Preparation method and application of mesoporous anti-perovskite structure electrocatalyst for producing formate through electrooxidation of glucose

Abstract

The invention discloses a preparation method and application of a mesoporous anti-perovskite structure electrocatalyst for producing formate through electrooxidation of glucose, and belongs to the technical field of catalysts. The preparation method of the catalyst comprises the following steps: (1) dispersing Kit-6, copper nitrate and nickel nitrate in a mixed solution to obtain a solution 1; (2) incubating the solution 1 in a drying oven, and evaporating to dryness to obtain a powder precursor 1; (3) transferring the powder precursor 1 into a muffle furnace, and calcining to obtain a powder precursor 2; (4) adding the powder precursor 2 into sodium hydroxide, etching in a drying oven, washing and drying to obtain a powder precursor 3; and (5) transferring the powder precursor 3 into a tubular furnace, and calcining in an NH3 atmosphere to obtain the mesoporous anti-perovskite structure electrocatalyst. The catalyst prepared by the invention uses non-noble metal, so that the synthesis cost is reduced; the preparation process is simple. The catalyst is applied to production of formate through electrooxidation of glucose, and has the advantages of high catalytic stability, high formate yield and the like.

Description

Technical Field

[0001] The present invention relates to the field of catalyst technology, and in particular to a preparation method and application of a mesoporous anti-perovskite structure electrocatalyst for producing formate by electrooxidation of glucose. Background Art

[0002] Formate (FA), an important class of chemicals, has a wide range of applications in industry, agriculture, environmental protection, and new energy due to its unique physical and chemical properties. For example, it can be used as a direct liquid fuel and hydrogen storage medium for fuel cells, as a deicer and snowmelt, and more. Currently, the traditional method for producing formate is to use CO and alkali under high temperature and high pressure. This not only has extremely high energy consumption but also easily produces byproducts such as CO2. Therefore, finding a green and pollution-free method for producing formate is of great significance.

[0003] Biomass is a rich and sustainable carbon resource that can replace non-renewable fossil resources for chemical and fuel production, aligning with national industrial decarbonization and denitrification goals. Unlike fossil feedstocks, biomass is typically rich in oxygen and carbon sources, making it an ideal starting material for the production of valuable oxygenates such as formic acid (FA), adipic acid (AA), and 2,5-furandicarboxylic acid (FDCA). Therefore, using renewable energy to generate formate via biomass electrocatalysis is an effective alternative for the synthesis and utilization of waste.

[0004] Glucose, a biomass source, is inexpensive and readily available because it can be directly extracted from starch collected from food processing waste and agricultural residues. Furthermore, its long carbon chain and abundant carbon reserves make it a promising candidate for producing formate via the electrocatalytic oxidation reaction (GOR). To improve glucose oxidation efficiency and formate yield to meet industrial production requirements, the development of high-performance glucose electrooxidation catalysts is crucial.

[0005] However, the excessively long carbon chain of glucose leads to incomplete cleavage of the C-C bond during catalysis, resulting in the generation of a variety of intermediates and byproducts. Furthermore, the inherently high reactivity of oxygen-containing functional groups in glucose often causes biomass upgrading to undergo undesirable reconstruction under extreme reaction conditions, further reducing the selectivity and Faradaic efficiency of electrocatalytic glucose-to-formate conversion. Furthermore, competition with the oxygen evolution reaction (OER) at the anodic potential significantly reduces the Faradaic efficiency of FA and increases energy consumption.

[0006] One potential catalyst design strategy is to exploit the direct oxidation mechanism of alloys or metalloids with low metal valence, thereby reducing the formation of intermediates. Recent research has led to significant efforts in designing Ni and Co DAC catalysts with Ni-N4 and Co-N4 coordination configurations, effectively enhancing the catalytic activity for glycerol oxidation. This has inspired the exploration of catalysts with active metal and nitrogen coordination to achieve efficient glucose oxidation to formate. Antiperovskite materials with the ABX3 chemical structure (A is a transition metal or nonmetal ion, B is a nonmetal anion, and X is a cation) are electron-inverted perovskite derivatives. They not only inherit the structural characteristics of perovskites but also exhibit unique physicochemical properties due to the abundance of cations at the X position. Among them, magnetic-element-rich antiperovskite nitrides (ANX3, where X = Co, Ni, Mn, Fe, etc.) exhibit exceptionally high electrical and thermal conductivity and mechanical properties, thus possessing strong electrocatalytic potential. Furthermore, mesoporous materials, with their abundant pores, not only expose numerous active sites but also exhibit confined properties that facilitate the adsorption and conversion of reactants. Therefore, designing antiperovskite materials with mesoporous and magnetic characteristics may be of great significance for developing high-performance catalysts for glucose oxidation to formate. Summary of the Invention

[0007] The purpose of the present invention is to provide a preparation method and application of a mesoporous antiperovskite structure electrocatalyst for producing formate by glucose electrooxidation, so as to solve technical problems such as high overpotential, low catalytic efficiency and poor catalyst stability during glucose electrooxidation.

[0008] To achieve the above objectives, the present invention provides the following technical solution: a method for preparing a mesoporous antiperovskite structure electrocatalyst for the electrooxidation of glucose to produce formate, the method comprising:

[0009] S1: Preparation of solution 1: Disperse pre-synthesized Kit-6, copper nitrate, and nickel nitrate in a mixed solution of ethanol and water, and mix well to obtain solution 1;

[0010] S2: Preparation of powder precursor 1: placing the solution 1 in an oven and incubating until the solution is evaporated to dryness to obtain the powder precursor 1;

[0011] S3: Preparation of powder precursor 2: transferring the powder precursor 1 to a muffle furnace for calcination to obtain the powder precursor 2;

[0012] S4: Preparation of powder precursor 3: Add the powder precursor 2 to sodium hydroxide and transfer it to an oven for etching to obtain an etched solid powder; wash the etched solid powder with an ethanol solution and dry it in a vacuum drying oven at 60° C. for 3 hours to obtain a powder precursor 3;

[0013] S5: Preparation of the final product - mesoporous antiperovskite structure electrocatalyst: The powder precursor 3 is transferred to a tube furnace and calcined under an NH3 atmosphere to obtain an electrocatalyst having a mesoporous antiperovskite structure.

[0014] Preferably, in S1, the method for preparing the pre-synthesized Kit-6 is:

[0015] H1: Prepare Pluronic P123 solution: Dissolve 7.9 g of concentrated HCl solution and 4.0 g of Pluronic P123 in 144 ml of distilled water, and stir at 35°C until completely dissolved and a white, clear state is obtained to obtain the Pluronic P123 solution; the mass fraction of the concentrated HCl solution is 37%;

[0016] H2: Preparation of solid product: 4.0 g of n-butanol was added to the Pluronic P123 solution, and the mixture was stirred at 35°C for 1 hour. 8.6 g of tetraethoxysilane was then added, and the mixture was stirred at 35°C for 24 hours to obtain a mixed solution. The mixed solution was then placed in a water bath at 75°C for 24 hours, and the solid product was collected by filtration.

[0017] H3: Preparation of pre-synthesized Kit-6: The solid product was washed with water / ethanol in a volume ratio of 3:1 and vacuum dried to obtain a solid powder; the solid powder was transferred to a muffle furnace, and the temperature was increased from room temperature to 550°C at a rate of 2°C / min, and calcined at 550°C for 6 h to obtain the pre-synthesized Kit-6.

[0018] Preferably, in S1, the method for preparing the solution 1 is:

[0019] 0.5 g of the pre-synthesized Kit-6, 0.1208 g of copper nitrate, and 0.436 g of nickel nitrate were added to a beaker, and 5 ml of ethanol and 1 ml of water were added and mixed well to prepare the solution 1.

[0020] Preferably, in said S2, the specific condition of incubation in the oven is incubation in an oven at 75°C for 10 hours.

[0021] Preferably, in S3, the powder precursor 1 is transferred to a muffle furnace for calcination, specifically placing the powder precursor 1 into a muffle furnace, heating it to 240°C at a rate of 5°C / min, maintaining it for 3 hours, and then heating it to 550°C for calcination for 6 hours.

[0022] Preferably, in S4, the amount of sodium hydroxide added to the powder precursor 2 is 20 mL 2 mol·L -1 Sodium hydroxide solution.

[0023] Preferably, in S4, the specific etching conditions in the oven are etching in an 80°C oven for 24 hours; the ethanol solution is a mixed solution of anhydrous ethanol and deionized water in a volume ratio of 3:1; the etched solid powder is washed with an ethanol solution and dried, and the drying conditions are drying at 60°C in a vacuum drying oven for 3 hours.

[0024] Preferably, in S5, the NH3 atmosphere is specifically an NH3 atmosphere with a flow rate of 0.04 L·min -1 .

[0025] Preferably, in S5, the calcination conditions are as follows: a heating rate of 5°C / min, a reaction temperature of 450°C, and a reaction time of 3h.

[0026] The prepared mesoporous antiperovskite structure electrocatalyst is used in the electrooxidation of glucose to produce formate.

[0027] Compared with the prior art, the present invention has the following beneficial effects:

[0028] (1) The catalyst prepared by the present invention has unique functional characteristics and is applicable to the oxidation of glucose to formate. The m-CuNi3N catalyst has a unique antiperovskite structure and a mesoporous structure with uniform and ordered pores, which can achieve a structural synergistic effect that promotes the electrooxidation of glucose to formate. The use of this catalyst can achieve high Faradaic efficiency, high selectivity, and high stability in the electrolysis of glucose to formate.

[0029] (2) The catalyst prepared by the present invention uses only non-precious metals, which greatly reduces the cost of raw materials; and the process is simple, easy to operate, and the product has good stability, and can be industrially produced.

[0030] (3) The catalyst prepared by the present invention can significantly enhance the glucose C-C bond cleavage rate, reduce the formation of byproducts, and inhibit the OER process. This not only improves the selectivity of glucose electrooxidation to formic acid but also reduces the energy consumption of the reaction. Therefore, the catalyst achieves a "win-win" in terms of biomass upgrading and energy consumption reduction. BRIEF DESCRIPTION OF THE DRAWINGS

[0031] Figure 1 1 is an X-ray diffraction pattern (XRD) of the mesoporous antiperovskite m-CuNi3N catalyst prepared in Example 1 of the present invention and the comparative catalyst mesoporous Ni4N (m-Ni4N);

[0032] Figure 2 is a transmission electron microscopy (TEM) image of the m-CuNi3N catalyst prepared in Example 1 of the present invention;

[0033] Figure 3Linear sweep voltammetry (LSV) curves of the m-CuNi3N catalyst prepared in Example 1 of the present invention and the comparative catalysts m-Ni4N and CuNi3N (with or without glucose);

[0034] Figure 4 The performance diagram of the m-CuNi3N catalyst prepared in Example 1 of the present invention and the comparative catalysts m-Ni4N and CuNi3N in the electrooxidation of glucose to formate (electrolysis at different voltages for 1 hour, the electrolyte is 1.0 mol·L -1 KOH + 0.1 mol L -1 Glucose);

[0035] Figure 5 is a graph showing the current density of the m-CuNi3N catalyst prepared in Example 1 of the present invention for the formation of formate;

[0036] Figure 6 The cyclic stability performance diagram of the m-CuNi3N catalyst prepared in Example 1 of the present invention (the electrolyte is 1.0 mol·L -1 KOH + 0.1 mol L -1 Glucose);

[0037] Figure 7 3 is a graph showing the relationship between current density and time for the m-CuNi3N catalyst prepared in Example 1 of the present invention at different voltages with or without glucose. DETAILED DESCRIPTION

[0038] The technical solutions in the embodiments of the present invention will be described clearly and completely below. Obviously, the embodiments described are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without making creative work are within the scope of protection of the present invention. The experimental methods described in the following embodiments are all conventional methods unless otherwise specified; the reagents and materials, unless otherwise specified, can be obtained from commercial channels.

[0039] Example 1

[0040] (1) Preparation of mesoporous antiperovskite structure electrocatalysts:

[0041] S1: Preparation of solution 1: 0.5 g of the pre-synthesized Kit-6 was mixed with 0.1208 g of copper nitrate and 0.436 g of nickel nitrate in a beaker, and 5 ml of ethanol and 1 ml of water were added and mixed well to obtain solution 1.

[0042] The steps for preparing pre-synthesized Kit-6 are as follows:

[0043] 7.9 g of concentrated HCl solution (37 wt%) and 4.0 g of Pluronic P123 were dissolved in 144 ml of distilled water and stirred at 35 ° C for several hours until completely dissolved into a white clear state; 4.0 g of n-butanol was continuously injected and stirred at 35 ° C for 1 hour; 8.6 g of tetraethoxysilane (TEOS) was directly poured into the above transparent solution, vigorously stirred at 35 ° C for 24 hours, and then in a water bath at 75 ° C for 24 hours. The solid product was collected by filtration and then washed with water / ethanol with a volume ratio of 3:1; after vacuum drying, the solid powder was transferred to a muffle furnace, heated from room temperature to 550 ° C at 2 ° C / min, and calcined at 550 ° C for 6 hours to obtain the pre-synthesized Kit-6.

[0044] S2: Preparation of powder precursor 1: Place the beaker containing solution 1 in an oven at 75° C. and incubate for 10 h until the solution is evaporated to dryness, thereby obtaining the powder precursor 1;

[0045] S3: Preparation of powder precursor 2: Transfer the powder precursor 1 to a muffle furnace, heat it to 240°C at 5°C / min, maintain it for 3 hours, and then continue heating it to 550°C and calcining it for 6 hours to obtain the powder precursor 2;

[0046] S4: Preparation of powdered precursor 3: Add the powdered precursor 2 to 20 mL of 2 mol·L -1 The resulting product was added to sodium hydroxide and transferred to an 80°C oven for etching for 24 h. The product was then washed with a mixed solution of anhydrous ethanol and deionized water in a volume ratio of 3:1 and dried in a vacuum drying oven at 60°C for 3 h to obtain a powder precursor 3.

[0047] S5: Preparation of the final product - mesoporous antiperovskite structure electrocatalyst: The powder precursor 3 was transferred to a tube furnace and calcined at a flow rate of 0.04 L min-1 of NH3 atmosphere. -1 , the heating rate was 5℃ / min, the reaction temperature was 450℃, the reaction time was 3h, and an electrocatalyst (m-CuNi3N) with a mesoporous antiperovskite structure was obtained.

[0048] (2) Preparation of working electrode

[0049] 5 mg of the prepared m-CuNi3N catalyst was weighed and thoroughly mixed with 2.5 mg of Vulcan XC-72 carbon black. 5 mg of the carbon black-loaded m-CuNi3N catalyst was mixed with 0.4 mL of deionized water, 0.52 mL of anhydrous ethanol, and 0.08 mL of naphthol solution. The mixed solution was ultrasonicated for 0.5 h to obtain 5 mg mL -1m-CuNi3N catalyst solution. Use a pipette to draw 0.005mL of catalyst solution and evenly apply it on a 1cm×0.5cm clean carbon paper to make the catalyst loading amount 0.05mg / cm -2 After drying, use it with the clip electrode as the working electrode. Before use, the carbon paper needs to be ultrasonically washed several times with an ethanol / water solution to remove possible contamination sources.

[0050] (3) Electrocatalytic oxidation of glucose to formate

[0051] The electrochemical oxidation of glucose to formate was carried out using a Chenhua 660e electrochemical workstation. The test used a typical three-electrode system, with m-CuNi3N as the working electrode, a saturated Hg / HgCl2 electrode as the reference electrode, and a 1cm×0.5cm platinum sheet electrode as the counter electrode. The electrolytic cell used was an H-type electrolytic cell with a concentration of 1.0 mol·L -1 KOH and 0.1 mol·L -1 The glucose mixed solution served as the electrolyte. In the electrochemical test, the reaction temperature was 25°C and the applied potential was +1.2V to +1.9V vs. RHE.

[0052] Comparative Example 1

[0053] Preparation of m-Ni4N

[0054] 0.4 g of pre-synthesized Kit-6 was mixed with 0.436 g of nickel nitrate in a beaker, and 5 ml of ethanol and 1 ml of water were added and mixed evenly. The beaker containing the solution was placed in an oven at 75 °C and incubated for 10 h. The fully dried solid powder was transferred to a muffle furnace and heated to 240 °C at 5 °C / min, maintained for 3 h, and then continued to heat to 550 °C and calcined for 6 h. The solid powder was taken out and added to 20 mL of 2 mol·L -1 The samples were then placed in a 80°C oven and etched for 24 h. The samples were then washed and dried using a mixture of anhydrous ethanol and deionized water in a volume ratio of 3:1. After sufficient drying, the samples were transferred to a tube furnace and calcined at an NH3 atmosphere flow rate of 0.04 L min. -1 , the heating rate was 5℃ / min, the reaction temperature was 450℃, the reaction time was 3h, and a Ni4N electrocatalyst with a mesoporous structure (m-CuNi3N) was obtained.

[0055] Comparative Example 2

[0056] Preparation of CuNi3N

[0057] 0.1208 g of copper nitrate and 0.436 g of nickel nitrate were mixed in a beaker, 5 ml of ethanol and 1 ml of water were added, and the mixture was mixed evenly. The beaker containing the solution was placed in an oven at 75 ° C for 10 h. The fully dried solid powder was transferred to a muffle furnace, heated to 240 ° C at 5 ° C / min, maintained for 3 h, and then continued to heat to 550 ° C and calcined for 6 h. The solid powder was removed and transferred to a tube furnace for calcination, wherein the NH3 atmosphere flow rate was 0.04 L·min -1 , the heating rate is 5℃ / min, the reaction temperature is 350℃, the reaction time is 3h, and an electrocatalyst (CuNi3N) with an antiperovskite structure is obtained.

[0058] In the test of electrocatalytic glucose oxidation to formate, linear sweep voltammetry (LSV) was used to record the current density (j) within the applied voltage range, which can be used to characterize the electrochemical behavior within this voltage range. The LSV scan rate was 10 mV s -1 The scanning voltage range is +1.2 V to +1.9 V vs. RHE relative to the reversible hydrogen electrode; the constant voltage method can be used to record the current-time (it) curve under the applied potential, which is used to record the charge (Q) to calculate the Faradaic efficiency (FE); the applied voltage range in the embodiment of the present invention is +1.5 V to +1.75 V vs. RHE relative to the reversible hydrogen electrode; the glucose oxidation product formate was analyzed using nuclear magnetic resonance (NMR).

[0059] The Faradaic efficiency of formate is calculated as follows:

[0060] FE FA =(2×F×C FA ×V×10 -6 ) / Q×100%

[0061] The formate yield was calculated as follows:

[0062] Yield rate (FA) = (C FA ×V) / (t×s)

[0063] Among them C FA is the measured formate concentration (mmol·L -1 ); V is the volume of the electrolyte (10 mL); s is the loading area of the catalyst (0.5 cm -2 ); t is the electrolysis time (1 h); F is the Faraday constant (96485 C mol· -1 ); Q(C) is the total charge passing through the electrode, which is the result of the integration of the it curve.

[0064] Analysis of the catalyst performance test results obtained in Example 1, Comparative Example 1 and Comparative Example 2:

[0065] Figure 1 The X-ray diffraction patterns (XRD) of the mesoporous antiperovskite m-CuNi3N catalyst prepared in Example 1 of the present invention and the comparative catalyst m-Ni4N in Comparative Example 1 show that both m-CuNi3N and m-Ni4N exhibit clear diffraction peaks. m-CuNi3N corresponds to the (111), (200), (220), and (311) planes of an antiperovskite nitride with a face-centered cubic structure (space group Fm-3m), while m-Ni4N corresponds to the (111), (200), and (220) planes of a face-centered cubic structure. Furthermore, m-CuNi3N was found to contain only the antiperovskite nitride phase, with no other phases present.

[0066] Figure 2 This is a scanning transmission electron microscopy (STEM) image of the m-CuNi3N catalyst prepared in Example 1 of the present invention. The image shows that the catalyst is a nanoparticle structure with abundant and ordered mesoporous channels ( Figure 2 a). In addition, high-resolution TEM (HRTEM) images and corresponding fast Fourier transform (FFT) patterns further revealed the crystal structure of the catalyst at the atomic scale ( Figure 2 bc), HRTEM shows that the lattice spacing of m-CuNi3N is 0.236nm, corresponding to the (111) crystal plane of m-CuNi3N, which confirms the successful preparation of the antiperovskite nitride catalyst m-CuNi3N. The FFT patterns observed from the two locations of m-CuNi3N are exactly the same, indicating that the (111) crystal plane of the catalyst is the main exposed crystal plane.

[0067] Figure 3 The LSV curves for the m-CuNi3N catalyst prepared in Example 1 and the comparative catalysts (m-Ni4N and CuNi3N) from Comparative Examples 1 and 2, in the presence and absence of glucose, are shown. The graph shows that the m-CuNi3N catalyst exhibits the highest glucose oxidation current density, demonstrating that the m-CuNi3N nanocatalyst possesses the best electrocatalytic glucose oxidation activity.

[0068] Figure 4 This figure shows the Faradaic efficiency and yield of formate produced by electrooxidation of glucose using the m-CuNi3N catalyst prepared in Example 1 of the present invention and the comparative catalysts (m-Ni4N, CuNi3N) from Comparative Examples 1-2. The figure shows that the m-CuNi3N catalyst achieved an optimal Faradaic efficiency of 92.99% at +1.55 V vs. RHE. Its highest formate yield was 3.375 mmol h-1. - 1 cm -2 , which is much higher than that of the comparative catalyst m-Ni4N (0.462 mmol h -1cm -2 ) and CuNi3N(0.568mmol h -1 cm -2 ).

[0069] Figure 5 Figure 2 shows the partial current density of glucose electrooxidation to formate using the m-CuNi3N catalyst prepared in Example 1 of the present invention and the comparative catalysts (m-Ni4N and CuNi3N) from Comparative Examples 1 and 2. The figure shows that the m-CuNi3N catalyst has the highest partial current density for formate at various voltages.

[0070] Figure 6 This is a graph showing the cyclic stability of the m-CuNi3N catalyst prepared in Example 1 of the present invention for the electrooxidation of glucose to formate. The graph shows that after 15 cycles, the performance of the m-CuNi3N catalyst has hardly decayed.

[0071] Figure 7 The graph shows the relationship between current density and time of the m-CuNi3N catalyst prepared in Example 1 of the present invention with or without 100 mM glucose at different voltages, which proves that the glucose oxidation reaction exhibits a current density much higher than that of the oxygen evolution reaction within a wide voltage range.

[0072] The present invention synthesized for the first time a mesoporous antiperovskite structure (m-CuNi3N) electrocatalyst with unique functional characteristics and applied it to the electrocatalytic oxidation of glucose to formate. The m-CuNi3N catalyst with an antiperovskite structure and abundant ordered mesopores can perfectly achieve the structural synergistic effect that promotes the electrocatalysis of glucose to formate. The main reason is that the reaction mediated by the mesoporous m-CuNi3N is a direct oxidation mechanism, and OOH* is not formed. It not only avoids the high overpotential caused by metal reconstruction in the indirect oxidation mechanism, but also the direct contact reaction between the catalyst and glucose reduces the formation of intermediates. The nano-confinement effect of the mesopores and the ultra-fast electron transport capability of the antiperovskite nitride structure allow a large amount of glucose to be quickly bound to the catalyst surface and realize rapid electron exchange, which suppresses the competing reaction of OER and thus improves the reaction efficiency. Therefore, the use of this catalyst can achieve better activity, selectivity and stability for the electroreduction of glucose to formic acid.

[0073] The catalyst prepared by this invention, due to its unique structural characteristics, can accelerate the attack of OH* on glucose, prompting rapid cleavage of C-C bonds, thereby achieving high-rate electrosynthesis of formate. Therefore, this invention achieves a "win-win" in terms of reducing energy consumption and upgrading biomass. More importantly, the catalyst prepared by this invention does not use precious metals, significantly reducing raw material costs. Furthermore, the process is simple, easy to operate, the product is stable, and can be produced in large quantities, making it suitable for large-scale industrial production.

[0074] Finally, it should be noted that the above descriptions are merely preferred embodiments of the present invention and are not intended to limit the present invention. Although the present invention has been described in detail with reference to the aforementioned embodiments, those skilled in the art will be able to modify the technical solutions described in the aforementioned embodiments or substitute equivalents for some of the technical features. Any modifications, equivalent substitutions, and improvements made within the spirit and principles of the present invention shall be included within the scope of protection of the present invention.

Claims

1. A method for preparing a mesoporous antiperovskite electrocatalyst for the electrooxidation of glucose to produce formate, characterized by: The preparation method of the mesoporous antiperovskite structure electrocatalyst comprises: S1: Preparation of solution 1: Disperse pre-synthesized Kit-6, copper nitrate, and nickel nitrate in a mixed solution of ethanol and water, and mix well to obtain solution 1; S2: Preparation of powder precursor 1: placing the solution 1 in an oven and incubating until the solution is evaporated to dryness to obtain the powder precursor 1; S3: Preparation of powder precursor 2: transferring the powder precursor 1 to a muffle furnace for calcination to obtain the powder precursor 2; S4: Preparation of powder precursor 3: adding the powder precursor 2 to sodium hydroxide and transferring it to an oven for etching to obtain an etched solid powder; washing the etched solid powder with an ethanol solution and drying it in a vacuum drying oven at 60° C. for 3 h to obtain the powder precursor 3; S5: Preparation of the final product - mesoporous antiperovskite structure electrocatalyst: The powder precursor 3 is transferred to a tube furnace and calcined under an NH3 atmosphere to obtain an electrocatalyst having a mesoporous antiperovskite structure.

2. The method for preparing a mesoporous antiperovskite structure electrocatalyst for producing formate by electrooxidation of glucose according to claim 1, characterized in that: In S1, the method for preparing the pre-synthesized Kit-6 is specifically: H1: Prepare Pluronic P123 solution: Dissolve 7.9 g of concentrated HCl solution and 4.0 g of Pluronic P123 in 144 ml of distilled water, and stir at 35°C until completely dissolved and a white, clear state is obtained to obtain the Pluronic P123 solution; the mass fraction of the concentrated HCl solution is 37%; H2: Preparation of solid product: 4.0 g of n-butanol was added to the Pluronic P123 solution, and the mixture was stirred at 35°C for 1 hour. 8.6 g of tetraethoxysilane was then added, and the mixture was stirred at 35°C for 24 hours to obtain a mixed solution. The mixed solution was then placed in a water bath at 75°C for 24 hours, and the solid product was collected by filtration. H3: Preparation of pre-synthesized Kit-6: The solid product was washed with water / ethanol in a volume ratio of 3:1 and vacuum dried to obtain a solid powder; the solid powder was transferred to a muffle furnace, and the temperature was increased from room temperature to 550°C at a rate of 2°C / min, and calcined at 550°C for 6 h to obtain the pre-synthesized Kit-6.

3. The method for preparing a mesoporous antiperovskite structure electrocatalyst for producing formate by electrooxidation of glucose according to claim 1, characterized in that: In S1, the method for preparing the solution 1 is specifically: 0.5 g of the pre-synthesized Kit-6, 0.1208 g of copper nitrate, and 0.436 g of nickel nitrate were added to a beaker, and 5 ml of ethanol and 1 ml of water were added and mixed well to prepare the solution 1.

4. The method for preparing a mesoporous antiperovskite structure electrocatalyst for producing formate by electrooxidation of glucose according to claim 1, characterized in that: In the step S2, the specific conditions for incubating in the oven are incubating in an oven at 75°C for 10 hours.

5. The method for preparing a mesoporous antiperovskite structure electrocatalyst for producing formate by electrooxidation of glucose according to claim 1, characterized in that: In S3, the powder precursor 1 is transferred to a muffle furnace for calcination. Specifically, the powder precursor 1 is placed in a muffle furnace, heated to 240° C. at a rate of 5° C. / min, maintained for 3 h, and then heated to 550° C. for calcination for 6 h.

6. The method for preparing a mesoporous antiperovskite structure electrocatalyst for producing formate by electrooxidation of glucose according to claim 1, characterized in that: In the step S4, the amount of sodium hydroxide added to the powder precursor 2 is specifically 20 mL 2 mol·L -1 Sodium hydroxide solution.

7. The method for preparing a mesoporous antiperovskite structure electrocatalyst for producing formate by electrooxidation of glucose according to claim 1, characterized in that: In S4, the specific etching conditions in the oven are etching in an 80°C oven for 24 hours; the ethanol solution is a mixed solution of anhydrous ethanol and deionized water in a volume ratio of 3:1; the etched solid powder is washed with an ethanol solution and dried, and the drying condition is drying in a vacuum drying oven at 60°C for 3 hours.

8. The method for preparing a mesoporous antiperovskite structure electrocatalyst for producing formate by electrooxidation of glucose according to claim 1, characterized in that: In the step S5, the NH3 atmosphere is specifically an NH3 atmosphere with a flow rate of 0.04 L·min -1 .

9. The method for preparing a mesoporous antiperovskite structure electrocatalyst for producing formate by electrooxidation of glucose according to claim 1, characterized in that: In S5, the calcination conditions are specifically: a heating rate of 5°C / min, a reaction temperature of 450°C, and a reaction time of 3 hours.

10. Use of the mesoporous antiperovskite structure electrocatalyst prepared according to any one of claims 1 to 9, characterized in that: The mesoporous antiperovskite structure electrocatalyst is used in the electrooxidation of glucose to produce formate.

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