CN103553204A - Method for treating water by using singlet oxygen produced from peroxymonosulfate under induction of inorganic solid peroxide - Google Patents

Method for treating water by using singlet oxygen produced from peroxymonosulfate under induction of inorganic solid peroxide Download PDF

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CN103553204A
CN103553204A CN201310589568.7A CN201310589568A CN103553204A CN 103553204 A CN103553204 A CN 103553204A CN 201310589568 A CN201310589568 A CN 201310589568A CN 103553204 A CN103553204 A CN 103553204A
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monosulfate
peroxy
singlet oxygen
peroxide
inoganic solids
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CN103553204B (en
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庞素艳
江进
王强
鲁雪婷
郭晓瑜
黄亮
郭仕达
王玲
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Harbin University of Science and Technology
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Abstract

The invention provides a method for treating water by using singlet oxygen produced from peroxymonosulfate under induction of inorganic solid peroxide and relates to a water treatment method. The water treatment method is used for solving the problems of a photosensitive method for generating singlet oxygen that a light source needs to be additionally added, secondary pollution is caused, and the utilization rate of singlet oxygen generated by adopting a chemical method is low. The method for treating water comprises the following steps: adding the inorganic solid peroxide and the peroxymonosulfate to water, reacting and stirring so as to complete the water treatment, wherein the water to be treated is source water and wastewater. According to the water treatment method, after the peroxide is dissolved in water, hydrogen peroxide slowly released reacts with the peroxymonosulfate rapidly to continuously generate the low-concentration high-activity singlet oxygen which can be efficiently utilized by pollutants, the self decomposition of the singlet oxygen is reduced, and the utilization rate of the singlet oxygen is increased. The method has the advantages that the pollution removal efficiency is high, no poisonous or harmful byproducts are generated, the additional equipment is not needed; and as solid reagents, the inorganic solid peroxide and the peroxymonosulfate are convenient to transport and store and are suitable for emergency treatment.

Description

A kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen
Technical field
The present invention relates to water treatment method, be specifically related to a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen.
Background technology
Singlet oxygen ( 1o 2) be a kind of molecular oxygen in excited 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 oxidation capacity is strong, reactive behavior is high, the survival time is short, do not produce the features such as poisonous and harmful by product after oxidation, belong to green, environmentally friendly oxygenant.
At present, the method for generation singlet oxygen mainly contains photosensitization method and chemical process.Photosensitization method produces singlet oxygen and relates to an optical excitation process, a kind of photosensitizers (rose-red, eosin, methylene blue, fluorescent yellow, chlorophyll and haematoporphyrin etc.), and under rayed condition, the photosensitizers of excited state and the ground state oxygen in system ( 3o 2) effect, and then obtain singlet oxygen ( 1o 2).Utilize photosensitization method can produce fast singlet oxygen, but the restriction (need stable light source) and the introducing of photosensitizers that exist light can produce the problem of secondary pollution.Chemical process 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 process to produce singlet oxygen is fast, and its second order rate constant is about 10 4m -1s -1, instantaneous generation is large, and self-decomposition speed is fast, and the survival time is short, and organism utilization ratio 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 water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen, address the problem: in (1) photosensitization method, producing singlet oxygen needs additional light source, be difficult to large-scale application, and the introducing of photosensitizers can produce secondary pollution; (2) chemical reaction method (H 2o 2-ClO -) in large, the easily self-decomposition of the singlet oxygen amount of instantaneous generation, be difficult to contaminated object height effect and utilize, and liquid hydrogen peroxide and hypochlorous acid solution or chlorine, transportation, store inconvenient, complicated operation and have potential safety hazard.
A kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen of the present invention is realized by following steps: by inoganic solids superoxide and peroxy-monosulfate, according to mass ratio, be 1:(0.5~5) ratio join in pending water, stir, controlling the concentration of peroxy-monosulfate in pending water is 0.3~300mg/L, hydraulic retention reaction 5~60min, completes the water treatment that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen; Wherein, described pending water is source water and sewage.
A kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen of the present invention, can according to mass ratio, be 1:(0.5~5 by inoganic solids superoxide, peroxy-monosulfate) make powder reagent and mix and to add or to add separately respectively, be dry type and add method; Also inoganic solids superoxide, peroxy-monosulfate can be made respectively to solution, add separately, be wet type and add method.
A kind of utilization in the water treatment method that inoganic solids peroxide-induced peroxy-monosulfate produces singlet oxygen of the present invention, inoganic solids superoxide (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 formula (1) and (2), this hydrogen peroxide producing at water situ by inoganic solids superoxide, can be rapidly and peroxy-monosulfate (HSO 5 -) reaction generation high reactivity singlet oxygen ( 1o 2), see reaction formula (3), the strong oxidizing property singlet oxygen that lower concentration continues to produce can contaminated object height effect utilize, and reduces its self-decomposition, improves its utilization ratio, and depollution is effective, and does not produce poisonous and harmful by product.
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 water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen of the present invention, tool has the following advantages: green emerging oxygenant peroxy-monosulfate is compared stable chemical nature with liquid hydrogen peroxide with hypochlorous acid solution or chlorine as pulverulent solids with inoganic solids superoxide, transportation stores convenient, moderate, business is easy to get, operation is simple, and not needing additionally increases operational outfit (as O 3, UV need to provide reaction unit and equipment), be subject to water condition to affect little (affected by pH larger as Fenton reagent), the environmentally friendly singlet oxygen with strong oxidizing property producing, depollution efficiency is high, in reaction process, do not produce poisonous and harmful by product, can in water factory, carry out large-scale application, as solid powder medicament, add the emergency processing when being more suitable for water and polluting outburst.
Accompanying drawing explanation
Fig. 1 is the clearance graphic representation of endocrine disrupter-dihydroxyphenyl propane in source water in embodiment 21.
Embodiment
Technical solution of the present invention is not limited to following cited embodiment, also comprises the arbitrary combination between each embodiment.
Embodiment one: present embodiment is a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen, it is realized by following steps: by inoganic solids superoxide and peroxy-monosulfate, according to mass ratio, be 1:(0.5~5) ratio join in pending water, stir, controlling the concentration of peroxy-monosulfate in pending water is 0.3~300mg/L, hydraulic retention reaction 5~60min, completes the water treatment that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen; Wherein, described pending water is source water and sewage.
Inoganic solids superoxide and peroxy-monosulfate in present embodiment are separately deposited before use.
The superoxide of inoganic solids 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 superoxide and peroxy-monosulfate can be made respectively to solution, add separately, be wet type and add method.
Present embodiment a kind of utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce in the water treatment method of singlet oxygen, after inoganic solids superoxide is water-soluble, can slowly release hydrogen peroxide (H 2o 2), this hydrogen peroxide producing at water situ by inoganic solids superoxide, can be rapidly and peroxy-monosulfate (HSO 5 -) reaction generation high reactivity singlet oxygen ( 1o 2), the strong oxidizing property singlet oxygen that lower concentration continues to produce can contaminated object height effect utilize, and reduces its self-decomposition, and depollution is effective, and does not produce poisonous and harmful by product.
A kind of advantage of utilizing inoganic solids peroxide-induced peroxy-monosulfate to produce the water treatment method of singlet oxygen of present embodiment is: green emerging oxygenant peroxy-monosulfate is compared stable chemical nature with liquid hydrogen peroxide with hypochlorous acid solution or chlorine as pulverulent solids with inoganic solids superoxide, transportation stores convenient, moderate, business is easy to get, operation is simple, do not need additionally to increase operational outfit, affected by water condition little, the strong oxidizing property singlet oxygen producing, depollution efficiency is high, in reaction process, do not produce poisonous and harmful by product, can in water factory, carry out large-scale application, be more suitable for emergency processing.
Embodiment two: present embodiment is different from embodiment one: described inoganic solids superoxide is sodium peroxide (Na 2o 2), calcium peroxide (CaO 2), Magnesium peroxide (MgO 2), barium peroxide (BaO 2), SPC-D (Na 2cO 4), antihypo (K 2cO 4) in one or more mixtures that are mixed by any ratio.Other parameter is identical with embodiment one.
Embodiment three: present embodiment is different from embodiment one or two: 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 embodiment one or two.
Embodiment four: present embodiment is different from one of embodiment one to three: permonosulphuric acid salt concn is 0.5~250mg/L.Other step and parameter are identical with one of embodiment one to three.
Embodiment five: present embodiment is different from one of embodiment one to four: permonosulphuric acid salt concn is 1~200mg/L.Other step and parameter are identical with one of embodiment one to four.
Embodiment six: present embodiment is different from one of embodiment one to five: permonosulphuric acid salt concn is 1.5~150mg/L.Other step and parameter are identical with one of embodiment one to five.
Embodiment seven: present embodiment is different from one of embodiment one to six: permonosulphuric acid salt concn is 2~100mg/L.Other step and parameter are identical with one of embodiment one to six.
Embodiment eight: present embodiment is different from one of embodiment one to seven: permonosulphuric acid salt concn is 5~75mg/L.Other step and parameter are identical with one of embodiment one to seven.
Embodiment nine: present embodiment is different from one of embodiment one to eight: permonosulphuric acid salt concn is 10~50mg/L.Other step and parameter are identical with one of embodiment one to eight.
Embodiment ten: present embodiment is different from one of embodiment one to nine: permonosulphuric acid salt concn is 15~30mg/L.Other step and parameter are identical with one of embodiment one to nine.
Embodiment 11: present embodiment is different from one of embodiment one to ten: permonosulphuric acid salt concn is 20mg/L.Other step and parameter are identical with one of embodiment one to ten.
Embodiment 12: present embodiment is different from one of embodiment one to 11: the mass ratio of inoganic solids superoxide and peroxy-monosulfate is 1:(0.6~4).Other parameter is identical with one of embodiment one by one to ten one.
Embodiment 13: present embodiment is different from one of embodiment one to 12: the mass ratio of inoganic solids superoxide and peroxy-monosulfate is 1:(0.7~3).Other parameter is identical with one of embodiment one to 12.
Embodiment 14: present embodiment is different from one of embodiment one to 13: the mass ratio of inoganic solids superoxide and peroxy-monosulfate is 1:(0.8~2).Other parameter is identical with one of embodiment one to 13.
Embodiment 15: present embodiment is different from one of embodiment one to 14: the mass ratio of inoganic solids superoxide and peroxy-monosulfate is 1:(0.9~1.5).Other parameter is identical with one of embodiment one to 14.
Embodiment 16: present embodiment is different from one of embodiment one to 15: the mass ratio of inoganic solids superoxide and peroxy-monosulfate is 1:1.Other parameter is identical with one of embodiment one to 15.
Embodiment 17: present embodiment is different from one of embodiment one to 16: controlling the reaction times is 10~50min.Other step and parameter are identical with one of embodiment one to 16.
Embodiment 18: present embodiment is different from one of embodiment one to 17: controlling the reaction times is 20~40min.Other step and parameter are identical with one of embodiment one to 17.
Embodiment 19: present embodiment is different from one of embodiment one to 18: controlling the reaction times is 30min.Other step and parameter are identical with one of embodiment one to 18.
Embodiment 20: present embodiment is a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen, it is realized by following steps: by inoganic solids superoxide and peroxy-monosulfate, according to mass ratio, be that 1:1 joins in treatment sewage, stir, controlling the concentration of peroxy-monosulfate in treatment sewage is 100mg/L, the hydraulic retention reaction times is 30min, completes the water treatment that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen.
The dosing method of the superoxide 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 superoxide in present embodiment is the SPC-D of any ratio and the mixture of antihypo; Peroxy-monosulfate is the permonosulphuric acid potassium of any ratio and the mixture of permonosulphuric acid sodium.
Present embodiment is a kind of utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce in the water treatment method of singlet oxygen, after oxide treatment, (chlorophenol, bromine phenol, iodine phenol, nitrophenol, aniline, atrazine, 2, clearance 4-D) reaches more than 90% pollutent in sewage.
Embodiment 21: present embodiment is a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen, it is realized by following steps: by inoganic solids calcium peroxide and permonosulphuric acid potassium, according to mass ratio, be that 1:2 joins in pending source water, stir, controlling the concentration of peroxy-monosulfate in treatment sewage is 20mg/L, the hydraulic retention reaction times is 30min, completes the water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen.
The dosing method of the 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.
Present embodiment is a kind of utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce in the water treatment method of singlet oxygen, endocrine disrupter-the dihydroxyphenyl propane that contains 0.1mg/L in source water, after oxide treatment, the clearance of dihydroxyphenyl propane reaches more than 99%, as shown in Figure 1.
Embodiment 22: present embodiment is a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen, it is realized by following steps: by inoganic solids calcium peroxide and permonosulphuric acid sodium, according to mass ratio, be that 1:2.5 joins in pending source water, stir, the hydraulic retention reaction times is 150mg/L, the hydraulic retention reaction times is 20min, completes the water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen.
The dosing method of the powder of solid bleach described in present embodiment and inoganic solids superoxide adds for being mixed with respectively solution form according to mass ratio 1:2.5.
Present embodiment is a kind of utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce in the water treatment method of singlet oxygen, after oxide treatment, the clearance of the pollutent in sewage (tsiklomitsin, penicillin, cephalo, Carbamzepine, triclosan, oestrone, nonyl phenol) reaches more than 90%.

Claims (10)

1. a water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen, the water treatment method that it is characterized in that utilizing inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen is realized by following steps: by inoganic solids superoxide and peroxy-monosulfate, according to mass ratio, be 1:(0.5~5) ratio join in pending water, stir, controlling the concentration of peroxy-monosulfate in pending water is 0.3~300mg/L, hydraulic retention reaction 5~60min, complete the water treatment that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen, wherein, described pending water is source water and sewage.
2. a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen according to claim 1, is characterized in that described inoganic solids superoxide is one or more mixtures that are mixed by any ratio in sodium peroxide, calcium peroxide, Magnesium peroxide, barium peroxide, SPC-D, antihypo.
3. a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen according to claim 1, 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 water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen described in claim 1,2 or 3, it is characterized in that described inoganic solids superoxide and the mass ratio of peroxy-monosulfate are 1:(0.6~4).
5. a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen according to claim 4, is characterized in that described inoganic solids superoxide and the mass ratio of peroxy-monosulfate are 1:(0.7~3).
6. a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen according to claim 5, is characterized in that described inoganic solids superoxide and the mass ratio of peroxy-monosulfate are 1:(0.8~2).
7. a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen according to claim 6, is characterized in that described inoganic solids superoxide and the mass ratio of peroxy-monosulfate are 1:(0.9~1.5).
8. a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen according to claim 7, is characterized in that described inoganic solids superoxide and the mass ratio of peroxy-monosulfate are 1:1.
9. according to a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen described in claim 1,2 or 3, it is characterized in that described peroxy-monosulfate concentration in pending water is 5~200mg/L.
10. a kind of water treatment method that utilizes inoganic solids peroxide-induced peroxy-monosulfate to produce singlet oxygen according to claim 9, is characterized in that described peroxy-monosulfate concentration in pending water is 20~100mg/L.
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CN105347458A (en) * 2015-11-16 2016-02-24 哈尔滨理工大学 Method for singlet state oxygen treatment on reverse osmosis concentrate
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