A method for highly selective electrocatalytic oxidation of simple aromatics via Fe-NC catalytic electrodes

Abstract

The invention discloses a method for the oxidation of simple aromatic hydrocarbons by highly selective electrocatalysis of Fe-N-C catalytic electrodes, wherein a mixed homogeneous solution containing aromatic compounds, water, electrolytes, and organic solvents is placed in an electrolytic cell provided with electrodes and oxygen is introduced to react to obtain a reaction solution containing aromatic ketone compounds. The cathode sheet of the electrolytic cell is a carbon paper electrode loaded with Fe-N-C material. The method provided by the present invention has simple experimental operation, high safety, more economical and environmentally friendly, green and practical, and high selectivity of the product. The shortcomings of traditional synthetic routes, such as long reaction time, high reaction temperature, disadvantageous for environmental protection, and high pressure, can be effectively overcome, and the problems of complicated steps, long reaction time, expensive catalysts, excessive strong oxidants, high reaction temperatures, and low atomic efficiency in the traditional reaction process are solved, and the reaction efficiency can be improved, which is suitable for industrial production.

Description

Technical Field

[0001] The invention belongs to the field of organic chemical synthesis, and in particular relates to a method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons through a novel Fe-NC catalytic electrode. Background Art

[0002] The efficient and selective oxidation of C-H bonds in organic substances is of vital importance in synthetic chemistry and plays a vital role in the manufacture of raw materials in the current chemical industry structure. However, the high bond energy and low polarity of C-H bonds pose a major challenge to their activation in a controllable and mild manner. Harsh operating conditions such as high temperature, high pressure, acidic solvents, stoichiometric additives, and strong oxidants (O 2 , H 2 O 2 , t-BuOOH, etc.). In addition, alkyl hydroperoxide intermediates are inevitably included in the process, and the combination of high temperature, strong chemical oxidants, and flammable organic substances raises particular concerns about potential explosions in large-scale production.

[0003] Precious metals are widely used as catalysts for energy conversion, chemical production, and emission control. However, the scarcity and high cost of precious metals constitute the main obstacle to large-scale practical application. Therefore, finding earth-abundant but effective catalysts to replace precious metals has become one of the central tasks of the catalysis community. Among them, MNC (M usually refers to Fe and Co) materials were originally obtained by pyrolysis of transition metal-containing macrocycles, and later they can be prepared by simply heating a mixture of more available and cheaper metal and nitrogen precursors on a carbon support. Due to their excellent performance in various typical platinum-catalyzed reactions such as oxygen reduction reaction (ORR), CO 2 They have attracted great attention due to their excellent catalytic performance in electroreduction reaction and hydrogen evolution reaction (HER) as well as fine chemical synthesis.

[0004] Electrochemical methods have the advantages of high reaction efficiency and mild temperature conditions. Using heterogeneous catalysts loaded on electrodes in the reaction can not only conveniently separate the product from the catalyst, but also improve the catalytic efficiency of the electrochemical reaction. With the development of society and the depletion of resources, the development of green chemistry has become one of the missions of scientists. Summary of the invention

[0005] Purpose of the invention: The technical problem to be solved by the present invention is to provide a method for achieving efficient oxidation of simple aromatics by electrocatalysis in view of the deficiencies in the prior art.

[0006] In order to achieve the above object, the technical solution adopted by the present invention is as follows:

[0007] A method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrodes, wherein a mixed homogeneous solution containing an aromatic compound represented by formula I, water, an electrolyte, and an organic solvent is placed in an electrolytic cell provided with electrodes and oxygen is introduced to react to obtain an aromatic ketone compound product represented by formula II;

[0008] Wherein, the cathode sheet in the electrolytic cell is a carbon paper electrode loaded with Fe-NC;

[0009] The aromatic compound shown in formula I is:

[0010]

[0011] The aromatic ketone compound shown in formula II is:

[0012]

[0013] In the formula, R 1 Any one selected from benzene, 4-methylbenzene, 4-ethylbenzene, 4-chlorobenzene, 4-methoxybenzene, 4-nitrobenzene or a naphthalene ring, preferably benzene, 4-methylbenzene, 4-chlorobenzene, 4-methoxybenzene or a naphthalene ring; more preferably benzene, 4-methylbenzene or 4-methoxybenzene.

[0014] Specifically, the electrolyte is any one of tetrabutylammonium hexafluorophosphate, tetrabutylammonium tetrafluoroborate, and tetrabutylammonium perchlorate, or a combination of two or more thereof.

[0015] Specifically, the organic solvent is any one of acetonitrile, methanol, N,N-dimethylformamide, and propylene carbonate, or a combination of two or more thereof; preferably, tetrabutylammonium hexafluorophosphate.

[0016] Furthermore, the concentration of the aromatic compound represented by Formula I in the mixed homogeneous solution is 5-15 mM, preferably 7-13 mM, and more preferably 10 mM.

[0017] Furthermore, the concentration of the electrolyte in the mixed homogeneous solution is 0.05-0.15M, preferably 0.07-0.13M, and more preferably 0.1M.

[0018] Furthermore, the mass ratio of water to organic solvent is 1:14 to 24, preferably 1:16 to 22, and more preferably 1:19.

[0019] Furthermore, the flow rate of oxygen introduced during the reaction is 10 to 30 mL / min, preferably 15 to 25 mL / min, and more preferably 20 mL / min.

[0020] Furthermore, the reaction temperature is controlled at 20-30°C, preferably room temperature; the current intensity introduced during the reaction is 1-5mA, preferably 2-4mA, and more preferably 3mA; the reaction residence time is controlled at 6-12h, preferably 7-11h, and more preferably 8h.

[0021] Specifically, the electrolytic cell provided with electrodes comprises a non-sealed electrolytic cell, a cathode sheet, an anode sheet and a DC power supply; the volume of the non-sealed electrolytic cell is preferably 25 mL; the distance between the cathode sheet and the anode sheet in the electrolytic cell is about 1 cm; the anode sheet is a graphite carbon electrode or a platinum sheet electrode, preferably a platinum sheet electrode; the cathode sheet is a carbon paper electrode loaded with Fe-NC;

[0022] The preparation method of the carbon paper electrode loaded with Fe-NC is as follows:

[0023] 2-Methylimidazole was dissolved in methanol to obtain solution A; zinc acetate and ferric triacetylacetonate were dissolved in methanol to obtain solution B; solution A and solution B were mixed and subjected to solvothermal reaction at 110-130°C for 5-6h to obtain a precursor; the precursor was placed in N 2 The Fe-NC material is obtained by calcining at 850-950° C. for 1-3 h in an atmosphere; finally, the obtained Fe-NC material is evenly coated on a carbon paper electrode.

[0024] Furthermore, after the reaction is completed, the liquid in the electrolytic cell is collected, the reaction solution is diluted with ethyl acetate (preferably diluted five times), washed with water, dried, filtered, and then eluted and separated with a mixed solvent of ethyl acetate and petroleum ether to obtain the aromatic ketone compound shown in formula II. Preferably, the volume ratio of the mixed solvent of ethyl acetate and petroleum ether is 1:10-30.

[0025] Beneficial effects:

[0026] The method provided by the present invention is simple to operate, highly safe, more economical, environmentally friendly, green and practical. It can effectively overcome the shortcomings of the traditional synthesis route, such as long reaction time, high reaction temperature, low atomic efficiency, high cost, and environmental disadvantages, solve the problems of complicated steps, long reaction time, excessive strong oxidant, high reaction temperature and low atomic efficiency in the traditional reaction process, and can improve the reaction efficiency, so as to be suitable for industrial production. BRIEF DESCRIPTION OF THE DRAWINGS

[0027] The present invention will be further described in detail below in conjunction with the accompanying drawings and specific embodiments, and the above and / or other advantages of the present invention will become more clear.

[0028] Figure 1 It is a reaction pathway diagram of the present invention.

[0029] Figure 2This is a diagram of the preparation of the catalytic electrode of the present invention.

[0030] Figure 3 This is the hydrogen spectrum of compound 2a prepared in Example 1.

[0031] Figure 4 This is the carbon spectrum of compound 2a prepared in Example 1.

[0032] Figure 5 This is the hydrogen spectrum of compound 2b prepared in Example 2.

[0033] Figure 6 This is the carbon spectrum of compound 2b prepared in Example 2.

[0034] Figure 7 This is the hydrogen spectrum of compound 2c prepared in Example 3.

[0035] Figure 8 This is the carbon spectrum of compound 2c prepared in Example 3.

[0036] Fig. 9 This is the hydrogen spectrum of compound 2d prepared in Example 4.

[0037] Fig.10 This is the carbon spectrum of compound 2d prepared in Example 4. DETAILED DESCRIPTION

[0038] The present invention can be better understood with reference to the following examples.

[0039] The present invention provides a method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrodes, wherein a mixed homogeneous solution containing an aromatic compound represented by Formula I, water, an electrolyte, and an organic solvent is placed in an electrolytic cell provided with electrodes and oxygen is introduced to react to obtain an aromatic ketone compound product represented by Formula II. The specific reaction pathway is shown in Figure 1 .

[0040] The electrolytic cell with electrodes used in the following examples includes a DC power supply, a 25 mL electrolytic cell, a cathode sheet and an anode sheet; wherein the electrolytic cell is provided with an anode sheet (platinum sheet) and a cathode sheet (Fe-NC loaded carbon paper electrode), respectively; the distance between the cathode sheet and the anode in the electrolytic cell is about 1 cm.

[0041] Among them, Figure 2 As shown in FIG. 1 , the cathode sheet was prepared by the following method: 1.3140 g of 2-methylimidazole was dissolved in 20 mL of methanol solution, 0.7335 g of zinc acetate and 0.0706 g of ferric triacetylacetonate were dissolved in 30 mL of methanol solution, the two were mixed, and a solvent thermal reaction was carried out at 120° C. for 4 h to obtain a precursor, and the precursor was placed in N 2The Fe-NC material was calcined at 900°C for 2h in an atmosphere; the Fe-NC material was evenly coated on a carbon paper electrode.

[0042] In the following examples, the following steps are followed: (1) adding a mixed homogeneous solution prepared in proportion to an electrolytic cell; (2) adjusting the required current; (3) collecting the reaction solution after the reaction is completed, and calculating the product yield by column weighing method; measuring the product yield by high performance liquid chromatography, and then separating by column chromatography to obtain the target product.

[0043] In the following examples, unless otherwise specified, the reaction temperature is room temperature.

[0044] In the following examples, the aromatic compounds used are listed in Table 1, and the corresponding products prepared are listed in Table 2.

[0045] Table 1

[0046]

[0047] Table 2

[0048]

[0049] Example 1 Synthesis of Compound 2a

[0050] (1) 0.1mmol ethylbenzene (compound 1a), 1mmol tetrabutylammonium hexafluorophosphate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 1mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction was completed, the reaction liquid was collected, and the product yield was calculated by HPLC to be 69%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2a, whose hydrogen spectrum and carbon spectrum are shown as follows Figure 3 and Figure 4 shown.

[0051] (2) 0.1mmol ethylbenzene (compound 1a), 1mmol tetrabutylammonium hexafluorophosphate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 3mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction was completed, the reaction liquid was collected, and the product yield was calculated by HPLC to be 89%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2a.

[0052] (3) 0.1mmol ethylbenzene (compound 1a), 1mmol tetrabutylammonium hexafluorophosphate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 5mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction was completed, the reaction liquid was collected, and the product yield was calculated by HPLC method to be 83%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2a.

[0053] (4) 0.1mmol ethylbenzene (compound 1a), 1mmol tetrabutylammonium hexafluoroborate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 3mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction was completed, the reaction liquid was collected, and the product yield was calculated by HPLC to be 86%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2a.

[0054] (5) 0.1mmol ethylbenzene (compound 1a), 1mmol tetrabutylammonium perchlorate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 3mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction was completed, the reaction liquid was collected, and the product yield was calculated by HPLC to be 70%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2a.

[0055] Example 2 Synthesis of Compound 2b

[0056] 0.1mmol 4-chloroethylbenzene (compound 1b), 1mmol tetrabutylammonium hexafluorophosphate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 3mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction, the reaction liquid was collected, and the product yield was calculated by HPLC to be 75%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2b, whose hydrogen spectrum and carbon spectrum are as follows Figure 5 and Figure 6 shown.

[0057] Example 3 Synthesis of Compound 2c

[0058] 0.1mmol 4-methylethylbenzene (compound 1c), 1mmol tetrabutylammonium hexafluorophosphate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 3mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction, the reaction liquid was collected, and the product yield was calculated by HPLC to be 92%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2c, whose hydrogen spectrum and carbon spectrum are as follows Figure 7 and Figure 8 shown.

[0059] Example 4 Synthesis of Compound 2d

[0060] 0.1mmol 4-methoxyethylbenzene (compound 1d), 1mmol tetrabutylammonium hexafluorophosphate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 3mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction, the reaction liquid was collected, and the product yield was calculated by HPLC to be 95%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2d, whose hydrogen spectrum and carbon spectrum are as follows Fig. 9 and Fig.10 shown.

[0061] In the following comparative example 1, the electrolytic cell is provided with a cathode sheet (a carbon paper electrode without Fe-NC material loaded thereon) and an anode sheet (a platinum sheet).

[0062] In the following comparative example 2, the reactor is not provided with an electrocatalytic related reaction device.

[0063] In the following comparative example 3, the electrolytic cell is provided with a cathode sheet (a carbon paper electrode loaded with Fe-NC material) and an anode sheet (a platinum sheet), and oxygen is not introduced into the system.

[0064] In the following comparative example 4, the electrolytic cell is provided with a cathode sheet (a carbon paper electrode loaded with Fe-NC material) and an anode sheet (a platinum sheet), and no water is added to the reaction solution.

[0065] Comparative Example 1: Electrocatalysis without Fe-NC loading for 1d Oxidation of 4-methoxyethylbenzene to 4-methoxyacetophenone for 2d

[0066] 0.1mmol 4-methoxyethylbenzene (compound 1d), 1mmol tetrabutylammonium hexafluorophosphate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 3mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction was completed, the reaction liquid was collected, and the product yield was calculated by HPLC method to be 3%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2d.

[0067] It can be seen from this comparative example that in the case of no supported catalyst, the catalytic efficiency of electrocatalytic aromatic compounds is low, and Fe-NC has good catalytic performance.

[0068] Comparative Example 2: Electrocatalytic oxidation of 4-methoxyethylbenzene to 4-methoxyacetophenone by Fe-NC without electricity for 1d

[0069] 0.1mmol 4-methoxyethylbenzene (compound 1d), 1mmol tetrabutylammonium hexafluorophosphate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to a reaction bottle; oxygen was injected into the solution before the reaction at an injection rate of 20mL / min; the reaction time was 8h; after the reaction was completed, the reaction liquid was collected and the product yield was calculated by HPLC method to be 0.

[0070] It can be seen from this comparative example that in the absence of current, the catalytic efficiency of aromatic compounds is low, indicating that current is a necessary means to catalyze the reaction.

[0071] Comparative Example 3: Electrocatalytic oxidation of 4-methoxyethylbenzene to 4-methoxyacetophenone by Fe-NC loading in an oxygen-free atmosphere for 1d

[0072] 0.1mmol 4-methoxyethylbenzene (compound 1d), 1mmol tetrabutylammonium hexafluorophosphate and 10mL water and acetonitrile (1:19) solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, argon gas was injected into the solution system for 30 minutes to ensure that the solution did not contain oxygen, the distance between the two electrodes was adjusted to 1cm, and the applied current was 3mA; the reaction time was 8h; after the reaction was completed, the reaction liquid was collected, and the product yield was calculated by HPLC method to be 0.

[0073] It can be seen from this comparative example that in the absence of oxygen, the catalytic efficiency of electrocatalytic aromatic compounds is low, indicating that oxygen is a necessary raw material.

[0074] Comparative Example 4: Electrocatalytic oxidation of 4-methoxyethylbenzene to 4-methoxyacetophenone under anhydrous conditions for 1d by Fe-NC support

[0075] 0.1mmol 4-methoxyethylbenzene (compound 1d), 1mmol tetrabutylammonium hexafluorophosphate and 10mL acetonitrile solvent were added to obtain a homogeneous solution, which was added to an electrolytic cell; before the reaction, the distance between the two electrodes was adjusted to 1cm, and the applied current was 3mA; oxygen was injected near the cathode at an injection rate of 20mL / min; the reaction time was 8h; after the reaction was completed, the reaction liquid was collected, and the product yield was calculated by HPLC method to be 5%. The reaction liquid was diluted five times with ethyl acetate, washed with water, dried, filtered, and then eluted with a mixed solvent of ethyl acetate / petroleum ether (1:30) to separate the product 2d.

[0076] It can be seen from this comparative example that in the absence of water as a solvent, the catalytic efficiency of the electrocatalytic aromatic compound is low, indicating that water must be present during the catalytic reaction.

[0077] The present invention provides a method and idea for a method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrodes. There are many methods and approaches to implement the technical solution. The above is only a preferred embodiment of the present invention. It should be pointed out that for ordinary technicians in this technical field, several improvements and modifications can be made without departing from the principle of the present invention. These improvements and modifications should also be regarded as the scope of protection of the present invention. All components not specified in this embodiment can be implemented by existing technologies.

Claims

1. A method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode, characterized in that: A mixed homogeneous solution containing an aromatic compound represented by Formula I, water, an electrolyte, and an organic solvent is placed in an electrolytic cell provided with electrodes and oxygen is introduced to react to obtain an aromatic ketone compound product represented by Formula II; Wherein, the cathode sheet in the electrolytic cell is a carbon paper electrode loaded with Fe-NC; The aromatic compound shown in formula I is: ； I； The aromatic ketone compound shown in formula II is: ； II; In the formula, R1 is selected from any one of benzene, 4-methylbenzene, 4-ethylbenzene, 4-chlorobenzene, 4-methoxybenzene or naphthalene ring.

2. The method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode according to claim 1, characterized in that: The electrolyte is any one of tetrabutylammonium hexafluorophosphate, tetrabutylammonium tetrafluoroborate and tetrabutylammonium perchlorate or a combination of two or more thereof.

3. The method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode according to claim 1, characterized in that: The organic solvent is any one of acetonitrile, methanol, N,N-dimethylformamide and propylene carbonate or a combination of two or more thereof.

4. The method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode according to claim 1, characterized in that: The concentration of the aromatic compound represented by formula I in the mixed homogeneous solution is 5-15 mM.

5. The method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode according to claim 1, characterized in that: The concentration of the electrolyte in the mixed homogeneous solution is 0.05-0.15M.

6. The method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode according to claim 1, characterized in that: The mass ratio of water to organic solvent is 1:14~24.

7. The method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode according to claim 1, characterized in that: The oxygen flow rate introduced during the reaction is 10~30mL / min.

8. The method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode according to claim 1, characterized in that: The reaction temperature is controlled at 20-30°C; the current intensity during the reaction is 1-5 mA; and the reaction residence time is controlled at 6-12 hours.

9. The method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode according to claim 1, characterized in that: The electrolytic cell provided with electrodes comprises a non-sealed electrolytic cell, a cathode sheet, an anode sheet and a DC power supply; the anode sheet is a graphite carbon electrode or a platinum sheet electrode; the cathode sheet is a carbon paper electrode loaded with Fe-NC; The preparation method of the carbon paper electrode loaded with Fe-NC is as follows: Dissolve 2-methylimidazole in methanol to obtain solution A; dissolve zinc acetate and ferric triacetylacetonate in methanol to obtain solution B; mix solution A and solution B, and perform a solvent thermal reaction at 110-130°C for 5-6 hours to obtain a precursor; place the precursor in a N2 atmosphere and calcine at 850-950°C for 1-3 hours to obtain a Fe-NC material; finally, evenly coat the obtained Fe-NC material on a carbon paper electrode.

10. The method for highly selective electrocatalytic oxidation of simple aromatic hydrocarbons by Fe-NC catalytic electrode according to claim 1, characterized in that: After the reaction is completed, the liquid in the electrolytic cell is collected, the reaction solution is diluted with ethyl acetate, washed with water, dried, filtered, and then rinsed and separated with a mixed solvent of ethyl acetate and petroleum ether to obtain the aromatic ketone compound shown in formula II.

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