid out, the operation such as nitrated.Waste water in production process mainly contains three sources: (1) reduction transposition; (2) acid out; (3) nitrated, wherein nitration waste water can reuse in sulfonation and acid out.The waste water main component that reduction transposition and acid out produce is naphthalene derivative, it forms complexity, containing gas chromatography, acidity is 5 ~ 8%, salinity is 8 ~ 15, colourity is 15000 ~ 35000 times, and COD is 10000 ~ 20000mg/L, belongs to the organic waste water of high density, highly acidity, high salinity, dark shade, difficult degradation.
The method of current this type of waste water of process mainly contains two kinds: (1) complexing abstraction, complexometric extraction process has high efficiency, highly selective, but due to the impurity in extraction and back-extraction process add up, repeatedly after circular treatment, extraction efficiency reduces, and strip liquor is difficult simultaneously.(2) traditional Fenton facture, traditional Fenton oxidation technology is mainly through neutralizing excessive acid with lime, produce the precipitations such as calcium sulfate, Adsorption organism, although percent of decolourization > 90% can be realized, but organic clearance lower (COD clearance is about 60%-70%), and H 2o 2the lower processing cost that causes of utilization ratio is high, because of oxygenizement thoroughly final outflow water be that brown color to brown is difficult to make discharged wastewater met the national standard, more difficultly reach reuse requirement, and produce a large amount of solid waste, raising enterprise production cost, impacts environment.
Summary of the invention
The present invention is directed to the deficiencies in the prior art, provide a kind of method of Fenton process 6-nitro-1,2,4-sulfonic acid co-production sodium sulfate, the method technique is simple, free from environmental pollution, simultaneously can co-producing sodium sulfate in process, reaches resource maximum using.
A method for Fenton process 6-nitro-1,2,4-sulfonic acid waste water co-production sodium sulfate, comprises the following steps:
(1) in 6-nitro-1,2,4-sulfonic acid waste water, add alkali and regulate its pH value to 2.0 ~ 3.0;
(2) in the waste water mixing up pH value, gac, FeSO is added under stirring 4and H 2o 2carry out oxidizing reaction;
(3) in the waste water after oxidation, add alkali and regulate its pH to 9 ~ 10;
(4) Al is added in the waste water processed to step (3) under stirring 2(SO 4) 3solution, until reaction system pH to 6 ~ 7, sufficient standing sedimentation obtains turbid liquid, filters obtain filtrate to this turbid liquid;
(5) if the filtrate that step (4) obtains reaches processing requirements, then technical grade sodium sulfate is obtained after evaporation concentration, drying; If the filtrate that step (4) obtains does not reach processing requirements, then repeating step (2) ~ (4), until reach processing requirements.
As preferably, described 6-nitro-1,2,4-sulfonic acid waste water is in 6-nitro-1,2,4-sulfonic acid production process, one or both composite wastes produced in reduction transposition or acid out step.Described 6-nitro-1,2,4-sulfonic acid is produced and referred to ethyl naphthol is main raw material, through nitrosification, sulfonation, reduction transposition, diazotization, acid out, nitrated etc. production technique.
As preferably, in step (1) and (3), alkali used is one or both in solid sodium carbonate or 25 ~ 35% aqueous sodium hydroxide solutions.
As preferably, in step (2), the FeSO added 4for solid, FeSO 4dosage is that 1 ~ 10mmol/L (refers to every 1L waste water and adds 1 ~ 10mmolFeSO 4);
The H added 2o 2mass percent concentration is 25 ~ 35%, H 2o 2dosage is 5 ~ 20ml/L.
As preferably, in step (2), gac dosage is 0.5 ~ 2g/L, at FeSO 4and H 2o 2add before.Wherein, first add gac and can make the abundant adsorb organic compound of gac, go into carbonium ion center, promote H 2o 2decompose speed and the efficiency of the hydroxyl radical free radical degradation of organic substances produced, improve H 2o 2utilization ratio.
As preferably, in step (2), temperature of reaction is 25 ~ 50 DEG C, and the reaction times is 1 ~ 2h, and reactive mode is standing.
As preferably, in step (4), the Al added 2(SO 4) 3mass percent concentration is 10 ~ 30%.
In the present invention, if filtrate does not reach requirement, then adjust ph to 2.0 ~ 3.0, repeating step (2) ~ (4), adjust ph can use sulfuric acid, also directly can use waste water, for most of waste water, the number of times of repeating step (2) ~ (4) is 2 ~ 4 times.
As preferably, as liquor C OD≤200mg/L, during colourity≤16 times, reach processing requirements, now, the sodium sulfate purity obtained is high, and waste water environmentally safe.
Compared with the method for existing Fenton process organic waste water, beneficial effect of the present invention is as follows:
(1) one or both composite wastes unification that this method will be reduced in 6-nitro-1,2,4-sulfonic acid process in transposition or acid out process processes, and improves waste water treatment efficiency and plant factor.
(2) with in solid sodium carbonate or 25 ~ 35% aqueous sodium hydroxide solutions, one or both regulate waste water, without limestone vegetation, not only can reduce the generation of solid waste, and the salinity in waste water can be made single, are convenient to recycle.
(3) at FeSO 4, H 2o 2add gac before, be convenient to charcoal absorption organism, go into chain carrier, promote H 2o 2decompose speed and the efficiency of the hydroxyl radical free radical degradation of organic substances produced, improve H 2o 2utilization ratio.
(4) gac can adsorb organism water-soluble in waste water, through sedimentation, filtration, removes together with organism mud, improves waste water treatment efficiency.And gac as flocculating aids, can improve filtering rate.
(5) with 10 ~ 30% Al 2(SO 4) 3, not only can adjust back wastewater pH, and generate flocculation agent again after adjusting pH to 6 ~ 7, the organism in waste water can be removed by sedimentation further.
(6) by continuous oxidation, sedimentation, filtration procedure 2 ~ 4 times, 6-nitro-1 can be realized, 2, the colourity of 4-acid oxysome waste water, COD efficiently remove that (chroma removal rate reaches 99.9%, COD clearance is greater than 98%), stable effluent quality, can by obtaining technical grade sodium sulfate after evaporation concentration, drying.
(7) present method is without the need to being equipped with particular device, only needs the simple operationss such as stirring, sedimentation, filtration, and treatment scheme is relatively simple, and processing costs is lower.
Embodiment
Embodiment 1
The 6-nitro-1,2,4-sulfonic acid of 200ml reduction transposition waste water is placed in beaker, adjusts pH to 2.5 with sodium carbonate, add 0.3g gac at 35 DEG C, the FeSO of 1mmol 4, and then add the H that 3ml mass percent concentration is 28% slowly 2o 2, keep temperature-resistant, standing and reacting 2h, be that 25% aqueous sodium hydroxide solution regulates pH to 10 with mass percent, under stirring, add the Al that massfraction is 10% slowly 2(SO 4) 3solution, adjusts pH to 6.2, leaves standstill 0.5h afterwards.Liquid turbid after described standing sedimentation is filtered.Repeated oxidation, sedimentation, filtration procedure 3 times, filtrate reaches processing requirements, and obtain technical grade sodium sulfate after evaporation concentration, drying, content reaches more than 98%.
Embodiment 2
The 6-nitro-1,2,4-sulfonic acid acid out waste water of 200ml is placed in beaker, adjusts pH to 2.0 with sodium carbonate, add 0.4g gac at 45 DEG C, the FeSO of 2mmol 4, and then add the H that 4ml mass percent concentration is 28% slowly 2o 2, keep temperature-resistant, standing and reacting 1.5h, regulate pH to 9.5 with 35% aqueous sodium hydroxide solution, under stirring, add the Al that massfraction is 30% slowly 2(SO 4) 3solution, adjusts pH to 6.5, leaves standstill 1h afterwards.Liquid turbid after described standing sedimentation is filtered.Repeated oxidation, sedimentation, filtration procedure 2 times, filtrate reaches processing requirements, and obtain technical grade sodium sulfate after evaporation concentration, drying, content reaches more than 98%.
Embodiment 3
The reduction transposition of the 6-nitro-1,2,4-sulfonic acid of each 100ml and acid out waste water are placed in beaker, adjust pH to 2.8 with 30% sodium hydroxide, add 0.1g gac at 25 DEG C, the FeSO of 0.5mmol 4, and then add the H that 2ml mass percent concentration is 28% slowly 2o 2, keep temperature-resistant, standing and reacting 1.5h, regulate pH to 9.3 with 30% aqueous sodium hydroxide solution, under stirring, add the Al that massfraction is 20% slowly 2(SO 4) 3solution, adjusts pH to 6.5, leaves standstill 0.5h afterwards.Liquid turbid after described standing sedimentation is filtered.Repeated oxidation, sedimentation, filtration procedure 4 times, filtrate reaches processing requirements, and obtain technical grade sodium sulfate after evaporation concentration, drying, content reaches more than 98%.
Embodiment 4
The 6-nitro-1,2,4-sulfonic acid acid out waste water of the reduction transposition of the 6-nitro-1,2,4-sulfonic acid of 50ml and 150ml is placed in beaker, adjusts pH to 2.3 with sodium carbonate, add 0.3g gac at 40 DEG C, the FeSO of 1.5mmol 4, and then add the H that 2ml mass percent concentration is 28% slowly 2o 2, keep temperature-resistant, standing and reacting 2h, regulate pH to 9.8 with 25% aqueous sodium hydroxide solution, under stirring, add the Al that massfraction is 30% slowly 2(SO 4) 3solution, adjusts pH to 6.3, leaves standstill 1h afterwards.Liquid turbid after described standing sedimentation is filtered.Repeated oxidation, sedimentation, filtration procedure 3 times, filtrate reaches processing requirements, and obtain technical grade sodium sulfate after evaporation concentration, drying, content reaches more than 98%.
Embodiment 5
The 6-nitro-1,2,4-sulfonic acid acid out waste water of the reduction transposition of the 6-nitro-1,2,4-sulfonic acid of 150ml and 50ml is placed in beaker, adjusts pH to 2.3 with sodium carbonate, add 0.2g gac at 40 DEG C, the FeSO of 2mmol 4, and then add the H that 3ml mass percent concentration is 28% slowly 2o 2, keep temperature-resistant, standing and reacting 1h, regulate pH to 9.0 with 35% aqueous sodium hydroxide solution, under stirring, add the Al that massfraction is 20% slowly 2(SO 4) 3solution, adjusts pH to 6.8, leaves standstill 1h afterwards.Liquid turbid after described standing sedimentation is filtered.Repeated oxidation, sedimentation, filtration procedure 3 times, filtrate reaches processing requirements, and obtain technical grade sodium sulfate after evaporation concentration, drying, content reaches more than 98%.
Comparative example 1
The reduction transposition of the 6-nitro-1,2,4-sulfonic acid of each 100ml and acid out waste water are placed in beaker, adjust pH to 2.8 with 30% sodium hydroxide, at 25 DEG C, add 0.4g gac, stir decolouring and filter for 1.5 hours, in filtrate, add the FeSO of 0.5mmol again 4, and then add the H that 2ml mass percent concentration is 28% slowly 2o 2, keep temperature-resistant, standing and reacting 1.5h, regulate pH to 9.3 with 30% aqueous sodium hydroxide solution, under stirring, add the Al that massfraction is 20% slowly 2(SO 4) 3solution, adjusts pH to 6.5, leaves standstill 0.5h afterwards.Liquid turbid after described standing sedimentation is filtered.Repeated oxidation, sedimentation, filtration procedure 4 times, filtrate reaches processing requirements, and obtain technical grade sodium sulfate after evaporation concentration, drying, detected result is in table 1.
By standard test method to COD, colourity before and after above embodiment wastewater treatment, and gained sodium sulfate measures, and its detected result is as shown in table 1.
The result of table 1 embodiment 1 ~ 5

Claims (9)

1. a method for Fenton process 6-nitro-1,2,4-sulfonic acid waste water co-production sodium sulfate, is characterized in that, comprise the following steps:
(1) in 6-nitro-1,2,4-sulfonic acid waste water, add alkali and regulate its pH value to 2.0 ~ 3.0;
(2) in the waste water mixing up pH value, gac, FeSO is added under stirring 4and H 2o 2carry out oxidizing reaction;
(3) in the waste water after oxidation, add alkali and regulate its pH to 9 ~ 10;
(4) Al is added in the waste water processed to step (3) under stirring 2(SO 4) 3solution, until reaction system pH to 6 ~ 7, sufficient standing sedimentation obtains turbid liquid, filters obtain filtrate to this turbid liquid;
(5) if the filtrate that step (4) obtains reaches processing requirements, then technical grade sodium sulfate is obtained after evaporation concentration, drying; If the filtrate that step (4) obtains does not reach processing requirements, then repeating step (2) ~ (4), until reach processing requirements.
2. Fenton process 6-nitro-1 according to claim 1,2, the method of 4-acid oxysome waste water co-production sodium sulfate, it is characterized in that, described 6-nitro-1,2,4-acid oxysome waste water is 6-nitro-1, in 2,4-acid oxysome production process, one or both composite wastes produced in reduction transposition or acid out step.
3. Fenton process 6-nitro-1 according to claim 1, the method of 2,4-acid oxysome waste water co-production sodium sulfate, is characterized in that, in step (1) and (3), alkali used is one or both in solid sodium carbonate or 25 ~ 35% aqueous sodium hydroxide solutions.
4. the method for Fenton process 6-nitro-1,2,4-sulfonic acid waste water co-production sodium sulfate according to claim 1, is characterized in that, in step (2), and the FeSO added 4for solid, FeSO 4dosage is 1 ~ 10mmol/L;
The H added 2o 2mass percent concentration is 25 ~ 35%, H 2o 2dosage is 5 ~ 20ml/L.
5. the method for Fenton process 6-nitro-1,2,4-sulfonic acid waste water co-production sodium sulfate according to claim 1, it is characterized in that, in step (2), gac dosage is 0.5 ~ 2g/L, at FeSO 4and H 2o 2add before.
6. the method for Fenton process 6-nitro-1,2,4-sulfonic acid waste water co-production sodium sulfate according to claim 1, it is characterized in that, in step (2), temperature of reaction is 25 ~ 50 DEG C, and the reaction times is 1 ~ 2h, and reactive mode is standing.
7. the method for Fenton process 6-nitro-1,2,4-sulfonic acid waste water co-production sodium sulfate according to claim 1, is characterized in that, in step (4), and the Al added 2(SO 4) 3mass percent concentration is 10 ~ 30%.
8. the method for the Fenton process 6-nitro-1,2,4-sulfonic acid waste water co-production sodium sulfate according to any one of claim 1 ~ 7, it is characterized in that, the number of times of repeating step (2) ~ (4) is 2 ~ 4 times.
9. the method for Fenton process 6-nitro-1,2,4-sulfonic acid waste water co-production sodium sulfate according to claim 1, is characterized in that, as liquor C OD≤200mg/L, during colourity≤16 times, reach processing requirements.
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陶明杰等: "活性炭协同芬顿试剂处理印染行业生化池出水的研究", 《兵器材料科学与工程》 *

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CN107381877A (en) * 2017-09-05 2017-11-24 湖北远大富驰医药化工股份有限公司 A kind of nitromethane treatment method for high-salinity wastewater
CN108046403A (en) * 2017-12-12 2018-05-18 合肥立方制药股份有限公司 A kind of processing method of sulfhydryl compound production waste liquid and its application
CN108046403B (en) * 2017-12-12 2021-04-23 合肥立方制药股份有限公司 Treatment method and application of mercapto compound production waste liquid
CN111392907A (en) * 2020-04-03 2020-07-10 贺利氏贵金属技术(中国)有限公司 Method for treating waste water
CN113292416A (en) * 2021-06-04 2021-08-24 枣庄市泰瑞精细化工有限公司 Production method for preparing sodium acetate by utilizing dihydroxy naphthalene waste liquid

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