CN107265602A - It is neutral to alkaline heterophase Fenton method for treating water - Google Patents
It is neutral to alkaline heterophase Fenton method for treating water Download PDFInfo
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- CN107265602A CN107265602A CN201710610515.7A CN201710610515A CN107265602A CN 107265602 A CN107265602 A CN 107265602A CN 201710610515 A CN201710610515 A CN 201710610515A CN 107265602 A CN107265602 A CN 107265602A
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- ferrous
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- organic pollution
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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
- C02F1/722—Oxidation by peroxides
-
- 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
- C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
- C02F2305/026—Fenton's reagent
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- Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Treatment Of Water By Oxidation Or Reduction (AREA)
Abstract
The invention belongs to field of environment pollution control, and in particular to neutral to alkaline heterophase Fenton method for treating water.Catalyst solid, which is added, in neutral or alkalescence Organic Pollution water body to be repaired contains ferrous materia and H2O2, the repairing organic polluted water body of heterogeneous Fenton system is built, the removal of pollutant is carried out；Described solid is the one or more in ferrous tartrate, acetylacetone,2,4-pentanedione ferrous iron, ferrous lactate, ferrous phosphate, ferrous oxalate or ferrous citrate containing ferrous materia.This method solve Fenton reaction systems can not be the problem of efficient renovation of organic pollution aquifer and Fenton reagent can not be recycled and reused under neutrality to alkalescence condition, available for the reparation of different pH Organic Pollution water body, there is efficient, non-selectivity, environment-friendly, non-secondary pollution.
Description
Technical field
The invention belongs to field of environment pollution control, and in particular to a kind of control of Organic Pollutants In Water and reparation side
Method, it is adaptable to print and dye, the neutral processing to alkaline organic wastewater in the field such as agricultural.
Background technology
With the economic sustained and rapid development of China, water pollution problems is increasingly serious, and the trend that presentation extends from point to face,
The healthy living of the mankind is seriously threatened.Fenton oxidation technology is a kind of hydroxyl radical free radical (OH) to produce strong oxidizing property
With the characteristics of high-level oxidation technology, the OH of generation can be with non-selectivity ground degradable organic pollutant., French scientist in 1894
H.J.Fenton has found Fe (II) and H2O2Mixed solution organic compound such as carboxylic acid, alcohol, esters quickly can be oxidized to nothing
Machine thing, afterwards Fe (II) and H2O2It is named as Fenton reagent.Fenton oxidation technology has that reaction efficiency is high, the time is short, dress
Put that simple, reaction condition is gentle, reactant advantages of environment protection, and the thorough mineralising of organic matter can be CO by it2、H2O and nothing
Machine salt, with good application prospect and great promotional value.Therefore, Fenton oxidation technology is to degrade to remove to have in environment
The optimal selection of organic pollutants.
In traditional Fenton (Fe (II)/H2O2) in oxidation system, Fe (II) and hydrogen peroxide (H2O2) reaction (76M-1s-1) production
Raw strong oxidizing property hydroxyl radical free radical (OH) and ferric ion, and ferric ion and H2O2React (0.02M-1s-1) regeneration
Ferrous process is slowly so that ferrikinetics is less efficient in system, causes H2O2It is unable to last decomposition utilization rate low.
And tradition Fenton reactions need to carry out under the conditions of relatively low pH (2.0~3.5).Heterogeneous Fenton system construction can
To widen the pH scope of applications of Fenton reactions to a certain extent, and realize that iron is reused, and attract wide attention.But it is existing
There is heterogeneous Fenton system still to have preferable oxidation efficiency below neutral range.And exist in practice many neutral
To the pollution environment of alkalescence, such as Sediment System, typically all in neutral and weak basic condition.Petrochemical industry, papermaking and weaving row
Industry can all produce alkaline waste water.General in alkaline sewage all to contain substantial amounts of organic matter, being discharged into natural water largely to consume
Dissolved oxygen in water body, causes fish anoxia asphyxia dead.Still can be with efficient degradation under neutrality to alkalescence condition so building
The heterogeneous Fenton system of organic pollution is very important.
The content of the invention
The technical problems to be solved by the invention are the deficiencies for above-mentioned Fenton oxidation technology, and there is provided neutrality extremely
Alkaline heterophase Fenton method for treating water.This method solve Fenton reaction systems can not be under neutrality to alkalescence condition efficiently
The problem of renovation of organic pollution aquifer and Fenton reagent can not be recycled and reused, the Organic Pollution available for different pH
The reparation of water body, has the advantages that efficient, non-selectivity, environment-friendly, non-secondary pollution.
The technical scheme that the present invention is used by solution the problem of set forth above for：
It is neutral to alkaline heterophase Fenton method for treating water, it is characterised in that：In neutral or alkalescence organic matter to be repaired
Catalyst solid is added in polluted-water and contains ferrous materia and H2O2, build heterogeneous Fenton system repairing organic polluted
Water body, carries out the removal of pollutant；Described solid containing ferrous materia be ferrous tartrate, acetylacetone,2,4-pentanedione ferrous iron, ferrous lactate,
One or more in ferrous phosphate, ferrous oxalate or ferrous citrate.
By such scheme, described solid concentration containing ferrous materia is 1~50mmol/L.
By such scheme, the neutral pH value to alkaline organic pollution aquifer to be repaired is 7~12.
By such scheme, the H2O2Concentration in Organic Pollution water body to be repaired is 5~200mmol/L.
By such scheme, the addition catalyst solid contains ferrous materia and H2O2System is stirred afterwards, solution is filled
Divide mixing, then repaired.System is not stirred, better effects can also be obtained.
There is Fe (II) in traditional Fenton oxidation system and be oxidized to Fe (III), Fe (III)/Fe (II) cycle efficieny
It is relatively low, the easy flocculation sediments of Fe (II), H2O2Utilization rate is low, and tradition Fenton reactions are needed in relatively low pH (2.0-3.5)
Under the conditions of carry out, iron ion is difficult to separate reuse after reaction.Building heterogeneous Fenton system can widen
The pH scope of applications of Fenton reactions, and realize that iron is reused.It is usually used in the material as heterogeneous Fenton catalyst
There are the iron-bearing materials such as di-iron trioxide, ferroso-ferric oxide, FeOOH and nano zero valence iron.The Fe on these iron-bearing materials surfaces
And H (III)2O2Reaction generation surface Fe (II), surface Fe (II) are to H2O2Transmission electronics makes H2O2Decompose and produce hydroxyl radical free radical.
However, can only have preferably oxidation effect below neutral range by the use of these materials as catalyst heterogeneous Fenton
Rate.Hydroxyl is the lewis base stronger compared with hydrogen peroxide, it is easier to be used as lewis acidic iron ion (Fe (II) with material surface
With Fe (III)) combine and adsorb in material surface, therefore under higher pH condition, these material surfaces are easier to adsorb hydrogen-oxygen
Root, in material characterization one layer of iron hydroxide shell of formation, it is difficult to contact generation electron transmission with iron ion again to make hydrogen peroxide, is caused
Decomposing hydrogen dioxide solution efficiency and the reduction of ferrikinetics efficiency.
The inventive method utilizes catalyst solid iron-bearing materials and H2O2The heterophase Fenton system of structure, catalyst surface
Fe (II) can transmit electronics (in neutral or basic conditions, catalyst solid iron-bearing materials will not dissolve, in solution detect
Less than Fe (II), illustrate that the Fe (II) of the catalyst surface under this pH value condition plays decomposing H2O2Leading role), make H2O2
Be excited generation strong oxidizing property OH, for the high poison persistence organic pollutant in the degraded water body of non-selectivity, and is catalyzed
The Fe (III) of agent plane of crystal causes catalyst surface to be not easily formed hydrogen-oxygen based on the effect with iron coordinating group in crystal
Change iron-clad layer, and can contact H2O2It is reduced into again as surface Fe (II), catalyst surface is there is good Fe (III)/Fe
(II) circulate, improve H under neutral and alkalescence condition2O2Decomposition efficiency, improves organic pollution aquifer remediation efficiency, thus solves
The problem of being difficult to circulation using traditional Fenton and general heterophase Fenton oxidation technology pH narrow application ranges and Fe.
The advantage of the invention is that：
1st, the neutrality that the present invention is built is into alkaline heterophase Fenton system, without obvious iron dissolution, H2O2Decompose in catalysis
Agent surface is carried out, and the surface Fe (III) that oxidation is produced can be by the H in system2O2Restore as surface Fe (II), so as to promote
Catalyst surface Fe (III)/Fe (II) circulations so that H2O2Last decomposition, under neutrality to alkalescence condition, to organic pollution
Degraded non-selectivity, efficiency high.
2nd, the inventive method is after neutrality to alkaline organic pollution aquifer is repaired, and catalyst can be reclaimed and reused,
Secondary pollution is not resulted in.
3rd, reaction condition is gentle, and normal temperature and pressure can fast reaction, simple to operate without complex appts, no danger, nothing
Professional need to be engaged to operate.
Brief description of the drawings
Fig. 1 is that the inventive method repairs the neutral design sketch to alkaline organic pollution aquifer using the catalyst reclaimed.
Embodiment
Describe the content of the invention of the present invention in detail below by specific implementation case, described specific embodiment is only used
To explain the present invention, it is not intended to limit the present invention.
Embodiment 1 is repaired neutral to alkaline organic pollution aquifer
Neutrality to alkaline organic pollution aquifer is derived from the different sample points of certain printing house six, six organic pollution aquifer samples
PH be respectively 7,8,9,10,11 and 12, after sampling, determine that pH has for 7,8,9,10,11 and 12 by chemical oxygen demand detection
The COD of machine polluted-water is respectively 365,354,351,342,335 and 387mg/L.
For the reparation of above-mentioned different pH organic pollution aquifer, into 50mL contaminant waters add catalyst ferrous phosphate and
H2O2, it is respectively 2mmol/L and 5mmol/L to make its concentration, is well mixed solution with magnetic stirrer, rotating speed is
400rpm, reacts 120min.It the results are shown in Table 1.While to dose same concentrations FeSO4·7H2O and H2O2Repair different pH pollutions
Water body is control experiment, the results are shown in Table 2.Shown in table 1, in the polluted-water that initial pH is respectively 7,8,9,10 and 11, reaction
120min, COD clearance has respectively reached 82%, 78%, 74%, 69%, 62% and 51%.Shown in table 2, first
Beginning pH value is in 7,8,9,10,11 and 12 polluted-water, reacts 120min, and COD clearance is 0.
Embodiment 2 is in different H2O2Alkaline organic pollution aquifer is repaired under concentration
Alkaline organic pollution aquifer is derived from certain printing house, and polluted-water sample pH value is 10, after sampling, passes through COD
Detection determines that pH is about 342mg/L for the chemical oxygen demand value of 10 organic pollution aquifer.
For the reparation that pH value is the organic pollution aquifer that 10, chemical oxygen demand value is 342mg/L, into 50mL contaminant waters
Catalyst ferrous phosphate is added, it is 2mmol/L to make its concentration, then adds H thereto2O2, it is respectively 2,5,7.5 and to make its concentration
10mmol/L, is well mixed solution, rotating speed is 400rpm with magnetic stirrer.It the results are shown in Table 3.
Shown in table 3, in the polluted-water that initial pH is 10, with H2O2The increase organic pollution aquifer of initial concentration
COD clearance is improved, and works as H2O2When initial concentration is respectively 2,5,7.5 and 10mmol/L, 120min is reacted, chemistry is needed
Oxygen amount clearance has respectively reached 43%, 69%, 75% and 82%.
Embodiment 3 repairs alkaline organic pollution aquifer under different catalysts concentration
Alkaline organic pollution aquifer is derived from certain printing house, and polluted-water sample pH value is 10, after sampling, passes through COD
Detection determines that pH is about 342mg/L for the chemical oxygen demand value of 10 organic pollution aquifer.
For the reparation that pH value is the organic pollution aquifer that 10, chemical oxygen demand value is 342mg/L, into 50mL contaminant waters
Add H2O2, it is 5mmol/L to make its concentration, then adds catalyst ferrous phosphate thereto, and it is respectively 1,2,4 and to make its concentration
6mmol/L, is well mixed solution, rotating speed is 400rpm with magnetic stirrer.It the results are shown in Table 4.
Shown in table 4, in the polluted-water that initial pH is 10, with the increase organic pollution aquifer of catalyst initial concentration
COD clearance improve, when catalyst initial concentration be 1,2,4 and 6mmol/L when, react 120min, chemical oxygen demand
Amount clearance has respectively reached 31%, 69%, 73% and 77%.
Embodiment 4 repairs neutral to alkaline organic pollution aquifer using the catalyst reclaimed
Neutrality is derived from certain printing house to alkaline organic pollution aquifer, and polluted-water sample pH value is divided into 7 and 10, after sampling, leads to
The COD for crossing the organic pollution aquifer that chemical oxygen demand detection determines that pH is 7 and 10 is respectively 365mg/L and 342mg/
L。
For pH value be respectively 7 and 10, COD be respectively 365mg/L and 342mg/L organic pollution aquifer
Repair, catalyst ferrous phosphate and H are added into 50mL contaminant waters2O2, it is respectively 2 and 5mmol/L to make its concentration, is stirred with magnetic force
Mixing device stirring is well mixed solution, and rotating speed is 400rpm.React after 120min, ferrous phosphate reclaimed, reuse 6 times,
As a result Fig. 1, table 5 and table 6 are seen.Shown in Fig. 1 and table 5, in initial pH in 7 organic pollution aquifer, ferrous phosphate is reclaimed 6 times
Afterwards, 120min is reacted, COD clearance has reached 79%.Shown in table 6, in the organic pollution aquifer that initial pH is 10
In, after ferrous phosphate is reclaimed 6 times, 120min is reacted, COD clearance has reached 64%.
Case study on implementation 5 repairs neutral to alkaline organic pollution aquifer using different catalysts
Neutrality is derived from certain printing house to alkaline organic pollution aquifer, and polluted-water sample pH value is divided into 7 and 10, after sampling, leads to
The COD for crossing the organic pollution aquifer that chemical oxygen demand detection determines that pH is 7 and 10 is respectively 365mg/L and 342mg/
L。
For pH value be respectively 7 and 10, COD be respectively 365mg/L and 342mg/L organic pollution aquifer
Repair, catalyst ferrous tartrate or acetylacetone,2,4-pentanedione ferrous iron or ferrous lactate or ferrous phosphate or grass are added into 50mL contaminant waters
Sour ferrous or ferrous citrate and H2O2, it is respectively 2 and 5mmol/L to make its concentration, makes solution mixing equal with magnetic stirrer
Even, rotating speed is 400rpm, after reaction 120min, the results are shown in Table 7 and table 8.Shown in table 7, in the organic pollution aquifer that initial pH is 7
In, adding catalyst ferrous tartrate or acetylacetone,2,4-pentanedione ferrous iron or ferrous lactate or ferrous phosphate or ferrous oxalate or citric acid
Ferrous and H2O2System in, react 120min, COD clearance has respectively reached 78%, 76%, 79%, 82%,
81% and 80%.Shown in table 8, in the organic pollution aquifer that initial pH is 10, catalyst ferrous tartrate or acetyl are being added
Acetone ferrous iron or ferrous lactate or ferrous phosphate or ferrous oxalate or ferrous citrate and H2O2System in, react 120min, change
Learn oxygen demand clearance and respectively reach 70%, 68%, 65%, 73%, 71% and 72.
Table 1
Table 2
Table 3
Table 4
Table 5
Table 6
Table 7
Table 8
Claims (5)
1. it is neutral to alkaline heterophase Fenton method for treating water, it is characterised in that：It is dirty in neutral or alkalescence organic matter to be repaired
Contaminate and catalyst solid is added in water body containing ferrous materia and H2O2, build the repairing organic polluted water of heterogeneous Fenton system
Body, carries out the removal of pollutant；Described solid is ferrous tartrate, acetylacetone,2,4-pentanedione ferrous iron, ferrous lactate, phosphorus containing ferrous materia
One or more in sour ferrous, ferrous oxalate or ferrous citrate.
2. it is according to claim 1 neutral to alkaline heterophase Fenton method for treating water, it is characterised in that：Described solid
Concentration containing ferrous materia is 1~50mmol/L.
3. it is according to claim 1 neutral to alkaline heterophase Fenton method for treating water, it is characterised in that：It is described to be repaired
The neutral pH value to alkaline organic pollution aquifer is 7~12.
4. it is according to claim 1 neutral to alkaline heterophase Fenton method for treating water, it is characterised in that：The H2O2
Concentration in Organic Pollution water body to be repaired is 5~200mmol/L.
5. it is according to claim 1 neutral to alkaline heterophase Fenton method for treating water, it is characterised in that：The addition is urged
Agent solid contains ferrous materia and H2O2System is stirred afterwards, solution is sufficiently mixed, is then repaired.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108191039A (en) * | 2018-02-24 | 2018-06-22 | 武汉纺织大学 | A kind of efficient compound Fenton reagent and preparation method thereof |
| CN110683993A (en) * | 2019-10-16 | 2020-01-14 | 黄冈师范学院 | Preparation method and application of ferrous phthalhydrazide |
| CN111018012A (en) * | 2019-11-26 | 2020-04-17 | 南京源泉环保科技股份有限公司 | Fluorescent wastewater high-COD (chemical oxygen demand) treating agent |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105967314A (en) * | 2016-06-27 | 2016-09-28 | 华中师范大学 | Method for restoring organic matter polluted water body using ferrous oxalate-activated persulfate system |
| CN106277278A (en) * | 2016-10-14 | 2017-01-04 | 合肥工业大学 | A kind of method utilizing iron oxides multiphase Fenton system to process arsenic-containing waste water |
-
2017
- 2017-07-25 CN CN201710610515.7A patent/CN107265602A/en active Pending
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105967314A (en) * | 2016-06-27 | 2016-09-28 | 华中师范大学 | Method for restoring organic matter polluted water body using ferrous oxalate-activated persulfate system |
| CN106277278A (en) * | 2016-10-14 | 2017-01-04 | 合肥工业大学 | A kind of method utilizing iron oxides multiphase Fenton system to process arsenic-containing waste water |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108191039A (en) * | 2018-02-24 | 2018-06-22 | 武汉纺织大学 | A kind of efficient compound Fenton reagent and preparation method thereof |
| CN110683993A (en) * | 2019-10-16 | 2020-01-14 | 黄冈师范学院 | Preparation method and application of ferrous phthalhydrazide |
| CN110683993B (en) * | 2019-10-16 | 2022-11-04 | 黄冈师范学院 | Preparation method and application of ferrous phthalhydrazide |
| CN111018012A (en) * | 2019-11-26 | 2020-04-17 | 南京源泉环保科技股份有限公司 | Fluorescent wastewater high-COD (chemical oxygen demand) treating agent |
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Application publication date: 20171020 |