CN104437468A - Catalyst composition for treating wastewater containing methylene blue dye as well as preparation method and application of catalyst composition - Google Patents
Catalyst composition for treating wastewater containing methylene blue dye as well as preparation method and application of catalyst composition Download PDFInfo
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- CN104437468A CN104437468A CN201410612692.5A CN201410612692A CN104437468A CN 104437468 A CN104437468 A CN 104437468A CN 201410612692 A CN201410612692 A CN 201410612692A CN 104437468 A CN104437468 A CN 104437468A
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- methylene blue
- sodium
- blue dye
- carbon monoxide
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Abstract
The invention discloses a catalyst composition for treating wastewater containing methylene blue dye as well as a preparation method and application of the catalyst composition. The preparation method comprises the following steps: sequentially adding a sodium compound, an aluminum salt, molybdate, a chromium salt and citric acid into water, and stirring and dissolving; adding ethylene glycol; heating to 100-130 DEG C and continually stirring to form gel; and heating the gel at 500-1000 DEG C for 5-15 hours to obtain the catalyst with a compound oxide NaAl(MoO4)2:xCr (x=0.005-0.05). According to the catalyst, the wastewater containing the methylene blue dye can be effectively treated at normal temperature and under normal pressure without an oxidant or light illumination, and the catalyst can be recycled for multiple times.
Description
Technical field
The invention belongs to inorganic functional material preparing technical field, relating to a kind of composite oxide catalysts and preparation method and application for the treatment of containing methylene blue dye wastewater.
Background technology
Along with the fast development of dye industry, organic dye waste water has become one of main pollution source of water body.This kind of waste water has that the water yield is large, concentration is high, complicated component, colourity are dark and the feature such as difficult degradation.Most of dyestuff also has toxicity, carcinogenicity, teratogenesis and mutagenic effect.Wherein, methylene blue is a kind of important organic chemical synthesis dye of positive ion, and commercial Application widely.Such as, can be applicable to fiber crops, silk fabric, the dyeing of paper and the painted of bamboo and wood, be applied to biology, bacterial organisms dyeing and be applied to manufacture ink and color lake etc.Methylene blue extensive use industrially also will cause containing methylene blue dye wastewater the severe contamination of water body.
At present, the processing method of organic dye waste water mainly contains bioanalysis, Coagulation Method, high-level oxidation technology, photocatalytic method, absorption method and membrane separation process etc.Bioanalysis, by the impact of the factors such as pH value, temperature, salt and kind of dyes, makes the effect of Biochemical method not ideal enough.The operating cost of Coagulation Method is higher, and body refuse amount is large and dehydration is difficult, and the pH value range be suitable for is narrow.High-level oxidation technology cost is high, conventional oxidant also can show oxidability strong, there is the shortcomings such as selective oxidation, and easily introduce impurity in processing procedure and cause secondary pollution.Photocatalytic method needs light source irradiation system, large by weather effect in actual applications.Absorption method is subject to the impacts such as suspension in water and grease, and adsorbent amount is large and costly.Membrane separation process is divided into electroosmose process, hyperfiltration, nano filtering process and ultrafiltration etc., wherein the advantage of electroosmose process, hyperfiltration, nano filtering process is that dyestuff clearance is high, the dyestuff in waste water can be reclaimed, technique is simple, but the cost of film used is higher, operating pressure is comparatively large, causes the energy consumption of embrane method higher, have impact on its industrial applications.Traditional ultrafiltration is comparatively large due to membrane aperture, is difficult to remove low-molecular-weight organic pollution.
In sum, the catalyst by researching and developing a kind of simple and efficient process methylene blue dye wastewater has important social effect and economic implications.
Summary of the invention
In view of the deficiencies in the prior art, the object of the invention is to solve the above-mentioned technical problem existed in prior art, thus carbon monoxide-olefin polymeric of the methylene blue dye in a kind of simple, effective degrading waste water and its preparation method and application is provided.
To achieve these goals, the present inventor, by lot of experiments research also persistent exploration, finally obtains following technical scheme:
For the treatment of the carbon monoxide-olefin polymeric containing methylene blue dye wastewater, comprise composite oxides, the general formula of described composite oxides is NaAl (MoO
4)
2: xCr, wherein x=0.005 ~ 0.05.
For the treatment of a preparation method for the carbon monoxide-olefin polymeric containing methylene blue dye wastewater, described carbon monoxide-olefin polymeric comprises composite oxides, and described composite oxides are prepared from as follows:
(1) sodium compound, chromic salts, molybdate and citric acid are added to the water successively, stirring and dissolving, the mol ratio of the aluminium in the sodium in described sodium compound, aluminium salt, the molybdenum in molybdate, the chromium in chromic salts, citric acid and water is 1:1:2:(0.005 ~ 0.05): (3-30): (250-450);
(2) add ethylene glycol, the addition of ethylene glycol is 3-5 times of citric acid molal quantity, after stirring 5-15min, is heated to 100 DEG C-130 DEG C, continues to stir to form gel;
(3) gel is calcined 5-15 hour at 500 DEG C-1000 DEG C, obtain that there is granular composite oxides NaAl (MoO
4)
2: xCr, wherein x=0.005 ~ 0.05.
In a most preferred embodiment of the present invention, as mentioned above for the treatment of the preparation method of the carbon monoxide-olefin polymeric of methylene blue dye wastewater, the mol ratio of the sodium wherein in sodium compound described in step (1), aluminium, the molybdenum in molybdate, the chromium in chromic salts, citric acid and water in aluminium salt is 1:1:2:0.01:13:333.
Preferably, as mentioned above for the treatment of the preparation method of the carbon monoxide-olefin polymeric of methylene blue dye wastewater, the calcining heat wherein in step (3) is 600 DEG C-900 DEG C, and calcination time is 6-10 hour.
Further preferably, as mentioned above for the treatment of the preparation method of the carbon monoxide-olefin polymeric containing methylene blue dye wastewater, wherein said sodium compound is selected from following one or more: NaOH, sodium chloride, sodium carbonate, sodium acid carbonate, sodium sulphate, niter cake, sodium nitrate, sodium phosphate, dibastic sodium phosphate, sodium dihydrogen phosphate, sodium formate, sodium acetate, natrium citricum.
Further preferably, as mentioned above for the treatment of the preparation method of carbon monoxide-olefin polymeric containing methylene blue dye wastewater, wherein said aluminium salt is selected from following one or more: aluminum nitrate, aluminum sulfate, aluminium chloride, aluminium triformate, aluminum acetate, aluminium citrate.
Further preferably, as mentioned above for the treatment of the preparation method of the carbon monoxide-olefin polymeric containing methylene blue dye wastewater, wherein said molybdate is that ammonium molybdate is or/and sodium molybdate.
Further preferably, as mentioned above for the treatment of the preparation method of the carbon monoxide-olefin polymeric containing methylene blue dye wastewater, wherein said chromic salts is one or more in chromic nitrate, chromium sulfate and chromium chloride.
Utilize above-mentioned carbon monoxide-olefin polymeric process containing the method for methylene blue dye wastewater, comprise described carbon monoxide-olefin polymeric to be suspended in methylene blue dye wastewater and process.
Described process, containing the method for methylene blue dye wastewater, preferably adds described composite oxides NaAl (MoO in the ratio of 0.5 ~ 2.0g/L waste water
4)
2: xCr, under agitation processes 20-60 minute.
Composite oxides NaAl (MoO of the present invention
4)
2: xCr (x=0.005 ~ 0.05) catalyst application in the processing method of methylene blue waste water is: with composite oxides NaAl (MoO
4)
2: xCr (x=0.005 ~ 0.05) is catalyst, and degradation conditions is: methylene blue concentration is in 5mg/L ~ 20mg/L scope, and the catalyst amount processing often liter of wastewater containing methylene blue is 0.5 ~ 2.0g, and solution system is in normal temperature and pressure.When methylene blue solution volume is 40mL, when concentration is 10mg/L, under agitation add catalyst 0.05g, catalytic degradation 30 minutes, the degradation rate of methylene blue reaches more than 85%.Residual solution color is close to colourless.Catalyst recycle use is carried out again after residual solution being replaced with new methylene blue solution.Result shows, catalyst can repeatedly recycle.
Compared with prior art, the present invention at normal temperatures and pressures, without the need to oxidant, effectively can process methylene blue dye wastewater under also penetrating without the need to illumination.Have catalytic degradation efficiency high, technological process is simple, and non-secondary pollution produces, and the feature such as operating cost is low, there is very high actual application value.Generally speaking, the method that the present invention relates to process methylene blue dye wastewater has following significant advantage with significant progressive:
(1) method for preparing catalyst of the present invention is simple.
(2) catalyst activity of the present invention is high, can in the short period of time fast and efficient degradation pollutant.
(3) method of wastewater treatment of the present invention can carry out at normal temperatures and pressures, and technological process is simple and cost is low.
(4) method of wastewater treatment of the present invention is without the need to using oxidant, does not also need to adopt any light source irradiation degraded system.
(5) catalyst of the present invention is repeatedly reusable.
Detailed description of the invention
Form is described in further detail foregoing of the present invention again by the following examples, but this should be interpreted as that the scope of the above-mentioned theme of the present invention is only limitted to following embodiment, all technology realized based on foregoing of the present invention all belong to scope of the present invention.
Embodiment 1
By 0.54g sodium carbonate (5.1 × 10
-3mol), 3.75g nine water aluminum nitrate (1.0 × 10
-2mol), 3.58g tetra-water ammonium molybdate (2.9 × 10
-3mol), 5.2 × 10
-3g nine water chromic nitrate (1.0 × 10
-4mol) and 25.47g citric acid (0.13mol) add 60mL(3.33 mol successively) in distilled water, stirring and dissolving.Add 32.28g ethylene glycol (0.52mol) and stir 10min afterwards, be warmed up to 120 DEG C and continue to stir, until form gel.Gel is heated 10 hours at 600 DEG C, obtains the granular composite oxides NaAl of 3.41g (MoO
4)
2: xCr (x=0.01) catalyst.
Get 0.05 gram of composite oxides NaAl (MoO prepared as stated above
4)
2: xCr (x=0.01) catalyst degradation aqueous solution of methylene blue.Methylene blue concentration is 10 mg/L, and volume is 40mL.Under stirring in normal temperature and pressure catalysis degradation of methylene blue, fixed time intervals samples, and within centrifugal 10 minutes on centrifuge, gets supernatant.Adopt spectrophotometer, measure absorbance in methylene blue maximum absorption wave strong point (660nm).The concentration of aqueous solution of methylene blue is converted into by absorbance-concentration working curve.When degradation time is 35 minutes, methylene blue degradation rate is 85.0 %.
Embodiment 2
By 0.54g sodium carbonate (5.1 × 10
-3mol), 3.75g nine water aluminum nitrate (1.0 × 10
-2mol), 3.58g tetra-water ammonium molybdate (2.9 × 10
-3mol), 5.2 × 10
-3g nine water chromic nitrate (1.0 × 10
-4mol) and 25.47g citric acid (0.13mol) add 60mL(3.33 mol successively) in distilled water, stirring and dissolving.Add 32.28g ethylene glycol (0.52mol) and stir 10min afterwards, be warmed up to 120 DEG C and continue to stir, until form gel.Gel is heated 7 hours at 700 DEG C, obtains the granular composite oxides NaAl of 3.30g (MoO
4)
2: xCr (x=0.01) catalyst.
Get 0.05 gram of composite oxides NaAl (MoO prepared as stated above
4)
2: xCr (x=0.01) catalyst degradation aqueous solution of methylene blue.Methylene blue concentration is 10 mg/L, and volume is 40mL.Under stirring in normal temperature and pressure catalysis degradation of methylene blue, fixed time intervals samples, and within centrifugal 10 minutes on centrifuge, gets supernatant.Adopt spectrophotometer, measure absorbance in methylene blue maximum absorption wave strong point (660nm).The concentration of aqueous solution of methylene blue is converted into by absorbance-concentration working curve.When degradation time is 35 minutes, methylene blue degradation rate is 86.0%.
Embodiment 3
By 0.54g sodium carbonate (5.1 × 10
-3mol), 3.75g nine water aluminum nitrate (1.0 × 10
-2mol), 3.58g tetra-water ammonium molybdate (2.9 × 10
-3mol), 5.2 × 10
-3g nine water chromic nitrate (1.0 × 10
-4mol) and 25.47g citric acid (0.13mol) add 60mL(3.33 mol successively) in distilled water, stirring and dissolving.Add 32.28g ethylene glycol (0.52mol) and stir 10min afterwards, be warmed up to 120 DEG C and continue to stir, until form gel.Gel is heated 6 hours at 900 DEG C, obtains the granular composite oxides NaAl of 3.13g (MoO
4)
2: xCr (x=0.01) catalyst.
Get 0.05 gram of NaAl (MoO prepared as stated above
4)
2: xCr (x=0.01) catalyst degradation aqueous solution of methylene blue.Methylene blue concentration is 10 mg/L, and volume is 40mL.Under stirring in normal temperature and pressure catalysis degradation of methylene blue, fixed time intervals samples, and within centrifugal 10 minutes on centrifuge, gets supernatant.Adopt spectrophotometer, measure absorbance in methylene blue maximum absorption wave strong point (660nm).The concentration of aqueous solution of methylene blue is converted into by absorbance-concentration working curve.When degradation time is 20 minutes, methylene blue degradation rate is 86.6%.
Claims (10)
1., for the treatment of the carbon monoxide-olefin polymeric containing methylene blue dye wastewater, comprise composite oxides, it is characterized in that: the general formula of described composite oxides is NaAl (MoO
4)
2: xCr, wherein x=0.005 ~ 0.05.
2., for the treatment of a preparation method for the carbon monoxide-olefin polymeric containing methylene blue dye wastewater, it is characterized in that: described carbon monoxide-olefin polymeric comprises composite oxides, described composite oxides are prepared from as follows:
(1) sodium compound, aluminium salt, molybdate, chromic salts and citric acid are added to the water successively, stirring and dissolving, the mol ratio of the aluminium in the sodium in described sodium compound, aluminium salt, the molybdenum in molybdate, the chromium in chromic salts, citric acid and water is 1:1:2:(0.005 ~ 0.05): (3-30): (250-450);
(2) add ethylene glycol, the addition of ethylene glycol is 3-5 times of citric acid molal quantity, after stirring 5-15min, is heated to 100 DEG C-130 DEG C, continues to stir to form gel;
(3) gel is calcined 5-15 hour at 500 DEG C-1000 DEG C, obtain that there is granular composite oxides NaAl (MoO
4)
2: xCr, wherein x=0.005 ~ 0.05.
3. according to claim 2 for the treatment of the preparation method of the carbon monoxide-olefin polymeric of methylene blue dye wastewater, it is characterized in that: the mol ratio of the sodium in sodium compound described in step (1), the aluminium in aluminium salt, the molybdenum in molybdate, the chromium in chromic salts, citric acid and water is 1:1:2: 0.01: 13:333.
4., according to claim 2 for the treatment of the preparation method of the carbon monoxide-olefin polymeric containing methylene blue dye wastewater, it is characterized in that: the calcining heat in step (3) is 600 DEG C-900 DEG C, calcination time is 6-10 hour.
5. according to claim 2 for the treatment of the preparation method of carbon monoxide-olefin polymeric containing methylene blue dye wastewater, it is characterized in that: described sodium compound is selected from following one or more: NaOH, sodium chloride, sodium carbonate, sodium acid carbonate, sodium sulphate, niter cake, sodium nitrate, sodium phosphate, dibastic sodium phosphate, sodium dihydrogen phosphate, sodium formate, sodium acetate, natrium citricum.
6. according to claim 2 for the treatment of the preparation method of carbon monoxide-olefin polymeric containing methylene blue dye wastewater, it is characterized in that: described aluminium salt is selected from following one or more: aluminum nitrate, aluminum sulfate, aluminium chloride, aluminium triformate, aluminum acetate, aluminium citrate.
7. according to claim 2 for the treatment of the preparation method of the carbon monoxide-olefin polymeric of methylene blue dye wastewater, it is characterized in that: described molybdate is that ammonium molybdate is or/and sodium molybdate.
8. according to claim 2 for the treatment of the preparation method of the carbon monoxide-olefin polymeric of methylene blue dye wastewater, it is characterized in that: described chromic salts is one or more in chromic nitrate, chromium sulfate and chromium chloride.
9. utilize carbon monoxide-olefin polymeric process described in claim 1 containing the method for methylene blue dye wastewater, it is characterized in that: comprise described carbon monoxide-olefin polymeric to be suspended in methylene blue dye wastewater and process.
10. process, containing the method for methylene blue dye wastewater, is characterized in that: add described composite oxides NaAl (MoO in the ratio of 0.5 ~ 2.0g/L waste water according to claim 9
4)
2: xCr, under agitation processes 20-60 minute.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105457650A (en) * | 2015-12-15 | 2016-04-06 | 湖北工业大学 | Catalyst composition and preparation method and application thereof in aspect of treating methylene blue industrial wastewater |
| CN106669725A (en) * | 2016-12-09 | 2017-05-17 | 湖北工业大学 | Preparation method of multi-component compound oxide catalyst composition for treating methylene blue wastewater |
| CN106698625A (en) * | 2016-12-26 | 2017-05-24 | 山东大学 | Application of formate as coagulant in high-concentration organic wastewater treatment |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102935359A (en) * | 2012-11-21 | 2013-02-20 | 湖北工业大学 | Catalyst composition for processing methylene blue dye wastewater and preparation method and applications of catalyst composition |
| CN103055844A (en) * | 2013-01-16 | 2013-04-24 | 湖北工业大学 | Catalyst composition for efficiently treating methylene blue dye wastewater and preparation method and application thereof |
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Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102935359A (en) * | 2012-11-21 | 2013-02-20 | 湖北工业大学 | Catalyst composition for processing methylene blue dye wastewater and preparation method and applications of catalyst composition |
| CN103055844A (en) * | 2013-01-16 | 2013-04-24 | 湖北工业大学 | Catalyst composition for efficiently treating methylene blue dye wastewater and preparation method and application thereof |
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105457650A (en) * | 2015-12-15 | 2016-04-06 | 湖北工业大学 | Catalyst composition and preparation method and application thereof in aspect of treating methylene blue industrial wastewater |
| CN105457650B (en) * | 2015-12-15 | 2018-09-25 | 湖北工业大学 | A kind of carbon monoxide-olefin polymeric and preparation method thereof and the application in terms of handling methylene blue industrial wastewater |
| CN106669725A (en) * | 2016-12-09 | 2017-05-17 | 湖北工业大学 | Preparation method of multi-component compound oxide catalyst composition for treating methylene blue wastewater |
| CN106698625A (en) * | 2016-12-26 | 2017-05-24 | 山东大学 | Application of formate as coagulant in high-concentration organic wastewater treatment |
| CN106698625B (en) * | 2016-12-26 | 2019-10-01 | 山东大学 | Application of the formates as coagulant in high concentrated organic wastewater processing |
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Application publication date: 20150325 |