GB2619004A - Nanoscale magnetite-modified activated carbon fiber (ACF) composite, and preparation method and use thereof - Google Patents

Nanoscale magnetite-modified activated carbon fiber (ACF) composite, and preparation method and use thereof Download PDF

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GB2619004A
GB2619004A GB2207202.9A GB202207202A GB2619004A GB 2619004 A GB2619004 A GB 2619004A GB 202207202 A GB202207202 A GB 202207202A GB 2619004 A GB2619004 A GB 2619004A
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acf
composite
modified
preparation
nanoscale magnetite
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Hou Junwei
Ren Jihong
Ma Liqiang
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Xinjiang Youmiao Environmental Protection Tech Co Ltd
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Xinjiang Youmiao Environmental Protection Tech Co Ltd
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Abstract

The present disclosure belongs to the technical field of catalytic materials for heterogeneous Electro-Fenton, and provides a nanoscale magnetite-modified activated carbon fiber (ACF) composite, and a preparation method and use thereof. The nanoscale magnetite-modified activated carbon fiber (ACF) composite comprises an ACF and iron(II,III) oxide particles loaded on a surface of the ACF. The preparation method of the nanoscale magnetite-modified ACF composite comprises the steps of: immersing the ACF in an inorganic acid for acid treatment to obtain a pretreated ACF; dissolving ferrous ions and ferric ions to obtain an iron ion solution; and soaking the pretreated ACF in the iron ion solution, and conducting precipitation and aging in sequence under alkaline conditions to obtain the nanoscale magnetite-modified ACF composite. In an aspect of the invention, the nanoscale magnetite-modified ACF composite is used in oxidative degradation of an organic pollutant by heterogeneous Electro-Fenton. Suitably, the nanoscale magnetite-modified ACF composite is used as a cathode and a conductive material as an anode, in an electrolyte containing the organic pollutant, wherein air may be blown in the electrolyte.

Description

NANOSCALE MAGNETITE-MODIFIED ACTIVATED CARBON FIBER (ACF) COMPOSITE, AND PREPARATION METHOD AND USE THEREOF
TECHNICAL FIELD
100011 The present disclosure relates to the technical field of catalytic materials for heterogeneous Electro-Fenton, in particular to a nanoscale magnetite-modified activated carbon fiber (ACF) composite, and a preparation method and use thereof
BACKGROUND ART
100021 Bio-organic substances such as coal, asphalt, wood and core shells can be screened, pretreated and carbonized to produce activated carbon with desired properties. Activated carbon, due to a desirable chemical stability, large specific surface area, low cost and easy availability, is widely used in industrial production and daily life. According to different shapes, the activated carbon can be prepared into powders, granules, and fibers. According to different source materials, the activated carbon includes coconut shell-derived activated carbon, rubber-derived activated carbon, synthetic resin-derived activated carbon, and mineral-derived activated carbon. 100031 ACE is a fibrous activated carbon. The ACF is an excellent adsorption material due to a huge specific surface area, developed pore structure, and abundant surface functional groups. At present, the ACF has been widely used in adsorption of pollutants and other harmful substances. However, ACF adsorption only transfer pollutant molecules to a surface of the ACF, which is a physical change and fails to destroy a structure of the pollutant molecules and completely remove the pollutants. As a result, the ACF after adsorbing harmful substances becomes a new harmful substance.
SUMMARY
100041 In view of this, an objective of the present disclosure is to provide a nanoscale magnetite-modified ACF composite, and a preparation method and use thereof The nanoscale magnetite-modified ACF composite can degrade and remove organic pollutants while adsorbing the organic pollutants.
100051 To achieve the above objective, the present disclosure provides the following technical solutions.
100061 The present disclosure provides a nanoscale magnetite-modified ACF composite, including an ACF and iron(H,III) oxide particles loaded on a surface of the ACF.
100071 Preferably, the iron(H,H1) oxide particles and the ACF may have a mass ratio of (0.3-1): 1.
[0008] The present disclosure further provides a preparation method of the nanoscale magnetite-modified ACF composite, including the following steps: [0009] immersing the ACF in an inorganic acid for acid treatment to obtain a pretreated ACF; 100101 dissolving ferrous ions and ferric ions to obtain an iron ion solution; and [0011] soaking the pretreated ACF in the iron ion solution, and conducting precipitation and aging in sequence under alkaline conditions to obtain the nanoscale magnetite-modified ACF composite.
[0012] Preferably, a reagent for the dissolving may include an alcohol aqueous solution; an alcohol in the alcohol aqueous solution may include ethanol; and the alcohol and water in the alcohol aqueous solution may have a volume ratio of 5:5 to 3:7.
[0013] Preferably, in the iron ion solution, the ferrous ions and the ferric ions may have a molar ratio of 1:(1.5-2); and the ferrous ions may have a concentration of 0.04 mol/L to 0.06 mol/L. [0014] Preferably, the soaking may be conducted at 70°C to 80°C for 30 min to 60 min. [0015] Preferably, the precipitation may be conducted at 70°C to 80°C and a pH value of 10 to 13 for] h to 2 h. [0016] Preferably, the aging may be conducted for 18 h to 36 h. [0017] The present disclosure further provides use of the nanoscale magnetite-modified ACF composite or a nanoscale magnetite-modified ACF composite prepared by the preparation method in oxidative degradation of an organic pollutant by heterogeneous Electro-Fenton.
[0018] Preferably, the use may include the following steps: [0019] placing the nanoscale magnetite-modified ACF composite as a cathode and a conductive material as an anode in an electrolyte containing the organic pollutant, blowing air in the electrolyte, and conducting electrification for the oxidative degradation by heterogeneous Electro-Fenton.
[0020] The present disclosure provides a nanoscale magnetite-modified ACF composite, including an ACF and iron(I1,111) oxide particles loaded on a surface of the ACF. In the composite, the ACF can adsorb pollutants, and the iron(II,III) oxide contains Fe' and Fen. Meanwhile, due to inherent H909-like catalytic enzyme properties, the iron(II,110 oxide can effectively stimulate the H202 to generate *OH. When being applied to an oxidative degradation system for the heterogeneous Electro-Fenton, the composite can simultaneously function as a catalyst source (Fe' and 11202) and as a functionalized cathode. Therefore, heterogeneous Electro-Fenton oxidation is simplified without a cost of external Fe feeding, thereby enabling degradation of the organic pollutants. In the composite, the iron (11,111) oxide particles have the highest catalytic activity for heterogeneous Electro-Fenton oxidation compared with other iron oxides such as wustite (FeO) and hematite (Fe203), to improve a degradation efficiency of the organic pollutants. In addition, the magnetic iron(II,M) oxide particles are beneficial to recycling of the nanoscale magnetite-modified ACF composite, thereby avoiding environmental pollution. [0021] The present disclosure further provides a preparation method of the nanoscale magnetite-modified ACF composite, including the following steps: immersing the ACF in an inorganic acid for acid treatment to obtain a pretreated ACF; dissolving ferrous ions and ferric ions to obtain an iron ion solution; and soaking the pretreated ACF in the iron ion solution, and conducting precipitation and aging in sequence under alkaline conditions to obtain the nanoscale magnetite-modified ACF composite. The acid treatment chemically etches the ACF, increases the number of micropores on a surface of the ACF, and increases a specific surface area of the ACF, thereby improving a subsequent loading rate of the iron(11,I11) oxide. The pretreated ACF is soaked in the iron ion solution, and ii-situ precipitation is conducted to form the iron(II,III) oxide and to deposit and load the iron(II,111) oxide particles on the surface or in the micropores of the pretreated ACF.
[0022] Further, a reagent for the dissolving includes an alcohol aqueous solution; an alcohol in the alcohol aqueous solution includes ethanol; and the alcohol and water in the alcohol aqueous solution have a volume ratio of 5:5 to 3:7. The alcohol aqueous solution can reduce a growth rate of iron(II,III) oxide crystals, reduce a particle size and agglomeration tendency of the iron(II,III) oxide crystals, and increase a specific surface area of iron(II,III) oxide nanomaterials. When participating in the oxidative degradation by heterogeneous Electro-Fenton, the aqueous alcohol solution can increase the space for a gas-liquid-solid three-phase reaction, shorten a mass transfer path, and enable more reactions to occur simultaneously, thereby further improving an efficiency of the oxidative degradation by heterogeneous Electro-Fenton.
100231 The present disclosure further provides use of the nanoscale magnetite-modified ACF composite or a nanoscale magnetite-modified ACF composite prepared by the preparation method in oxidative degradation of an organic pollutant by heterogeneous Electro-Fenton. Since in the nanoscale magnetite-modified ACF composite, the iron(II,III) oxide has 11202-like catalytic enzyme properties, and contains Fe' and Fe". Therefore, the nanoscale magnetite-modified ACF composite can effectively stimulate the 11202 to generate.011. When being applied to an oxidative degradation system for the heterogeneous Electro-Fenton, the composite can simultaneously function as a catalyst source (Fe" and H202) and as a functionalized cathode. Therefore, the composite can be applied to the field of oxidative degradation of organic pollutants by heterogeneous Electro-Fenton.
BRIEF DESCRIPTION OF THE DRAWINGS
[0024] FIG. 1 shows a comparison diagram of a nanoscale magnetite-modified ACF composite (n-Fe304/ACF) obtained in Example 1 and a Fe304 spectrum standard card; [0025] FIG. 2 shows an X-ray photoelectron spectroscopy (XPS) wide-spectrum scanning spectrogram of the nanoscale magnetite-modified ACF composite obtained in Example 1; [0026] FIG. 3 shows an energy dispersive spectroscopy (EDS) layered image of the nanoscale magnetite-modified ACF composite obtained in Example 1; [0027] FIG. 4 shows a transmission electron microscope (TEM) image of the nanoscale magnetite-modified ACF composite obtained in Example 1; [0028] FIG. 5 shows a mapping diagram of C element distribution of the nanoscale magnetite-modified ACF composite obtained in Example 1; [0029] FIG. 6 shows a mapping diagram of 0 element distribution of the nanoscale magnetite-modified ACF composite obtained in Example 1; [0030] FIG. 7 shows a mapping diagram of Fe element distribution of the nanoscale magnetite-modified ACF composite obtained in Example I; [0031] FIG. 8 shows a TEM image and an analysis image of an interplanar spacing of the nanoscale magnetite-modified ACF composite obtained in Example 1; [0032] FIG. 9 shows a curve comparison of a catalytic performance test on an n-Fe304/ACF obtained in Example 1 and a pure-ACF obtained in Comparative Example 1 in degradation of methyl blue; [0033] FIG. 10 shows a curve comparison of a catalytic performance test on the n-Fe304/ACF obtained in Example 1 in degradation of the methyl blue, methyl orange and methyl violet; [0034] FIG. 11 shows a curve comparison of a catalytic performance test on the n-Fe304/ACF obtained in Example 1 in degradation of the methyl blue after 5 cycles; and [0035] FIG. 12 shows a curve comparison of a catalytic performance test on the n-Fe304/ACF obtained in Example 1 in degradation of a chemical oxygen demand (COD) after 5 cycles.
DETAILED DESCRIPTION OF THE EMBODIMENTS
[0036] The present disclosure provides a nanoscale magnetite-modified ACF composite, including an ACF and iron(II,III) oxide particles loaded on a surface of the ACF.
[0037] In the present disclosure, the iron(II,III) oxide particles have a particle size of 4 nm to 12 nm.
[0038] In the present disclosure, the iron(11,111) oxide particles and the ACF have a mass ratio of preferably (0.3-1):1. The mass ratio of the iron(II,III) oxide and the ACF is controlled at (0.3-1):1, to ensure that enough iron(H,III) oxide particles are loaded on the ACF to participate in heterogeneous Electro-Fenton oxidation; meanwhile, the loading of iron(II,III) oxide cannot affect an adsorption effect of the ACF on pollutants.
[0039] The present disclosure further provides a preparation method of the nanoscale magnetite-modified ACF composite, including the following steps: [0040] immersing the ACF in an inorganic acid for acid treatment to obtain a pretreated ACF; [0041] dissolving ferrous ions and ferric ions to obtain an iron ion solution; and 100421 soaking the pretreated ACF in the iron ion solution, and conducting precipitation and aging in sequence under alkaline conditions to obtain the nanoscale magnetite-modified ACF composite.
[0043] In the present disclosure, the raw materials provided herein are all preferably commercially-available products unless otherwise specified.
[0044] In the present disclosure, the ACF is immersed in the inorganic acid for acid treatment to obtain the pretreated ACF.
[0045] In the present disclosure, the inorganic acid includes preferably hydrochloric acid, and the hydrochloric acid has a concentration of preferably 0.05 mol/L to 0.15 mol/L, more preferably 0.1 mol/L. The acid treatment is conducted preferably by standing. The acid treatment is conducted preferably at room temperature without additional cooling or additional heating. The acid treatment is conducted for preferably 6 h to 8 h, more preferably 7 h. The acid treatment achieves chemical etching of the ACF, increases the specific surface area of the ACF, and introduces a rich pore structure for the ACF, thereby exposing more reactive active sites (02 adsorption sites and active sites for electrochemical reduction of 02 to H207), and more defects and sp3-C.
100461 In the present disclosure, before the acid treatment, the ACF is preferably further subjected to ultrasonic water washing preferably 2 to 3 times for preferably 5 min in each time. The ultrasonic water washing can remove impurities and ash that may be adsorbed by unmodified activated carbon during transportation and other processes.
[0047] In the present disclosure, after the acid treatment, an acid-treated ACF is preferably subjected to water washing and drying. There is no special limitation on parameters of the water washing, as long as excess impurities on a surface of the ACF can be removed. There is no special limitation on a temperature and time of the drying, as long as excess water and hydrogen chloride on the surface of the ACF can be removed.
[0048] In the present disclosure, ferrous ions and ferric ions are dissolved to obtain the iron ion solution.
[0049] In the present disclosure, the ferrous ions are preferably provided by ferrous sulfate heptahydrate; and the ferric ions are preferably provided by ferric chloride hexahydrate.
[0050] In the present disclosure, a reagent for the dissolving includes preferably an alcohol aqueous solution; an alcohol in the alcohol aqueous solution includes preferably ethanol; and the alcohol and water in the alcohol aqueous solution have a volume ratio of preferably 5:5 to 3:7. [0051] In the present disclosure, in the iron ion solution, the ferrous ions and the ferric ions have a molar ratio of preferably 1:(1.5-2); and the ferrous ions have a concentration of preferably 0.04 mol/L to 0.06 mol/L.
[0052] In the present disclosure, the dissolving is conducted at preferably 60°C to 80°C, more preferably 70°C. The dissolving is conducted preferably by stirring for preferably 30 min. [0053] In the present disclosure, the pretreated ACF is soaked in the iron ion solution, and precipitation and aging are conducted in sequence under alkaline conditions to obtain the nanoscale magnetite-modified ACF composite.
[0054] In the present disclosure, the soaking is conducted at preferably 70°C to 80°C, more preferably 75°C for preferably 30 min to 60 min, more preferably 40 min to 50 min. The soaking is conducted preferably by stirring.
[0055] In the present disclosure, the alkaline conditions are at a pH value of preferably 10 to 13, more preferably 11 to 12. The alkaline conditions are provided preferably by an inorganic alkali preferably in an inorganic alkali aqueous solution with a concentration of preferably 5 mol/L. The inorganic alkali aqueous solution is preferably added dropw-ise at preferably 10 mL/min to 20 mL/min. The inorganic alkali includes preferably sodium hydroxide.
[0056] In the present disclosure, the precipitation is conducted at preferably 70°C to 80°C, more preferably 75°C for preferably 1 h to 2 h, more preferably 1.5 h. The precipitation is conducted preferably by stirring.
[0057] In the present disclosure, the aging is conducted for preferably 18 h to 36 h, more preferably 24 h to 30 h. [0058] In the present disclosure, after the aging, an aged ACF is preferably further taken out for water washing and drying in sequence to obtain the nanoscale magnetite-modified ACF composite. There is no special limitation on a method of the water washing, as long as excess substances can be washed away. The drying is conducted at preferably 60°C.
[0059] The present disclosure further provides use of the nanoscale magnetite-modified ACF composite or a nanoscale magnetite-modified ACF composite prepared by the preparation method in oxidative degradation of an organic pollutant by heterogeneous El ectro-Fenton.
100601 In the present disclosure, the organic pollutants include preferably one or more of methyl blue, methyl orange, and methyl violet.
[0061] In the present disclosure, the use preferably includes the following steps: [0062] placing the nanoscale magnetite-modified ACF composite as a cathode and a conductive material as an anode in an electrolyte containing the organic pollutant, blowing air in the electrolyte, and conducting electrification for the oxidative degradation by heterogeneous El ectro-Fenton.
100631 In the present disclosure, the conductive material includes preferably platinum or graphite.
[0064] In the present disclosure, the air is blown at preferably 0.2 L/min to 0.8 L/min.
[0065] In the present disclosure, the oxidative degradation by heterogeneous Electro-Fenton is conducted at a current density of preferably 20 mA/cm2 to 40 mA/cm2, more preferably 40 mA/cm2.
[0066] The nanoscale magnetite-modified ACF composite, and the preparation method and the use thereof provided by the present disclosure will be described in detail in connection with the following examples, but they should not be construed as limiting the claimed scope of the present disclosure.
[0067] Example 1
[0068] A preparation method of a nanoscale magnetite-modified ACF composite (n-Fe304/ACF) included the following steps: 100691 (1) ACF pretreatment: a pure ACF was added in a 200 mL beaker filled with deionized water, and placed in an ultrasonic cleaner for ultrasonic cleaning for 5 min; after taking out, impurities and ash remaining on a surface were removed 3 times; after taking out, the ACF was treated in a 0.1 mol/L dilute HCI solution for 8 h, washed with water and dried at 60 °C to obtain a pretreated ACF (pure-ACF).
[0070] (2) Deposition of nano-Fe304: at 70°C, 13.14 g of ferric chloride hexahydrate (FeC13 6H90) and 7.2 g of ferrous sulfate heptahydrate (FeSO4 7H20) were dissolved in 450 mL of an ethanol aqueous solution (where the ethanol to water had a volume ratio of 3:7), followed by magnetic stirring for 30 min to obtain an iron ion solution.
[0071] (3) The pure-ACF obtained in step (1) was placed in the iron ion solution obtained in step (2), stirred for 30 min and heated to 75°C in a water bath; a 5 mol/L sodium hydroxide aqueous solution was added dropwise to a pH value of 11, 60 min of precipitation was conducted by stirring, and the beaker was allowed to stand for aging for 24 h and cooled to room temperature; a product was washed with deionized water, and dried at 60°C in a preheated vacuum drying oven, to obtain the n-Fe304/ACF.
[0072] FIG. 1 shows a comparison diagram of a nanoscale magnetite-modified ACF composite and a Fe304 spectrum standard card. It can be seen from FIG. 1 that the existence of C elementary substance and Fe304 in the n-Fe304/ACF can be confirmed by comparing the XRD spectrum of the sample with the spectrum standard cards of the Fe304 and C elementary substance.
[0073] FIG. 2 shows an XPS wide-spectrum scanning spectrogram of the nanoscale magnetite-modified ACF composite. It can be seen from FIG. 2 that a surface of the sample mainly contains three elements: C, 0 and Fe; the existence of an 0 is peak and a Fe 2p peak can confirm the existence of magnetite in this sample, namely the n-Fe304/ACF.
[0074] FIG. 3 shows an EDS layered image of the nanoscale magnetite-modified ACF composite; FIG. 4 shows a TEM image of the nanoscale magnetite-modified ACF composite; FIG. 5 shows a mapping diagram of C element distribution of the nanoscale magnetite-modified ACF composite; FIG. 6 shows a mapping diagram of 0 element distribution of the nanoscale magnetite-modified ACF composite; and FIG. 7 shows a mapping diagram of Fe element distribution of the nanoscale magnetite-modified ACF composite. It can be seen from FIG. 3 to FIG. 7 that the surface of the sample mainly contains three elements: C, 0 and Fe, with highly uniform distribution, confirming that the sample has the Fe304, namely the n-Fe304/ACF.
[0075] FIG. 8 shows a l'EM image and an analysis image of an interplanar spacing of the nanoscale magnetite-modified ACF composite. It can be seen from FIG. 8 that the nanoscale magnetite-modified ACF composite is composed of a plurality of nano-Fe304 particles with small spacing.
[0076] Comparative Example 1 [0077] Only step (1) in Example 1 was conducted to obtain a pure-ACF.
[0078] Experiment 1. Use of oxidative degradation by heterogeneous Electro-Fenton in organic dye methyl blue included the following steps: [0079] The experiment was conducted in a beaker with an effective volume of 250 mL as a reactor. A 20 mm*20 mm Pt sheet electrode was used as an anode, and 20 mm*20 mm of the n-Fe304/ACF of Example 1 and the pure-ACF of Comparative Example 1 were used as a cathode separately; methyl blue solutions of 200 mL and 100 mg/L were to a beaker, air was pumped into the methyl blue solutions at 200 mL/min, and electrification (at a current density of 30 mA/cm2) was conducted to form a oxidative degradation system by heterogeneous Electro-Fenton, during the entire heterogeneous Electro-Fenton, the solutions were stirred and homogenized with a magnetic stirrer at a current of 30 mA/cm2 supplied by an adjustable constant-voltage DC power supply. At room temperature, a supernatant was collected every 30 min to measure an absorbance using a UV-Vis spectrophotometer, a concentration was calculated according to an F factor, and a degradation rate curve was drawn; meanwhile, a COD was measured, and a COD removal rate curve was drawn by a rapid digestion spectrophotometry (COD tester: China DR1010). The results are shown in FIG. 9. It can be seen from FIG. 9 that a degradation rate of methyl blue is 45.14% after the adsorption of pure ACF for 120 min; the n-Fe304/ACF has a catalytic adsorption and degradation efficiency by heterogeneous Electro-Fenton on methyl blue of 98.87%.
[0080] Experiment 2. Use of oxidative degradation by heterogeneous Electro-Fenton in organic dye methyl blue, methyl orange, and methyl violet included the following steps: [0081] The experiment was conducted in a beaker with an effective volume of 250 mL as a reactor. A 20 mm*20 mm Pt sheet electrode was used as an anode, and 20 mm*20 mm of the n-Fe304/ACF of Example 1 was used as a cathode; methyl blue, methyl orange, or methyl violet solutions of 200 mL and 100 mg/L were to a beaker, air was pumped into the methyl blue, methyl orange, or methyl violet solutions at 200 naL/min, and electrification (at a current density of 30 mA/cm2) was conducted to form a oxidative degradation system by heterogeneous Electro-Fenton; during the entire heterogeneous Electro-Fenton, the solutions were stirred and homogenized with a magnetic stirrer at a current of 30 mA/cm2 supplied by an adjustable constant-voltage DC power supply. At room temperature, a supernatant was collected every 30 min to measure an absorbance using a UV-Vis spectrophotometer, a concentration was calculated according to an F factor, and a degradation rate curve was drawn; meanwhile, a COD was measured, and a COD removal rate curve was drawn by a rapid digestion spectrophotometry (COD tester: China DR1010). The results are shown in FIG. 10. It can be seen from FIG. 10 that the nanoscale magnetite-modified ACF composite has an excellent degradation effect on the methyl blue, the methyl orange and the methyl violet, and an optimal degradation effect on the methyl blue.
[0082] Example 2 Repeated experiment [0083] The n-Fe:304/ACF in Example 1 in Experiment 1 was subjected to an electrocatalytic test for 120 min, rinsed with deionized water 3 times to remove adsorbed organic pollutants, and fully dried in a vacuum drying oven preset at 60°C, and proceed to a next cycle test [0084] The experiment was conducted in a beaker with an effective volume of 250 mL as a reactor. A Pt sheet electrode was used as an anode, and the n-Fe304/ACF composite was used as a functionalized cathode (both being 20 mm*20 mm), methyl blue solutions of 200 mL and 100 mg/L (at a pH value of about 5.73) were to a beaker, air was pumped into the methyl blue solutions at 200 mL/min, to form a oxidative degradation system by heterogeneous Electro-Fenton; during the entire heterogeneous Electro-Fenton, the solutions were stirred and homogenized with a magnetic stirrer at a current of 30 mA/cm2 supplied by an adjustable constant-voltage DC power supply. At room temperature, a supernatant was collected every 30 min to measure an absorbance using a UV-Vis spectrophotometer, a concentration was calculated according to an F factor, and a degradation rate curve was drawn; meanwhile a COD was measured, and a COD removal rate curve was drawn by a rapid digestion spectrophotometry (COD tester: China DR1010).
[0085] The above process was repeated 4 times. The experimental results are shown in FIG. 11 and FIG. 12.
[0086] It can be seen from FIG. 11 that the heterogeneous Electro-Fenton system of n-Fe304/ACF has an extremely stable treatment effect, with removal rates of the methyl blue in the five treatments being 98.87%, 98.32%, 97.95%, 97.23%, and 95.89%, respectively; and after five reuses, the n-Fe304/ACF still has a methyl blue removal rate remained within 3%. This indicates that the catalysis of n-Fe504/ACF composite by heterogeneous Electro-Fenton has a desirable stability and excellent electrochemical performances.
[0087] It can be seen from FIG. 12 that the heterogeneous Electro-Fenton system of n-Fe304/ACF has an extremely stable treatment effect, with removal rates of the methyl blue in the five treatments being 98.47%, 97.77%, 92.65%, 91.68%, and 87.58%, respectively; and after five reuses, the n-Fe204/ACF still has a reduction of a single COD removal rate remained within 6%, and a reduction of five-time COD degradation rate remained within 11%. This indicates that the catalysis of n-Fe304/ACF composite by heterogeneous Electro-Fenton has a desirable stability and excellent electrochemical performances.
[0088] The present disclosure belongs to the technical field of catalytic materials for heterogeneous Electro-Fenton, and provides a nanoscale magnetite-modified activated carbon fiber (ACF) composite, and a preparation method and use thereof In the composite, the ACF can adsorb pollutants, and the iron(11,1I1) oxide contains Fe' and Fe'. Meanwhile, due to inherent H202-like catalytic enzyme properties, the iron(ILIM oxide can effectively stimulate the 11202 to generate.0H. When being applied to an oxidative degradation system for the heterogeneous Electro-Fenton, the composite can simultaneously function as a catalyst source (Fe' and H902) and as a functionalized cathode. Therefore, heterogeneous Electro-Fenton oxidation is simplified without a cost of external Fe feeding, thereby enabling degradation of the organic pollutants. In addition, the magnetic iron(II,IM oxide particles are beneficial to recycling of the nanoscale magnetite-modified ACF composite.
100891 The above descriptions are merely preferred implementations of the present disclosure. It should be noted that a person of ordinary skill in the art may further make several improvements and modifications without departing from the principle of the present disclosure, but such improvements and modifications should be deemed as falling within the protection scope of the present disclosure

Claims (10)

  1. CLAIMS: 1. A nanoscale magnetite-modified activated carbon fiber (ACF) composite, comprising an ACF and iron(11,I11) oxide particles loaded on a surface of the ACF.
  2. 2. The nanoscale magnetite-modified ACF composite according to claim 1, wherein the iron(II,III) oxide particles and the ACF have a mass ratio of (0.3-1): I.
  3. 3. A preparation method of the nanoscale magnetite-modified ACF composite according to claim 1 or 2, comprising the following steps: immersing the ACF in an inorganic acid for acid treatment to obtain a pretreated ACF; dissolving ferrous ions and ferric ions to obtain an iron ion solution; and soaking the pretreated ACF in the iron ion solution, and conducting precipitation and aging in sequence under alkaline conditions to obtain the nanoscale magnetite-modified ACF composite.
  4. 4. The preparation method according to claim 3, wherein a reagent for the dissolving comprises an alcohol aqueous solution; an alcohol in the alcohol aqueous solution comprises ethanol; and the alcohol and water in the alcohol aqueous solution have a volume ratio of 5:5 to 3:7.
  5. 5. The preparation method according to claim 3 or 4, wherein in the iron ion solution, the ferrous ions and the ferric ions have a molar ratio of 1:0.5-2); and the ferrous ions have a concentration of 0.04 mol/L to 0.06 mol/L.
  6. 6 The preparation method according to claim 3, wherein the soaking is conducted at 70°C to 80°C for 30 min to 60 min
  7. 7. The preparation method according to claim 3, wherein the precipitation is conducted at 70°C to 80°C and a pH value of 10 to 13 for I h to 2 h.
  8. 8. The preparation method according to claim 3, wherein the aging is conducted for 18 h to 36 h.
  9. 9. Use of the nanoscale magnetite-modified ACF composite according to claim 1 or 2 or a nanoscale magnetite-modified ACF composite prepared by the preparation method according to any one of claims 3 to 8 in oxidative degradation of an organic pollutant by heterogeneous El ectro-Fenton.
  10. 10. The use according to claim 9, comprising the following steps: placing the nanoscale magnetite-modified ACF composite as a cathode and a conductive material as an anode in an electrolyte containing the organic pollutant, blowing air in the electrolyte, and conducting electrification for the oxidative degradation by heterogeneous Electro-Fenton.
GB2207202.9A 2022-05-17 2022-05-17 Nanoscale magnetite-modified activated carbon fiber (ACF) composite, and preparation method and use thereof Pending GB2619004A (en)

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