Method for activating feiii driven fenton-like reaction system by pda@mon and application thereof
By activating the FeIII-driven Fenton-like reaction system with PDA@MoN, the problems of narrow pH application range and iron sludge formation in the existing homogeneous Fenton system are solved. This achieves efficient degradation of organic pollutants and improved H2O2 utilization efficiency over a wide pH range, without the formation of iron sludge.
Patent Information
- Application Number
- CN202311254736.7
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- Filing Date
- 2023-09-27
- Publication Date
- 2025-10-17
- Estimated Expiration
- 2043-09-27
AI Technical Summary
The existing homogeneous Fenton system has a narrow pH application range, low H2O2 utilization efficiency, and iron sludge is generated during the reaction process.
A PDA@MoN-activated FeIII-driven Fenton-like reaction system was constructed by using a PDA@MXene-FeIII-H2O2 homogeneous Fenton-like reaction system. By utilizing the electron-donating ability of PDA and the conductivity and coordination ability of MXene, FeIII was stabilized and the FeIII/FeII redox cycle was activated, the pH range was broadened, and the formation of iron sludge was inhibited.
It achieves efficient degradation within a pH range of 3.0-10.0, improves H2O2 catalytic efficiency, generates strong oxidizing free radicals, and efficiently removes organic pollutants in water, including antibiotics, organic dyes, chemical industrial agents, and complexed heavy metals, without producing iron sludge.
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Abstract
Description
TECHNICAL FIELD
[0001] The application belongs to the technical field of environmental protection, and particularly relates to a method for degrading water organic pollutants by high-efficiency driving homogeneous Fenton reaction based on MXene (transition metal nitride) interface activation of trivalent iron ions (Fe III ) and application thereof. BACKGROUND
[0002] The homogeneous Fenton technology is the most mature advanced oxidation water treatment technology at present due to its simple operation, low cost, high pollutant treatment efficiency and other advantages. II The reaction mechanism is based on Fe III / Fe II redox cycle, catalytic H2O2 to form free radical chain reaction, and strong oxidizing hydroxyl radical (·OH) is generated, so as to oxidize and degrade pollutants. III Therefore, the cycle efficiency of Fe III / Fe II is the key to determine the catalytic efficiency of the system. Since the process of Fe III being reduced to Fe II is the main speed control step in the catalytic reaction, the conversion of Fe III to Fe II is blocked, which leads to various technical bottlenecks of the homogeneous Fenton method, such as narrow pH range, low H2O2 utilization efficiency, and a large amount of iron sludge generated in the reaction process. Therefore, developing a kind of catalyst that can effectively prevent the precipitation of Fe III ions in the Fenton reaction and efficiently drive the Fe III / Fe II redox cycle to construct a Fe III activated Fenton-like system is an upgrading strategy of Fenton technology with great development and application potential.
[0003] However, the existing homogeneous Fenton system has a small pH range, low H2O2 utilization efficiency, and generates iron sludge in the reaction process. SUMMARY
[0004] The application provides a degradation complex based on a Fenton-like system and application thereof, and aims to solve the problems of the existing homogeneous Fenton system, such as small pH range, low H2O2 utilization efficiency, and generation of iron sludge in the reaction process.
[0005] Technical scheme
[0006] The application provides a method for activating Fe III to drive a Fenton-like reaction system by PDA@MoN, and the steps are as follows:
[0007] The Mxene is ultrasonically dispersed in ultrapure water for 1-2h, the concentration of the MXene is 1-10mg / mL, dopamine is added, the mass ratio of the MXene and dopamine is 5-2:1, the pH of the solution is adjusted to 8.0, the dopamine is polymerized on the surface of the MXene by fully stirring, after reaction for 4-5h, standing, removing the supernatant, and repeatedly washing the obtained material with ultrapure water until impurities are removed, vacuum freeze-drying to obtain PDA@MoN; PDA@MoN, Fe III and H2O2 are mixed in a mass ratio of 1:1:1 to form a Fenton-like reaction system.
[0008] Further, the MXene is molybdenum nitride, which is alternately stacked by transition metal layers and nitrogen atom layers to form a stable layered structure through covalent bonding.
[0009] Preferably, the preparation method of the Mxene is: (NH4)4Mo7O 24 ·4H2O is dissolved in ultrapure water to form a 0.05-1.0mM Mo 4+ ion solution, and a 0.01-1.0g / L solution of cyclohexane methylene tetramine is prepared, the two are mixed in equal volume, and after standing for 5-7h, observing whether colorless crystals are generated, removing the supernatant, slowly washing the obtained crystals with ultrapure water until impurities are removed, and drying at 60℃ to obtain a precursor; the obtained precursor is calcined at 400℃ for 5-7h with continuous ammonia gas to obtain the Mxene.
[0010] Preferably, the reagent for adjusting the pH of the solution is hydrochloride-Tris buffer reagent.
[0011] The application also provides a method for activating Fe III The Fenton-like reaction system prepared by the method is used for treating pollutants.
[0012] Further, the Fenton-like reaction system is used for degrading antibiotics, organic dyes, chemical industrial preparations and complex heavy metals.
[0013] Further, the pH application range of the Fenton-like reaction system is 3.0-10.0, and no iron mud is generated in the degradation reaction process.
[0014] Compared with the existing homogeneous Fenton technology, the above technical scheme of the application can achieve the following
[0015] Beneficial effects:
[0016] (1) The good electron donating ability of PDA and the excellent conductivity and strong coordination ability of MXene to high charge state iron ions are combined, so that Fe IIIStable on the catalytically active interface to prevent its precipitation inactivation, and further activation of Fe III Promote Fe III / Fe II Circulation, and continuous release of Fe II PDA@MXene composite catalyst;
[0017] (2) PDA@MXene-Fe III -H2O2 Fenton system can effectively broaden the pH value of Fenton reaction, and Fe III In the system is not easy to precipitate inactivation under higher pH conditions, effectively inhibits the generation of iron mud in homogeneous Fenton system.
[0018] (3) The existence of transition metal layer and hole can not only provide new active sites for the catalysis of H2O2, but also can reduce the catalytic energy barrier of Fe II / III H2O2, effectively improve the catalytic efficiency of H2O2 in the system, and promote the generation of ·OH.
[0019] (4) PDA@MXene-Fe III -H2O2 Fenton system with catalytic activity Fe II Comes completely from the activation and conversion of Fe III The conversion efficiency is high. And the reaction condition is mild, without adding high energy consumption auxiliary process, the preparation process of the added catalyst is simple, and can be reused, which is economic and feasible, green and pollution-free, and has great application and development prospect.
[0020] (5) The degradation complex of the application can efficiently treat various water organic pollutants, including antibiotics (90%-98%), organic dyes (94%-99%), chemical industrial preparations (74%-81%), and complex heavy metals (85%-98%). The pH range is wide (3.0-10.0), and no iron mud is generated during the reaction process. DETAILED DESCRIPTION
[0021] In order to make the purpose, technical scheme and application advantages of the application more clear and explicit, the following will be further described in detail combined with examples. It should be understood that the specific embodiments described herein are only used to explain the application, and are not used to limit the application. In addition, the technical features involved in each embodiment of the application described below can be combined with each other as long as they do not conflict with each other.
[0022] MXene is a two-dimensional material that has attracted much attention in recent years. It is mainly composed of transition metal layers and nitrogen atom layers stacked alternately, forming a stable layered structure through covalent bonding. Its high specific surface area, excellent electrical conductivity and unique chemical reactivity make it stand out in the field of electrocatalysis and energy conversion, especially its common metal layer mainly composed of molybdenum (Mo) and vanadium (V), which is a promising cocatalyst metal. Polydopamine (PDA) is a kind of green and safe biomimetic material. Its good adhesion properties enable it to be stably modified on the surface of almost any material and endow the material with unique physical and chemical properties. It has rich amine and phenolic hydroxyl structures and is an excellent electron donor, so it can activate Fe III and mediate Fe III / Fe II redox cycle, which has great advantages. However, existing research has not focused on the great application potential of this material as a cocatalyst in Fenton and Fenton-like technology. The research on Fe III activation driven Fenton-like system based on this kind of cocatalyst is also insufficient.
[0023] The present application directly activates Fe III by cocatalyst, prevents Fe III precipitation, mediates Fe III / Fe II redox cycle, broadens the pH range of Fenton reaction, and strengthens the generation of OH, thereby efficiently removing organic pollutants in water.
[0024] The present application proposes a method for activating Fe III driven Fenton-like reaction system by PDA@MoN, which comprises the following steps: step S1, dissolving (NH4)4Mo7O 24 ·4H2O in ultrapure water to form a 0.05-1.0mM Mo 4+ ion solution, at the same time, preparing a 0.01-1.0g / L solution of cyclohexane methylene tetramine, mixing the two solutions in equal volume, and then standing for 6h. After observing whether colorless crystals are generated, remove the supernatant, wash the obtained crystals with ultrapure water slowly to remove impurities, and dry them at 60℃ to obtain a precursor.
[0025] Step S2, the precursor obtained in step S1 is calcined at 400 DEG C for 6h with continuous ammonia gas, to obtain Mxene; Step S3, then the Mxene is ultrasonically dispersed in ultrapure water for 1-2h, the concentration of MXene is 1-10mg / mL, dopamine is added, the mass ratio of MXene and dopamine is 5-2:1, the pH of the solution is adjusted to 8.0 using hydrochloride-Tris buffer reagent, and the dopamine is polymerized on the surface of MXene by fully stirring, and after reaction for 4h, it is placed, the supernatant is removed, and the obtained material is repeatedly washed with ultrapure water until impurities are removed, and vacuum freeze-drying to obtain PDA@MoN; Step S4, PDA@MoN, Fe III and H2O2 are mixed in a mass ratio of 1:1:1 to form a Fenton-like system.
[0026] The principle of the application is to construct a PDA@MXene-Fe III -H2O2 homogeneous Fenton-like reaction system by using PDA modified MXene composite material, and the catalytically active species Fe II is activated and converted in situ through the interface action between PDA@MXene and Fe III . III Therefore, the PDA@MXene-Fe II system has excellent Fe III / Fe III cycle efficiency, can efficiently drive the Fenton reaction, and realizes the degradation of organic pollutants.
[0027] The activation and catalysis mechanism of PDA@MXene to Fe III is mainly to use the adsorption and reduction of FeIII by the composite material, to use the surface electrostatic action of MXene and polydopamine to drive the enrichment of Fe III on the surface of the catalyst, and then to use the lone pair electrons in the nitrogen atom layer of MXene to effectively prevent Fe III from precipitating, thereby widening the pH range of the Fenton reaction; and the catechol structure in PDA combined with the graphene-like structure of MXene can effectively donate electrons to Fe II , the coordination ability of the generated Fe III is weakened, and the change in the surface charge properties of the PDA oxidized by Fe II will further promote the release of Fe III , so as to ensure that the catalyst can provide enough reaction sites to continuously activate Fe III in the system.
[0028] The transition metal layer and the hole in MXene can also reduce the catalytic reaction energy barrier of H2O2, and mediate Fe IIThe PDA@MoN-Fe can activate H2O2 through a redox cycle, thereby improving the catalytic efficiency of H2O2 and strengthening the oxidative complete degradation of organic pollutants in water.
[0029] PDA@MoN-Fe III The interface activation catalytic reaction mechanism of H2O2 is shown in reactions (1)-(9). First, PDA@MoN cooperates with the surface electrostatic effect and chemical coordination to anchor the free Fe III in the system on the surface of the cocatalyst, and the electron-donating structure in PDA@MoN further conducts electrons to the surface Fe III , so that it is converted into Fe II . At the same time, the binding ability of PDA@MoN to FeII weakens, and Fe II is released into the solution. At the same time, a certain surface defect is formed on the surface, as shown in reactions (1)-(4). The generated Fe II and the ≡Mo III structure in the cocatalyst further catalyze H2O2 to induce free radical chain reactions to generate ROSs such as ·OH and ·O2 - , as shown in reactions (5)-(8). In addition, ·O2 - can further react with the surface defect formed by the activation of FeIII by PDA@MoN to generate singlet oxygen (O2), as shown in reaction (9). 1
[0030] Liquid phase (activation): PDA@MoN + Fe III → PDA@MoN≡Fe III (coordination complexation) (1)
[0031] Solid phase (activation): ≡Mo III –e - → ≡Mo IV (2)
[0032] ≡Ph-OH (PDA) –e - → ≡C6H4O2 (PDA) (3)
[0033] Solid-liquid (activation): PDA@MoN≡Fe III + e-→ PDA@MoN-h + + Fe II (4)
[0034] Liquid phase (catalysis): Fe II + H2O2→ Fe III + OH - + ·OH (5)
[0035] Liquid phase (catalysis): H2O2 + ·OH→ HO2· + H2O (6)
[0036] Liquid (catalysis): HO2·→ H + +·O2 - (7)
[0037] Solid-liquid (catalysis): ≡Mo III +H2O2→≡Mo IV +OH - +·OH (8)
[0038] Solid-liquid (catalysis): PDA@MoN-h + +·O2 - →PDA@MoN+ 1 O2 (9)
[0039] Example 1
[0040] A PDA@MoN activates Fe III drives a Fenton reaction system, specifically as follows:
[0041] First, PDA@MoN is prepared, and the specific steps are as follows: 5.0 g of (NH4)4Mo7O 24 ·4H2O is dissolved in 100 mL of ultrapure water, 0.8 g of hexamethylene tetramine (HMT) is dissolved in 100 mL of ultrapure water, both are mixed in equal volume, and after standing for 6 h, no colorless crystals are observed. After removing the supernatant, the obtained crystals are slowly washed with ultrapure water to remove impurities, and dried at 60°C. Then the obtained precursor is placed in a muffle furnace, and ammonia gas is continuously introduced, and calcined at 400°C for 6 h to obtain MoN MXene. Then 0.5 g of MoN is ultrasonically dispersed in 500 mL of ultrapure water, and 0.1 g of dopamine is added to the system, and the pH of the system is adjusted to 8.0 with hydrochloride-Tris buffer reagent. After stirring, dopamine is polymerized on the surface of MXene, and after reaction for 4 h, the supernatant is removed, and the obtained material is repeatedly washed with ultrapure water, and then vacuum freeze-dried to obtain PDA@MoN.
[0042] Example 2
[0043] MoN MXene is prepared as in Example 1, then 1.0 g of MoN is ultrasonically dispersed in 100 mL of ultrapure water, and 0.5 g of dopamine is added to the system, and the pH of the system is adjusted to 8.0 with hydrochloride-Tris buffer reagent. After stirring, dopamine is polymerized on the surface of MXene, and after reaction for 24 h, the supernatant is removed, and the obtained material is repeatedly washed with ultrapure water, and then vacuum freeze-dried to obtain PDA@MoN. And using 0.5 g / L PDA@MoN, 10 mM Fe IIIFenton-like system was constructed with 0.2 g / L PDA@MoN, 2 mM Fe III The pollutant treatment efficiency of the H2O2 system. The oxidation degradation effect of terramycin is shown in Table 1, wherein the concentration of terramycin is determined by using a high performance liquid chromatograph (Waters 1525, USA).
[0044] Table 1: PDA@MoN-Fe III H2O2 system for oxidatively degrading terramycin
[0045]
[0046] As shown in Table 1, the PDA@MoN-Fe III The Fenton-like system formed by H2O2 has excellent pollutant treatment efficiency, and has a fast reaction kinetics process for degrading antibiotics in water. Within 30 min, 98.2% of terramycin in the system can be degraded. It is proved that the Fenton-like technology proposed in the application can be applied to remove tetracycline antibiotic pollutants in water. Within 10 min, the degradation rate can reach 90.9-98.2%.
[0047] Example 3
[0048] The preparation of MoN MXene is as same as that in Example 1. Then, 0.2 g of MoN is ultrasonically dispersed in 100 mL of ultrapure water, and 0.05 g of dopamine is added to the system. The pH of the system is adjusted to 8.0 by using a hydrochloride-Tris buffer reagent. The dopamine is polymerized on the surface of the MXene by fully stirring. After 24 h of reaction, the supernatant is removed, and the obtained material is repeatedly washed with ultrapure water. Then, PDA@MoN is obtained by vacuum freeze-drying. Then, 0.2 g / L PDA@MoN, 2 mM Fe III Fenton-like system was constructed with 0.2 g / L PDA@MoN, 2 mM Fe III The pollutant treatment efficiency of the H2O2 system. The oxidation degradation effect of terramycin is shown in Table 1, wherein the concentration of terramycin is determined by using a high performance liquid chromatograph (Waters 1525, USA).
[0049] Table 2: PDA@MoN-Fe III H2O2 system for oxidatively degrading terramycin
[0050]
[0051] As shown in Table 2, the PDA@MoN-Fe IIIThe Fenton-like system formed by H2O2 has excellent pollutant treatment efficiency, and 90.4% of sulfadiazine in the system can be removed after 30 min of reaction, which shows that the Fenton-like technology proposed in the application can be applied to degradation of sulfonamide antibiotic pollutants in water.
[0052] Example 4
[0053] MoN MXene is prepared as in Example 1, then 0.5g MoN is ultrasonically dispersed in 200mL ultrapure water, and 0.3g dopamine is added to the system, the pH of the system is adjusted to 8.0 by hydrochloride-Tris buffer reagent, the dopamine is polymerized on the surface of MXene by fully stirring, and after 12h of reaction, the supernatant is removed, and the obtained material is repeatedly washed with ultrapure water, and then vacuum freeze-dried to obtain PDA@MoN. And 0.1g / L PDA@MoN, 8mM Fe III and 5mM H2O2 are used to construct a Fenton-like system, the pH value of the system is adjusted to 5.0, and 50mg / L methyl orange is oxidatively degraded at room temperature (25℃), so as to investigate the pollutant treatment efficiency of the PDA@MoN-Fe III -H2O2 system. The oxidative degradation effect of methyl orange is shown in Table 2, wherein the concentration of methyl orange is determined by using an ultraviolet spectrophotometer (A360, AOE, China).
[0054] Table 3: PDA@MoN-Fe III -H2O2 system oxidatively degrades methyl orange
[0055]
[0056] As shown in Table 3, the PDA@MoN-Fe III -H2O2 system has excellent pollutant treatment efficiency, and the removal rate of methyl orange in the system can reach 94.1% after 120min of reaction. It shows that the Fenton-like technology proposed in the application can be applied to degradation and removal of dye pollutants, and the removal rate can reach 92.0-94.1% after 90min of reaction.
[0057] Example 5
[0058] MoN MXene is prepared as in Example 1, then 0.5g MoN is ultrasonically dispersed in 200mL ultrapure water, and 0.3g dopamine is added to the system, the pH of the system is adjusted to 8.0 by hydrochloride-Tris buffer reagent, the dopamine is polymerized on the surface of MXene by fully stirring, and after 12h of reaction, the supernatant is removed, and the obtained material is repeatedly washed with ultrapure water, and then vacuum freeze-dried to obtain PDA@MoN. And 0.1g / L PDA@MoN, 8mM Fe IIIFenton-like system was constructed with 0.3 g / L PDA@MoN, 20 mM Fe III The pollutant treatment efficiency of the H2O2 system is shown in Table 2, wherein the concentration of methylene blue was determined by ultraviolet spectrophotometry (A360, AOE, China) as in Example 4.
[0059] Table 4: PDA@MoN-Fe III Oxidative degradation of methylene blue by the H2O2 system
[0060]
[0061] As shown in Table 5, PDA@MoN-Fe III The Fenton-like system formed by H2O2 has excellent pollutant treatment efficiency, and the removal rate of the dye methylene blue in the system can reach 99.1% after 120 min of reaction. It is shown that the Fenton-like technology proposed in the application can be applied to the degradation and removal of dye pollutants, and the reaction kinetics is fast, and the removal rate of pollutants can reach 91.9-99.1% after 60 min of reaction.
[0062] Example 6
[0063] MoN MXene was prepared as in Example 1, then 0.5 g of MoN was ultrasonically dispersed in 300 mL of ultrapure water, and 0.4 g of dopamine was added to the system. The pH of the system was adjusted to 8.0 with hydrochloric acid-Tris buffer reagent, and the dopamine was polymerized on the surface of the MXene by fully stirring. After 8 h of reaction, the supernatant was removed, and the obtained material was repeatedly washed with ultrapure water, and then vacuum freeze-dried to obtain PDA@MoN. A Fenton-like system was constructed with 0.3 g / L PDA@MoN, 20 mM Fe III A Fenton-like system was constructed with 0.3 g / L PDA@MoN, 20 mM Fe III The pollutant treatment efficiency of the H2O2 system is shown in Table 3, wherein the concentration of phenol was determined as in Example 2.
[0064] Table 5: PDA@MoN-Fe III Oxidative degradation of phenol by the H2O2 system
[0065]
[0066] As shown in Table 6, PDA@MoN-Fe IIIThe removal rate of phenol in the Fenton-like system formed by H2O2 can reach 74.1% at 60 min of reaction, which shows that the Fenton-like technology proposed in the application has good degradation and removal capacity for small-molecule organic pollutants in water.
[0067] Example 7
[0068] MoN MXene is prepared as in Example 1, then 0.6 g of MoN is ultrasonically dispersed in 300 mL of ultrapure water, and 0.4 g of dopamine is added to the system, the pH of the system is adjusted to 8.0 by using hydrochloride-Tris buffer reagent, the dopamine is polymerized on the surface of MXene by fully stirring, after 8 h of reaction, standing, removing the supernatant, and repeatedly washing the obtained material with ultrapure water, PDA@MoN is obtained by vacuum freeze-drying. And 0.3 g / L of PDA@MoN, 20 mM of Fe III and 8 mM of H2O2 are used to construct a Fenton-like system, the pH value of the system is adjusted to 6.5, and 10 mg / L of nitrobenzene is oxidatively degraded at room temperature (25 °C), so as to investigate the pollutant treatment efficiency of the PDA@MoN-Fe III -H2O2 system. The oxidative degradation effect of phenol is shown in Table 3, wherein the concentration determination method of nitrobenzene is as shown in Example 2.
[0069] Table 6: Oxidative degradation of nitrobenzene by PDA@MoN-Fe III -H2O2 system
[0070]
[0071] As shown in Table 7, the removal rate of nitrobenzene in the Fenton-like system formed by PDA@MoN-Fe III -H2O2 can reach 81.3% at 60 min of reaction, which shows that the Fenton-like technology proposed in the application has good degradation and removal capacity for small-molecule organic pollutants in water.
[0072] Example 8
[0073] MoN MXene is prepared as in Example 1, then 0.6 g of MoN is ultrasonically dispersed in 300 mL of ultrapure water, and 0.4 g of dopamine is added to the system, the pH of the system is adjusted to 8.0 by using hydrochloride-Tris buffer reagent, the dopamine is polymerized on the surface of MXene by fully stirring, after 8 h of reaction, standing, removing the supernatant, and repeatedly washing the obtained material with ultrapure water, PDA@MoN is obtained by vacuum freeze-drying. And 0.3 g / L of PDA@MoN, 20 mM of Fe III and 10 mM of H2O2 are used to construct a Fenton-like system, the pH value of the system is adjusted to 10.0, and 2 mg / L of EDTA-Ni is removed by breaking the complex at room temperature (25 °C), so as to investigate the pollutant treatment efficiency of the PDA@MoN-FeIII The pollutant treatment efficiency of the H2O2 system. The oxidative removal effect of EDTA-Ni is shown in Table 5, wherein the concentration of EDTA-Ni is determined by using a high-performance liquid chromatograph (Waters 1525, USA), and the concentration of NiII ions is determined by using an atomic absorption spectrophotometer.
[0074] Table 7: PDA@MoN-Fe III -H2O2 system breaks the complex to remove EDTA-Ni
[0075]
[0076] As shown in Table 7, PDA@MoN-Fe III The degradation rate of EDTA-Ni in the system is as high as 98.3% when the Fenton-like system formed by H2O2 reacts for 120 min, and the complex breaking efficiency of complexed Ni can reach 85.9%. It is shown that the Fenton-like technology proposed in the application can effectively realize the complex breaking and removal of complexed heavy metals in water bodies.
[0077] In summary, the application is based on a polydopamine (PDA) modified MXene (transition metal nitride) cocatalyst. The PDA and MXene have strong coordination ability and electronic conductivity for high-charged iron ions. The free FeIII in the liquid phase is anchored on the surface of the cocatalyst and activated in situ, thereby releasing Fe II Catalyze hydrogen peroxide (H2O2) to generate various reactive oxygen species (ROSs). The Fenton-like system has extremely high Fe III / Fe II Cyclic conversion efficiency, which can effectively expand the pH range of the system, improve the utilization efficiency of H2O2, and does not generate iron sludge, greatly improving the oxidation and degradation ability of homogeneous Fenton-like system for water organic pollutants and the potential for practical application. The degradation complex can efficiently treat various water organic pollutants, including antibiotics (90%-98%), organic dyes (94%-99%), chemical industrial preparations (74%-81%), and complexed heavy metals (85%-98%). The pH range is widely applicable (3.0-10.0), and no iron sludge is generated during the reaction process.
Claims
1. A PDA@MoN activated Fe III The preparation method of a Fenton-type driving reaction system is characterized in that: The steps are: MXene was ultrasonically dispersed in ultrapure water for 1-2 hours. The concentration of MXene was 1-10 mg / mL. Dopamine was added. The mass ratio of MXene to dopamine was 5-2:
1. The pH of the solution was adjusted to 8.
0. The solution was stirred thoroughly to allow dopamine to polymerize on the surface of MXene. After the reaction was allowed to stand for 4-5 hours, the supernatant was removed. The obtained material was repeatedly washed with ultrapure water to remove impurities and then freeze-dried in vacuum to obtain PDA@MoN; PDA@MoN, Fe III and H2O2 in a mass ratio of 1:1:1 to form a Fenton-like reaction system; The MXene is molybdenum nitride, which is a stable layered structure formed by alternating stacking of transition metal layers and nitrogen atomic layers through covalent bonding.
2. A PDA@MoN activated Fe according to claim 1 III The preparation method of a Fenton-type driving reaction system is characterized in that: The preparation method of Mxene is as follows: (NH4)4Mo7O 24 4H2O is dissolved in ultrapure water to form 0.05-1.0 mM Mo 4+ ion solution, and simultaneously prepare 0.01-1.0 g / L hexamethylenetetramine solution, mix the two in equal volumes thoroughly and let it stand for 5-7 hours. After observing the formation of colorless crystals, remove the supernatant, slowly rinse the resulting crystals with ultrapure water to remove impurities, and dry at 60°C to obtain a precursor; the resulting precursor is calcined at 400°C with ammonia gas continuously introduced for 5-7 hours to obtain Mxene.
3. A PDA@MoN activated Fe according to claim 1 III The preparation method of a Fenton-type driving reaction system is characterized in that: The reagent for adjusting the pH of the solution is hydrochloride-Tris buffer.
4. Use of a Fenton-like reaction system prepared by the preparation method of claim 1 in pollutant treatment.
5. The use according to claim 4, characterized in that The Fenton-like reaction system is used for degrading antibiotics, organic dyes and complexed heavy metals.
6. The use according to claim 4, characterized in that The Fenton-like reaction system is used for degrading chemical industrial preparations.
7. The use according to claim 5, characterized in that The applicable pH range of the Fenton-like reaction system is 3.0-10.0, and no iron sludge is generated during the degradation reaction.
Citation Information
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