CN109721148B - Heterojunction interface electron transfer induced ozone catalytic oxidation water treatment method with bromate reduction capability - Google Patents
Heterojunction interface electron transfer induced ozone catalytic oxidation water treatment method with bromate reduction capability Download PDFInfo
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Abstract
The invention provides a heterojunction interface electron transfer induced ozone catalytic oxidation water treatment method with bromate reduction capability, and belongs to the field of water treatment technology and environment functional materials. The invention successfully prepares CeO by one-step method2/α‑Fe2O3The heterojunction catalyst simplifies the preparation steps of the catalyst; using CeO2And alpha-Fe2O3The heterogeneous junctions are formed by uniform compounding, and active sites are increased; by Ce3+/Ce4+And Fe2+/Fe3+The oxidation-reduction reaction between the two components promotes the electron transfer of a catalytic ozonation system, and improves the catalytic performance; bound Ce3+Capacity to capture bromine radicals and complexes [ Fe ]3+‑H2O2]sMiddle H2O2The double inhibition effect of bromate is realized by the reduction capability of bromate.
Description
Technical Field
The invention relates to a water treatment method of ozone catalytic oxidation with bromate reduction capacity induced by heterojunction interface electron transfer.
Background
At present, the problem of water environment pollution in China is remarkable, the appearance of novel pollutants such as benzotriazole ultraviolet stabilizers and the like greatly threatens the water quality safety of drinking water, and a new challenge is provided for drinking water treatment technology in China. Benzotriazole ultraviolet stabilizers are widely applied to sunscreen products, plastics, coatings and airplane deicers, and once the benzotriazole ultraviolet stabilizers enter water, the benzotriazole ultraviolet stabilizers pose great threats to the health of ecological systems and human beings.
Ozone has strong capabilities of disinfection, sterilization, degradation of macromolecular organic matters, deodorization and the like, and is widely applied. However, when bromide is present in the water, ozone oxidizes the bromide to bromate by strong oxidation of the bromide. Bromate has carcinogenicity and mutagenicity and has been identified as a class 2B potential carcinogen by the International agency for research on cancer. Once formed, bromate is difficult to remove in conventional processing. Common means for bromate inhibition are: removing bromide ions at the front end, removing bromate at the tail end and inhibiting the generation of bromate in the reaction process.
In the prior art, the generation of bromate can be successfully reduced by removing bromide ions at the front end. Patent CN105236691A provides a method for controlling bromide ion as a bromate precursor, which comprises adding sodium hypochlorite into water to react, oxidizing bromide ion in water into hypobromous acid, adding ammonium chloride into water, and reacting hypobromous acid with ammonium ion to generate ammonium bromide, thereby reducing the concentration of bromide ion in water. However, the addition of sodium hypochlorite and ammonium chloride may result in the increase of toxic by-products during the disinfection process. Patent CN102020372A provides an ozone water purification method for reducing bromate, and an adsorption filtration device is arranged at the front end of ozone oxidation to adsorb bromide ions, and the filter material of the pre-filtration is activated carbon or high-purity copper-zinc alloy or a combination of the activated carbon and the high-purity copper-zinc alloy. However, the above front-end bromide removal processes all add cost and are not economically cost effective.
The end control mainly comprises a membrane filtration method, a photocatalytic reduction method, an electrochemical method, a biological method and the like. The patent CN201353482Y discloses a hollow fiber membrane filter element, which can efficiently filter and remove harmful substances such as trace bromate in water. However, the membrane filtration method is expensive, and therefore, the use thereof is limited. Patent CN105772037A provides a method for removing bromate in water by ultraviolet light catalysis, and the technology adopts a catalyst to modify TiO through HF and graphene2The bromate in water can be efficiently removed in the ultraviolet catalytic oxidation process. However, the photocatalytic method requires an increased light source and equipment and consumes a high amount of energy, and the presence of organic matter competes with the reduction of bromate, reducing the reduction of bromate. The patent CN103420453A discloses an electrode for removing bromate in water and an application method thereof, the technology uses carbon paper as a carrier, precious metals and iron are electrodeposited on the surface of the carbon paper in sequence by an electrodeposition method to form the electrode, and the electrode has the capability of removing bromate in water by reduction. However, the electrochemical method has high energy consumption of electric energy and increased operation cost, and therefore, the electrochemical method cannot be generally utilized. The patent CN103103146A adopts the genus Sphingomonas to degrade bromate, the degradation efficiency is high, and the genus Sphingomonas can be inoculated and applied to a biological activated carbon process to effectively remove bromate. However, biodegradation has slow start-up period, long residence time, and the problem of biostability remains to be solved.
The removal of bromide ions at the front end and the removal of bromate at the tail end both increase the process and the cost, so that the practical application is greatly limited. Therefore, a novel, efficient and economic advanced treatment technology for the feed water or the reclaimed water is developed, the generation of bromate byproducts is synchronously and effectively controlled in the process of degrading organic pollutants by ozone oxidation, and the safety of the feed water is guaranteed.
The method for controlling bromate in the ozone oxidation reaction process comprises the following steps: ammonia water is added, pH is reduced, OH scavenger is added, hydrogen peroxide is added, ozone oxidation technology is catalyzed, and the like. The addition of ammonia reduces the amount of bromate formed, and under sufficient ozone conditions, the addition of ammonia results in BrO3 -The formation of bromate is delayed, but the formation of bromate cannot be really and effectively controlled, so the use of the bromate is limited. The generation of bromate can be effectively controlled by reducing the pH value, and the pH value is O3Lowering the pH by 50% to 63% per unit prior to oxidation reduces the amount of bromate formed, but lowering the pH is a process that adds cost and therefore limits the utility of the process. There are many kinds of OH scavengers, different OH scavengers are used for BrO3 -The effect of the amount of formation is also different, however, the addition of OH scavengers introduces new organic species, increasing the organic load of the water treatment process. Therefore, the major research is focused on the addition of chemical reagents and the catalytic ozonation technology to remove the ozone-oxidized organic pollutants and simultaneously inhibit the generation of bromate.
In the prior art, the method for controlling bromate by adding chemical reagent comprises the following steps: the patent CN101967020A controls the main path of bromate generation by adding hydrogen peroxide into the ozone oxidation device, thereby effectively inhibiting the bromate generation in the drinking water treatment process and enhancing the removal effect of organic matters. Patent CN10327985A provides a method for removing organic pollutants in water by catalytic ozonation, which adopts metal oxide or metal oxyhydroxide as a catalyst, and adds ozone and hydrogen peroxide as oxidants, thereby not only removing the organic pollutants in water, but also reducing the generation of bromate. The method can effectively control the generation of the bromate, but hydrogen peroxide is added, and the generation of the bromate can be effectively reduced only by adding excessive hydrogen peroxide, so that the operation cost is increased. Patent CN102701425A discloses the inhibition of bromate by adding hydroxylamine during the ozone oxidation process, and by the reaction of hydroxylamine and ozone, thereby depleting ozone. However, the addition of hydroxylamine not only increases the cost, but also increases the risk of nitrogen-containing sterilization by-products during the sterilization process. The bromate is controlled by adding a chemical reagent method, so that the operation cost is increased, secondary pollution is possibly caused, and the practical application is limited to a certain extent.
The heterogeneous ozone catalytic oxidation technology is one of advanced water treatment oxidation technologies, and can realize the reinforced removal of organic pollutants difficult to degrade in water. Researchers develop various composite metal oxide catalysts and successfully apply the catalysts to the degradation of various organic pollutants which are difficult to degrade, such as pesticides, dyes, PPCPs and the like in water through heterogeneous ozone catalytic oxidation, thereby obtaining satisfactory treatment effect. In addition, in the prior art, some patents disclose that catalysts such as metal oxides, metal oxide composites, metal oxyhydroxides and activated carbon are used in an ozone oxidation system for degrading organic pollutants in water, wherein some technologies have the capability of synchronously inhibiting the generation of a toxic byproduct, namely bromate.
The patent CN102234153A discloses that the Ce-MCM-48 catalyst is applied to a catalytic ozone oxidation system to successfully reduce the generation of bromate, and the Ce-MCM-48 catalyst can promote the effect of ozone oxidation of organic matters. Patent CN101050036A discloses a catalytic ozonation method of transition metal oxide doped cerium oxide or a supported cerium oxide catalyst to control the generation of bromate in the process of drinking water treatment, which overcomes the limitation of the method of adding chemical agents to control bromate, and has a higher bromate inhibition effect. Rare earth cerium oxide composite oxide catalyst (Ce-Zr-O) invented by patent CN102218309A 2) Can be effectively applied to the catalytic ozonation technology, and has good performance on organic matter degradation and bromate generation inhibition. In patent CN102513088A, cerium nitrate and titanium nitrate are used as main raw materials, and are calcined to prepare a composite catalyst, and the generation of bromate in the ozone oxidation process is controlled by controlling the generation of hydroxyl radicals. Patent CN102616916A introduces nano TiO2The catalyst is used for controlling bromate in the ozone oxidation process of drinking water, and the method is used for concentrating high bromide ionsThe control of the amount of bromate generated in the process of oxidizing the test water also has a remarkable effect. Patent CN108671920A invents a mesoporous gamma-Fe-Ti-Al2O3The catalyst can degrade ibuprofen and block the generation of bromate in the catalytic ozone oxidation process.
The catalysts in the above patents all show good catalytic activity and high stability, but the catalyst preparation steps are relatively complicated. More importantly, the metal ion Men+With Me(n+m)+The limited rate of inter-cycle conversion becomes a major limiting factor in catalytic activity. Therefore, bromate is synchronously inhibited in the catalytic ozonation process, research and development of a high-activity catalyst with high electron transfer capacity are carried out, the electron transfer rate is accelerated, the catalytic ozonation activity is promoted, and the method has important significance for heterogeneous catalytic ozonation degradation of organic pollutants and synchronous inhibition of the toxic byproduct bromate in wide application.
Thus, CeO2And alpha-Fe2O3Recombination to form a heterojunction by CeO2And alpha-Fe2O3And use of Ce3+Has remarkable capture effect on bromine free radicals (formulas (1) to (2)), and forms an indirect path for inhibiting bromate generation; bound Fe3+With the surface hydroxyl of the composite catalyst and H generated in the system2O2Promoting the complexing action of the complex [ Fe ] (formula (3))3+-H2O2]sMiddle H2O2Bromate is reduced into hypobromous acid, so that a double path of inhibiting the bromate is realized; by Ce3+/Ce4+And Fe2+/Fe3+The oxidation-reduction reaction (formula (4)) between the above two, and the transfer of electrons in the catalytic ozonation system is promoted by Ce4+Oxidation of Fe2+Production of Ce at the same time3+And Fe3+Generated Ce3+And Fe3+The inhibition of bromate can be further promoted; the catalytic performance of a catalytic ozonation system is improved, the enhanced removal of trace organic pollutants and the efficient control of bromate are realized, the water quality safety is ensured, and the method has very important theoretical and practical significance.
Ce3++Br·→Ce4++Br- (1)
Ce3++BrO·+H+→Ce4++HOBr (2)
Ce4++Fe2+→Ce3++Fe3+ (4)
Disclosure of Invention
Aiming at the polluted water body containing trace organic pollutants which are difficult to degrade such as ultraviolet stabilizer and bromide ions, the invention solves the problems that the conventional feedwater treatment process and the sewage secondary treatment have poor effect and cannot inhibit the generation of a toxic byproduct, namely bromate, and innovatively provides the method for treating the polluted water body by using CeO 2/α-Fe2O3The advanced oxidation technology of heterogeneous catalytic ozonation water treatment by taking a heterojunction as a catalyst and aiming at CeO2/α-Fe2O3The preparation and application conditions of the heterojunction catalyst are explained. The invention adopts the following technical scheme:
using CeO2/α-Fe2O3The bimetallic oxide heterojunction is used as a catalyst, and the preparation is completed by a one-step method: (1) weighing 2.0-4.0 mmol of cerium nitrate, 4.0-8.0 mmol of ferric nitrate and 6.0-12.0 mmol of citric acid, wherein the molar ratio of metal to citric acid is 1: adding 10-30 ml of ethanol and 5-15 ml of distilled water to prepare a complexing solution with a certain concentration, and stirring at room temperature for 12 hours; (2) drying and grinding the solution obtained in the step (1) at 90-100 ℃; (3) calcining the dry powder obtained in the step (2) at 600-900 ℃ for 4h (the heating rate is 2 ℃/min); (4) cooling and naturally cooling to room temperature.
The invention provides CeO2/α-Fe2O3The application condition of the bimetallic oxide heterojunction in a catalytic ozonation system is characterized in that the process is realized by the following steps: (1) required for the process O3The concentration is 0.5-2.5 mg/L; (2) process for the preparation of a coatingRequired CeO2/α-Fe2O3The dosage is 0.1-2.0 g/L; (3) the concentration of pollutants in the water body to be treated is 2.0-10.0 mg/L; (4) the concentration of bromide ions in the water body to be treated is 50-500 mug/L; (5) the contact time is 60-120 min; (6) the pH value of the reaction system is 2.63-11.00.
The invention provides an ozone catalytic oxidation water treatment method with a bromide reduction capability induced by heterojunction interface electron transfer, which can be applied to a drinking water deep treatment process, and can be used for pretreatment, coagulation, precipitation, filtration and CeO (CeO) treatment of a polluted water body2/α-Fe2O3After the catalytic ozonation advanced treatment-disinfection treatment, the problems of pollutant removal and synchronous control of the generation of ozone byproduct bromate in the treatment of bromine-containing water can be realized, so that the quality of drinking water is improved.
The invention provides a heterojunction interface electron transfer induced ozone catalytic oxidation water treatment method with bromate reduction capability, which can be applied to regeneration treatment process of urban domestic sewage, wherein polluted water passes through a grid, a grit chamber, a primary sedimentation tank, an aeration biochemical tank, a secondary sedimentation tank, a biological filter, an ultrafiltration membrane separation and CeO2/α-Fe2O3After catalytic ozonation-disinfection treatment, the method not only has a good effect of removing pollutants, but also can effectively inhibit the generation of a toxic byproduct, namely bromate, and has a good application prospect without an additional process.
Compared with the prior art, the invention has the advantages that:
1. the invention provides a water treatment method of ozone catalytic oxidation with bromate reduction capability induced by heterojunction interface electron transfer, which is implemented by using CeO 2And alpha-Fe2O3The catalyst has the advantages of increasing the reaction active sites of the catalyst and promoting the transfer rate of interface electrons, realizing the accelerated decomposition of ozone into active oxygen species, accelerating the degradation of ultraviolet stabilizers in water, ensuring the safety of water quality and improving the water quality environment.
2. The method for treating water by ozone catalytic oxidation with the heterojunction interface electron transfer induction and bromate reduction capacity, provided by the invention, has good catalytic oxidation performance, the removal rate of the ultraviolet stabilizer in 10 minutes can reach 100%, the reaction time is greatly shortened, the removal rate is improved by 30% compared with that of a single ozone oxidation system, and the rapid and efficient removal of the ultraviolet stabilizer in water is realized.
3. According to the method for treating water by ozone catalytic oxidation with the heterojunction interface electron transfer induction and the bromate reduction capacity, provided by the invention, through a double inhibition approach to bromate, the pollutants are degraded by ozone oxidation and the generation of bromate is synchronously inhibited, and compared with a single ozone oxidation system, the bromate inhibition rate is up to 84%, so that the problem that the generation of a toxic byproduct bromate cannot be inhibited in the traditional water treatment process is solved, and the method has great significance for further improving the water quality.
4. The CeO provided by the invention 2/α-Fe2O3The bimetallic oxide heterojunction is synthesized by a one-step method, is simple and convenient to operate, has high catalytic oxidation capacity and has wide application prospect.
Brief description of the drawings
FIG. 1 shows CeO in different compounding ratios2/α-Fe2O3Catalytic ozone oxidative degradation BZA potency diagram.
FIG. 2 shows CeO in different compounding ratios2/α-Fe2O3The bromate inhibition efficacy of the catalytic ozonation system is shown in the figure.
Detailed Description
This CeO was added to2/α-Fe2O3The preparation method of the heterojunction and the application of the heterojunction in the research on the efficiency of catalyzing and degrading the ultraviolet stabilizer in water and synchronously inhibiting bromate are illustrated, and the technical scheme of the invention is not limited to the specific embodiments listed below and also comprises any combination of the specific embodiments.
The first embodiment is as follows: CeO of the present embodiment2/α-Fe2O3The preparation method of the heterojunction comprises the following steps: (1) weighing 4.0mmol of cerium nitrate, 4.0mmol of ferric nitrate and 8.0mmol of citric acid, wherein the molar ratio of metal to citric acid is 1: 1, adding 15ml of ethanol and 5ml of distilled water to prepare a complexing solution with a certain concentration, and stirring at room temperature for 12 hours; (2) drying and grinding the solution obtained in the step (1) at 90 ℃; (3) will be provided withCalcining the dry powder obtained in the step (2) at 750 ℃ for 4h (the heating rate is 2 ℃/min); (4) cooling and naturally cooling to room temperature.
The second embodiment is as follows: CeO of the present embodiment2/α-Fe2O3The preparation method of the heterojunction comprises the following steps: (1) weighing 4.0mmol of cerium nitrate, 8.0mmol of ferric nitrate and 12.0mmol of citric acid, wherein the molar ratio of metal to citric acid is 1: 1, adding 15ml of ethanol and 5ml of distilled water to prepare a complexing solution with a certain concentration, and stirring at room temperature for 12 hours; (2) drying and grinding the solution obtained in the step (1) at 90 ℃; (3) calcining the dry powder obtained in the step (2) at 750 ℃ for 4h (the heating rate is 2 ℃/min); (4) cooling and naturally cooling to room temperature.
The third concrete implementation mode: CeO of the present embodiment2/α-Fe2O3The preparation method of the heterojunction comprises the following steps: (1) weighing 2.0mmol of cerium nitrate, 8.0mmol of ferric nitrate and 10.0mmol of citric acid, wherein the molar ratio of metal to citric acid is 1: 1, adding 15ml of ethanol and 5ml of distilled water to prepare a complexing solution with a certain concentration, and stirring at room temperature for 12 hours; (2) drying and grinding the solution obtained in the step (1) at 90 ℃; (3) calcining the dry powder obtained in the step (2) at 750 ℃ for 4h (the heating rate is 2 ℃/min); (4) cooling and naturally cooling to room temperature.
The fourth concrete implementation mode: the decontamination technology in the catalytic ozonation system is realized according to the following steps of (1) O required by the process3The concentration is 2.0 mg/L; (2) CeO required by the process 2/α-Fe2O3The dosage is 0.25 g/L; (3) the concentration of pollutants in the water body to be treated is 10.0 mg/L; (4) the concentration of bromide ions in the water body to be treated is 100 mug/L; (5) the contact time is 120 min; (6) the pH of the reaction system was in the range of 6.40.
CeO prepared in the present embodiment2/α-Fe2O3The heterojunction catalyst can realize the rapid and efficient removal of the ultraviolet stabilizer, and the attached figure 1 shows that CeO2/α-Fe2O3The removal rate of the catalytic ozone oxidation system to BZA reaches 100%, and the rapid reinforced removal of the ultraviolet stabilizer BZA is realized; meanwhile, the inhibition effect of bromate can be synchronously realized. As shown in figure 2, the bromate inhibition rate reaches 8 after 30min4 percent. CeO prepared by the invention2/α-Fe2O3The catalyst simplifies the preparation steps of the conventional composite catalyst, has simple preparation process and low price, enhances the efficiency of removing pollutants by catalyzing ozone oxidation under the synergistic action of the catalyst, improves the mineralization and detoxification effects, makes up the defects of the traditional drinking water treatment process, and is a catalyst with wide prospect.
The fifth concrete implementation mode: CeO prepared by the present embodiment2/α-Fe2O3The application method of the heterojunction catalyst in the drinking water treatment comprises the following steps: pretreatment-coagulation-precipitation-filtration-CeO2/α-Fe2O3Catalyzing ozone oxidation for advanced treatment, and discharging water after disinfection. CeO used in the present embodiment 2/α-Fe2O3The catalytic ozonation advanced treatment technology is completely the same as the existing ozonation system of a water plant, no water treatment equipment is needed to be added, and the catalytic ozonation reactor can be a batch reactor, a continuous reactor or a multi-stage combined reaction system.
The sixth specific implementation mode: the present embodiment is different from the fifth embodiment in that CeO2/α-Fe2O3The application method of the heterojunction catalyst in the regeneration treatment of the urban domestic sewage comprises the following steps: performing primary treatment in a grating-grit chamber-primary sedimentation tank, introducing the effluent of the primary sedimentation tank into biological treatment equipment such as an aeration biochemical tank, introducing the effluent after biological treatment into a secondary sedimentation tank, performing advanced treatment on the effluent after secondary treatment by using a coupling technology of biological filter-ultrafiltration membrane separation, and finally adopting CeO2/α-Fe2O3Catalyzing ozone oxidation for advanced treatment, and discharging water after treatment.
CeO obtained in the present embodiment2/α-Fe2O3The heterojunction catalyst is applied to advanced treatment of drinking water or treatment of urban domestic sewage, can realize enhanced removal of low-concentration and high-toxicity PPCPs novel organic pollutants in water, can inhibit generation of toxic byproduct bromate, and has great significance for guaranteeing water quality safety.
Claims (2)
1. A water treatment method of ozone catalytic oxidation induced by heterojunction interface electron transfer and having bromate reduction capability is characterized in that CeO synthesized by one-step method is adopted 2/α-Fe2O3The bimetallic oxide heterojunction is a catalyst for catalytic oxidation treatment of ozone, and the interface Ce is strengthened3+/Ce4+And Fe2+/Fe3+The oxidation-reduction reaction between the two components promotes the neutron transfer rate of a catalytic ozone oxidation system and induces Ce4+Oxidation of Fe2+Production of Ce at the same time3+And Fe3+Generated Ce3+Trapping of bromine radicals, binding Fe3+With the surface hydroxyl of the composite catalyst and H generated in the system2O2Promoting the complexing action of the complex [ Fe ]3+-H2O2]sMiddle H2O2The method has the advantages that the bromate is reduced into the hypobromous acid, the dual-path inhibition of the bromate is promoted, the degradation of trace refractory organic pollutants in water is enhanced, the mineralization capability is improved, the reaction time is effectively shortened, the high-efficiency reduction of the bromate which is a toxic byproduct is synchronously realized, the purpose of water purification is realized, and the method is prepared through the following steps:
(1) weighing 2.0-4.0 mmol of cerium nitrate, 4.0-8.0 mmol of ferric nitrate and 6.0-12.0 mmol of citric acid, wherein the molar ratio of metal cations to citric acid is 1: adding 10-30 ml of ethanol and 5-15 ml of distilled water to prepare a complexing solution with a certain concentration, and stirring at room temperature for 12 hours;
(2) drying and grinding the solution obtained in the step (1) at 90-100 ℃;
(3) calcining the dry powder obtained in the step (2) at 600-900 ℃ for 4h, wherein the heating rate is 2 ℃/min;
(4) Cooling and naturally cooling to room temperature.
2. The application of the method for treating water through ozone catalytic oxidation with the bromate reduction capability induced by electron transfer at the heterojunction interface as claimed in claim 1, wherein the advanced treatment process applied to drinking water comprises the steps of pretreating, coagulating, precipitating, filtering and CeO (CeO) polluted water2/α-Fe2O3Catalytic ozone oxidation advanced treatment, disinfection and water discharge; the process flow applied to the regeneration of urban domestic sewage comprises the steps of putting the polluted water into a grid, a grit chamber, a primary sedimentation tank, a biochemical tank, a secondary sedimentation tank, a biological filter, ultrafiltration membrane separation and CeO2/α-Fe2O3Catalytic ozone oxidation advanced treatment, disinfection and water discharge; the method is applied by the following steps:
(1) required for the process O3The concentration is 0.5-2.5 mg/L;
(2) CeO required by the process2/α-Fe2O3The dosage is 0.1-2.0 g/L;
(3) the concentration of pollutants in the water body to be treated is 2.0-10.0 mg/L;
(4) the concentration of bromide ions in the water body to be treated is 50-500 mug/L;
(5) the contact time is 60-120 min;
(6) the pH range of the reaction system is 2.63-11.00;
(7) the catalytic ozonation reactor is one of a batch reactor, a continuous reactor or a multi-stage combined reaction system.
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| CN111151280A (en) * | 2019-12-30 | 2020-05-15 | 同济大学 | Cerium-based ozone catalyst containing double active sites and preparation method and application thereof |
| CN113171739B (en) * | 2021-04-25 | 2023-07-04 | 中南民族大学 | Method for producing superoxide anion free radical by catalytic activation of bromate and application of superoxide anion free radical produced by method |
| CN113880204A (en) * | 2021-10-29 | 2022-01-04 | 昆山市供排水水质检测中心有限公司 | Control method of bromate content in water and detection method of bromate content in sodium hypochlorite |
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| CN104478171A (en) * | 2014-12-15 | 2015-04-01 | 北京桑德环境工程有限公司 | Reusing treatment method and system for municipal wastewater |
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