CN114100657B - alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 /MXene material and preparation method and application thereof - Google Patents
alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 /MXene material and preparation method and application thereof Download PDFInfo
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- 229910017771 LaFeO Inorganic materials 0.000 title claims abstract description 157
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- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/24—Nitrogen compounds
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- 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
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- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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- C02F1/30—Treatment of water, waste water, or sewage by irradiation
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Abstract
The invention provides alpha-Fe 2 O 3 /LaFeO 3 /g‑C 3 N 4 A/MXene material and a preparation method and application thereof belong to the technical field of photocatalysis. The invention combines two narrow band gap semiconductors (LaFeO) 3 And alpha-Fe 2 O 3 ) With a wide band gap semiconductor (g-C) 3 N 4 ) The double heterojunction is formed by compounding, so that the response range of sunlight can be widened, the separation of photoinduced electrons and holes can be promoted, the redox capability is improved, and meanwhile, the metal MXene material is compounded on the surface of the material, so that the conductivity of the material is increased, the photon-generated carriers are separated, and the photocatalytic performance of the whole system is greatly improved. The photocatalyst is used for treating polluted wastewater, has excellent capability of removing organic pollutants and heavy metal ions, and has good removal effect on methylene blue, rhodamine B, tetracycline hydrochloride, heavy metal hexavalent chromium and the like.
Description
Technical Field
The invention relates to the technical field of photocatalysis, in particular to alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 A/MXene material and a preparation method and application thereof.
Background
Due to rapid industrialization and population growth, energy crisis and environmental pollution have become two major challenges facing today's society. Groundwater is an important component of water resources and has a significant impact on human production and life. However, with the progress of industrialization and urbanization, underground water resources in China are polluted to different degrees, and the discharge of industrial wastewater not only causes serious underground water pollution, but also indirectly harms human health. The photocatalysis technology is a pollutant treatment technology which integrates the advantages of high efficiency, energy conservation, simple and convenient operation, mild reaction conditions and the like. Therefore, the development of a simple and efficient photocatalyst for removing pollutants in water is urgently needed.
Solar energy is a renewable energy source with abundant reserves, low cost, cleanness and no pollution, and is attracted by people. In 1972, scientists Fujishima and Honda, tokyo university, japan, discovered TiO 2 Can electrolyze water under the irradiation of ultraviolet light to generate H 2 And O 2 . Since then, efforts have been made to design and develop semiconductor photocatalysts that can efficiently collect solar energy and convert it into chemical fuels. However, the single semiconductor photocatalyst has a wide forbidden band, and photo-generated electrons and holes are easy to recombine, so that the photocatalytic performance is poor.
Disclosure of Invention
The invention aims to provide alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 /MXene material, preparation method and application thereof, and alpha-Fe provided by the invention 2 O 3 /LaFeO 3 /g-C 3 N 4 the/MXene material has good photocatalytic performance as a catalyst.
In order to achieve the above object, the present invention provides the following technical solutions:
the invention provides alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The preparation method of the/MXene material comprises the following steps:
mixing lanthanum nitrate, ferric nitrate, water, citric acid and glycol, forming wet gel under the water bath heating condition, drying the wet gel to obtain dry gel, and calcining the dry gel to obtain alpha-Fe 2 O 3 /LaFeO 3 (ii) a Said calcinedThe temperature is 900 ℃;
subjecting the alpha-Fe to a reaction 2 O 3 /LaFeO 3 And g-C 3 N 4 Mixing the dispersion liquid, and carrying out solvothermal reaction on the obtained mixed liquid to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 ；
Subjecting the alpha-Fe to a reaction 2 O 3 /LaFeO 3 /g-C 3 N 4 Protonating to obtain protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 ；
Protonating the protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing in water, mixing the obtained dispersion with MXene dispersion, and performing solid-liquid separation to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The material of/MXene.
Preferably, the molar ratio of lanthanum nitrate to ferric nitrate to citric acid is 0.85; the molar ratio of ethylene glycol to citric acid is 1:1.
Preferably, the calcination is carried out with a holding time of 2 hours.
Preferably, the alpha-Fe 2 O 3 /LaFeO 3 And g-C 3 N 4 The mass ratio of (1) is 10.
Preferably, the temperature of the solvothermal reaction is 120 ℃, and the holding time is 6 hours.
Preferably, the protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 And MXene in a mass ratio of 10.
Preferably, MXene is Ti 3 C 2 Said Ti 3 C 2 Is less than 5 layers.
Preferably, the protonation comprises: alpha-Fe is mixed 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing in hydrochloric acid, sequentially performing ultrasonic treatment and stirring, and drying to obtain protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 (ii) a The concentration of the hydrochloric acid is 0.4mol/L.
The invention provides alpha-Fe prepared by the preparation method in the scheme 2 O 3 /LaFeO 3 /g-C 3 N 4 The material of/MXene.
The invention provides the alpha-Fe in the scheme 2 O 3 /LaFeO 3 /g-C 3 N 4 The application of the/MXene material as a photocatalyst in photocatalytic treatment of polluted wastewater.
The invention provides alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The preparation method of the/MXene material comprises the following steps: mixing lanthanum nitrate, ferric nitrate, water, citric acid and glycol, forming wet gel under the water bath heating condition, drying the wet gel to obtain dry gel, and calcining the dry gel to obtain alpha-Fe 2 O 3 /LaFeO 3 (ii) a The calcining temperature is 900 ℃; subjecting the alpha-Fe to a reaction 2 O 3 /LaFeO 3 And g-C 3 N 4 Mixing the dispersion liquid, and carrying out solvothermal reaction on the obtained mixed liquid to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 (ii) a Subjecting the alpha-Fe to a reaction 2 O 3 /LaFeO 3 /g-C 3 N 4 Protonating to obtain protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 (ii) a Protonating the protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing in water, mixing the obtained dispersion with MXene dispersion, and performing solid-liquid separation to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The material of/MXene.
The invention combines two semiconductors (LaFeO) with narrow band gap 3 And alpha-Fe 2 O 3 ) With a wide band gap semiconductor (g-C) 3 N 4 ) The double heterojunction is formed by compounding, the response range of sunlight can be widened, the separation of photoinduced electrons and holes can be promoted, the redox capability is improved, and meanwhile, the metalloid MXene material is compounded on the surface of the material, so that the conductivity of the material is increased, the photogenerated carriers are separated, and the material is largeGreatly improves the photocatalytic performance of the whole system.
alpha-Fe of the invention 2 O 3 /LaFeO 3 /g-C 3 N 4 the/MXene material is used as a photocatalyst for treating polluted wastewater, has excellent capability of removing organic pollutants and heavy metal ions, and has good removal effect on Methylene Blue (MB), rhodamine B (RhB), tetracycline hydrochloride (TC), heavy metal hexavalent chromium (Cr (VI)), and the like.
Drawings
FIG. 1 shows g-C 3 N 4 、LaFeO 3 、α-Fe 2 O 3 /LaFeO 3 And alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 、α-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 XRD pattern of/MXene material;
FIG. 2 is a view of alpha-Fe 2 O 3 /LaFeO 3 And alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 SEM image of/MXene material;
FIG. 3 is a diagram showing the effect of different catalysts on the removal of methylene blue, rhodamine B, tetracycline hydrochloride and the heavy metal hexavalent chromium.
Detailed Description
The invention provides alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The preparation method of the/MXene material comprises the following steps:
mixing lanthanum nitrate, ferric nitrate, water, citric acid and glycol, forming wet gel under the water bath heating condition, drying the wet gel to obtain dry gel, and calcining the dry gel to obtain alpha-Fe 2 O 3 /LaFeO 3 (ii) a The calcining temperature is 900 ℃;
subjecting the alpha-Fe to a reaction 2 O 3 /LaFeO 3 And g-C 3 N 4 Mixing the dispersion liquid, and carrying out solvothermal reaction on the obtained mixed liquid to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 ；
Subjecting the alpha-Fe to a reaction 2 O 3 /LaFeO 3 /g-C 3 N 4 Protonating to obtain protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 ；
Protonating the protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing in water, mixing the obtained dispersion with MXene dispersion, and performing solid-liquid separation to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The material of/MXene.
In the present invention, the starting materials used are all commercially available products well known in the art, unless otherwise specified.
Lanthanum nitrate, ferric nitrate, water, citric acid and glycol are mixed to form wet gel under the water bath heating condition, the wet gel is dried to obtain dry gel, and the dry gel is calcined to obtain alpha-Fe 2 O 3 /LaFeO 3 。
In the present invention, the lanthanum nitrate is preferably La (NO) 3 ) 3 ·xH 2 O, the ferric nitrate is preferably Fe (NO) 3 ) 3 ·9H 2 And O. In the present invention, the citric acid functions as a complexing agent to form a complex with the metal, and the ethylene glycol is advantageous to make the prepared particles finer.
In the present invention, mixing lanthanum nitrate, iron nitrate, water, citric acid and ethylene glycol preferably comprises: lanthanum nitrate and ferric nitrate are dissolved in water, then citric acid is added into the obtained mixed solution, after the citric acid is completely dissolved, ethylene glycol is added, and the mixture is stirred for 1 hour at room temperature.
In the present invention, the molar ratio of lanthanum nitrate, ferric nitrate and citric acid is preferably 0.85; the molar ratio of ethylene glycol to citric acid is preferably 1:1. the invention has no special requirement on the dosage of the water, and can completely dissolve the lanthanum nitrate, the ferric nitrate and the citric acid.
In the present invention, the temperature of the water bath heating is preferably 80 ℃, and the water bath heating is preferably carried out under stirring in the present invention. The invention has no special requirement on the time of water bath heating, and the water bath heating is stopped until a red brown wet gel is formed.
After the wet gel is formed, the wet gel is dried to obtain the dry gel. In the present invention, the temperature of the drying is preferably 120 ℃, and the time of the drying is preferably 24 hours.
After obtaining the xerogel, the invention calcines the xerogel to obtain alpha-Fe 2 O 3 /LaFeO 3 . The xerogel is preferably ground into powder and then calcined. In the present invention, the calcination temperature is 900 ℃, and the holding time is preferably 2 hours. The invention controls the calcining temperature to ensure that the perovskite La 0.85 FeO 3-δ Oxygen defects in the perovskite are aggregated, and then alpha-Fe is formed through enrichment in the perovskite 2 O 3 Finally form alpha-Fe 2 O 3 /LaFeO 3 A composite material.
To obtain alpha-Fe 2 O 3 /LaFeO 3 Then, the invention uses the alpha-Fe 2 O 3 /LaFeO 3 And g-C 3 N 4 Mixing the dispersion liquid, and carrying out solvothermal reaction on the obtained mixed liquid to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 。
In the present invention, the alpha-Fe 2 O 3 /LaFeO 3 The dispersant used in the dispersion of (3) is preferably ethanol. The invention has no special requirement on the dosage of the ethanol, and can convert alpha-Fe into alpha-Fe 2 O 3 /LaFeO 3 Dispersing uniformly. In the examples of the present invention, for 100mg of alpha-Fe 2 O 3 /LaFeO 3 The amount of ethanol used was 40mL. For alpha-Fe 2 O 3 /LaFeO 3 The preparation method of the dispersion liquid has no special requirements, and the alpha-Fe is directly prepared 2 O 3 /LaFeO 3 Adding into ethanol, and ultrasonically dispersing for 30 min.
In the present invention, the g-C 3 N 4 The dispersant used in the dispersion of (3) is preferably ethanol. The invention has no special requirements on the dosage of the ethanol, and g-C can be added 3 N 4 Dispersing uniformly. In the practice of the inventionIn the examples, 30mg of g-C was targeted 3 N 4 The amount of ethanol used was 40mL. Invention pair g-C 3 N 4 The dispersion of (A) is prepared by directly mixing g-C 3 N 4 Adding into ethanol, and ultrasonically dispersing for 30 min.
In the present invention, the g-C 3 N 4 Preferably by preparation, of said g-C 3 N 4 The preparation method of (A) is not particularly required, and a preparation method well known in the art can be adopted. In the examples of the present invention, the g-C 3 N 4 The preparation steps are as follows: putting melamine powder into a crucible, covering the crucible with a cover, heating to 550 ℃ in a muffle furnace at the speed of 5 ℃/min in the air atmosphere, and preserving the temperature for 4 hours to obtain yellow blocky g-C 3 N 4 (ii) a Subjecting the block g-C to 3 N 4 Grinding, heating the obtained powder to 500 ℃ in air atmosphere, and keeping the temperature for 2 hours at the heating rate of 5 ℃/min to obtain light yellow g-C with a nanosheet structure 3 N 4 。
In the present invention, the α -Fe is added 2 O 3 /LaFeO 3 And g-C 3 N 4 The dispersion mixing of (a) preferably comprises: subjecting the alpha-Fe to a reaction 2 O 3 /LaFeO 3 Is added dropwise to g-C 3 N 4 The dispersion of (3) was stirred for 12 hours. The invention has no special requirement on the dropping speed, and the dropping can be carried out drop by drop. The present invention does not require any particular speed of agitation, and can employ agitation speeds well known in the art. The invention realizes alpha-Fe by dropwise adding 2 O 3 /LaFeO 3 And g-C 3 N 4 And (4) uniformly mixing.
In the present invention, the alpha-Fe 2 O 3 /LaFeO 3 And g-C 3 N 4 Is preferably 10.
In the present invention, the solvothermal reaction is preferably carried out in a polytetrafluoroethylene reaction vessel. In the present invention, the temperature of the solvothermal reaction is preferably 120 ℃ and the incubation time is preferably 6 hours. The invention adopts the solvent thermal reactionIn the process, g-C 3 N 4 Uniformly grown in alpha-Fe 2 O 3 /LaFeO 3 The surfaces form chemical bonds with the surfaces and are tightly combined together.
After the solvothermal reaction is finished, the obtained reaction product system is cooled, then water and ethanol are alternately washed, centrifuged and dried overnight in a drying oven at the temperature of 80 ℃ to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 。
To obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Then, the invention uses the alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Protonating to obtain protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 。
In the present invention, the protonation preferably includes: alpha-Fe is mixed 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing in hydrochloric acid, sequentially performing ultrasonic treatment and stirring, and drying to obtain protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 . In the present invention, the concentration of the hydrochloric acid is preferably 0.4mol/L; the alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 And the amount ratio of hydrochloric acid is preferably 100mg:100mL. In the present invention, the time of the ultrasonic treatment is preferably 2 hours, and the time of the stirring is preferably 4 hours. The invention has no special requirements on the power of the ultrasound and the stirring speed. After the stirring is completed, the obtained alpha-Fe is preferably mixed in the invention 2 O 3 /LaFeO 3 /g-C 3 N 4 Washed to be neutral and then dried. In the present invention, the drying is preferably performed for 12 hours under vacuum at 60 ℃. The invention uses protonation to lead alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The powder surface is positively charged and thus assembled with negatively charged MXene by electrostatic adsorption.
Obtaining protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Then, the present invention converts the protonation α-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing in water, mixing the obtained dispersion with MXene dispersion, and performing solid-liquid separation to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The material of/MXene.
The invention preferably treats the alpha-Fe under ultrasonic conditions 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersed in water. The invention has no special requirement on the dosage of the water and can convert alpha-Fe into alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing uniformly.
In the present invention, the concentration of the MXene dispersion is preferably 5mg/mL. In the present invention, the dispersant of the MXene dispersion is preferably water.
In the present invention, the MXene preferably comprises Ti 3 C 2 Said Ti 3 C 2 Preferably less than 5 layers. In the present invention, the protonated α -Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 And MXene are preferably in a mass ratio of 10.
In the present invention, the obtained α -Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The dispersion of (3) is preferably mixed with the dispersion of MXene: dropwise adding MXene dispersion to alpha-Fe under the stirring condition of ice-water bath 2 O 3 /LaFeO 3 /g-C 3 N 4 The dispersion of (4) was magnetically stirred for 12 hours. The invention is mixed under the condition of ice-water bath to prevent MXene from oxidative decomposition at normal temperature. In the mixing process, the alpha-Fe with positive charges on the surface 2 O 3 /LaFeO 3 /g-C 3 N 4 And MXene with negative charges are assembled together through electrostatic adsorption.
The invention has no special requirement on the solid-liquid separation mode, and the solid-liquid separation mode which is well known in the field, such as centrifugation, can be adopted.
After solid-liquid separation, the solid obtained is preferably dried in vacuum to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The material of/MXene. In the present invention, the temperature of the vacuum drying is preferably 60 ℃, and the time of the vacuum drying is preferably 12 hours.
The invention provides alpha-Fe prepared by the preparation method in the scheme 2 O 3 /LaFeO 3 /g-C 3 N 4 a/MXene material comprising alpha-Fe 2 O 3 、LaFeO 3 、g-C 3 N 4 And MXene. In the present invention, the alpha-Fe 2 O 3 In-situ grown in LaFeO 3 Surface of alpha-Fe 2 O 3 /LaFeO 3 (ii) a The g to C 3 N 4 Growth on alpha-Fe by solvothermal method 2 O 3 /LaFeO 3 Surface of alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 (ii) a The alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Is adsorbed together with MXene through electrostatic interaction to form alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 a/MXene material. In the present invention, the α -Fe 2 O 3 /LaFeO 3 The diameter of (A) is preferably 80 to 120nm. In the present invention, the LaFeO 3 The crystal system of (A) is a monoclinic perovskite crystal system.
The invention combines two semiconductors (LaFeO) with narrow band gap 3 And alpha-Fe 2 O 3 ) With a wide band gap semiconductor (g-C) 3 N 4 ) The double heterojunction is formed by compounding, the response range of sunlight can be widened, the separation of photoinduced electrons and holes can be promoted, the oxidation reduction capability is improved, meanwhile, the metalloid MXene material is compounded on the surface of the material, and the two-dimensional MXene material has similar metallicity, so that electrons can be captured, the electron transmission performance is improved, hole electron pairs are separated, the conductivity of the material is increased, photocarriers are separated, and the photocatalysis performance of the whole system is greatly improved.
The invention provides the alpha-Fe in the scheme 2 O 3 /LaFeO 3 /g-C 3 N 4 The application of the/MXene material as a photocatalyst in photocatalytic treatment of polluted wastewater.
In the present invention, the polluted wastewater is preferably organic pollutant wastewater and/or heavy metal wastewater, and the organic pollutants in the organic pollutant wastewater preferably comprise one or more of methylene blue, rhodamine B and tetracycline hydrochloride; the heavy metal in the heavy metal wastewater preferably comprises heavy metal hexavalent chromium. The concentration of the contaminant is not particularly required by the present invention, and in the examples of the present invention, is specifically 10mg/mL.
In the present invention, the photocatalysis is preferably carried out under visible light. In the embodiment of the invention, a 300W xenon lamp is adopted and a filter plate (lambda is more than 420 nm) is installed to simulate visible light.
The following examples are given to provide alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 the/MXene materials and their preparation and use are described in detail but they should not be construed as limiting the scope of the invention.
Example 1
Taking 1.105g La (NO) 3 ) 3 ·xH 2 O with 1.616g Fe (NO) 3 ) 3 ·9H 2 Adding 100mL of deionized water into the solution, stirring the solution for dissolving, then adding 2.6g of citric acid into the mixed solution, adding 2mL of ethylene glycol after dissolving, stirring the solution for 1 hour at room temperature, heating the mixed solution in a water bath at 80 ℃ and magnetically stirring the solution to form a red brown wet sol, drying the wet sol at 120 ℃ for 24 hours to form dry gel, grinding the dry gel into powder, calcining the powder at 900 ℃ for 2 hours to obtain alpha-Fe 2 O 3 /LaFeO 3 。
Putting melamine powder into a crucible, covering the crucible, heating the melamine powder to 550 ℃ in a muffle furnace in the air atmosphere at the speed of 5 ℃/min, and then preserving the heat for 4 hours to obtain yellow block-shaped g-C 3 N 4 Mixing the blocks g-C 3 N 4 Grinding into powder, and mixing the powder with the block g-C 3 N 4 The powder is kept at 500 ℃ for 2 hours in the air atmosphere, the heating rate is 5 ℃/min, and light yellow g-C with a nano lamellar structure is obtained 3 N 4 And (3) powder.
Taking 100mg of alpha-Fe 2 O 3 /LaFeO 3 And 30mg g-C 3 N 4 The powder is respectively dispersed in 40mL ethanol and is subjected to ultrasonic treatment for 30 minutes to obtain alpha-Fe 2 O 3 /LaFeO 3 And g-C 3 N 4 And then dispersing alpha-Fe 2 O 3 /LaFeO 3 Is added dropwise to g-C 3 N 4 The solution is poured into a 100mL polytetrafluoroethylene reaction kettle, the solvent at 120 ℃ undergoes a thermal reaction for 6 hours, then the solution is cooled, alternately washed by water and ethanol, centrifuged and dried in a drying oven at 80 ℃ overnight to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 And (3) powder.
Taking 100mg of alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing in 100mL 0.4mol/L hydrochloric acid, ultrasonic stirring for 2 hours, magnetic stirring for 4 hours, washing to neutrality, and vacuum drying at 60 ℃ for 12 hours to obtain protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 And (3) powder.
Protonating 20mg of alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing the powder in 100mL deionized water by ultrasonic for 30 minutes, and dropwise adding 0.8mL of 5 mg/mL-concentration small-layer Ti 3 C 2 Magnetically stirring the solution in ice-water bath for 12 hours, centrifugally separating the obtained product, and then drying the product in vacuum at 60 ℃ for 12 hours to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The material of/MXene.
Structural characterization:
for g-C 3 N 4 、LaFeO 3 、α-Fe 2 O 3 /LaFeO 3 And alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 、α-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 the/MXene materials were separately subjected to X-ray diffraction analysis, and the results are shown in FIG. 1. In FIG. 1, the perovskite LaFeO 3 Has a diffraction peak matching with that of a standard PDF card (JCPDS No. 37-1493) and has no other diffraction peak except that, which shows that LaFeO 3 Sample only existsPhase of perovskite structure, indicating the synthesized LaFeO 3 The samples were pure monoclinic perovskite phases. And alpha-Fe in FIG. 1 2 O 3 /LaFeO 3 Not only has corresponding perovskite LaFeO 3 The diffraction peak of (2) can also find alpha-Fe 2 O 3 The peak diffraction peak of (A) was matched with that of a standard PDF card (JCPDS No. 33-0664), indicating that alpha-Fe 2 O 3 /LaFeO 3 Is made of perovskite LaFeO 3 And alpha-Fe 2 O 3 Two phases are formed. In the complex alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 In (B), not only LaFeO can be observed 3 And alpha-Fe 2 O 3 The diffraction peak of (A) can be clearly seen, and g-C can be also clearly seen 3 N 4 The (002) crystal face corresponding to the strong diffraction peak at 27.4 degrees indicates that the invention successfully synthesizes alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 And (c) a complex.
Scanning electron microscopy on alpha-Fe 2 O 3 /LaFeO 3 And alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The morphology of the/MXene material is characterized, and the result is shown in FIG. 2. In FIG. 2, (a) is. Alpha. -Fe 2 O 3 /LaFeO 3 SEM picture of (b) is alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 SEM image of/MXene material; from FIG. 2 (a), alpha-Fe can be seen 2 O 3 /LaFeO 3 Is formed by the mutual connection of nano particles, alpha-Fe 2 O 3 /LaFeO 3 The nano particles are small in size and about 100nm in diameter. As can be seen from FIG. 2 (b), the small nanoparticles are uniformly coated with g-C 3 N 4 And MXene.
α-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The MXene photocatalysis performance test:
application examples 1 to 4
A300W xenon lamp is used as a visible light source and is arranged right above the reaction device. The reaction device is arranged on the magnetic stirrer to keep a stirring state and is connected with the cooling circulating water to ensure the light degradationThe assay was performed at 22 ℃ at room temperature. 60mL of 10mg/L pollutant solution (the pollutants in application examples 1-4 are respectively Methylene Blue (MB), rhodamine B (RhB), tetracycline hydrochloride (TC) and heavy metal hexavalent chromium (Cr (VI))) is put into a reactor, 20mg of catalyst is added, and the reactor is wrapped by tinfoil and stirred for 30min in a dark adsorption mode to achieve absorption and desorption balance. Then, a light source is turned on, 4mL of solution is taken at regular intervals under the irradiation of visible light, the catalyst is centrifugally separated, and the degradation condition of the catalyst to the dye under the irradiation of the visible light, namely the change of the dye concentration (C) in the photocatalytic performance test, is researched by researching the absorbance (A) of the obtained liquid. The conversion formula between them is C/C 0 ＝A/A 0 In which C is 0 Representing the initial concentration of the contaminant after dark adsorption before illumination, C representing the real-time concentration of the contaminant after reaction for a corresponding time, A 0 The initial absorbance of the contaminant before illumination after dark adsorption is indicated, and A represents the real-time concentration of the contaminant after the reaction for the corresponding time.
For comparison of catalytic performance, laFeO was also used 3 、α-Fe 2 O 3 /LaFeO 3 And alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The catalytic performance of the catalyst is tested, the testing method is the same as that of application examples 1-4, the catalytic performance of different catalysts is shown in figure 3, and specific data corresponding to figure 3 are shown in tables 1-4.
In FIG. 3, (a) catalyst degrades MB; (b) catalyst degradation RhB; (c) catalyst degradation TC; (d) catalyst degradation of Cr (VI); in FIG. 3, blank represents a Blank control group, and CN represents g-C 3 N 4 L represents LaFeO 3 And alpha L represents alpha-Fe 2 O 3 /LaFeO 3 And alpha LC represents alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 And alpha LCM represents alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The material of/MXene.
As can be seen from FIG. 3, laFeO 3 、α-Fe 2 O 3 /LaFeO 3 、α-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 And alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The degradation performance of the/MXene material shows an increasing trend. LaFeO 3 Exhibits weak photocatalytic performance under visible light when LaFeO is used 3 Growing alpha-Fe in situ 2 O 3 Of alpha-Fe 2 O 3 /LaFeO 3 The photocatalytic performance of the photocatalyst is improved to a certain extent. When in alpha-Fe 2 O 3 /LaFeO 3 Surface recombination of g-C 3 N 4 And a double heterojunction is formed, so that the transition of a photon-generated carrier is greatly improved, and the photocatalytic performance of a sample is improved. In the presence of alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Surface recombination of MXene to form alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The MXene material has the largest catalytic performance, and the MB is degraded to 91.3 percent in 40min and is pure LaFeO 3 6.6 times of the total weight; the RhB is degraded at 180min to 85.5 percent and is pure LaFeO 3 3.9 times of; the degradation TC reaches 87.2 percent in 60min and is pure LaFeO 3 6.2 times of the total weight; cr (VI) degraded in 60min reaches 71.6 percent and is pure LaFeO 3 2.83 times of.
TABLE 1 degradation Effect of the catalysts on Methylene Blue (MB)
| Sample (I) | Is free of | CN | L | αL | αLC | |
| Degradation rate | ||||||
| 0％ | 13.21％ | 13.89％ | 31.36％ | 87.38％ | 91.28％ |
TABLE 2 degradation Effect of each catalyst on rhodamine B (RhB)
| Sample (I) | Is free of | CN | L | αL | αLC | αLCM |
| Rate of |
0％ | 1.34％ | 2.45％ | 12.37％ | 67.39％ | 84.42％ |
TABLE 3 degradation Effect of each catalyst on Tetracycline hydrochloride (TC)
| Sample (I) | Is free of | CN | L | αL | αLC | αLCM |
| Rate of |
0％ | 10.31％ | 13.90％ | 19.59％ | 31.49％ | 86.11％ |
TABLE 4 degradation Effect of the catalysts on Cr (VI)
| Sample(s) | Is free of | CN | L | αL | αLC | |
| Degradation rate | ||||||
| 0％ | 18.39％ | 24.24％ | 28.22％ | 49.49％ | 91.60 |
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.
Claims (6)
1. alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The application of the/MXene material in photocatalytic degradation of hexavalent chromium is characterized in that the alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 The preparation method of the/MXene material comprises the following steps:
mixing lanthanum nitrate, ferric nitrate, water, citric acid and glycol, forming wet gel under the condition of water bath heating, drying the wet gel,obtaining dry gel, calcining the dry gel to obtain alpha-Fe 2 O 3 /LaFeO 3 (ii) a The calcining temperature is 900 ℃;
subjecting the alpha-Fe to a reaction 2 O 3 /LaFeO 3 And g-C 3 N 4 Respectively dispersing the mixture into ethanol to obtain alpha-Fe 2 O 3 /LaFeO 3 And g-C 3 N 4 The dispersion of (4);
subjecting the alpha-Fe to a reaction 2 O 3 /LaFeO 3 And g-C 3 N 4 Mixing the dispersion liquid, and carrying out solvothermal reaction on the obtained mixed liquid to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 (ii) a The alpha-Fe 2 O 3 /LaFeO 3 And g-C 3 N 4 The mass ratio of (A) to (B) is 10;
subjecting the alpha-Fe to 2 O 3 /LaFeO 3 /g-C 3 N 4 Protonating to obtain protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 ；
Protonating the protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing in water, mixing the obtained dispersion with MXene dispersion, and performing solid-liquid separation to obtain alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 a/MXene material; the protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 And MXene in a mass ratio of 10;
the g to C 3 N 4 The preparation steps are as follows: putting melamine powder into a crucible, covering the crucible, heating to 550 ℃ in a muffle furnace at the speed of 5 ℃/min under the air atmosphere, and preserving the heat for 4 hours to prepare yellow blocky g-C 3 N 4 (ii) a Mixing the blocks g-C 3 N 4 Grinding, heating the obtained powder to 500 ℃ in air atmosphere, and keeping the temperature for 2 hours at the heating rate of 5 ℃/min to obtain light yellow g-C with a nanosheet structure 3 N 4 。
2. The use according to claim 1, wherein the molar ratio of lanthanum nitrate, ferric nitrate and citric acid is 0.85; the molar ratio of ethylene glycol to citric acid is 1:1.
3. Use according to claim 1, characterized in that the calcination is carried out with a holding time of 2 hours.
4. Use according to claim 1, wherein the solvothermal reaction is carried out at a temperature of 120 ℃ and for a holding time of 6 hours.
5. Use according to claim 1, wherein MXene is Ti 3 C 2 Said Ti 3 C 2 Is less than 5 layers.
6. Use according to claim 1, characterized in that the protonation comprises: alpha-Fe is mixed 2 O 3 /LaFeO 3 /g-C 3 N 4 Dispersing in hydrochloric acid, sequentially performing ultrasonic treatment and stirring, and drying to obtain protonated alpha-Fe 2 O 3 /LaFeO 3 /g-C 3 N 4 (ii) a The concentration of the hydrochloric acid is 0.4mol/L.
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