CN106232531A - Containing cyanogen and the processing method of the waste water of ammonia - Google Patents
Containing cyanogen and the processing method of the waste water of ammonia Download PDFInfo
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- CN106232531A CN106232531A CN201580019750.6A CN201580019750A CN106232531A CN 106232531 A CN106232531 A CN 106232531A CN 201580019750 A CN201580019750 A CN 201580019750A CN 106232531 A CN106232531 A CN 106232531A
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B11/00—Oxides or oxyacids of halogens; Salts thereof
- C01B11/20—Oxygen compounds of bromine
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/76—Treatment of water, waste water, or sewage by oxidation with halogens or compounds of halogens
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Abstract
Even if providing in the case of dissolubility concentration of iron height, it is also possible to make that cyanogen and ammonia is fully decomposed containing cyanogen and the processing method of the water of ammonia.A kind of containing cyanogen with the processing method of the waste water of ammonia, it has and adds the operation comprising Hydrogen oxybromide (HOBr) and/or hypochlorous chemical solution and make cyanogen and ammoxidation decompose in the waste water containing cyanogen and ammonia.The liquid that bromide solution and aqueous hypochlorite solution mixing generate Hydrogen oxybromide (HOBr) and/or hypobromite adds in the waste water containing cyanogen and ammonia.By aqueous sodium bromide and aqueous sodium hypochlorite solution by equimolar ratio or with sodium hypochlorite excess in the way of mix and add.
Description
Technical field
The present invention relates to containing cyanogen and the processing method of the waste water of ammonia, particularly relate to the improved method utilizing Pomolio-Celdecor process to containing
The method that the waste water containing cyanogen and ammonia of dissolubility ferrum carries out processing.
Background technology
As discharge from the industrial plants such as Electroplate Factory, steel plant, Metallurgical Factory, power plant, coke manufacturer containing cyanogen
The processing method of waste water, the most extensive adopted method is Pomolio-Celdecor process.In the method, by chlorine source, such as sodium hypochlorite
Add under alkalescence in the waste water containing cyanogen, the cyanogen in waste water is carried out oxidation processes (patent documentation 1,2).
In the Pomolio-Celdecor process of patent documentation 1, with 2 step reactions of pH and ORP (oxidation-reduction potential) controlling value as follows
Make cyanogen compound oxidation Decomposition.
The first step is reacted: more than pH10, ORP controlling value 300~350mV
NaCN+NaOCl→NaCNO+NaCl…(1)
Second step reacts: pH7~8, ORP controlling value 600~650mV
2NaCNO+3NaClO+H2O→N2+3NaCl+2NaHCO3…(2)
Patent documentation 2 is recorded the water reuse containing cyanogen comprising free Cyanide, cyano complex and ammonia has been had little
In the method that the Pomolio-Celdecor process of the 1st oxidation operations of 80 DEG C and this 2 step operation of the 2nd oxidation operation of more than 80 DEG C carries out processing.
Patent documentation 3 is recorded and has carried out processing at pH11 Pomolio-Celdecor process utilized above by the waste water containing cyanogen and ammonium ion
Method.In the method for this patent documentation 3, after cyanogen compound decomposition reaction, still so that free residual cl concn is 0.1mg/L
Above mode adds chlorine source.In patent documentation 3 record, the most of dissolubility ferrum in the waste water containing cyanogen and ammonium ion with
Presented in ferrum cyano complex;This ferrum cyano complex is difficult to be decomposed in Pomolio-Celdecor process, therefore, and useless containing cyanogen and ammonium ion
Dissolubility concentration of iron in water should be below 0.4mg/L (the 0025th section of patent documentation 3).
Patent documentation 1: Japanese Unexamined Patent Publication 2001-269674
Patent documentation 2: Japanese Unexamined Patent Publication 2006-334508
Patent documentation 3: Japanese Unexamined Patent Publication 2013-208550
As described in patent documentation 3, in the case of the dissolubility concentration of iron height in the waste water containing cyanogen and ammonium ion,
In existing Pomolio-Celdecor process, cyanogen is not sufficiently oxidized decomposition.
The method of above-mentioned patent documentation 3 exists for making the waste water containing cyanogen and ammonium ion become the alkaline agent of more than pH11
The problem that cost increases.And then there are the different risks producing chlorine of the addition according to chlorine source.
Summary of the invention
Even if it is a first object of the present invention to provide also being able to make in the case of dissolubility concentration of iron height in waste water
Cyanogen decomposed fully containing cyanogen and the processing method of the waste water of ammonia.
Even if it is a second object of the invention to provide also being able to make cyanogen be sufficiently oxidized containing of decomposition at below pH11
The processing method of the waste water of cyanogen and ammonia.
The processing method containing cyanogen and the waste water of ammonia of the present invention has interpolation in the waste water containing cyanogen and ammonia and comprises secondary
Bromic acid and/or hypochlorous chemical solution and make the operation of cyanogen oxidation Decomposition.It should be noted that in the present invention, " ammonia " includes
" ammonium ion ".It addition, " cyanogen " expression " cyanide ion " and " cyanogen compound such as cyano complex ".
In one mode of the present invention, chemical solution the most only comprises Hydrogen oxybromide (HOBr) and/or hypobromite as oxidant
Composition.In the another way of the present invention, chemical solution comprises Hydrogen oxybromide (HOBr) and/or hypobromite and hypochlorous acid and/or hypochlorous acid
Salt is as oxidizer composition.
The effect of invention
In the processing method containing cyanogen and the waste water of ammonia of the present invention, by Hydrogen oxybromide (HOBr) radical ion, anti-according to following formula of ammonia
Should oxidized decomposition.
OBr-+NH4 +→NH3Br++OH-…………………(3)
2NH3Br++OBr-→N2+3Br-+H2O+2H+………(4)
2NH4 ++3OBr-→N2+3Br-+3H2O+2H+………(5)
It addition, by the oxidisability of Hydrogen oxybromide (HOBr), cyanogen is decomposed.
In the inventive method, such as (3) formula, Hydrogen oxybromide (HOBr) radical ion reacts with ammonia, generation bromo-amine (bromoamine), but bromo-amine
Stronger than the oxidisability of the chloramines generated by chlorine agent.Therefore, it also is able to make cyanogen decompose with bromo-amine.
In the present invention, due to few without chlorine agent or its addition, therefore bonding chlorine and organic reaction cause
Cyanogen generates and is prevented or suppressed, and processes in the way of the abundant step-down of cyanogen concentration.
In the present invention, the Oxidation of the ferrum cyano complex also strength of dimension bromate ion, bromo-amine and be decomposed.Cause
This, in the case of the dissolubility concentration of iron in the waste water containing cyanogen and ammonia is up to more than 0.1mg/L, cyanogen is also divided fully
Solve.It addition, at below pH11, cyanogen is also decomposed fully.
Detailed description of the invention
Below, the present invention is illustrated in further detail.
In the present invention, for become process object containing cyanogen and the waste water of ammonia, give up exemplified with steel plant wastewater, Electroplate Factory
Water, electronics industry waste water, oil refinery waste water etc. are containing cyanogen and the waste water of ammonia, but are not limited to this.
In normal circumstances, total cyanogen concentration of such waste water containing cyanogen and ammonia is 0.1~about 400mg/L, ammonia
Concentration be calculated as more than 10mg/L, for example, 10~about 10000mg/L with ammonium ion.It addition, pH is 6~about 10.
Waste water containing cyanogen and ammonia is sometimes with the Organic substance from coal, coke etc..Organic concentration is usually 1mg/L
Above, for example, 1~about 1500mg/L.
The dissolubility ferrum major part comprised in plant chimney stalk more than pH neutrality containing cyanogen compound is with ferrum cyano complex
Presented in.In cyanogen compound oxidative decomposition according to the inventive method, also decompose ferrum cyano complex, therefore as this
Even if the waste water containing cyanogen processing object of inventive method comprise dissolubility more than ferrum 0.1mg/L, such as 0.1~5mg/L, outstanding
It is 1~3mg/L years old, it is also possible to fully cyanogen and ammonia are carried out resolution process.
From the viewpoint of the generation avoiding HCN gas, containing when adding Hydrogen oxybromide (HOBr) and/or hypobromite and process
The pH having the waste water of cyanogen and ammonia is preferably more than 9.
The ORP containing cyanogen and the waste water of ammonia after making interpolation Hydrogen oxybromide (HOBr) and/or hypobromite is more than 400mV, preferably
For more than 500mV.By making ORP be more than 400mV, it is possible to maintain the oxidisability in water system, it is possible to decompose hard-decomposed ferrum
Cyano complex.On the other hand, about the upper limit of ORP, chemically from the viewpoint of reagent cost, for below 800mV, it is preferably
Below 650mV.
In the present invention, such waste water containing cyanogen and ammonia adds the chemistry comprising Hydrogen oxybromide (HOBr) and/or hypobromite
Solution decomposes cyanogen.
In one mode of the present invention, chemical solution the most only comprises Hydrogen oxybromide (HOBr) and/or hypobromite as oxidant
Composition.In the another way of the present invention, chemical solution comprises Hydrogen oxybromide (HOBr) and/or hypobromite and hypochlorous acid and/or hypochlorous acid
Salt is as oxidizer composition.
As above-mentioned salt, sodium salt or potassium salt, particularly preferred sodium salt can be enumerated.
Hydrogen oxybromide (HOBr) or hypobromite preferably make hypochlorous acid or its salt (preferably sodium hypochlorite) and bromine and/or bromide, excellent
Sodium bromide reaction is selected to generate.Hypochlorous acid and sodium bromide generate Hydrogen oxybromide (HOBr) according to following formula with reaction with same mole.
HOCl+NaBr→HOBr+NaCl
Sodium hypochlorite and sodium bromide generate sodium hypobromite according to following formula with reaction with same mole.
NaOCl+NaBr→NaOBr+NaCl
It should be noted that the hypochlorous acid reacted with bromine and/or bromide can also be to make chlorine be dissolved in the water and generate
The hypochlorous water being dissolved with chlorine.
For containing Hydrogen oxybromide (HOBr) and/or hypobromite or containing Hydrogen oxybromide (HOBr) and/or hypobromite and hypochlorous acid and/
Or the liquid (chemical solution) of hypochlorite is relative to the addition of the waste water containing cyanogen and ammonia, the ORP value of water system can be measured in limit
While be determined.Specifically, as it was previously stated, interpolation to ORP value reaches more than 400mV, preferably reaches more than 500mV.
When adding Hydrogen oxybromide (HOBr) and/or hypobromite and hypochlorous acid and/or hypochlorite in the waste water containing cyanogen and ammonia,
Make Hydrogen oxybromide (HOBr) and/or hypobromite the interpolation mole that interpolation mole is hypochlorous acid and/or hypochlorite 0.1~1.0
Again, particularly preferably 0.3~0.5 times.
For the process of the waste water containing cyanogen and ammonia, intermittently can carry out in groove;Can also make containing cyanogen and ammonia
Waste water be continuously flowed into reactive tank, and be allowed to continuously flow out from this reactive tank, this reactive tank carry out cyanogen and decomposes anti-
Should;The waste water flow ipe containing cyanogen and ammonia can also be made, in this pipeline, add chemical solution and carry out pipeline.
In the present invention, can make the water temperature containing cyanogen and the waste water of ammonia become more than 40 DEG C, for example, 40~80 DEG C, especially
It is about 50~70 DEG C, thus strengthens cyanogen decomposition reaction velocity.In order to suppress heating cost, to make water temperature be less than 80 DEG C, especially
It is preferably less than 70 DEG C.
Embodiment
Below, embodiment and comparative example are illustrated.It should be noted that in the following examples and comparative example, molten
Solution property concentration of iron, ammonium concentration and total cyanogen analysis measure according to JIS K 0102.Total residual chlorine and free residual chlorine
It is to use DPD reagent the residual chlorine meter mensuration utilizing Hach Company to manufacture.
[embodiment 1 (utilizing the process of the liquid containing sodium hypobromite)]
As test water, use the steel plant wastewater of following water quality.
PH:8.3,
Total cyanogen concentration: 0.8mg/L,
Ammonium concentration: 532mg/L,
TOC:22mg/L,
Dissolubility ferrum: 1.3mg/L
ORP:90mV
For the liquid containing sodium hypobromite as chemical solution, use the sodium bromide solution of 40wt% concentration and
The liquor natrii hypochloritis of 12wt% concentration mixes in the way of NaBr:NaOCl=1:1 (mol ratio) and generates the secondary of sodium hypobromite
Sodium bromate and aqueous sodium hypochlorite solution.
Test water 1000mL is stored in glass container, water temperature is held in 50 DEG C, utilize NaOH to make pH become 12
Afterwards, under conditions of table 1, add above-mentioned chemical solution (sodium hypobromite and aqueous sodium hypochlorite solution).Anti-by cyanogen decomposition reaction
1 hour it is set between Ying Shi.
By chemical reagent addition (wherein, the conversion NaBr adding rate of back-to-back test water, NaOCl adding rate) and process
Free residual cl concn, ORP, total cyanogen concentration, total cyanogen resolution ratio, ammonium concentration and ammonium ion after the above-mentioned response time
Resolution ratio is shown in table 1.
[embodiment 2]
As test water, use the steel plant wastewater of following water quality.
PH:8.15,
Total cyanogen concentration: 0.7mg/L,
Ammonium concentration: 354mg/L,
TOC:17mg/L,
Dissolubility ferrum: 1.4mg/L
ORP:230mV
For the liquid containing sodium hypobromite as chemical solution, use liquid same as in Example 1.And, remove
Utilize the NaOH to make pH become beyond 9, process similarly to Example 1.By chemical reagent addition, through previous reaction
Free residual cl concn, ORP, total cyanogen concentration, total cyanogen resolution ratio, ammonium concentration and ammonium ion resolution ratio after time are shown
In table 1.
[embodiment 3]
As test water, use the steel plant wastewater of following water quality.
PH:8.6,
Total cyanogen concentration: 1.2mg/L,
Ammonium concentration: 410mg/L,
TOC:18mg/L,
Dissolubility ferrum: 1.0mg/L
ORP:264mV
Add in the way of becoming 9.6 by pH in addition to NaOH, process test water similarly to Example 2.Result is shown
In table 1.
[comparative example 1 (utilizing the process of sodium hypochlorite)]
As test water, use the steel plant wastewater of following water quality.
PH:8.7,
Total cyanogen concentration: 0.7mg/L,
Ammonium concentration: 451mg/L,
TOC:13mg/L,
Dissolubility ferrum: 1.3mg/L
ORP:230mV
Substitute the liquid containing sodium hypobromite and use sodium hypochlorite (12wt% aqueous solution), in the way of pH becomes 11.1
Add NaOH, for NaOCl, be added with the addition shown in table 1, in addition, similarly to Example 1 to test water
Process.Show the result in table 1.
[comparative example 2 (utilizing the process of sodium hypochlorite)]
As test water, use the steel plant wastewater of following water quality.
PH:8.7,
Total cyanogen concentration: 3.0mg/L,
Ammonium concentration: 120mg/L,
TOC:10mg/L,
Dissolubility ferrum: 0.1mg/L
ORP:210mV
Substitute sodium hypobromite and use sodium hypochlorite (12wt% aqueous solution), in the way of pH becomes 11.3, add NaOH,
For NaOCl, it is added with the addition shown in table 1, in addition, similarly to Example 1 test water is processed.
Show the result in table 1.
Table 1
Such as table 1, contain the embodiment 1~3 of the liquid of sodium hypobromite according to use, with the comparative example only using sodium hypochlorite
1,2 comparing, cyanogen is decomposed fully.It should be noted that high at dissolubility concentration of iron, only use the comparative example 1 of sodium hypochlorite
In, the result of process, total cyanogen concentration also increases than test water.In the present invention, even if dissolubility concentration of iron is high, even and if little
Under conditions of pH11, cyanogen is also decomposed fully.
[embodiment 4 (utilizing the process of the liquid containing sodium hypobromite)]
As test water, use the steel plant wastewater of following water quality.
PH:8.2
Ammonium concentration: 410mg/L
TOC:21mg/L
Dissolubility ferrum: 0.8mg/L
ORP:187mV
As chemical solution (containing sodium hypobromite and the liquid of sodium hypochlorite), use molten for the sodium bromide of 40wt% concentration
Liquid mixes in the way of becoming NaBr:NaOCl=1:1 (mol ratio) with the aqueous sodium hypochlorite solution of 12wt% concentration and generates secondary
The liquid of sodium bromate.
Test water 1000mL is stored in glass container, water temperature is held in 50 DEG C, utilize NaOH to make pH become 9.6
Afterwards, above-mentioned chemical solution is added.To be set in the response time 5 minutes.
By chemical reagent addition (wherein, the conversion NaBr adding rate of back-to-back test water, NaOCl adding rate) and process
Concentration of residual chlorine after the above-mentioned response time is shown in table 2.
[comparative example 3 (utilizing the process of sodium hypochlorite)]
As chemical solution, only add sodium hypochlorite (12wt% aqueous solution) with the addition shown in table 2, in addition,
Similarly to Example 4 same test water is processed.Show the result in table 2.
[embodiment 5~9 (utilizing the process of the liquid containing sodium hypobromite)]
As test water, use the steel plant wastewater of following water quality.
PH:8.3
Ammonium concentration: 532mg/L
TOC:22mg/L
Dissolubility ferrum: 1.3mg/L
ORP:90mV
As chemical solution (containing sodium hypobromite or sodium hypobromite and the liquid of sodium hypochlorite), use 40wt%
The sodium bromide solution of concentration generates sodium hypobromite with the aqueous sodium hypochlorite solution of 12wt% concentration so that the compounding amount of table 2 mixes
Liquid.
Test water 1000mL is stored in glass container, water temperature is held in 50 DEG C, utilize NaOH to make pH become 9.7
After (embodiment 5) or 9.6 (embodiments 6~9), add sodium hypobromite aqueous solution.To be set in the response time 5 minutes.
By chemical reagent addition (wherein, the conversion NaBr adding rate of back-to-back test water, NaOCl adding rate) and process
Concentration of residual chlorine after the above-mentioned response time is shown in table 2.
Table 2
Table 2-1
Table 2-2
<investigation>
Such as table 2, according to the embodiment 4~9 that with the addition of containing sodium hypobromite and the liquid of sodium hypochlorite, though dissolubility ferrum
Concentration is high, and compared with the comparative example 3 only adding sodium hypochlorite, residual chlorine is also few.Thus, it can be known that the present invention can suppress halogen
The generation of gas.
Although use specific mode that the present invention is illustrated in detail, but without departing from the intent and scope of the present invention
Various change can be carried out, will be readily apparent to one having ordinary skill.
The Japanese patent application 2014-084692 that the application proposed based on April 16th, 2014, it is in full by quoting
It is incorporated herein.
Claims (11)
1., containing cyanogen and a processing method for the waste water of ammonia, it has interpolation in the waste water containing cyanogen and ammonia and comprises Hydrogen oxybromide (HOBr)
And/or the chemical solution of hypobromite and make the operation of cyanogen oxidation Decomposition.
The most according to claim 1 containing cyanogen with the processing method of the waste water of ammonia, it is characterised in that described chemical solution is
Bromine and/or bromide solution are mixed with hypochlorous acid and/or aqueous hypochlorite solution and generate Hydrogen oxybromide (HOBr) and/or hypobromite
Liquid.
The most according to claim 2 containing cyanogen with the processing method of the waste water of ammonia, it is characterised in that bromine and/or bromide
It is equimolar amounts with the combined amount of hypochlorous acid and/or hypochlorite.
The most according to claim 1 containing cyanogen with the processing method of the waste water of ammonia, it is characterised in that described chemical solution is
By hypochlorous acid and/or hypochlorite relative to bromine and/or bromide more than equimolar amounts mixing with containing Hydrogen oxybromide (HOBr) and/or secondary
Liquid prepared by the mode of bromate and hypochlorous acid and/or hypochlorite.
5. according to according to any one of claim 2~4 containing cyanogen and the processing method of the waste water of ammonia, it is characterised in that bromine
Compound is sodium bromide, and hypochlorite is sodium hypochlorite.
6. according to according to any one of Claims 1 to 5 containing cyanogen and the processing method of the waste water of ammonia, it is characterised in that contain
Having the dissolubility concentration of iron in the waste water of cyanogen and ammonia is more than 0.1mg/L.
7. according to according to any one of claim 1~6 containing cyanogen and the processing method of the waste water of ammonia, it is characterised in that make
ORP is more than 400mV.
8. according to according to any one of claim 1~7 containing cyanogen and the processing method of the waste water of ammonia, it is characterised in that contain
The waste water having cyanogen and ammonia is steel plant wastewater, waste water from plating plant, electronics industry waste water or oil refinery waste water.
9. according to according to any one of claim 1~8 containing cyanogen and the processing method of the waste water of ammonia, it is characterised in that contain
The total cyanogen concentration having the waste water of cyanogen and ammonia is 0.1~400mg/L, and ammonia density is calculated as 10~10000mg/L with ammonium ion.
10. according to according to any one of claim 1~9 containing cyanogen and the processing method of the waste water of ammonia, it is characterised in that add
The pH containing cyanogen and the waste water of ammonia when adding Hydrogen oxybromide (HOBr) and/or hypobromite and process is more than 9.
11. is according to claim 1 containing cyanogen with the processing method of the waste water of ammonia, it is characterised in that it is to containing cyanogen
Hydrogen oxybromide (HOBr) and/or hypobromite and hypochlorous acid and/or the method for hypochlorite is added, Hydrogen oxybromide (HOBr) and/or secondary with the waste water of ammonia
0.1~1.0 times of the interpolation mole that interpolation mole is hypochlorous acid and/or hypochlorite of bromate.
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JP2014084692A JP5867538B2 (en) | 2014-04-16 | 2014-04-16 | Treatment method for wastewater containing cyanide and ammonia |
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PCT/JP2015/058833 WO2015159653A1 (en) | 2014-04-16 | 2015-03-24 | Method for treating wastewater containing cyanogen and ammonia |
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CN106745961B (en) * | 2016-11-25 | 2019-03-01 | 中冶赛迪工程技术股份有限公司 | A kind of method and system of coking wastewater deep treatment decarburization decoloration decyanation |
CN111111086B (en) * | 2019-12-24 | 2021-06-11 | 东北大学 | Treatment method of cyanide-containing barren solution precipitation slag |
CN113003800A (en) * | 2021-02-25 | 2021-06-22 | 上海金厦实业有限公司 | Wastewater quality-based treatment process |
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CN111517507A (en) * | 2019-02-01 | 2020-08-11 | 兆联实业股份有限公司 | Water treatment system |
CN109911975A (en) * | 2019-03-20 | 2019-06-21 | 江南大学 | A kind of mesoporous material and the preparation method and application thereof that halogen amine macromolecular compound is modified |
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CN106232531B (en) | 2019-08-30 |
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