CN104591369A - Composite chemical agent for promoting hydrogen peroxide to produce hydroxyl free radicals and application thereof - Google Patents
Composite chemical agent for promoting hydrogen peroxide to produce hydroxyl free radicals and application thereof Download PDFInfo
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- CN104591369A CN104591369A CN201410805779.4A CN201410805779A CN104591369A CN 104591369 A CN104591369 A CN 104591369A CN 201410805779 A CN201410805779 A CN 201410805779A CN 104591369 A CN104591369 A CN 104591369A
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- Prior art keywords
- hydroxylamine
- azanol
- hydrogen peroxide
- compound
- chemical agent
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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
- 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
-
- 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
- C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
Abstract
The invention discloses a composite chemical agent for promoting hydrogen peroxide to produce hydroxyl free radicals and application thereof. The application comprises the following steps of adding hydrogen peroxide and the composite chemical agent into water containing organic pollutants, uniformly mixing and reacting, wherein the molar concentration ratio of total addition amount of the composite chemical agent to hydrogen peroxide is between 1:10 and 10:1. The invention relates to the composite chemical agent for promoting hydrogen peroxide to produce hydroxyl free radicals and application thereof, the composite chemical agent can effectively promote hydrogen peroxide to produce hydroxyl free radicals and the hydroxyl free radicals can be used for removing the organic pollutants in various waste water, groundwater, surface water and drinking water, the composite chemical agent has the characteristics of simplicity and convenience in operation, safety and economical efficiency, the reaction applicable pH is wider, the water body does not need to be adjusted to be strongly acidic, no metal oxide precipitates are formed, and the composite chemical agent has good practicability.
Description
Technical field
The invention belongs to the high-level oxidation technology field of water treatment, being specifically related to a kind of compound and application thereof for impelling hydrogen peroxide to produce hydroxyl radical free radical.
Background technology
High-level oxidation technology is study hotspot both domestic and external, is also one of the further treatment technique of water and the important directions of based technique for in-situ remediation.Be utilize different systems to produce hydroxyl radical free radical to carry out degradable organic pollutant in simple terms, improve its bio-degradable, reduce its bio-toxicity, or even organic pollutant is thoroughly mineralized into carbonic acid gas and water.In advanced oxidation system, activated hydrogen peroxide produces one of the most direct way of hydroxyl radical free radical, and the hydrogen peroxide of a part can be excited and generate the reactive hydroxyl radical of a part.The redox potential of hydroxyl radical free radical, can fast and without most of organic pollutant of obviously optionally degrading up to 2.73 V.
Summary of the invention
Goal of the invention: for the deficiencies in the prior art, the object of this invention is to provide a kind of compound for impelling hydrogen peroxide to produce hydroxyl radical free radical, is used for impelling hydrogen peroxide to produce hydroxyl radical free radical.Another object of the present invention is to provide and a kind ofly uses the described compound for impelling hydrogen peroxide to produce hydroxyl radical free radical to remove the method for dirty organic pollutants, has simple, convenient, safe, economic feature.
Technical scheme: in order to realize foregoing invention object, the technical solution used in the present invention is as follows:
For the compound impelling hydrogen peroxide to produce hydroxyl radical free radical, described compound is selected from quinhydrones, chloro quinone, S-WAT, lithium sulfite, potassium sulfite, magnesium sulfite, calcium sulfite, ammonium sulphite, sulfurous acid, Sodium Pyrosulfite, pyrosulphite lithium, potassium pyrosulfite, pyrosulphite magnesium, pyrosulphite calcium, ammonium pyrosulfite, V-Brite B, SODIUM HYDROSULPHITE lithium, potassium hyposulfite, magnesium hyposulfite, calcium hyposulfite, ammonium hyposulfite, azanol, N-methyl hydroxylamine, O-methyl hydroxylamine, N, N-dimethyl hydroxylamine, N-ethylhydroxyl amine, O-ethylhydroxyl amine, N, N-diethyl hydroxylamine, N, O-dimethyl hydroxylamine, N, N, O-trimethylammonium azanol, N-t-butylhydroxylamine, O-t-butylhydroxylamine, sulfonation azanol, N-isopropylhydroxyla, metaraminol, isobutyl oxygen amine salt, aromatic hydroxylamine, N-ethyl-O-methyl hydroxylamine, N-methyl-O-ethylhydroxyl amine, N, N, O-tripropyl azanol, O-Cvclopropvlmethvl azanol, humic acid, ammonium chloride, quadrol-N, N-disuccinic acid trisodium salt, disodium ethylene diamine tetraacetate, nitrilotriacetic acid(NTA), trisodium phosphate, citric acid, Trisodium Citrate, one or more in oxalic acid and sodium oxalate.
Described azanol is selected from oxammonium hydrochloride, hydroxylamine perchlorate, oxammonium sulfate, phosphatic hydroxylamine or aqueous hydroxylamine.
Described compound is selected from azanol, N-methyl hydroxylamine, N, N-dimethyl hydroxylamine, N-ethylhydroxyl amine, N, N-diethyl hydroxylamine, N, O-dimethyl hydroxylamine, N, N, O-trimethylammonium azanol, N-t-butylhydroxylamine, one or more in sulfonation azanol and aromatic hydroxylamine; Wherein, azanol is selected from oxammonium hydrochloride, hydroxylamine perchlorate, oxammonium sulfate, phosphatic hydroxylamine or aqueous hydroxylamine.
Use the described method removing dirty organic pollutants for the compound impelling hydrogen peroxide to produce hydroxyl radical free radical: add hydrogen peroxide and a compound to containing in the water of organic pollutant, mix, react; Wherein, total throwing amount of compound and total dosage molar ratio of hydrogen peroxide are at 1:10 ~ 10:1.
Described compound is selected from azanol, N-methyl hydroxylamine, N, N-dimethyl hydroxylamine, N-ethylhydroxyl amine, N, N-diethyl hydroxylamine, N, O-dimethyl hydroxylamine, N, N, O-trimethylammonium azanol, N-t-butylhydroxylamine, one or more in sulfonation azanol and aromatic hydroxylamine; Wherein, azanol is selected from oxammonium hydrochloride, hydroxylamine perchlorate, oxammonium sulfate, phosphatic hydroxylamine or aqueous hydroxylamine.
Beneficial effect: compared with prior art, compound and application thereof for impelling hydrogen peroxide to produce hydroxyl radical free radical of the present invention, can be used for impelling hydrogen peroxide to produce hydroxyl radical free radical, the speed producing hydroxyl radical free radical is fast, efficiency is high, all kinds of waste water, underground water, surface water can be removed with the organic pollutant in tap water, there is simple, convenient, safe, economic feature, the pH that reaction is suitable for is wider, without the need to regulating water body to strongly-acid, do not form metal oxide deposits, there is good practicality.
Accompanying drawing explanation
Fig. 1 is the mensuration figure of hydroxyl radical free radical signal in compound/hydrogen peroxide system;
Fig. 2 is that the composition of embodiment 3 compound and throwing amount are to hydroxyl radical free radical effect of signals figure;
Fig. 3 is that the composition of embodiment 4 compound and throwing amount are to hydroxyl radical free radical effect of signals figure;
Fig. 4 is that the composition of embodiment 5 compound and throwing amount are to hydroxyl radical free radical effect of signals figure;
Fig. 5 is that the composition of embodiment 6 compound and throwing amount are to hydroxyl radical free radical effect of signals figure;
Fig. 6 is that different composite medicament composition and throwing amount activated hydrogen peroxide are degraded and benzoicly affected result figure;
To be different pH on compound activated hydrogen peroxide degrade Fig. 7 benzoicly affects result figure.
Embodiment
Below in conjunction with specific embodiment, the present invention is described further.
Embodiment 1
For the compound impelling hydrogen peroxide to produce hydroxyl radical free radical, be selected from quinhydrones, chloro quinone, S-WAT, lithium sulfite, potassium sulfite, magnesium sulfite, calcium sulfite, ammonium sulphite, sulfurous acid, Sodium Pyrosulfite, pyrosulphite lithium, potassium pyrosulfite, pyrosulphite magnesium, pyrosulphite calcium, ammonium pyrosulfite, V-Brite B, SODIUM HYDROSULPHITE lithium, potassium hyposulfite, magnesium hyposulfite, calcium hyposulfite, ammonium hyposulfite, azanol (oxammonium hydrochloride, hydroxylamine perchlorate, oxammonium sulfate, phosphatic hydroxylamine, hydroxylamine solution etc.), N-methyl hydroxylamine, O-methyl hydroxylamine, N, N-dimethyl hydroxylamine, N-ethylhydroxyl amine, O-ethylhydroxyl amine, N, N-diethyl hydroxylamine, N, O-dimethyl hydroxylamine, N, N, O-trimethylammonium azanol N-t-butylhydroxylamine, O-t-butylhydroxylamine, sulfonation azanol, N-isopropylhydroxyla, metaraminol, isobutyl oxygen amine salt, aromatic hydroxylamine, N-ethyl-O-methyl hydroxylamine, N-methyl-O-ethylhydroxyl amine, N, N, O-tripropyl azanol, O-Cvclopropvlmethvl azanol, humic acid, ammonium chloride, quadrol-N, N-disuccinic acid trisodium salt, disodium ethylene diamine tetraacetate, nitrilotriacetic acid(NTA), trisodium phosphate, citric acid, Trisodium Citrate, acetic acid, sodium acetate, oxalic acid and sodium oxalate.When in present embodiment, the promotor of hydrogen peroxide is mixture, can by any combination between each component.
Embodiment 2
Impel hydrogen peroxide generation hydroxyl radical free radical to remove a method for dirty organic pollutants, hydrogen peroxide and compound are added to the water, uniform stirring reacts, and impels hydrogen peroxide to produce hydroxyl radical free radical; Hydrogen peroxide throwing amount is 10 mM, compound (azanol, N-methyl hydroxylamine, N-ethylhydroxyl amine, O-methyl hydroxylamine, O-ethylhydroxyl amine, acetic acid and sodium acetate, can mix according to arbitrary proportion (or mol ratio 1:2:2:1:1:5)) total throwing amount is 0.7 g/L, DMPO throwing amount is 20 mM, water temperature is 20 DEG C, pH=3.0 ± 0.2, the reaction times is 30 s.。Adopt DMPO as the trapping agent of free radical, detect with the equipment of electron paramagnetic resonance, when producing the fignal center of 1:2:2:1, hydroxyl radical free radical is had to generate in explanation system, result as shown in Figure 1, Fig. 1 generates the fignal center of 1:2:2:1, illustrates that this compound can produce hydroxyl radical free radical with hydroperoxidation.
In the present embodiment staying water before treatment its pH value need not be adjusted to less than 4, pH value can be extended to 6, the acid of adjust ph and alkali before and after process can be saved, even do not need additionally to add bronsted lowry acids and bases bronsted lowry.
Do not need in the present embodiment in staying water, to add the metals such as iron and compound thereof again, do not need additionally to carry out uv irradiation, microwave exposure, ultrasonic cavitation, additional electromagnetic field and heating yet.Have that operation is simple, need not increase other treatment facilities, applied widely, not easily produce molysite mud, disposable input cost is low, and working cost is low, activator safety, and effectively can generate the advantages such as hydroxyl radical free radical.
Embodiment 3
Method is with embodiment 2, unlike: compound (sulphite, N, N, O-trimethylammonium azanol,, N, N, O-tripropyl azanol, O-Cvclopropvlmethvl azanol, metaraminol, quinhydrones and sulfonation azanol, can mix according to arbitrary proportion (or making mol ratio 1:3:3:1:1:2:3 into)) total throwing measures 0.5 g.Result as shown in Figure 2, generates the fignal center of 1:2:2:1, illustrates that this compound can produce hydroxyl radical free radical with hydroperoxidation.
Embodiment 4
Method, with embodiment 2, is 0.6g unlike the total throwing amount of: compound (pyrosulfite, N, N-dimethyl hydroxylamine, N-methyl-O-ethylhydroxyl amine, aromatic hydroxylamine and humic acid, can mix according to arbitrary proportion (or mol ratio 1:3:2:2:1)).Result as shown in Figure 3, generates the fignal center of 1:2:2:1, illustrates that this compound can produce hydroxyl radical free radical with hydroperoxidation.
Embodiment 5
Method, with embodiment 2, is 0.8 g unlike the total throwing amount of: compound (hyposulfite, N-ethyl-O-methyl hydroxylamine, N, N-diethyl hydroxylamine, oxalic acid and sodium oxalate, can mix according to arbitrary proportion (or mol ratio 1:2:3:1:1)).Result as shown in Figure 4, generates the fignal center of 1:2:2:1, illustrates that this compound can produce hydroxyl radical free radical with hydroperoxidation.
Embodiment 6
Method is with embodiment 2, unlike: compound throwing amount is (N, O-dimethyl hydroxylamine, N-t-butylhydroxylamine, O-t-butylhydroxylamine, chloro quinone, quinhydrones, citric acid and Trisodium Citrate, can mix according to arbitrary proportion (or mol ratio 1:3:1:1:1:2:2:1)) 1.0 g, wherein compound is by forming.Result as shown in Figure 5, generates the fignal center of 1:2:2:1, illustrates that this compound can produce hydroxyl radical free radical with hydroperoxidation.
Embodiment 7
Do not add nonmetal activator in present embodiment in hydrogen peroxide to use in the steps below: be that benzoic staying water pH value is adjusted to 3 with perchloric acid by pollutent, hydrogen peroxide and compound is added in water body, uniform stirring reacts: wherein, benzoic starting point concentration is 40 μMs, reaction times is 8h, and temperature of reaction is 25 DEG C.Result as shown in Figure 6.
In Fig. 6, F curve is benzoic removal effect, and condition is: concentration of hydrogen peroxide is 0.4mM, and the compound added is consistent with in embodiment 2, and throwing amount is 30 mg/L.The benzoic removal effect of E curve, condition is: concentration of hydrogen peroxide is 0.4 mM, and the compound added is consistent with in embodiment 3, and throwing amount is 25 mg/L.D curve is benzoic removal effect, and condition is: concentration of hydrogen peroxide is 2 mM, and the compound added is consistent with in embodiment 4, and throwing amount is 20mg/L.C curve is benzoic removal effect, and condition is: be that benzoic staying water pH value is adjusted to 4 with acetic acid/sodium acetate buffer by pollutent, and concentration of hydrogen peroxide is 2 mM, and the compound added is consistent with in embodiment 5, and throwing amount is 10 mg/L.B curve is benzoic removal effect, and condition is: be that benzoic staying water pH value is adjusted to 4.5 with acetic acid/sodium acetate buffer by pollutent, and concentration of hydrogen peroxide is 2 mM, and the compound added is consistent with in embodiment 6, and throwing amount is 8 mg/L.A figure is the background not adding compound, phenylformic acid almost without any degraded, further illustrate add compound can effectively impel hydrogen peroxide produce hydroxyl radical free radical, thus degraded phenylformic acid.
Embodiment 8
In present embodiment, damping fluid (as perchloric acid, acetic acid/sodium acetate) is first used to be that benzoic staying water pH value tune is respectively 2.0,3.0,4.0,5.0,5.5,6.0 by pollutent, compound throwing amount is 25 mg/L, benzoic starting point concentration is 40 μMs, concentration of hydrogen peroxide is 0.4 mM, the compound added is consistent with in embodiment 2, and temperature of reaction is 25 DEG C.Total removal effect after phenylformic acid 1.5h is shown in Fig. 7.As can be seen from Figure 7, pH value be between 3.0-5.5 using compound as activator time, phenylformic acid clearance is the highest.Still have when pH value is 6 up to 12% phenylformic acid clearance, illustrate that adopting compound to produce when hydroxyl radical free radical removes the activator of organic contamination as hydrogen peroxide has widened the scope of application of pH value greatly.
Compound in the present invention can make hydrogen peroxide slowly-releasing hydroxyl radical free radical, is very suitable for repairing by the underground water of organic contamination and soil.
Claims (5)
1. the compound for impelling hydrogen peroxide to produce hydroxyl radical free radical, is characterized in that: described compound is selected from quinhydrones, chloro quinone, S-WAT, lithium sulfite, potassium sulfite, magnesium sulfite, calcium sulfite, ammonium sulphite, sulfurous acid, Sodium Pyrosulfite, pyrosulphite lithium, potassium pyrosulfite, pyrosulphite magnesium, pyrosulphite calcium, ammonium pyrosulfite, V-Brite B, SODIUM HYDROSULPHITE lithium, potassium hyposulfite, magnesium hyposulfite, calcium hyposulfite, ammonium hyposulfite, azanol, N-methyl hydroxylamine, O-methyl hydroxylamine, N, N-dimethyl hydroxylamine, N-ethylhydroxyl amine, O-ethylhydroxyl amine, N, N-diethyl hydroxylamine, N, O-dimethyl hydroxylamine, N, N, O-trimethylammonium azanol, N-t-butylhydroxylamine, O-t-butylhydroxylamine, sulfonation azanol, N-isopropylhydroxyla, metaraminol, isobutyl oxygen amine salt, aromatic hydroxylamine, N-ethyl-O-methyl hydroxylamine, N-methyl-O-ethylhydroxyl amine, N, N, O-tripropyl azanol, O-Cvclopropvlmethvl azanol, humic acid, ammonium chloride, quadrol-N, N-disuccinic acid trisodium salt, disodium ethylene diamine tetraacetate, nitrilotriacetic acid(NTA), trisodium phosphate, citric acid, Trisodium Citrate, one or more in oxalic acid and sodium oxalate.
2. the compound for impelling hydrogen peroxide to produce hydroxyl radical free radical according to claim 1, is characterized in that: described azanol is selected from oxammonium hydrochloride, hydroxylamine perchlorate, oxammonium sulfate, phosphatic hydroxylamine or aqueous hydroxylamine.
3. the compound for impelling hydrogen peroxide to produce hydroxyl radical free radical according to claim 1, it is characterized in that: described compound is selected from azanol, N-methyl hydroxylamine, N, N-dimethyl hydroxylamine, N-ethylhydroxyl amine, N, N-diethyl hydroxylamine, N, O-dimethyl hydroxylamine, N, N, O-trimethylammonium azanol, one or more in N-t-butylhydroxylamine, sulfonation azanol and aromatic hydroxylamine; Wherein, azanol is selected from oxammonium hydrochloride, hydroxylamine perchlorate, oxammonium sulfate, phosphatic hydroxylamine or aqueous hydroxylamine.
4. one kind uses the method removing dirty organic pollutants for the compound impelling hydrogen peroxide to produce hydroxyl radical free radical described in claim 1, it is characterized in that: add hydrogen peroxide and compound to containing in the water of organic pollutant, mix, react; Wherein, total throwing amount of compound and total dosage molar ratio of hydrogen peroxide are at 1:10 ~ 10:1.
5. the method impelling hydrogen peroxide generation hydroxyl radical free radical to remove dirty organic pollutants according to claim 4, it is characterized in that: described compound is selected from azanol, N-methyl hydroxylamine, N, N-dimethyl hydroxylamine, N-ethylhydroxyl amine, N, N-diethyl hydroxylamine, N, O-dimethyl hydroxylamine, N, N, O-trimethylammonium azanol, N-t-butylhydroxylamine, one or more in sulfonation azanol and aromatic hydroxylamine; Wherein, azanol is selected from oxammonium hydrochloride, hydroxylamine perchlorate, oxammonium sulfate, phosphatic hydroxylamine or aqueous hydroxylamine.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN108640209A (en) * | 2018-05-04 | 2018-10-12 | 南京林业大学 | A method of strengthening microwave treatment organic wastewater |
| CN113198302A (en) * | 2021-04-15 | 2021-08-03 | 成都安捷芮环保科技有限公司 | SRR free radical cluster medicament for treating various VOCs (volatile organic compounds) foul waste gas |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN108640209A (en) * | 2018-05-04 | 2018-10-12 | 南京林业大学 | A method of strengthening microwave treatment organic wastewater |
| CN113198302A (en) * | 2021-04-15 | 2021-08-03 | 成都安捷芮环保科技有限公司 | SRR free radical cluster medicament for treating various VOCs (volatile organic compounds) foul waste gas |
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