CN103551044A - Method for cleaning polluted membrane by using singlet oxygen produced from peroxymonosulfate under induction of inorganic solid peroxide - Google Patents
Method for cleaning polluted membrane by using singlet oxygen produced from peroxymonosulfate under induction of inorganic solid peroxide Download PDFInfo
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- CN103551044A CN103551044A CN201310589567.2A CN201310589567A CN103551044A CN 103551044 A CN103551044 A CN 103551044A CN 201310589567 A CN201310589567 A CN 201310589567A CN 103551044 A CN103551044 A CN 103551044A
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Abstract
The invention provides a method for cleaning polluted membrane by using singlet oxygen produced from peroxymonosulfate under induction of inorganic solid peroxide and relates to a membrane cleaning method. The method for cleaning a polluted membrane comprises the following steps: adding the inorganic solid peroxide and the peroxymonosulfate in a tank containing a polluted membrane module, stirring, soaking, and finally rinsing. According to the method, after the peroxide is dissolved in water, hydrogen peroxide slowly released reacts with the peroxymonosulfate rapidly to generate the high-activity singlet oxygen which directly acts on biological cells polluting the membrane to rapidly destroy enzymatic structures, thus achieving a good membrane cleaning effect. As environmentally-friendly reagents, the inorganic solid peroxide and the peroxymonosulfate do not generate poisonous and harmful byproducts in the cleaning process, and waste liquid can be directly discharged after the membrane is cleaned; and as solid reagents, the inorganic solid peroxide and the peroxymonosulfate can be directly added for use without need of additional equipment. The method has the advantages that the operation is simple and practicable, and the reagents are convenient to transport and store, low in cost and easy to obtain.
Description
Technical field
The present invention relates to a kind of film cleaning method, be specifically related to a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes and produce the method that singlet oxygen cleans film pollution.
Background technology
Along with the requirement to the high isolation and purification of material, membrane filtration technique arises at the historic moment, and becomes a newborn high score from, concentrated, purification and purification techniques.Because it is without phase change, the advantage such as energy consumption is low, system is clean, has been widely used in the ， countries in the world, field such as medicine, food, chemical industry and water treatment and has obtained fast development.But, along with the film growth of running time, inorganic matter in processed material liquid, suspension, organic matter and microorganism etc. are by physics, chemistry and mechanism with membrane material existence, adsorb or be deposited in film surface or fenestra, membrane aperture is diminished or stop up, formation film pollutes, and causes membrane flux to decline, and causes the separating effect variation of film.
It is by adopting rational cleaning method that contaminated film is cleaned and regenerated that film cleans object, destroys the Adsorption of solute layer on film surface, removes the impurity in fenestra road, makes film return to as far as possible original flux.Film cleaning method can be divided into physical cleaning method and chemical cleaning method.Physical cleaning comprises waterpower cleaning, gas pulses cleaning, Ultrasonic Cleaning etc., can remove preferably the pollutant on film surface, but can not remove the pollutant in fenestra road, and cleaning performance is not good.Chemical cleaning is by using chemical agent to reach loosening, dissolve dirt, oxidation of organic compounds, deactivation microorganism are removed the effect that film pollutes.Conventional cleaning method has pickling, alkali cleaning, alcohol wash, oxidant and bactericide (as ozone, hypochlorous acid, potassium permanganate etc.) to clean film pollution etc. by oxidation reaction.
Singlet oxygen (
1o
2) be a kind of molecular oxygen in excitation state, with superoxide radical (O
2 -), hydroxyl radical free radical (OH), sulfate radical free radical (SO
4 -) isoreactivity oxygen species seemingly, chemical property is active, unstable, be widespread in nature, one of the longest active oxygens that relate in field such as chemistry, environment, medical science, have that oxidability is strong, reactivity is high, the time-to-live is short, do not produce the features such as poisonous and harmful accessory substance after oxidation, belong to green, environmentally friendly oxidant.
At present, the method for generation singlet oxygen mainly contains photoactivate method and chemical method.Photoactivate method produces singlet oxygen and relates to an optical excitation process, a kind of sensitising agent (rose-red, eosin, methylene blue, fluorescein, chlorophyll and haematoporphyrin etc.), and under irradiation condition, the sensitising agent of excitation state and the ground state oxygen in system (
3o
2) effect, and then obtain singlet oxygen (
1o
2).Utilize photoactivate method can produce fast singlet oxygen, but the restriction (need stable light source) and the introducing of sensitising agent that exist light can produce the problem of secondary pollution.Chemical method produces singlet oxygen and realizes by there is chemical reaction, and the most classical method is by hydrogen peroxide (H
2o
2) and chlorine (Cl
2) the aqueous solution or hypochlorous acid solution mix and can produce singlet oxygen.This formation speed that utilizes chemical method to produce singlet oxygen is fast, and its second order reaction speed constant is about 10
4m
-1s
-1, instantaneous generation is large, and selfdecomposition speed is fast, and the time-to-live is short, and organic matter utilization rate is low; Chemical reagent is liquid hydrogen peroxide and hypochlorous acid solution or chlorine, and transportation stores inconvenient, complex operation and have the problem of potential safety hazard.
Summary of the invention
The object of this invention is to provide a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes and produce the method that singlet oxygen cleans film pollution, to solve the above-mentioned problem existing.
Of the present inventionly a kind ofly utilize inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen to clean the method that film pollutes and realize by following steps: a, contaminated membrane module to be cleaned is put into the pond that running water is housed; B, by inoganic solids peroxide and peroxy-monosulfate, according to mass ratio, be 1:(0.5～5) ratio join in the pond of step 1, stir, controlling permonosulphuric acid salinity is 50～1000mg/L, soaks 10～180min; C, the membrane module after soaking is put into another pond that running water is housed carry out rinsing, completed and utilized inoganic solids peroxide-induced persulfate to produce singlet oxygen to clean film and pollute.
A kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes of the present invention produces the method that singlet oxygen cleans film pollution, can according to mass ratio, be 1:(0.5～5 by inoganic solids peroxide, peroxy-monosulfate) make powder reagent and mix and to add or to add separately respectively, be dry type and add method; Also inoganic solids peroxide, peroxy-monosulfate can be made respectively to solution, add separately, be wet type and add method.
A kind of inoganic solids peroxide-induced peroxy-monosulfate generation singlet oxygen that utilizes of the present invention cleans in the method for film pollution, inoganic solids peroxide (Na
2o
2, CaO
2, MgO
2, BaO
2, Na
2cO
4, K
2cO
4) can slowly release hydrogen peroxide (H after water-soluble
2o
2), see reaction equation (1) and (2), this hydrogen peroxide producing at water situ by inoganic solids peroxide, can be rapidly and peroxy-monosulfate (HSO
5 -) reaction generation high activity singlet oxygen (
1o
2), see reaction equation (3), it is strong that the singlet oxygen of generation has oxidability, can directly act on the biological cell that film pollutes, and destructive enzyme structure, does not produce poisonous and harmful accessory substance rapidly, and film cleaning performance is good.
O
2 2-+2H
2O→H
2O
2+2OH
- (1)
CO
4 2-+H
2O→H
2O
2+CO
3 2- (2)
H
2O
2+HSO
5 -→
1O
2+SO
4 2-+H
2O+H
+ (3)
A kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes of the present invention produces the method that singlet oxygen cleans film pollution, tool has the following advantages: green emerging oxidant peroxy-monosulfate is compared stable chemical nature with liquid hydrogen peroxide with hypochlorous acid solution or chlorine as pulverulent solids with inoganic solids peroxide, transportation stores convenient, moderate, business is easy to get, operation is simple, do not need additionally to increase operational outfit; The high activity singlet oxygen producing is because its oxidability is strong, the biological cell can snap action polluting in film, and destructive enzyme structure rapidly, film cleaning performance is good; As environmental friendliness reagent, in cleaning process, do not produce poisonous and harmful accessory substance, after cleaning, waste liquid can directly discharge without processing, and has avoided biological pollution in conventional film cleaning method not wash clean clearly, easily produce poisonous and harmful accessory substance, produce the problem that waste liquid need to be processed again.
Accompanying drawing explanation
Fig. 1 is the variation that in the specific embodiment 21, film cleans front and back membrane flux, and is the membrane flux before film pollutes, and ■ is the membrane flux after film pollutes,
for cleaning the membrane flux after film pollutes.
The specific embodiment
Technical solution of the present invention is not limited to the following cited specific embodiment, also comprises any combination between each specific embodiment.
The specific embodiment one: present embodiment is a kind ofly to utilize inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen to clean the method that film pollutes, and it is realized by following steps: a, contaminated membrane module to be cleaned is put into the pond that running water is housed; B, by inoganic solids peroxide and peroxy-monosulfate, according to mass ratio, be 1:(0.5～5) ratio join in the pond of step 1, stir, controlling permonosulphuric acid salinity is 50～1000mg/L, soaks 10～180min; C, the membrane module after step b is soaked are put into another pond that running water is housed and are carried out rinsing, have completed to utilize inoganic solids peroxide-induced persulfate to produce singlet oxygen to clean film and pollute.
The membrane material of the contaminated membrane module described in present embodiment is Kynoar (PVDF), polyether sulfone (PES), polyethylene (PE) or polyvinyl chloride (PVC).
Inoganic solids peroxide and peroxy-monosulfate in present embodiment are separately deposited before use.
Inoganic solids peroxide described in present embodiment and peroxy-monosulfate can be 1:(0.5～5 according to mass ratio) make powder reagent and mix and to add or to add separately respectively, be dry type and add method; Also inoganic solids peroxide and peroxy-monosulfate can be made respectively to solution, add separately, be wet type and add method.
A kind of inoganic solids peroxide-induced peroxy-monosulfate generation singlet oxygen that utilizes of present embodiment cleans in the method for film pollution, after inoganic solids peroxide is water-soluble, can slowly release hydrogen peroxide (H
2o
2), can be rapidly and peroxy-monosulfate (HSO
5 -) reaction generation high activity singlet oxygen (
1o
2), it is strong that the singlet oxygen of generation has oxidability, can directly act on the biological cell that film pollutes, and destructive enzyme structure, does not produce poisonous and harmful accessory substance rapidly, and film cleaning performance is good.
A kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes of present embodiment produces the method that singlet oxygen cleans film pollution, tool has the following advantages: green emerging oxidant peroxy-monosulfate is compared stable chemical nature with liquid hydrogen peroxide with hypochlorous acid solution or chlorine as pulverulent solids with inoganic solids peroxide, transportation stores convenient, moderate, business is easy to get, operation is simple, do not need additionally to increase operational outfit; The high activity singlet oxygen producing is because its oxidability is strong, the biological cell can snap action polluting in film, and destructive enzyme structure rapidly, film cleaning performance is good; As environmental friendliness reagent, in cleaning process, do not produce poisonous and harmful accessory substance, after cleaning, waste liquid can directly discharge without processing, and has avoided biological pollution in conventional film cleaning method not wash clean clearly, easily produce poisonous and harmful accessory substance, produce the problem that waste liquid need to be processed again.
The specific embodiment two: present embodiment is different from the specific embodiment one: described inoganic solids peroxide is sodium peroxide (Na
2o
2), calper calcium peroxide (CaO
2), peromag (MgO
2), barium peroxide (BaO
2), SODIUM PERCARBONATE (Na
2cO
4), potassium percarbonate (K
2cO
4) in one or more mixture.Other parameter is identical with the specific embodiment one.
When in present embodiment, inoganic solids peroxide is wherein several mixture, with arbitrarily than mixing.
The specific embodiment three: what present embodiment was different from the specific embodiment one or two is that peroxy-monosulfate is: permonosulphuric acid sodium (NaHSO
5), permonosulphuric acid potassium (KHSO
5), permonosulphuric acid ammonium (NH
4hSO
5), permonosulphuric acid calcium (Ca (HSO
5)
2), permonosulphuric acid magnesium (Mg (HSO
5)
2) in one or more mixtures that are mixed by any ratio.Other parameter is identical with the specific embodiment one or two.
The specific embodiment four: present embodiment is different from one of specific embodiment one to three: permonosulphuric acid salinity is 60～900mg/L.Other step and parameter are identical with one of specific embodiment one to three.
The specific embodiment five: present embodiment is different from one of specific embodiment one to four: permonosulphuric acid salinity is 70～800mg/L.Other step and parameter are identical with one of specific embodiment one to four.
The specific embodiment six: present embodiment is different from one of specific embodiment one to five: permonosulphuric acid salinity is 80～700mg/L.Other step and parameter are identical with one of specific embodiment one to five.
The specific embodiment seven: present embodiment is different from one of specific embodiment one to six: permonosulphuric acid salinity is 90～600mg/L.Other step and parameter are identical with one of specific embodiment one to six.
The specific embodiment eight: present embodiment is different from one of specific embodiment one to seven: permonosulphuric acid salinity is 100～500mg/L.Other step and parameter are identical with one of specific embodiment one to seven.
The specific embodiment nine: present embodiment is different from one of specific embodiment one to eight: permonosulphuric acid salinity is 120～400mg/L.Other step and parameter are identical with one of specific embodiment one to eight.
The specific embodiment ten: present embodiment is different from one of specific embodiment one to nine: permonosulphuric acid salinity is 150～300mg/L.Other step and parameter are identical with one of specific embodiment one to nine.
The specific embodiment 11: present embodiment is different from one of specific embodiment one to ten: permonosulphuric acid salinity is 200mg/L.Other step and parameter are identical with one of specific embodiment one to ten.
The specific embodiment 12: present embodiment is different from one of specific embodiment one to 11: the mass ratio of inoganic solids peroxide and peroxy-monosulfate is 1:(0.6～4).Other parameter is identical with one of specific embodiment one to 11.
The specific embodiment 13: present embodiment is different from one of specific embodiment one to 12: the mass ratio of inoganic solids peroxide and peroxy-monosulfate is 1:(0.7～3).Other parameter is identical with one of specific embodiment one to 12.
The specific embodiment 14: present embodiment is different from one of specific embodiment one to 13: the mass ratio of inoganic solids peroxide and peroxy-monosulfate is 1:(0.8～2).Other parameter is identical with one of specific embodiment one to 13.
The specific embodiment 15: present embodiment is different from one of specific embodiment one to 14: the mass ratio of inoganic solids peroxide and peroxy-monosulfate is 1:(0.9～1.5).Other parameter is identical with one of specific embodiment one to 14.
The specific embodiment 16: present embodiment is different from one of specific embodiment one to 15: the mass ratio of inoganic solids peroxide and peroxy-monosulfate is 1:1.Other parameter is identical with one of specific embodiment one to 15.
The specific embodiment 17: present embodiment is different from one of specific embodiment one to 16: soak time is 20～120min.Other step and parameter are identical with one of specific embodiment one to 16.
The specific embodiment 18: present embodiment is different from one of specific embodiment one to 17: soak time is 30～90min.Other step and parameter are identical with one of specific embodiment one to 17.
The specific embodiment 19: present embodiment is different from one of specific embodiment one to 18: soak time is 60min.Other step and parameter are identical with one of specific embodiment one to 18.
The specific embodiment 20: present embodiment is a kind ofly to utilize inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen to clean the method that film pollutes, and it is realized by following steps: a, contaminated membrane module to be cleaned is put into the pond that running water is housed; B, by inoganic solids peroxide and peroxy-monosulfate, according to mass ratio, be that 1:1 joins in pond, stir, controlling permonosulphuric acid salinity is 500mg/L, and soak time is 60min; C, soaked membrane module is put into another pond that running water is housed carry out rinsing, completed and utilized inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen to clean film and pollute.
The membrane material of the contaminated membrane module described in present embodiment is Kynoar (PVDF), polyether sulfone (PES), polyethylene (PE) or polyvinyl chloride (PVC).
The singlet oxygen of present embodiment through producing cleans after film pollution, and membrane flux recovers more than 90%.
The dosing method of the peroxide of inoganic solids described in present embodiment and peroxy-monosulfate adds for making mixed-powder reagent form according to mass ratio 1:1.Inoganic solids peroxide in present embodiment is the sodium peroxide of any ratio and the mixture of calper calcium peroxide; Peroxy-monosulfate is the permonosulphuric acid potassium of any ratio and the mixture of permonosulphuric acid sodium.
The specific embodiment 21: present embodiment is a kind ofly to utilize inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen to clean the method that film pollutes, and it is realized by following steps: a, contaminated membrane module to be cleaned is put into the pond that running water is housed; B, by inoganic solids calper calcium peroxide and permonosulphuric acid potassium, according to mass ratio, be that 1:2 joins in pond, stir, controlling permonosulphuric acid salinity is 300mg/L, and soak time is 60min; C, soaked membrane module is put into another pond that running water is housed carry out rinsing, completed and utilized inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen to clean film and pollute.
The membrane material of present embodiment membrane module is Kynoar (PVDF), polyether sulfone (PES), polyethylene (PE) and polyvinyl chloride (PVC).
Present embodiment membrane flux recovery rate is shown in Fig. 1, as shown in Figure 1, singlet oxygen through producing cleans after film pollution, and the membrane flux recovery rate of Kynoar (PVDF), polyether sulfone (PES), polyethylene (PE) and polyvinyl chloride (PVC) all reaches more than 90%.
The dosing method of the calper calcium peroxide of inoganic solids described in present embodiment and permonosulphuric acid potassium is for to add with powder reagent form respectively according to mass ratio 1:2.
The specific embodiment 22: present embodiment is a kind ofly to utilize inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen to clean the method that film pollutes, and it is realized by following steps: a, contaminated membrane module to be cleaned is put into the pond that running water is housed; B, by inoganic solids peroxide and peroxy-monosulfate, according to mass ratio, be that 1:1.5 joins in pond, stir, controlling permonosulphuric acid salinity is 800mg/L, and soak time is 60min; C, cleaned membrane module is put into another pond that running water is housed carry out rinsing, completed and utilized inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen to clean film and pollute.
The membrane material of the contaminated membrane module described in present embodiment is Kynoar (PVDF), polyether sulfone (PES), polyethylene (PE) or polyvinyl chloride (PVC).
The singlet oxygen of present embodiment through producing cleans after film pollution, and membrane flux recovers more than 90%.
The dosing method of the peroxide of inoganic solids described in present embodiment and peroxy-monosulfate adds for making mixed-powder reagent form according to mass ratio 1:1.5.Inoganic solids peroxide in present embodiment is the SODIUM PERCARBONATE of any ratio and the mixture of potassium percarbonate; Peroxy-monosulfate is the permonosulphuric acid potassium of any ratio and the mixture of permonosulphuric acid sodium.
Claims (10)
1. utilize inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen and clean the method that film pollutes, it is characterized in that utilizing inoganic solids peroxide-induced persulfate to produce singlet oxygen and clean the method that film pollutes and realize by following steps: a, contaminated membrane module to be cleaned is put into the pond that running water is housed; B, by inoganic solids peroxide and peroxy-monosulfate, according to mass ratio, be 1:(0.5～5) ratio join in the pond of step 1, stir, controlling permonosulphuric acid salinity is 50～1000mg/L, soaks 10～180min; C, the membrane module after soaking is put into another pond that running water is housed carry out rinsing, completed and utilized inoganic solids peroxide-induced persulfate to produce singlet oxygen to clean film and pollute.
2. a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes according to claim 1 produces the method that singlet oxygen cleans film pollution, it is characterized in that described inoganic solids peroxide is one or more mixtures that are mixed by any ratio in sodium peroxide, calper calcium peroxide, peromag, barium peroxide, SODIUM PERCARBONATE, potassium percarbonate.
3. a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes according to claim 1 produces the method that singlet oxygen cleans film pollution, it is characterized in that described peroxy-monosulfate is one or more mixtures that are mixed by any ratio in permonosulphuric acid sodium, permonosulphuric acid potassium, permonosulphuric acid ammonium, permonosulphuric acid calcium, permonosulphuric acid magnesium.
4. according to a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes described in claim 1,2 or 3, produce the method that singlet oxygen cleans film pollution, it is characterized in that described inoganic solids peroxide and the mass ratio of peroxy-monosulfate are 1:(0.6～4).
5. a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes according to claim 4 produces the method that singlet oxygen cleans film pollution, it is characterized in that described inoganic solids peroxide and the mass ratio of peroxy-monosulfate are 1:(0.7～3).
6. a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes according to claim 5 produces the method that singlet oxygen cleans film pollution, it is characterized in that described inoganic solids peroxide and the mass ratio of peroxy-monosulfate are 1:(0.8～2).
7. a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes according to claim 6 produces the method that singlet oxygen cleans film pollution, it is characterized in that described inoganic solids peroxide and the mass ratio of peroxy-monosulfate are 1:(0.9～1.5).
8. a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes according to claim 7 produces the method that singlet oxygen cleans film pollution, it is characterized in that described inoganic solids peroxide and the mass ratio of peroxy-monosulfate are 1:1.
9. according to a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes described in claim 1,2 or 3, produce the method that singlet oxygen cleans film pollution, it is characterized in that described control permonosulphuric acid salinity is 100～800mg/L.
10. a kind of inoganic solids peroxide-induced peroxy-monosulfate that utilizes according to claim 9 produces the method that singlet oxygen cleans film pollution, it is characterized in that described control permonosulphuric acid salinity is 200～500mg/L.
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| CN115463559A (en) * | 2022-09-08 | 2022-12-13 | 哈尔滨工业大学水资源国家工程研究中心有限公司 | Method for enhanced cleaning of polluted delta-manganese dioxide modified membrane based on peroxymonosulfate catalytic oxidation |
| CN115463559B (en) * | 2022-09-08 | 2024-05-31 | 哈尔滨工业大学水资源国家工程研究中心有限公司 | Method for performing enhanced cleaning on polluted delta-manganese dioxide modified membrane based on peroxymonosulfate catalytic oxidation |
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