CN115043481A - Method for oxidizing As (III) in water body by using supported manganese-based catalyst - Google Patents

Method for oxidizing As (III) in water body by using supported manganese-based catalyst Download PDF

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CN115043481A
CN115043481A CN202210719123.5A CN202210719123A CN115043481A CN 115043481 A CN115043481 A CN 115043481A CN 202210719123 A CN202210719123 A CN 202210719123A CN 115043481 A CN115043481 A CN 115043481A
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iii
manganese
based catalyst
oxidizing
solution
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徐志峰
杨裕东
李玉虎
金贵忠
龚福保
金承永
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HSIKWANG SHAN TWINKLING STAR CO Ltd
Jiangxi University of Science and Technology
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HSIKWANG SHAN TWINKLING STAR CO Ltd
Jiangxi University of Science and Technology
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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
    • C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/32—Manganese, technetium or rhenium
    • B01J23/34—Manganese
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
    • B01J29/16—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y containing arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J29/163—X-type faujasite
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
    • B01J29/78—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J29/7807—A-type
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/0201—Impregnation
    • 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
    • C02F1/727—Treatment of water, waste water, or sewage by oxidation using pure oxygen or oxygen rich gas
    • 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
    • C02F2101/10—Inorganic compounds
    • C02F2101/103—Arsenic compounds
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/16—Nature of the water, waste water, sewage or sludge to be treated from metallurgical processes, i.e. from the production, refining or treatment of metals, e.g. galvanic wastes

Abstract

The invention discloses a method for oxidizing As (III) in water by using a supported manganese-based catalyst, which comprises the steps of successfully loading soluble manganese salt on a carrier by using an impregnation method, drying and roasting to prepare the supported manganese-based catalyst, then adding the manganese-based catalyst into a solution containing As (III), adjusting the pH of the solution to be alkaline by using an alkaline solution, introducing air/oxygen, stirring and reacting for 1-3 hours, and oxidizing the As (III) in the solution into As (V); meanwhile, the manganese-based catalyst after oxidation can be recycled, and a new part of solution containing As (III) is continuously oxidized. The method is suitable for treating As (III) -containing waste liquid and water, and has the advantages of low energy consumption, wide application range, simple operation, recyclable catalyst and the like.

Description

Method for oxidizing As (III) in water body by using supported manganese-based catalyst
Technical Field
The invention relates to the technical field of hydrometallurgy arsenic oxide, in particular to a method for oxidizing As (III) in water by a supported manganese-based catalyst.
Background
Arsenic (As) is a toxic element widely distributed in the earth crust, arsenic contamination in drinking water has become a major concern worldwide, and signs and symptoms of arsenic poisoning have occurred in many parts of the world, endangering human health and sustainable development. The world health organization sets the maximum allowable level of As in drinking water to 10ug/L due to its high toxicity and carcinogenicity. It is reported that at least 1.4 million people worldwide are exposed to environments above this tentative standard. In natural waters, arsenic is present predominantly in the form of two oxyanions, arsenite (as (iii)) and arsenate (as (v)), depending on their oxidation state and redox potential. As (V) can be effectively removed by common water treatment methods, including precipitation/coagulation, adsorption, ion exchange, membrane treatment and the like, but As (III) is more difficult to remove from solution than As (V), and the removal efficiency is often greatly reduced, and particularly, As (III) has higher toxicity and mobility than As (V). Therefore, in order to effectively remove arsenic from the solution, it is necessary to oxidize As (III) to As (V).
As (III) is relatively easy to oxidize and can be achieved using oxidants such as chlorine, hydrogen peroxide, sodium permanganate, and ozone. Although these agents are highly effective in oxidizing As (III), some of them may be caused by the formation of by-products or the presence of residuesHis minor problem. In addition, these chemicals are expensive, which makes the use of the chemical expensive and difficult for the user to bear. The oxidation of As (III) by using air as an oxidizing agent is undoubtedly the most attractive method, but the oxidation of As (III) by air has the problems of low efficiency and poor oxidation depth. Therefore, the technical proposal of directly using air or oxygen as the oxidant for As (III) oxidation is not feasible, and a catalyst is required to accelerate the oxidation rate of As (III). On the other hand, the researchers found that Pt-TiO could be introduced into the reaction system 2 And nano silver, etc. can improve the oxidation efficiency of air to As (III) (Kim et al, 2020, Guo et al, 2018). For example, patent CN101492199A discloses a method for removing arsenic by platinum-doped titanium dioxide through photoelectrocatalysis oxidation; during reaction, air is introduced from the bottom of the reactor through an aeration device, active carbon loaded platinum doped nano titanium dioxide is used as an anode, a carbon rod is used as a cathode, an ultraviolet lamp is placed at the top of the reactor or in the reactor, and direct current is applied to the ultraviolet lamp, and the As (III) is fully oxidized under the synergistic action of light, electricity and air. The existing catalyst for catalytic oxidation of As (III) generally has the defects of high price, complex preparation method, high use cost, incapability of recycling the catalyst and the like, so that the research on the catalyst which is prepared at low cost, good in catalytic performance and high in recycling performance is necessary.
Disclosure of Invention
The invention relates to a method for oxidizing As (III) in water by a supported manganese-based catalyst, which realizes the low-cost preparation of the catalyst and the high-efficiency oxidation of As (III) in water.
In order to achieve the purpose, the technical scheme disclosed by the invention is a method for oxidizing As (III) in water by using a supported manganese-based catalyst, which comprises the following steps: activating the carrier by adopting a soluble manganese salt solution impregnation method, and drying and roasting to prepare a supported manganese-based catalyst;
putting the solution containing As (III) into a reaction vessel, adjusting the initial alkalinity of the solution, stirring and heating to a specified temperature, then blowing oxygen-containing gas, adding a certain amount of manganese-based catalyst, and starting the catalytic oxidation of As (III);
the manganese-based catalyst after oxidation is returned to the oxidation process to re-oxidize a new portion of the As (III) -containing solution.
Preferably, the carrier is selected from one of molecular sieve 13X, molecular sieve 4A, zeolite, activated carbon and diatomaceous earth.
Preferably, the soluble manganese salt comprises one or more of manganese sulfate, manganese nitrate and manganese chloride.
Preferably, the concentration of the soluble manganese salt solution is 1-4 mol/L, the solid-to-solid ratio of the impregnation solution is 3: 1-8: 1, the impregnation temperature is 20-60 ℃, and the impregnation time is 1-2 hours.
Preferably, the solution containing As (III) has an initial pH of 11-13 and an initial As (III) concentration of 1-5 g/L.
Preferably, the oxygen-containing gas is selected from one or two of air and industrial pure oxygen, and the flow rate of the oxygen-containing gas is 0-0.4 m 3 /h。
Preferably, the addition amount of the manganese-based catalyst is 2-33 g/L.
Preferably, the solution temperature during the oxidation of As (III) is 20-80 ℃.
Preferably, the reaction vessel is equipped with aeration strips.
Preferably, the reaction time is controlled to be 1-3 h.
The technical idea and principle of the invention are as follows:
the carriers such as the molecular sieve 13X, the molecular sieve 4A, the zeolite, the activated carbon, the diatomite and the like are taken as typical porous minerals, so that the catalyst has the characteristics of low cost, rich reserves, stable chemical properties and strong adsorption capacity, and the unique porous structure enables the carriers to become high-quality catalyst carriers, thereby obtaining the composite catalyst with excellent adsorption capacity and dispersibility. Soluble manganese salt can be well loaded on the carriers by using an impregnation method, and the manganese-based catalyst is successfully prepared. When the manganese-based catalyst is added into the water containing As (III) and oxygen-containing gas is introduced, the manganese-based catalyst releases Mn (II) ions, but due to the excellent adsorption capacity of the manganese-based catalyst, Mn (II) ions are adsorbed on the surface of the catalyst, and dissolved oxygen in the solution reacts with the Mn (II) ions to oxidize the Mn (II) ions into MnOOH, MnO 2 . The catalyst has strong adsorption and surface formationThe manganese oxide has a large number of reactive active sites, As (III) and dissolved oxygen in the solution can be adsorbed to the active sites and vacancy sites at the edge of the catalyst particle layer, the reaction rate of As (III) and the dissolved oxygen is accelerated along with the electron transfer, the process is accompanied with the reduction of Mn (IV), As (III) and Mn (IV) are oxidized into As (V) after being reacted, Mn (IV) is reduced into Mn (II) and adsorbed on the surface of the catalyst, and then the manganese oxide with catalytic capability is generated by the reaction of the manganese oxide and the dissolved oxygen, so that the regeneration and the recycling of the catalyst are realized. Along with the continuous bubbling of the oxygen-containing gas, the dissolved oxygen in the solution is continuously supplemented, so that the manganese-based catalyst can be regenerated circularly, and has better direct oxidation and catalytic oxidation performances.
Based on the technical thought, the inventor provides a method for oxidizing As (III) in water by using a supported manganese-based catalyst.
Compared with the prior art, the invention has the following advantages:
(1) the method has the advantages of cleanness, high efficiency, low cost, simple operation, low energy consumption, no special equipment requirement, convenience for subsequent treatment process and easy realization of industrialization.
(2) The manganese-based catalyst prepared by the invention adopts a porous mineral carrier, has the advantages of low cost, rich reserves and the like, and can effectively reduce the preparation cost. The oxidant used for catalytically oxidizing As (III) is oxygen-containing gas which is cheap and easy to obtain, and the manganese-based catalyst can be recycled while the As (III) in the water body is efficiently oxidized. Therefore, the method is environment-friendly and generates no waste gas and waste residue.
Drawings
FIG. 1 is a schematic flow chart of a method for oxidizing As (III) in a water body by using a supported manganese-based catalyst according to the present invention;
FIG. 2 is a graph showing the effect of different manganese-based catalysts on the catalytic air oxidation of As (III);
FIG. 3 is a graph showing the effect of different reaction temperatures on catalytic air oxidation of As (III);
FIG. 4 is a graph showing the effect of atmospheric and air flow rates on catalytic air oxidation of As (III);
FIG. 5 is a graph showing the effect of initial As (III) concentration in solution on catalytic air oxidation of As (III);
FIG. 6 is a graph showing the effect of manganese-based catalyst addition on catalytic air oxidation of As (III);
FIG. 7 shows the effect of Mn-based diatomaceous earth on the catalytic air oxidation of As (III) during recycling.
Detailed Description
The present invention will be further described with reference to the accompanying drawings, and it should be noted that the following examples are provided to illustrate the detailed embodiments and specific operations based on the technical solutions of the present invention, but the scope of the present invention is not limited to the examples.
Example 1:
500mL of 2mol/L manganese sulfate solution is taken, carrier molecular sieve 13X, molecular sieve 4A, zeolite, activated carbon and diatomite are respectively added according to the liquid-solid ratio of 4:1, the mixture is immersed for 2 hours at the temperature of 40 ℃ for activation treatment, and the supported manganese-based catalyst is prepared through drying and roasting. Taking 500mL of water containing As (III), the initial concentration of As (III) is 1g/L, the initial pH of the solution is 11.3-11.5, stirring and heating to 50 ℃ at 300r/min, and then blowing in at the flow rate of 0.2m 3 H, air, 20g/L of manganese-based molecular sieve 13X, manganese-based molecular sieve 4A, manganese-based zeolite, manganese-based activated carbon, manganese-based diatomite and a blank are added respectively, and the reaction is carried out for 3 hours, wherein the result is shown in figure 2.
After 3 hours, the contents of As (III) detected by taking liquid samples are respectively 110mg/L (adding manganese-based zeolite), 70.6mg/L (adding manganese-based diatomite), 116mg/L (adding manganese-based activated carbon), 501.4mg/L (adding manganese-based molecular sieve 13X), 255mg/L (adding manganese-based molecular sieve 4A) and 995.8mg/L (blank sample), and the oxidation rates of As (III) to As (V) are respectively 89%, 92.94%, 88.4%, 49.86%, 74.5% and 0.42%. Under the condition of introducing oxygen-containing gas, the manganese-based diatomite shows a better catalytic oxidation effect on As (III) in the water body, and can efficiently oxidize As (III) in a short time.
Example 2:
500mL of 2mol/L manganese chloride solution is taken, added with carrier diatomite according to the liquid-solid ratio of 4:1, immersed for 2 hours at the temperature of 40 ℃ for activation treatment, and dried and roasted to prepare the load-type manganese-based diatomite. 500mL of a solution containingAs (III) water body, the initial concentration of As (III) is 1g/L, the initial pH of the solution is 12.2-12.3, stirring is carried out at 300r/min, and then the blowing-in flow rate is 0.2m 3 Air/h, and 20g/L of manganese-based diatomite, and the reaction temperature was controlled at 20 deg.C, 50 deg.C, 60 deg.C, 80 deg.C, respectively, and the results were as shown in FIG. 3.
After 3 hours, the As (III) contents assayed in the liquid samples were 176.4mg/L (reaction temperature: 20 ℃), 75.5mg/L (reaction temperature: 50 ℃), 79.6mg/L (reaction temperature: 60 ℃), 61.3mg/L (reaction temperature: 80 ℃), and the As (III) oxidation rates to As (V) were 82.36%, 92.45%, 92.04%, 93.87%, respectively. The reaction temperature has a great influence on the catalytic oxidation of As (III) by manganese-based diatomite, and is preferably selected to be 50 ℃ based on the consideration of the oxidation efficiency and energy consumption of As (III).
Example 3:
500mL of 2mol/L manganese nitrate solution is taken, added with carrier diatomite according to the liquid-solid ratio of 4:1, immersed for 2 hours at the temperature of 40 ℃ for activation treatment, and dried and roasted to prepare the load-type manganese-based diatomite. Taking 500mL of water containing As (III) with initial concentration of 1g/L and initial pH of 11.5-11.7, heating to 50 ℃ with stirring at 300r/min, blowing air, adding 20g/L of manganese-based diatomite, and respectively controlling air flow rate to be 0m 3 /h、0.2m 3 /h、0.3m 3 /h、0.4m 3 Reaction time was 3 hours with a nitrogen stream, and the results are shown in FIG. 4.
After 3 hours, the As (III) content of the liquid sample is 709.1mg/L (nitrogen is introduced) and 398.8mg/L (air flow rate is 0 m) 3 H) and 75.5mg/L (air flow rate of 0.2 m) 3 H) and 70.8mg/L (air flow rate of 0.4 m) 3 H) and 71.4mg/L (air flow rate of 0.3 m) 3 And/h), the oxidation rates of As (III) to As (V) are 29.09%, 60.12%, 92.45%, 92.92% and 92.86%, respectively. The extra blowing of air is beneficial to supplement the consumed dissolved oxygen in the reaction system and quicken the oxidation rate of As (III), but when the dissolved oxygen is close to or reaches a saturated state, the further increase of the air flow rate cannot improve the concentration of the dissolved oxygen in the reaction system, so that the oxidation effect of As (III) cannot be further improved. Based on As (III)Considering the effect of oxidation, an air flow of 0.3m is selected 3 Preferably,/h.
Example 4:
500mL of 2mol/L manganese sulfate solution is taken, carrier diatomite is added according to the liquid-solid ratio of 4:1, the carrier diatomite is immersed for 2 hours at the temperature of 40 ℃ for activation treatment, and the carrier diatomite is prepared through drying and roasting. Taking 500mL of As (III) -containing water body, the initial pH of the solution is 12.4-12.6, heating to 50 ℃ with stirring at 300r/min, and then blowing in water with the flow rate of 0.2m 3 Air/h, and 20g/L of manganese-based diatomite, the initial concentrations of As (III) were controlled to be 1g/L, 2g/L, 3g/L, and 5g/L, respectively, and the reaction time was 3 hours, the results are shown in FIG. 5.
After 3 hours, the As (III) content of the liquid sample assay is respectively 75.5mg/L (As (III)) with the initial concentration of 1g/L, 617.4mg/L (As (III)) with the initial concentration of 2g/L, 1131.3mg/L (As (III)) with the initial concentration of 3g/L and 1990mg/L (As (III)) with the initial concentration of 5g/L, and the As (III) oxidation rate to As (V) is respectively 92.45%, 69.13%, 62.29% and 60.20%. When the air flow rate and the catalyst amount are constant, the dissolved oxygen participating in the reaction in unit time is fixed, namely the oxidation amount of As (III) in the air oxidation catalyzed by the catalyst is kept unchanged, and the total oxidation rate of As (III) is reduced due to the increase of the initial concentration of As (III); on the other hand, as the As (III) oxidation reaction proceeds, the higher initial As (III) concentration to alkali consumption is higher than that of the lower initial As (III) concentration system, which causes the pH value of the solution to rapidly decrease, which is not beneficial to the oxidation of As (III). Therefore, the higher the initial concentration of As (III), the poorer the oxidation effect. For the solution with higher initial As (III) concentration, the complete oxidation of As (III) can be promoted by adding lye.
Example 5:
500mL of 2mol/L manganese sulfate solution is taken, carrier diatomite is added according to the liquid-solid ratio of 4:1, the carrier diatomite is immersed for 2 hours at the temperature of 40 ℃ for activation treatment, and the carrier diatomite is prepared through drying and roasting. Taking 500mL of water containing As (III), the initial concentration of As (III) is 1g/L, the initial pH of the solution is 11.7-11.9, stirring and heating to 50 ℃ at 300r/min, and then blowing in at the flow rate of 0.2m 3 H air, 2g/L, 10g/L, 20g/L and 33g/L manganese base are respectively added in a controlled mannerDiatomaceous earth, 3 hours, the results are shown in FIG. 6.
After 3 hours, the As (III) content of the liquid sample assay is 427.1mg/L (added with 2g/L of manganese-based diatomite), 157.9mg/L (added with 10g/L of manganese-based diatomite), 70.6mg/L (added with 33g/L of manganese-based diatomite), 71mg/L (added with 20g/L of manganese-based diatomite), and the oxidation rate of As (III) to As (V) is 57.29%, 84.21%, 92.94% and 92.9% respectively. Therefore, in order to realize the efficient oxidation of As (III), the catalyst dosage is preferably selected to be 20 g/L.
Example 6:
500mL of 2mol/L manganese chloride solution is taken, a carrier diatomite is added according to the liquid-solid ratio of 4:1, the mixture is immersed for 2 hours at the temperature of 40 ℃ for activation treatment, and the supported manganese-based diatomite is prepared through drying and roasting. Taking 500mL of water containing As (III), the initial concentration of As (III) is 1g/L, the initial pH of the solution is 12.6-12.8, stirring and heating to 50 ℃ at 300r/min, and then blowing in at the flow rate of 0.2m 3 Adding 20g/L manganese-based diatomite into air per hour, reacting for 3 hours, filtering and collecting the manganese-based diatomite after the oxidation reaction, oxidizing a new part of water containing As (III) again, and circulating for 4 times. The cycling results are shown in FIG. 7.
As (III) content of the liquid sample to be tested is 39.6mg/L (primary cycle), 41.7mg/L (secondary cycle), 66.7mg/L (tertiary cycle) and 73.3mg/L (quaternary cycle) after reaction for 3 hours in each cycle, and the oxidation rate of As (III) to As (V) is 96.04%, 95.83%, 93.33% and 92.67% respectively. The results show that the performance of manganese-based diatomaceous earth in As (III) oxidation does not change significantly after 4 cycles of repeated use. After reacting for 3h, the oxidation degree of As (III) continuously reaches more than 90 percent, which shows that the manganese-based diatomite has good recycling performance and is beneficial to reducing the oxidation cost of As (III).
Various corresponding changes and modifications can be made by those skilled in the art based on the above technical solutions and concepts, and all such changes and modifications should be included in the protection scope of the present invention.

Claims (10)

1. A method for oxidizing As (III) in water by a supported manganese-based catalyst is characterized in that:
activating the carrier by adopting a soluble manganese salt solution impregnation method, and drying and roasting to prepare a supported manganese-based catalyst;
putting the solution containing As (III) into a reaction vessel, adjusting the initial alkalinity of the solution, stirring and heating to a specified temperature, then blowing oxygen-containing gas, adding a certain amount of manganese-based catalyst, and starting the catalytic oxidation of As (III);
the manganese-based catalyst after oxidation is returned to the oxidation process to re-oxidize a new portion of the As (III) -containing solution.
2. The method of claim 1, wherein the carrier is selected from the group consisting of molecular sieves 13X, molecular sieves 4A, zeolites, activated carbon, and diatomaceous earth.
3. The method for oxidizing As (III) in a water body by using the supported manganese-based catalyst according to claim 1, wherein the soluble manganese salt comprises one or more of manganese sulfate, manganese nitrate and manganese chloride.
4. The method for oxidizing As (III) in water by using the supported manganese-based catalyst according to claim 1, wherein the concentration of the soluble manganese salt solution is 1-4 mol/L, the solid-to-solid ratio of the impregnation solution is 3: 1-8: 1, the impregnation temperature is 20-60 ℃, and the impregnation time is 1-2 hours.
5. The method for oxidizing As (III) in water body by using the supported manganese-based catalyst according to claim 1, wherein the initial pH of the As (III) -containing solution is 11-13, and the initial As (III) concentration is 1-5 g/L.
6. The method for oxidizing As (III) in water by using the supported manganese-based catalyst as claimed in claim 1, wherein the oxygen-containing gas is selected from one or two of air and industrially pure oxygen, and containsThe flow rate of the oxygen gas is 0-0.4 m 3 /h。
7. The method for oxidizing As (III) in water by using the supported manganese-based catalyst as claimed in claim 1, wherein the amount of the manganese-based catalyst is 2-33 g/L.
8. The method for oxidizing As (III) in water by using the supported manganese-based catalyst according to claim 1, wherein the solution temperature of As (III) during the oxidation is 20-80 ℃.
9. The method for oxidizing As (III) in water by using the supported manganese-based catalyst according to claim 1, wherein aeration strips are additionally arranged in the reaction vessel.
10. The method for oxidizing As (III) in water by using the supported manganese-based catalyst according to claim 1, wherein the reaction time is controlled to be 1-3 h.
CN202210719123.5A 2022-06-23 2022-06-23 Method for oxidizing As (III) in water body by using supported manganese-based catalyst Pending CN115043481A (en)

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Citations (4)

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