CN104609597A - Method for removing organic pollutants in water at ultrahigh speed - Google Patents
Method for removing organic pollutants in water at ultrahigh speed Download PDFInfo
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- CN104609597A CN104609597A CN201410846501.1A CN201410846501A CN104609597A CN 104609597 A CN104609597 A CN 104609597A CN 201410846501 A CN201410846501 A CN 201410846501A CN 104609597 A CN104609597 A CN 104609597A
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Abstract
The invention relates to a method for removing organic pollutants in water at an ultrahigh speed. The method comprises the following steps: firstly, adding a reducing agent to water to be treated; secondly, adjusting the pH value of the water to be treated to be within the range of 3-7; thirdly, adding an oxidizing agent to the water to be treated. According to the method, bisulfite radicals are utilized for reacting with potassium permanganate or manganese dioxide, the removal of the organic pollutants in the water at the ultrahigh speed is realized by quickly generating a highly active oxidizing agent Mn(III) (at a non-complexing state), the rate of removing the pollutants by potassium permanganate and manganese dioxide can be improved by one thousand to one million times and is ten thousand times higher than the apparent oxidation rate of a general advanced oxidation technology, and the degradation for the pollutants can be completed in ten seconds or several seconds. According to the method, the pollutants incapable of being oxidized by potassium permanganate and manganese dioxide can also be oxidized, and even nitrobenzene capable of being oxidized by hydroxyl radicals only in traditional meanings can be oxidized, so that the oxidizing capacity of potassium permanganate and manganese dioxide is greatly improved, and the application range of potassium permanganate and manganese dioxide is expanded.
Description
Technical field
The invention belongs to water and technical field of sewage, relate to a kind of method of supper-fast removal organic pollutants, can be applicable to drinking water treatment, treatment of domestic sewage advanced and Industrial Wastewater Treatment.
Background technology
Water is the very important precious resources of occurring in nature, and the life of the mankind is produced and the progress of society all be unable to do without water resources, and the water resources of safe and high quality is more related to the national future economy and social development in an all-round way.Along with the develop rapidly of China's industrial or agricultural in recent years, water surrounding is faced with severe challenge and the pressure of resource and water quality lack of water two aspect to be formed by problems such as such as water pollution, water quality deterioration and high-quality shortage of water resources at present.In the world today that industrialization and development of globalization are constantly deepened, water pollution problem has become the problem that the whole world is paid close attention to.The seventies, EPA detected some organic pollutants in tap water, allowed water environment pollution problem become more complicated and serious.Some investigators had found POPs(persistence organic pollutant again in succession in drinking water source in recent years), EDCs(endocrine disrupter) and PPCPs(medicine and personal care articles) etc. emerging organic pollutant, the organic contamination problem in water becomes focus and the study hotspot of people's extensive concern just day by day.Chemical oxidization method is one of the most frequently used water treatment method, is oxidizing, the treatment process that decomposes and transform water pollutant that utilize oxidation capacity stronger.Oxygenant conventional in Water purification has ozone, chlorine, potassium permanganate, dioxide peroxide, ferrate and hydrogen peroxide etc.Ozone has very strong oxidation capacity, and redox potential reaches 2.07V, can pollute by great majority in oxidizing water, but when there is bromide anion in water, bromide anion is oxidized to the bromate of strong carinogenicity by ozone; Chlorine is a kind of widely used Water Disinfection agent, but current research finds likely to react with organism in chlorine oxidation process to generate poisonous halogenated organic matters; Potassium permanganate is a kind of oxygenant of green, poisonous, harmful halogenated disinfection by-products can not be produced in oxidative degradation organism process, and easy handling uses, be convenient to transport, cheap, but potassium permanganate oxidation is limited in one's ability, comparatively slow for most organic pollutant rate of oxidation, can not oxidation removal to some constitutionally stable organic pollutants; Dioxide peroxide has stronger oxidation capacity, affects little by temperature and pH, does not produce the by product such as haloform and halogen acetic acid, does not produce mutagenic matter, but disinfection by chlorine dioxide produces Inorganic Disinfectant By-products chlorition (ClO
2 -) and chloranion (ClO
3 -).Ferrate is also a kind of oxygenant of green, and oxidation products ferric iron can also strengthen removal to pollutent as coagulating agent, but ferrate poor stability, be not easy to preserve and use; The redox potential of hydrogen peroxide reaches 1.77 V, but has labile shortcoming, limits its practical application.Except the oxidation technology of routine, also obtain application in water treatment and advanced treatment of wastewater field in recent years with the high-level oxidation technology that hydroxyl radical free radical or potentiometric titrations are active oxidation component.Although hydroxyl radical free radical oxidation capacity is very strong, with the oxidation rate constant of most pollutent between 10
8-10
10m
-1s
-1.But due to common high-level oxidation technology (O
3/ H
2o
2, Fe
2+/ H
2o
2, UV/O
3, UV/O
3/ H
2o
2, UV/H
2o
2) hydroxy free radical concentration that produces in process is low to moderate 10
-14-10
-16mol L
-1be that the observed rate constant that the high-level oxidation technology of active oxidizer is oxidized organic pollutant is not high with hydroxyl radical free radical, and hydroxyl radical free radical does not have selectivity, in actual water, humic acid except target contaminant, bicarbonate radical etc. all can consume hydroxyl radical free radical, thus reduce oxidation efficiency further.Potentiometric titrations is more weak than the oxidation capacity of hydroxyl radical free radical and have certain selectivity, therefore causes the concern of investigator in recent years, but is that the rate of oxidation of technology to pollutent of active oxidizer is slower with potentiometric titrations.Therefore the more efficient oxidation technology of development is needed badly to realize the quick removal of organic pollutants.
Correlative study display manganic has important role in natural redox processes.Bivalent manganese can be oxidized to tetravalent manganese by oxygenizement by bacterium, thus controls the concentration of bivalent manganese in the circulation of manganese and ocean, in the working cycle of manganese, have manganic generation; In ocean, bivalent manganese can be oxidized to manganic at the top of anaerobic zone, and Manganse Dioxide can be reduced to manganic in the bottom of anaerobic zone, then by the ligands stabilize in seawater.Manganic is by obtaining electronics or losing the existence of anaerobic zone in electronically controlled ocean.Manganese In Soils element and oxide compound thereof to plant-growth and environmental pollution improvement significant, the pollutent that the manganic in soil can be oxidized as oxygenant and degrade in soil, affects the Transport And Transformation of pollutent.The manganic of free state has very high oxidation activity, there is the possibility as high-efficient oxidant, but free state manganic is unstable, be very easy to be hydrolyzed to bivalent manganese and Manganse Dioxide, part can extend manganic lifetime by generating complex state manganic, so the manganic reported in document detects under all having part existence condition, but part also reduces manganic oxidation activity complexing is manganic simultaneously.CN101503242B discloses a kind of water treatment agent utilizing the manganese strengthened potassium permanganate depollution of intermediate state, adds complexing agent or in potassium permanganate oxidation process, add complexing agent (part) and inductor simultaneously in potassium permanganate oxidation process.This method only improves several times to tens times to the speed of potassium permanganate oxidation pollutent, mainly because of the oxidation activity that can affect intermediate state manganese after part and the complexing of intermediate state manganese, reduce the oxidation capacity of intermediate state manganese, make the highly active oxidation advantage of intermediate state manganese can not get playing.Therefore find a kind of new original position and produce the manganic method of free state, play manganic high oxidation activity advantage, make it be applied to being very important of efficient degradation water pollutant.
Summary of the invention
In order to make full use of the feature of the manganic high oxidation activity of free state, the invention provides a kind of method of supper-fast removal organic pollutants.The method utilizes bisulfite and potassium permanganate or Manganse Dioxide to react, by producing rapidly highly active oxygenant Mn (III) (non-complexing state), realize the supper-fast removal to organic pollutants, the speed that potassium permanganate and manganese dioxide remove pollutent can be improved 1 thousand to one hundred ten thousand times, exceed about 10,000 times than the apparent rate of oxidation of general high-level oxidation technology, the degraded to pollutent in 1 second or in several seconds, can be completed.This method is oxidable potassium permanganate and the Manganse Dioxide pollutent that originally cannot be oxidized also, even can be oxidized the oil of mirbane that traditional sense only has hydroxyl radical free radical to be oxidized, substantially increase the oxidation capacity of potassium permanganate and Manganse Dioxide, expand the range of application of potassium permanganate and Manganse Dioxide.
The object of the invention is to be achieved through the following technical solutions:
A method for supper-fast removal organic pollutants, comprises the steps:
One, in pending water, add reductive agent, described reductive agent is sulphite or hydrosulphite;
Two, by pending water pH regulator in the scope of 3-7;
Three, in pending water, add oxygenant, described oxygenant is permanganate or Manganse Dioxide, and the mol ratio controlling reductive agent and oxygenant is 3-10.
In the present invention, described reductive agent is the sulphite or hydrosulphite storing solution that have dissolved in advance, and oxygenant is the potassium permanganate storing solution or Manganse Dioxide colloid storing solution that have dissolved in advance, and solvent for use is distilled water.
In the present invention, adding the pending water after sulphite or hydrosulphite must by pH regulator to 3-7, the pK of sulfurous acid
a1be 7.2, low ph value ensure that in the sulphite or bisulfite solution added has a large amount of bisulfites to exist.
In the present invention, reductive agent used, except sulphite and hydrosulphite, can also be other the material that Mn (III) can be induced to produce.
In the present invention, described sulphite is S-WAT, potassium sulfite or other sulphite; Described hydrosulphite is sodium bisulfite, Potassium hydrogen sulfite or other hydrosulphite.
In the present invention, by measuring the change in concentration of water pollutant, evaluate the palliating degradation degree of water pollutant.
In the present invention, water treatment method carries out in complete or magnetic stirring apparatus.
In the present invention, pending water is surface water, underground water, sanitary sewage or trade effluent.
In the present invention, the key of described method is the mol ratio controlling bisulfite and potassium permanganate (or Manganse Dioxide), when the mol ratio <3 of bisulfite and potassium permanganate (or Manganse Dioxide) time, sulphite or adding of hydrosulphite can accelerate the degraded of potassium permanganate to pollutent, but tens-tens times can only be improved, supper-fast degradation of contaminant cannot be realized; When mol ratio >=20 of bisulfite/potassium permanganate (or Manganse Dioxide) time, sulphite or adding of hydrosulphite start to play restraining effect to potassium permanganate oxidation pollutent; When the mol ratio 10-20 of bisulfite/potassium permanganate (or Manganse Dioxide) time, although pretty good to the degradation effect of pollutent, the medicament that needs add is too many, and cost is too high; Therefore, the application selects the mol ratio 3-10 of bisulfite/potassium permanganate (or Manganse Dioxide).
Take oxygenant as potassium permanganate be example, sulfite hydrogen root of the present invention and potassium permanganate react the principle that original position produces high reactivity free state manganic and supper-fast oxidation removal organic pollutant thereof: bisulfite and potassium permanganate are swift in response and generate free state Mn (III) (non-complexing state), free state Mn (III) has superelevation oxidation activity, can remove various organic pollutants in water by Quick Oxidation.The present invention's utilize bisulfite and potassium permanganate to produce supper-fast degraded that highly active Mn (III) (non-complexing state) realizes organic pollutants, can by inoxidizable for potassium permanganate pollutent rapid oxidation, the pollutent that can be oxidized for potassium permanganate drastically increases rate of oxidation.
Compared with existing water treatment method for oxidation, there is following outstanding superiority:
(1) reagent that the present invention uses is potassium permanganate (or Manganse Dioxide) and sulphite (or hydrosulphite), it is all the solid reagent of green safety, convenient transportation and cheap, do not need extra processing unit, being applied to existing technique does not need to transform technique;
(2) the oxidant reaction after product that the present invention uses is Manganse Dioxide (or Mn
2+) and sulfate radical, Manganse Dioxide has absorption, helps solidifying effect, can strengthen the removal of pollutent; Sulfate radical is nontoxic, is the background ions in water; Mn
2+manganse Dioxide can be generated by atmospheric oxidation of exposing to the sun and filter removal.
(3) mild condition of this reaction needed, does not need strongly-acid or strong alkaline condition, is easy to practical application;
(4) in the present invention, the removal " instantaneously " (-several seconds a few tens of milliseconds) of pollutent completes, about 10,000 times are exceeded than traditional high-level oxidation technology speed of reaction, and this technology of pollutent that potassium permanganate and manganese dioxide cannot be removed also can be removed, its effect is more much better than the effect reported in CN101503242B, also reflects the difference of reaction mechanism from the side.
Accompanying drawing explanation
When Fig. 1 is initial pH=5, in S-WAT activation potassium permanganate treatment of simulated surface water, phenol (schemes a) (to scheme effect contrast figure b) with independent potassium permanganate process phenol;
When Fig. 2 is initial pH=7, in S-WAT activation potassium permanganate treatment of simulated underground water, phenol (schemes a) (to scheme effect contrast figure b) with independent potassium permanganate process phenol;
When Fig. 3 is initial pH=5, in potassium sulfite activation potassium permanganate process sanitary sewage disposal secondary effluent, Ciprofloxacin (schemes a) (to scheme effect contrast figure b) with independent potassium permanganate process Ciprofloxacin;
When Fig. 4 is initial pH=7, in potassium sulfite activation potassium permanganate process trade effluent, reactive blue 4 (schemes a) (to scheme effect contrast figure b) with independent potassium permanganate process reactive blue 4;
When Fig. 5 is initial pH=3, sodium bisulfite activates the effect contrast figure of oil of mirbane and independent potassium permanganate oil of mirbane in potassium permanganate treatment of simulated surface water;
When Fig. 6 is initial pH=7, sodium bisulfite activates the effect contrast figure of caffeine and independent potassium permanganate caffeine in potassium permanganate treatment of simulated surface water;
The effect contrast figure of phenol and independent manganese dioxide phenol in S-WAT activated manganese dioxide treatment of simulated surface water when Fig. 7 is initial pH=6;
When Fig. 8 is initial pH=7, S-WAT activation potassium permanganate coexists to phenol and Ciprofloxacin in simulation surface water the treatment effect of water sample.
Embodiment
Below in conjunction with accompanying drawing, technical scheme of the present invention is further described; but be not limited thereto; everyly technical solution of the present invention modified or equivalent to replace, and not departing from the spirit and scope of technical solution of the present invention, all should be encompassed in protection scope of the present invention.
Embodiment one: the method for the supper-fast removal organic pollutants in present embodiment is carried out in complete, and concrete steps are as follows:
To containing 5 μm of ol L
-1250 μm of ol L are added in the simulation surface water water of phenol
-1s-WAT, regulates pH=5, by 50 μm of ol L
-1potassium permanganate (that is: sulphite/potassium permanganate mol ratio=5) joins in above-mentioned simulation surface water, as long as 80 milliseconds of removals completely that can realize phenol.When being used alone potassium permanganate, need the removal completely that could realize phenol for 4 hours.Because the observed rate constant making phenol remove that adds of S-WAT improves 42.25 ten thousand times.Concrete effect comparison data are shown in Fig. 1.
Embodiment two: present embodiment and embodiment one are unlike the pH=7 of reaction.Because the observed rate constant making phenol remove that adds of sulphite improves 4100 times.Concrete effect comparison data are shown in Fig. 2.
Embodiment three: present embodiment and embodiment one unlike: the dosage of sulphite is 150 μm of ol L
-1(that is: sulphite/potassium permanganate mol ratio=3).Because the observed rate constant making phenol remove that adds of sulphite improves 400,000 times.
Embodiment four: present embodiment and embodiment one unlike: the dosage of sulphite is 500 μm of ol L
-1(that is: sulphite/potassium permanganate mol ratio=10).Because the observed rate constant making phenol remove that adds of sulphite improves 450,000 times.
Embodiment five: present embodiment and embodiment one are Ciprofloxacin in sanitary sewage disposal secondary effluent unlike: the pollutent in handled water and sulphite used is potassium sulfite.Ciprofloxacin in potassium sulfite and potassium permanganate conbined usage process sanitary sewage secondary effluent, as long as 45.6 milliseconds of removals completely that can realize Ciprofloxacin.When being used alone potassium permanganate, the Ciprofloxacin of 57% within 80 minutes, only can be removed.Because the observed rate constant making Ciprofloxacin remove that adds of potassium sulfite improves 1,531 ten thousand times.Concrete effect comparison data are shown in Fig. 3.
Embodiment six: present embodiment and embodiment one are reactive blue 4 in trade effluent unlike: the pollutent in handled water and the initial pH reacted is 7 and sulphite used is potassium sulfite.Compared with independent potassium permanganate oxidation, conbined usage potassium sulfite and potassium permanganate can make the oxidation removal speed of reactive blue 4 improve 1258 times.Concrete effect comparison data are shown in Fig. 4.
Embodiment seven: the method for the supper-fast removal organic pollutants in present embodiment utilizes in magnetic stirring apparatus carries out, and concrete steps are as follows:
To containing 5 μm of ol L
-1150 μm of ol L are added in the simulation surface water of oil of mirbane
-1sodium bisulfite, regulates pH=3, by 50 μm of ol L
-1potassium permanganate (that is: hydrosulphite/potassium permanganate mol ratio=3) joins in above-mentioned simulation surface water, can remove the oil of mirbane of 33% in 10 seconds.When being used alone potassium permanganate, the removal of oil of mirbane can be ignored.Concrete effect comparison data are shown in Fig. 5.Present embodiment shows, and utilizes the method can improve the oxidation capacity of potassium permanganate, and not only improves its rate of oxidation to pollutent.
Embodiment eight: present embodiment and embodiment seven unlike: the pH of handled water is 7, and pollutent is caffeine.As hydrosulphite and the process of potassium permanganate conbined usage are simulated surface water containing caffeine, the caffeine of 38.3% in 10 seconds, can be removed.When being used alone potassium permanganate, the removal of caffeine can be ignored.Concrete effect comparison data are shown in Fig. 6.Present embodiment display utilizes the method can improve the oxidation capacity of potassium permanganate, and not only improves its rate of oxidation to pollutent.
Embodiment nine: the technology of the supper-fast removal organic pollutants in present embodiment is carried out in complete, and concrete steps are as follows:
First dropped into by sodium bisulfite in pending water, in water, contained pollutent is Ciprofloxacin, adds potassium permanganate again, mol ratio=3 of hydrosulphite/potassium permanganate after regulating pH=7 of handled water.Compared with independent potassium permanganate oxidation, hydrosulphite and potassium permanganate conbined usage make the oxidation removal speed of Ciprofloxacin improve 35.7 ten thousand times.
Embodiment ten: present embodiment and embodiment nine unlike: the pH of handled water is 3, mol ratio=5 of hydrosulphite/potassium permanganate.Compared with independent potassium permanganate oxidation, sulphite and potassium permanganate conbined usage can make the oxidation removal speed of Ciprofloxacin improve 21.2 ten thousand times.
Embodiment 11: present embodiment and embodiment nine unlike: the pH of handled water is 5, mol ratio=10 of hydrosulphite/potassium permanganate.Compared with independent potassium permanganate oxidation, hydrosulphite and potassium permanganate conbined usage can make the oxidation removal speed of Ciprofloxacin improve 1,502 ten thousand times.
Embodiment 12: present embodiment and embodiment one unlike: the initial pH=6 of reaction, the oxygenant added is Manganse Dioxide.Sulphite and the process of Manganse Dioxide conbined usage contain the simulation surface water of phenol, as long as within 10 seconds, can realize the removal completely of phenol.When being used alone Manganse Dioxide, the phenol of 10% within 45 minutes, only can be removed.Concrete effect comparison data are shown in Fig. 7.
Embodiment 13: present embodiment and embodiment one unlike: the pollutent in handled water is Ciprofloxacin and phenol.Sulphite and potassium permanganate combination treatment contain the simulation surface water of Ciprofloxacin and phenol, as long as 60 milliseconds of removals completely that can realize Ciprofloxacin and phenol.Concrete effect comparison data are shown in Fig. 8.
Claims (7)
1. a method for supper-fast removal organic pollutants, is characterized in that described method steps is as follows:
One, in pending water, add reductive agent, described reductive agent is sulphite or hydrosulphite;
Two, by pending water pH regulator in the scope of 3-7;
Three, in pending water, add oxygenant, described oxygenant is permanganate or Manganse Dioxide, and the mol ratio controlling reductive agent and oxygenant is 3-10.
2. the method for supper-fast removal organic pollutants according to claim 1, it is characterized in that described reductive agent is the sulphite or hydrosulphite storing solution that have dissolved in advance, solvent for use is distilled water.
3. the method for supper-fast removal organic pollutants according to claim 1 and 2, is characterized in that described sulphite is S-WAT, potassium sulfite or other sulphite.
4. the method for supper-fast removal organic pollutants according to claim 1 and 2, is characterized in that described hydrosulphite is sodium bisulfite, Potassium hydrogen sulfite or other hydrosulphite.
5. the method for supper-fast removal organic pollutants according to claim 1, it is characterized in that oxygenant is the potassium permanganate storing solution or Manganse Dioxide colloid storing solution that have dissolved in advance, solvent for use is distilled water.
6. the method for supper-fast removal organic pollutants according to claim 1, is characterized in that described water treatment method carries out in complete or magnetic stirring apparatus.
7. the method for supper-fast removal organic pollutants according to claim 1, is characterized in that described pending water is surface water, underground water, sanitary sewage or trade effluent.
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