CN114733523A - Preparation method and application of iron monatomic catalyst - Google Patents
Preparation method and application of iron monatomic catalyst Download PDFInfo
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 60
- 239000003054 catalyst Substances 0.000 title claims abstract description 29
- 229910052742 iron Inorganic materials 0.000 title claims abstract description 25
- 238000002360 preparation method Methods 0.000 title claims abstract description 10
- 238000000034 method Methods 0.000 claims abstract description 25
- 230000004913 activation Effects 0.000 claims abstract description 13
- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 claims abstract description 12
- 230000003197 catalytic effect Effects 0.000 claims abstract description 6
- 238000006731 degradation reaction Methods 0.000 claims description 26
- WBZFUFAFFUEMEI-UHFFFAOYSA-M Acesulfame k Chemical compound [K+].CC1=CC(=O)[N-]S(=O)(=O)O1 WBZFUFAFFUEMEI-UHFFFAOYSA-M 0.000 claims description 25
- 230000015556 catabolic process Effects 0.000 claims description 24
- 239000000619 acesulfame-K Substances 0.000 claims description 20
- 235000010358 acesulfame potassium Nutrition 0.000 claims description 19
- 229960004998 acesulfame potassium Drugs 0.000 claims description 17
- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(3+);trinitrate Chemical compound [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 claims description 16
- 239000006229 carbon black Substances 0.000 claims description 14
- 229960005164 acesulfame Drugs 0.000 claims description 10
- YGCFIWIQZPHFLU-UHFFFAOYSA-N acesulfame Chemical compound CC1=CC(=O)NS(=O)(=O)O1 YGCFIWIQZPHFLU-UHFFFAOYSA-N 0.000 claims description 10
- 238000003756 stirring Methods 0.000 claims description 10
- 229910021642 ultra pure water Inorganic materials 0.000 claims description 10
- 239000012498 ultrapure water Substances 0.000 claims description 10
- 239000000203 mixture Substances 0.000 claims description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 8
- 239000008122 artificial sweetener Substances 0.000 claims description 7
- 235000021311 artificial sweeteners Nutrition 0.000 claims description 7
- 239000012692 Fe precursor Substances 0.000 claims description 6
- 238000002156 mixing Methods 0.000 claims description 6
- 239000000725 suspension Substances 0.000 claims description 6
- 230000008569 process Effects 0.000 claims description 5
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 4
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 4
- 239000004202 carbamide Substances 0.000 claims description 4
- 229910017604 nitric acid Inorganic materials 0.000 claims description 4
- 239000000843 powder Substances 0.000 claims description 4
- 238000001132 ultrasonic dispersion Methods 0.000 claims description 4
- 230000000593 degrading effect Effects 0.000 claims description 3
- 241000872198 Serjania polyphylla Species 0.000 claims description 2
- 239000012736 aqueous medium Substances 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims description 2
- 239000002904 solvent Substances 0.000 claims description 2
- 238000002336 sorption--desorption measurement Methods 0.000 claims description 2
- 239000000463 material Substances 0.000 abstract description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract description 6
- 229910052751 metal Inorganic materials 0.000 abstract description 5
- 239000002184 metal Substances 0.000 abstract description 5
- 150000002500 ions Chemical class 0.000 abstract description 4
- 238000000197 pyrolysis Methods 0.000 abstract description 4
- 239000003344 environmental pollutant Substances 0.000 abstract description 2
- 230000003993 interaction Effects 0.000 abstract description 2
- 239000002923 metal particle Substances 0.000 abstract description 2
- 125000002524 organometallic group Chemical group 0.000 abstract description 2
- 239000000243 solution Substances 0.000 description 15
- 238000005265 energy consumption Methods 0.000 description 7
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 6
- 238000004128 high performance liquid chromatography Methods 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 239000000047 product Substances 0.000 description 4
- 239000011550 stock solution Substances 0.000 description 4
- 238000001308 synthesis method Methods 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000004659 sterilization and disinfection Methods 0.000 description 3
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 239000003153 chemical reaction reagent Substances 0.000 description 2
- 238000005660 chlorination reaction Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000012467 final product Substances 0.000 description 2
- MVFCKEFYUDZOCX-UHFFFAOYSA-N iron(2+);dinitrate Chemical compound [Fe+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MVFCKEFYUDZOCX-UHFFFAOYSA-N 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 238000010992 reflux Methods 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 238000009210 therapy by ultrasound Methods 0.000 description 2
- 241000894006 Bacteria Species 0.000 description 1
- CZMRCDWAGMRECN-UGDNZRGBSA-N Sucrose Chemical compound O[C@H]1[C@H](O)[C@@H](CO)O[C@@]1(CO)O[C@@H]1[C@H](O)[C@@H](O)[C@H](O)[C@@H](CO)O1 CZMRCDWAGMRECN-UGDNZRGBSA-N 0.000 description 1
- 229930006000 Sucrose Natural products 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 230000003213 activating effect Effects 0.000 description 1
- 230000001154 acute effect Effects 0.000 description 1
- 238000003556 assay Methods 0.000 description 1
- 235000013361 beverage Nutrition 0.000 description 1
- 210000002798 bone marrow cell Anatomy 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 229940112822 chewing gum Drugs 0.000 description 1
- 235000015218 chewing gum Nutrition 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000007857 degradation product Substances 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 235000013305 food Nutrition 0.000 description 1
- 235000003599 food sweetener Nutrition 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 231100000086 high toxicity Toxicity 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 229920002521 macromolecule Polymers 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- 239000005416 organic matter Substances 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 125000001997 phenyl group Chemical class [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 1
- 235000021110 pickles Nutrition 0.000 description 1
- 125000005575 polycyclic aromatic hydrocarbon group Chemical group 0.000 description 1
- HDMGAZBPFLDBCX-UHFFFAOYSA-M potassium;sulfooxy sulfate Chemical compound [K+].OS(=O)(=O)OOS([O-])(=O)=O HDMGAZBPFLDBCX-UHFFFAOYSA-M 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229960004793 sucrose Drugs 0.000 description 1
- 239000003765 sweetening agent Substances 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
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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
- B01J35/391—Physical properties of the active metal ingredient
-
- 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
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/74—Iron group metals
- B01J23/745—Iron
-
- 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
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/40—Organic compounds containing sulfur
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Catalysts (AREA)
Abstract
The invention belongs to the technical field of water body micro-pollutant treatment, and particularly relates to a preparation method and application of an iron monatomic catalyst. According to the invention, the Fe-SACs are synthesized by an ion adsorption-pyrolysis method, and the material improves the utilization efficiency of atoms and the surface free energy thereof by reducing the size of metal particles, so that the catalytic activity of Fe is improved, and the consumption of metal is reduced; the strong metal-carrier interaction generates electronic characteristics similar to those of the organometallic complex, and can also effectively mediate charge transfer between a metal atom and a carrier so as to realize high-efficiency persulfate activation.
Description
Technical Field
The invention belongs to the technical field of water body micro-pollutant treatment, and particularly relates to a preparation method and application of an iron monatomic catalyst.
Background
Acesulfame potassium is a common artificial sweetener, and is widely used as an organic compound for replacing cane sugar in various foods such as solid beverages, pickles, preserves, chewing gum, table sweeteners and the like. At present, the global annual consumption of acesulfame-K reaches 4000 tons, and because of the characteristics of strong polarity and high water solubility, the acesulfame-K can not be metabolized by human bodies almost, and can exist stably in the environment, and the removing effect of the traditional water treatment process is very limited. The introduction of improperly handled acesulfame k and its degradation products into the environment can pose a serious threat to the ecosystem and human health. In recent years, researches show that acesulfame potassium can damage DNA of mouse bone marrow cells, and the accumulation of metabolites of acesulfame potassium also has an acute inhibitory effect on luminescent bacteria and obviously enhances the toxicity of organisms. Because of the stable physicochemical characteristics of the acesulfame, the chemical method removal is the current mainstream acesulfame degradation technology, and mainly comprises chlorination disinfection, ozone oxidation, an ultraviolet irradiation method, a Fenton (like) method and the like. The chlorination disinfection method has strong treatment capacity, but is easy to generate high-toxicity disinfection byproducts in the water treatment process; the ozone oxidation method has high reaction rate, no secondary pollution, large energy consumption and high operating cost; the ultraviolet irradiation method has high active oxygen species yield, but has higher energy consumption and general treatment effect. Therefore, an acesulfame potassium degradation technology which is simple in process, high in degradation efficiency and environment-friendly is needed.
The persulfate-based advanced oxidation method can generate SO with strong oxidizing power by activating persulfate4H-and OH, can oxidize and degrade various persistent organic pollutants including chlorohydrocarbon, polycyclic aromatic hydrocarbon, benzene series and the like. At present, homogeneous phase activation mode exists that the energy consumption is big, and the medicament is thrown the dosage height, has secondary pollution risk scheduling problem, and the heterogeneous persulfate activation mode that utilizes monatomic catalyst can reduce the consumption and the reaction energy consumption of metal, improves the output and the selectivity of active oxygen material, realizes the degradation of macromolecule organic matter green economically. Therefore, the persulfate advanced oxidation method based on the activation of the monatomic catalyst is expected to solve the problems of low degradation efficiency, high energy consumption, secondary pollution risk and the like in the acesulfame treatment process of the existing method.
Disclosure of Invention
Therefore, the technical problem to be solved by the invention is to overcome the defects of low conversion efficiency, high energy consumption and secondary pollution risk of the acesulfame potassium degradation method in the prior art, so that the preparation method and the application of the iron monatomic catalyst are provided.
Therefore, the invention provides the following technical scheme,
the invention provides a preparation method of an iron monatomic catalyst, which comprises the following steps,
s1: mixing Fe (NO)3)3·6H2Dissolving O in ultrapure water to obtain a ferric nitrate solution;
s2: dispersing carbon black in a concentrated nitric acid solution for activation, then mixing the activated carbon black with ultrapure water, and performing ultrasonic dispersion to obtain a carbon black suspension;
s3: dropwise adding a ferric nitrate solution into a carbon black solution, stirring and centrifuging to obtain an iron precursor;
s4: mixing the prepared iron precursor powder with urea, heating the mixture to 800 ℃ in a tubular furnace in an Ar atmosphere of 60-100sccm, and keeping the temperature for 1 hour to obtain the iron monatomic catalyst.
Optionally, the concentration of the ferric nitrate solution is 3 mg/mL.
Optionally, the activation time is 3 h;
and/or, the activation temperature is 90 ℃.
Optionally, the concentration of the carbon black suspension is 0.0025 g/mL;
and/or the ultrasonic dispersion time is 30-40 min.
Optionally, the stirring time is 10-12 h.
The invention also provides application of the iron monatomic catalyst prepared by the preparation method in degradation of artificial sweetener acesulfame potassium.
Optionally, the method comprises the following steps,
(1) preparing a degradation system: the degradation system consists of acesulfame potassium and an aqueous medium;
(2) adding an iron monatomic catalyst with the mass concentration of 0.1g/L into the degradation system to form a mixture, and then stirring to establish adsorption-desorption balance;
(3) adding persulfate with the mass concentration of 0.1-2.4g/L into the mixture in the step (2), and performing catalytic degradation in the formed solution with the pH value of 3-7.
Optionally, the molar concentration of the acesulfame potassium in the solvent in the step (1) is 0.2 mM.
Optionally, the stirring speed in the step (2) is 200 rpm;
and/or the stirring time in the step (2) is 30 min.
Optionally, the persulfate in step (3) is oxone;
and/or the time for catalytic degradation in the step (3) is 0-60 min.
The technical proposal provided by the invention has the advantages that,
1. according to the invention, the Fe-SACs are synthesized by an ion adsorption-pyrolysis method, and the material improves the utilization efficiency of atoms and the surface free energy thereof by reducing the size of metal particles, so that the catalytic activity of Fe is improved, and the consumption of metal is reduced; the strong metal-carrier interaction generates electronic characteristics similar to those of the organometallic complex, and can also effectively mediate charge transfer between a metal atom and a carrier so as to realize high-efficiency persulfate activation.
2. The invention utilizes Fe-SACs as the iron monatomic catalyst to efficiently activate persulfate, thereby realizing the efficient degradation of the artificial sweetener, and can realize the near 100 percent degradation of the acesulfame potassium with the concentration of 0.2mM within 60min under the conditions of 0.1g/L of the catalyst, 2.4g/L of the persulfate and the room temperature (25 ℃) with the pH value of 7. Compared with other treatment methods, the method is rapid and efficient, has low energy consumption and small potential safety hazard and environmental risk, and meanwhile, the material synthesis method is simpler and more convenient compared with other monatomic material synthesis methods, provides a more green, economic and efficient means for degrading the microcontaminant acesulfame in the water body, and is expected to solve a series of ecological problems caused by the fact that the artificial sweetener exists in the environment for a long time.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below, and it is obvious that the drawings in the following description are some embodiments of the present invention, and other drawings can be obtained by those skilled in the art without creative efforts.
FIG. 1 is an XRD pattern of Fe-SACs catalysts;
FIG. 2 is a graph of acesulfame potassium degradation efficiency under different pH conditions;
FIG. 3 is a graph of acesulfame potassium degradation efficiency for different persulfate dosages;
Detailed Description
The following examples are provided to further understand the present invention, not to limit the scope of the present invention, but to provide the best mode, not to limit the content and the protection scope of the present invention, and any product similar or similar to the present invention, which is obtained by combining the present invention with other prior art features, falls within the protection scope of the present invention.
The examples do not show the specific experimental steps or conditions, and can be performed according to the conventional experimental steps described in the literature in the field. The reagents or instruments used are not indicated by manufacturers, and are all conventional reagent products which can be obtained commercially.
Example 1
The synthesis method of the iron monatomic catalyst provided by the embodiment comprises the following steps: preparing Fe-SACs (iron single-atom catalysts) by an ion adsorption-pyrolysis method: firstly Fe (NO)3)3·6H2O was dissolved in ultrapure water to prepare a 3mg/mL stock solution of ferric nitrate. 2g of carbon black was dispersed in 100mL of concentrated nitric acid solution, followed by activation at 90 ℃ under reflux for 3 hours. 1g of activated carbon black is mixed with 400ml of ultrapure water, and the mixture is subjected to ultrasonic treatment for 30-40min to obtain a uniformly dispersed carbon black suspension. Then, 40mL of iron nitrate stock solution was added dropwise to the carbon black solution, stirred to be sufficiently adsorbed, and centrifuged to collect a product iron precursor (Fe)3+-CB). Prepared Fe3+-CB powder was mixed with urea in a mass ratio of 1:10, and it was put in a tube furnace in an Ar atmosphere of 80sccmHeating to 800 ℃ and keeping for 1 hour to obtain the final product Fe-SACs.
The prepared Fe-SACs material is used in an acesulfame potassium degradation system, and the specific degradation process is implemented according to the following steps:
s1: 0.004g of acesulfame potassium is mixed with 100ml of ultrapure water to prepare a 0.2mM acesulfame potassium solution.
S2: 0.01g of Fe-SACs was added to the solution and stirred at 200rpm for 30min to reach adsorption equilibrium.
S3: 0.01g of oxone was added to the S2 blend system using 1M H2SO4And 1M NaOH was added to adjust pH 3/7, stirred at 200rpm for 60min, 1mL was taken out every 10min, quenched with methanol, and passed through a 0.22 μm filter.
S4: and (4) determining the concentration of the acesulfame in the system by HPLC (high performance liquid chromatography), thereby calculating the acesulfame removal efficiency.
As shown in FIG. 2, the results showed that the removal rate of acesulfame from Fe-SACs under the conditions of this example was 13%, and the removal effect was hardly affected by the pH change.
Example 2
The synthesis method of the iron monatomic catalyst provided by the embodiment comprises the following steps: preparing Fe-SACs (iron single-atom catalysts) by an ion adsorption-pyrolysis method: firstly Fe (NO)3)3·6H2O was dissolved in ultrapure water to prepare a 3mg/mL stock solution of ferric nitrate. 2g of carbon black was dispersed in 100mL of concentrated nitric acid solution, followed by activation at 90 ℃ under reflux for 3 hours. Then 1g of activated carbon black is mixed with 400ml of ultrapure water, and the mixture is subjected to ultrasonic treatment for 30min to obtain a uniformly dispersed carbon black suspension. Then, 40mL of iron nitrate stock solution was added dropwise to the carbon black solution, stirred to be sufficiently adsorbed, and centrifuged to collect a product iron precursor (Fe)3+-CB). Prepared Fe3+-CB powder is mixed with urea in a mass ratio of 1:10, heated to 800 deg.C in a tube furnace at 80sccm Ar atmosphere and held for 1 hour to obtain the final product Fe-SACs.
The prepared Fe-SACs material is used in an acesulfame potassium degradation system, and the specific degradation process is implemented according to the following steps:
s1: 0.004g of acesulfame potassium is mixed with 100ml of ultrapure water to prepare a 0.2mM acesulfame potassium solution.
S2: 0.01g of Fe-SACs was added to the solution and stirred at 200rpm for 30min to reach adsorption equilibrium.
S3: adding 0.01/0.04/0.12/0.24g of potassium hydrogen persulfate into the S2 mixed system, and utilizing 1MH2SO4And 1M NaOH was added to adjust pH to 7, stirred at 200rpm for 60min, 1mL was taken out every 10min, quenched with methanol, and passed through a 0.22 μ M filter for assay.
S4: and (4) determining the concentration of the acesulfame in the system by HPLC (high performance liquid chromatography), thereby calculating the acesulfame removal efficiency.
As shown in FIG. 3, the results showed that the removal rates of Fe-SACs for acesulfame K were 13%, 25%, 88%, 93% at the addition of 0.01/0.04/0.12/0.24g of oxone.
It should be understood that the above examples are only for clarity of illustration and are not intended to limit the embodiments. Other variations and modifications will be apparent to persons skilled in the art in light of the above description. And are neither required nor exhaustive of all embodiments. And obvious variations or modifications therefrom are within the scope of the invention.
Claims (10)
1. A preparation method of an iron monatomic catalyst is characterized by comprising the following steps,
s1: mixing Fe (NO)3)3·6H2Dissolving O in ultrapure water to obtain a ferric nitrate solution;
s2: dispersing carbon black in a concentrated nitric acid solution for activation, then mixing the activated carbon black with ultrapure water, and performing ultrasonic dispersion to obtain a carbon black suspension;
s3: dropwise adding a ferric nitrate solution into a carbon black solution, stirring and centrifuging to obtain an iron precursor;
s4: mixing the prepared iron precursor powder with urea, heating the mixture to 800 ℃ in a tubular furnace in an Ar atmosphere of 60-100sccm, and keeping the temperature for 1 hour to obtain the iron monatomic catalyst.
2. The method according to claim 1, wherein the concentration of the ferric nitrate solution is 3 mg/mL.
3. The method for preparing an iron monatomic catalyst according to claim 1 or 2, wherein the activation time is 3 hours;
and/or, the activation temperature is 90 ℃.
4. A method of preparing an iron monatomic catalyst according to any one of claims 1 to 3, characterized in that the concentration of the carbon black suspension is 0.0025 g/mL;
and/or the ultrasonic dispersion time is 30-40 min.
5. A process for the preparation of an iron monatomic catalyst according to any one of claims 1 to 4, characterized in that the stirring time is 10 to 12 hours.
6. The use of the iron monatomic catalyst prepared by the preparation method of any one of claims 1 to 5 for degrading artificial sweetener acesulfame potassium.
7. The use of the iron monatomic catalyst of claim 6 for degrading the artificial sweetener acesulfame k, characterized in that it comprises the following steps,
(1) preparing a degradation system: the degradation system consists of acesulfame and an aqueous medium;
(2) adding an iron monatomic catalyst with the mass concentration of 0.1g/L into the degradation system to form a mixture, and then stirring to establish adsorption-desorption balance;
(3) adding persulfate with the mass concentration of 0.1-2.4g/L into the mixture in the step (2), and performing catalytic degradation in the formed solution with the pH value of 3-7.
8. The use of an iron monatomic catalyst as set forth in claim 7 for the degradation of the artificial sweetener acesulfame k, wherein the molar concentration of acesulfame k in the solvent in step (1) is 0.2 mM.
9. Use of the iron monatomic catalyst according to claim 7 or 8, characterized in that, in step (2), the stirring rate is 200 rpm;
and/or the stirring time in the step (2) is 30 min.
10. Use of an iron monatomic catalyst according to any one of claims 7 to 9, wherein in step (3) said persulfate is oxone;
and/or the time for catalytic degradation in the step (3) is 0-60 min.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN109731605A (en) * | 2019-02-28 | 2019-05-10 | 哈尔滨工业大学 | A kind of metal composite situ Nitrogen Doping carbon microspherical catalyst and its application |
| CN112452346A (en) * | 2020-10-14 | 2021-03-09 | 浙江大学 | Universal method for preparing metal single-atom carbon-based catalyst and application |
| CN113042081A (en) * | 2021-03-24 | 2021-06-29 | 中南大学 | Iron-nitrogen-carbon composite material containing single-atom active site, and preparation and application methods thereof |
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| CN113549935A (en) * | 2021-05-20 | 2021-10-26 | 中国科学技术大学 | Heteroatom-doped transition metal monoatomic catalyst and preparation method and application thereof |
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| CN112452346A (en) * | 2020-10-14 | 2021-03-09 | 浙江大学 | Universal method for preparing metal single-atom carbon-based catalyst and application |
| CN113097508A (en) * | 2021-03-17 | 2021-07-09 | 国家电投集团氢能科技发展有限公司 | Noble metal supported electrocatalyst and preparation method and application thereof |
| CN113042081A (en) * | 2021-03-24 | 2021-06-29 | 中南大学 | Iron-nitrogen-carbon composite material containing single-atom active site, and preparation and application methods thereof |
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