Transition metal catalyst electrode for hydrogen production by reforming polyethylene glycol as well as preparation method and application of transition metal catalyst electrode

Abstract

The invention belongs to the field of waste polymer electrochemical reforming hydrogen production, and particularly relates to a transition metal catalyst electrode for polyethylene glycol reforming hydrogen production and a preparation method and application thereof. The transition metal catalyst electrode is composed of a conductive self-supporting substrate and a transition metal ion-dopamine complexing layer coated on the self-supporting substrate. The novel self-supporting catalyst electrode for polyethylene glycol electrochemical reforming hydrogen production provided by the invention can realize electrochemical upgrading and recovery of polyethylene glycol, and a polyethylene glycol oxidation reaction with more dynamic advantages is used for replacing an anode oxygen evolution reaction of traditional water electrolysis, so that the polyethylene glycol is upgraded and recovered into a chemical value-added product at an anode; and high-efficiency hydrogen evolution is realized at the cathode, so that the method has dual environment-friendly practical significance.

Description

Technical Field

[0001] The present invention belongs to the field of electrochemical reforming of waste polymers to produce hydrogen, and specifically relates to a transition metal catalyst electrode for polyethylene glycol reforming to produce hydrogen, and a preparation method and application thereof. Background Art

[0002] Polyethylene glycol (PEG) is a colorless, odorless and lubricating compound commonly used in medicine, cosmetics, industry and chemistry. Currently, the global polyethylene glycol market is worth over US$40 billion. With the booming polyethylene glycol market, a large amount of polyethylene glycol waste is also generated. Therefore, the recycling technology of waste polyethylene glycol has attracted widespread attention. Traditional polyethylene glycol recovery methods require high energy input, which is accompanied by expensive solutions. Electrochemical recycling is a new alternative method that can be powered by green energy (wind, water and solar energy) and can convert and recycle waste polyethylene glycol at relatively low energy.

[0003] Hydrogen energy stands out among many new energy sources due to its high energy density and clean and pollution-free characteristics. Hydrogen production is located at the upstream of the industrial chain. Therefore, the core issue is to develop simple and efficient hydrogen production technology to improve the efficiency of hydrogen energy production. Hydrogen production through water electrolysis is considered to be a promising way. However, the commercial application of electrochemical water electrolysis is still limited by the slow kinetics and high overpotential of the anodic oxygen evolution reaction (OER), which leads to limited hydrogen production efficiency. Compared with OER, the anodic polyethylene glycol oxidation reaction (PEGOR) can have a lower kinetic barrier and produce chemical value-added products, making it a favorable candidate to replace OER.

[0004] Therefore, the development of anodic polyethylene glycol oxidation electrocatalysts with high electroactivity, high selectivity and high stability for electrochemical reforming to produce hydrogen has attracted increasing attention. Summary of the Invention

[0005] The purpose of the present invention is to provide a transition metal catalyst electrode that can be used for the electrochemical reuse of polyethylene glycol and realize reforming hydrogen production, which enables the anodic polyethylene glycol oxidation reaction to replace the kinetically slow anodic oxygen evolution reaction, greatly improving the efficiency of hydrogen production by electrolysis of water.

[0006] To achieve the above object, the present invention is implemented through the following technical solutions:

[0007] In one aspect, the present invention provides a transition metal catalyst electrode for polyethylene glycol reforming to produce hydrogen, wherein the transition metal catalyst electrode comprises a conductive self-supporting substrate and a transition metal ion-dopamine complex layer coated on the self-supporting substrate.

[0008] Furthermore, the self-supporting substrate is selected from metal or alloy mesh, foam metal or foam alloy, metal or alloy sheet, and non-metallic substrate.

[0009] Furthermore, the metal or alloy mesh is a stainless steel mesh or a nickel mesh, the foam metal or foam alloy is foam nickel, foam iron, foam titanium or foam nickel-iron alloy, the metal or alloy sheet is a nickel sheet, iron sheet, titanium sheet or nickel-iron alloy sheet, and the non-metallic substrate is carbon paper, carbon cloth or carbon fiber.

[0010] Furthermore, the transition metal ions are selected from one or more of Fe, Co, Ni and Cu.

[0011] Furthermore, the dopamine is dopamine hydrochloride.

[0012] In another aspect, the present invention provides a method for preparing a transition metal catalyst electrode for polyethylene glycol reforming to produce hydrogen as described herein, comprising the following steps:

[0013] (1) pre-treating the conductive self-supporting substrate to obtain a clean self-supporting substrate;

[0014] (2) placing the pretreated self-supporting substrate in an alkaline mixed solvent;

[0015] (3) adding transition metal ions and dopamine to react to form a transition metal ion-dopamine complex layer coated on the self-supporting substrate;

[0016] (4) washing the product and drying it to obtain the transition metal catalyst electrode.

[0017] Furthermore, the pretreatment includes ultrasonically cleaning the self-supporting substrate in dilute hydrochloric acid, acetone and deionized water respectively.

[0018] Furthermore, the concentration of the dilute hydrochloric acid is 0.1-2 mol L -1 .

[0019] Furthermore, the ultrasonic cleaning time may be 15 minutes.

[0020] Furthermore, the alkaline mixed solvent is prepared from deionized water, ethanol and ammonia water.

[0021] Furthermore, the transition metal ions are selected from one or more of Fe, Co, Ni and Cu.

[0022] Furthermore, the transition metal ions are provided by chlorides, nitrates or hydrates of transition metals such as Fe, Co, Ni and Cu.

[0023] Furthermore, the dopamine is dopamine hydrochloride.

[0024] Furthermore, the molar ratio of the added transition metal ions to dopamine is 1:2-4.

[0025] Furthermore, when the transition metal ion includes two different metal ions, the molar ratio of the two metal ions is 1:1.

[0026] Furthermore, the reaction in step (3) comprises reacting at room temperature for 24-72 hours.

[0027] Furthermore, the reaction in step (3) can be carried out under stirring.

[0028] Furthermore, deionized water can be used for washing in step (4).

[0029] Furthermore, the drying in step (4) may include drying at 60° C. overnight.

[0030] In other aspects, the present invention also provides the use of the transition metal catalyst electrode for polyethylene glycol reforming to produce hydrogen as described herein or the transition metal catalyst electrode for polyethylene glycol reforming to produce hydrogen obtained by the preparation method described herein in the electrochemical reuse of waste polyethylene glycol.

[0031] Furthermore, the transition metal catalyst electrode is used to catalyze the reforming of waste polyethylene glycol to produce hydrogen.

[0032] Advantageous Effects of the Invention

[0033] The novel self-supporting catalyst electrode for electrochemical reforming of polyethylene glycol to produce hydrogen provided by the present invention has the following advantages: (1) The present invention provides a novel self-supporting catalyst electrode and uses it for electrochemical upgrading and recovery of polyethylene glycol, with a mild reaction process, safe preparation and production, and a simple preparation process; (2) The present invention replaces the anode oxygen evolution reaction of traditional water electrolysis with a polyethylene glycol oxidation reaction with greater kinetic advantages, achieving the technical effects of low starting voltage and large potential reduction, and significantly improving the cathode hydrogen energy production efficiency.

[0034] In summary, the present invention combines the electrochemical upgrading and recycling of polyethylene glycol with the electrolytic hydrogen evolution of water, realizing the upgrading and recycling of polyethylene glycol into chemical value-added products at the anode and achieving efficient hydrogen evolution at the cathode, which has dual environmental protection practical significance. BRIEF DESCRIPTION OF THE DRAWINGS

[0035] Figure 1 Scanning electron microscopy and transmission electron microscopy images of the NiCu catalyst electrode prepared in Example 1: (a) SEM image, (b-c) HRTEM images, and (dh) selected areas and corresponding element mapping of C, N, O, Ni, and Cu.

[0036] Figure 2This is the X-ray photoelectron spectrum of the NiCu catalyst electrode prepared in Example 1.

[0037] Figure 3 For Example 1-2 in KOH (1 mol L -1 ) in the linear sweep voltammetry curve.

[0038] Figure 4 For comparative examples 1-8, the KOH (1 mol L -1 ) in the linear sweep voltammetry curve.

[0039] Figure 5 The value of Example 1 at 100 mA cm -2 Stability curves in KOH (1 mol L-1) with and without polyethylene glycol (PEG 200) at different current densities. DETAILED DESCRIPTION

[0040] The present invention relates to a transition metal catalyst electrode, and a preparation method thereof comprises the following steps:

[0041] First, nickel foam was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and deionized water for 15 minutes. The pretreated clean nickel foam was then placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia water (1.5 mL). Subsequently, a certain amount of metal ions and dopamine hydrochloride (1 g) were added to the above mixture and stirred at room temperature for 48 hours. After the reaction, the product was washed with deionized water and dried in an oven at 60°C overnight to obtain a metal ion composite membrane (transition metal ion-dopamine complex layer) catalyst electrode coated on the nickel foam.

[0042] Wherein, the metal ions are chlorides or nitrates of Fe, Co, Ni, Cu and hydrates thereof.

[0043] The present invention is further described below with reference to specific examples, which, however, are not intended to limit the present invention in any way. Unless otherwise specified, the reagents, methods, and equipment used in the present invention are conventional reagents, methods, and equipment in the art.

[0044] Example 1

[0045] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0046] S2: The clean nickel foam was placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia (1.5 mL).

[0047] S3: Add nickel chloride hexahydrate (0.9 mmol), cupric chloride dihydrate (0.9 mmol), and dopamine hydrochloride (DA, 1 g) to the mixture and react at room temperature for 48 hours. After the reaction, rinse the product with deionized water and dry it in a vacuum oven at 60°C overnight to obtain a NiCu free-standing electrode.

[0048] Example 2

[0049] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0050] S2: The clean nickel foam was placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia (1.5 mL).

[0051] S3: Cobalt dichloride hexahydrate (0.9 mmol), copper chloride dihydrate (0.9 mmol), and dopamine hydrochloride (DA, 1 g) were added to the mixture and allowed to react at room temperature for 48 hours. After the reaction, the product was washed with deionized water and dried in a vacuum oven at 60°C overnight to obtain a CoCu free-standing electrode.

[0052] Comparative Example 1

[0053] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0054] S2: The clean nickel foam was placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia (1.5 mL).

[0055] S3: Add ferric chloride (1.8 mmol) and dopamine hydrochloride (DA, 1 g) to the mixture and react at room temperature for 48 hours. After the reaction, rinse the product with deionized water and dry it in a vacuum oven at 60°C overnight to obtain an Fe self-supporting electrode.

[0056] Comparative Example 2

[0057] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0058] S2: The clean nickel foam was placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia (1.5 mL).

[0059] S3: Cobalt dichloride hexahydrate (1.8 mmol) and dopamine hydrochloride (DA, 1 g) were added to the mixture and allowed to react at room temperature for 48 hours. After the reaction, the product was washed with deionized water and dried in a vacuum oven at 60°C overnight to obtain a Co self-supporting electrode.

[0060] Comparative Example 3

[0061] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0062] S2: The clean nickel foam was placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia (1.5 mL).

[0063] S3: Add nickel chloride hexahydrate (1.8 mmol) and dopamine hydrochloride (DA, 1 g) to the mixture and react at room temperature for 48 hours. After the reaction, rinse the product with deionized water and dry it in a vacuum oven at 60°C overnight to obtain a Ni free-standing electrode.

[0064] Comparative Example 4

[0065] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0066] S2: The clean nickel foam was placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia (1.5 mL).

[0067] S3: Copper chloride dihydrate (1.8 mmol) and dopamine hydrochloride (DA, 1 g) were added to the mixture and allowed to react at room temperature for 48 hours. After the reaction, the product was washed with deionized water and dried in a vacuum oven at 60°C overnight to obtain a Cu free-standing electrode.

[0068] Comparative Example 5

[0069] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0070] S2: The clean nickel foam was placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia (1.5 mL).

[0071] S3: Add ferric chloride (0.9 mmol), cobalt dichloride hexahydrate (0.9 mmol), and dopamine hydrochloride (DA, 1 g) to the mixture and react at room temperature for 48 hours. After the reaction, rinse the product with deionized water and dry it in a vacuum oven at 60°C overnight to obtain a FeCo self-supporting electrode.

[0072] Comparative Example 6

[0073] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0074] S2: The clean nickel foam was placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia (1.5 mL).

[0075] S3: Cobalt dichloride hexahydrate (0.9 mmol), nickel chloride hexahydrate (0.9 mmol), and dopamine hydrochloride (DA, 1 g) were added to the mixture and reacted at room temperature for 48 hours. After the reaction, the product was washed with deionized water and dried in a vacuum oven at 60°C overnight to obtain a CoNi self-supporting electrode.

[0076] Comparative Example 7

[0077] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0078] S2: The clean nickel foam was placed in a mixture of deionized water (180 mL), ethanol (80 mL) and ammonia (1.5 mL).

[0079] S3: Nickel chloride hexahydrate (0.9 mmol) and cupric chloride dihydrate (0.9 mmol) were added to the mixture and reacted at room temperature for 48 hours. After the reaction, the product was washed with deionized water and dried in a vacuum oven at 60°C overnight to obtain a NiCu (without the dopamine complex layer) free-standing electrode.

[0080] Comparative Example 8

[0081] S1: Nickel foam (1.0 cm × 2.0 cm × 0.1 cm) was dissolved in dilute hydrochloric acid (1 mol L -1 ), acetone and ultrasonic cleaning in deionized water for 15 minutes.

[0082] S2: The clean nickel foam was placed in a mixture of deionized water (30 mL), sodium hydroxide (0.15 mol) and sodium carbonate (0.013 mol).

[0083] S3: Nickel chloride hexahydrate (0.9 mmol) and cupric chloride dihydrate (0.9 mmol) were added to the mixture and hydrothermally reacted at 100°C for 24 hours. After the reaction, the product was washed with deionized water and dried in a vacuum oven at 60°C overnight to obtain a NiCuLDH (without a dopamine complexing layer) free-standing electrode.

[0084] Performance testing:

[0085] Figure 1 The scanning electron microscope and transmission electron microscope images of the NiCu catalyst electrode prepared in Example 1 are shown. Figure 1 a Flake-like protrusions can be observed, Figure 1 bh It can be observed that the NiCu catalyst electrode has no obvious lattice structure, and the C, N, O, Ni, and Cu elements are evenly distributed in the catalyst, which indicates that the metal ions exist in the catalyst electrode in the form of "metal-PDA complex".

[0086] Figure 2 This is the X-ray photoelectron spectrum of the NiCu catalyst electrode prepared in Example 1. Figure 2 In the full spectrum of a, five main elements, C, N, O, Ni and Cu, can be observed. Figure 2 In the C1s spectrum of b, the typical peaks of PDA can be observed at 284.8 eV for CC / C=C bond, 285.8 eV for CO / CN bond, and 288.8 eV for C=O / / C=N bond. Figure 2 In the N1s spectrum of c, peaks at 398.6 eV, 400.9 eV, and 405.6 eV can be observed, corresponding to pyridinic nitrogen, pyrrolic nitrogen, and ON bond, respectively. Figure 2 In the O1s spectrum of d, peaks at 529.9 eV and 531.6 eV can be observed, corresponding to MO / M-OH and C=O bonds, respectively, indicating the presence of metal oxy(hydroxide) species. Figure 2 In the Ni 2p spectrum of e, the peaks at 856.1eV and 876.3.0eV correspond to Ni 2+ 2p 3 / 2 and 2p 1 / 2 The satellite peaks at 858.2 eV, 861.4 eV, 865.2 eV, 876.9 eV, and 880.7 eV are typical features of the formation of Ni oxides. Figure 2 In the Cu 2p spectrum of f, the peaks at 933.2eV and 952.8eV correspond to Cu 1+2p 3 / 2 and 2p 1 / 2 orbital. The peaks at 935.0eV and 954.7eV are from Cu 2+ 2p 3 / 2 and 2p 1 / 2 The satellite peaks at around 941.8e, 944.5eV, and 963.1eV are typical characteristics of the formation of copper oxide. This indicates the successful preparation of Example 1 and the feasibility of the preparation method designed by the present invention.

[0087] Figure 3 and Figure 4 The linear sweep voltammograms of Examples 1-2 and Comparative Examples 1-8 are shown. The catalytic activities of Examples 1-2 and Comparative Examples 1-8 were tested using linear sweep voltammograms (LSV). The electrochemical measurements were performed using a CHI660e (CHInstruments, Inc, Shanghai) electrochemical workstation. In a typical three-electrode system, the catalytic activities of the samples were tested in pure KOH (1 mol L -1 ) and added PEG200 (75 mg mL -1 ) of KOH (1 mol L -1 ) electrolyte, where Hg / HgO was used as the reference electrode and platinum was used as the counter electrode. All potentials were calibrated using the following equation: RHE =E Hg / HgO +0.098+0.0591*pH. All potential values are iR compensated and calibrated to the reversible hydrogen electrode (RHE). All current densities are converted to the geometric area of nickel foam. -1 The LSV curve was tested at a scan rate of .

[0088] Using 50mA cm -2 The potential difference between PEGOR and OER at the current density is used to describe the improvement effect of PEGOR on OER, that is, the promotion effect on the cathode hydrogen evolution reaction. The specific test results are as follows Figure 3 and Figure 4 As shown. Figure 3 and Figure 4It can be seen that in Examples 1-2 and Comparative Examples 1-8, after adding PEG200 to the electrolyte, the anodic oxidation potential of all electrodes decreased significantly. Among them, the initial oxidation potential of Example 1 is the lowest, only 1.33V vs.RHE, and PEGOR has the most significant improvement effect on OER (Δη=384mV). Although the Δη (430mV) of Comparative Example 4 is higher than that of Example 1, its initial oxidation potential (1.37Vvs.RHE) is higher, and it shows the defect of insufficient power at high potential. Therefore, among all the electrodes designed in the present invention, Example 1 has the best comprehensive performance. The performances of the remaining electrodes are: Example 2 (1.33 V vs. RHE, Δη = 248 mV), Comparative Example 1 (1.38 V vs. RHE, Δη = 61 mV), Comparative Example 2 (1.35 V vs. RHE, Δη = 20 mV), Comparative Example 3 (1.34 V vs. RHE, Δη = 217 mV), Comparative Example 4 (1.37 V vs. RHE, Δη = 430 mV), Comparative Example 5 (1.36 V vs. RHE, Δη = 99 mV), Comparative Example 6 (1.35 V vs. RHE, Δη = 17 mV), Comparative Example 7 (1.36 V vs. RHE, Δη = 286 mV) and Comparative Example 8 (1.35 V vs. RHE, Δη = 135 mV).

[0089] Figure 5 The chronoamperometry diagram of Example 1. The durability test of Example 1 with the best comprehensive performance was conducted using chronoamperometry (it). The initial PEG concentration was 75 mg / mL. As the test progressed, the current density increased from 100 mA cm -2 down to 74 mA cm -2 After PEG was added to the electrolyte at 20 h, the current density returned to 100 mA cm -2 This indicates that the oxidation current in Example 1 is entirely provided by PEGOR. Furthermore, this indicates that Example 1 itself has excellent durability as a catalyst electrode; as long as PEG is continuously added to the electrolyte, the reaction can continue.

[0090] In the above test experiment, the structure of PEG 200 added to the electrolyte is as follows:

[0091]

[0092] It should be noted that the preferred embodiments of the present invention are given in the specification and drawings of the present invention. However, the present invention can be implemented in many different forms and is not limited to the embodiments described in this specification. These embodiments are not intended to be additional limitations on the content of the present invention. The purpose of providing these embodiments is to make the understanding of the disclosure of the present invention more thorough and comprehensive. In addition, the above-mentioned technical features can be combined with each other to form various embodiments not listed above, which are all considered to be within the scope of the description of the present invention. Furthermore, it is obvious to those skilled in the art that improvements or changes can be made based on the above description, and all such improvements and changes should fall within the scope of protection of the claims attached to the present invention.

Claims

1. A transition metal catalyst electrode for polyethylene glycol reforming to produce hydrogen, characterized in that: The transition metal catalyst electrode consists of a conductive self-supporting substrate and a transition metal ion-dopamine complex layer coated on the self-supporting substrate.

2. The transition metal catalyst electrode according to claim 1, characterized in that The self-supporting substrate is selected from metal or alloy mesh, foam metal or foam alloy, metal or alloy sheet, non-metallic substrate; Furthermore, the metal or alloy mesh is a stainless steel mesh or a nickel mesh, the foam metal or foam alloy is foam nickel, foam iron, foam titanium or foam nickel-iron alloy, the metal or alloy sheet is a nickel sheet, iron sheet, titanium sheet or nickel-iron alloy sheet, and the non-metallic substrate is carbon paper, carbon cloth or carbon fiber.

3. The transition metal catalyst electrode according to claim 1, characterized in that The transition metal ion is selected from one or more of Fe, Co, Ni and Cu; The dopamine is dopamine hydrochloride.

4. A method for preparing a transition metal catalyst electrode for polyethylene glycol reforming to produce hydrogen according to any one of claims 1 to 3, characterized in that: The following steps are involved: (1) pre-treating the conductive self-supporting substrate to obtain a clean self-supporting substrate; (2) placing the pretreated self-supporting substrate in an alkaline mixed solvent; (3) adding transition metal ions and dopamine to react to form a transition metal ion-dopamine complex layer coated on the self-supporting substrate; (4) washing the product and drying it to obtain the transition metal catalyst electrode.

5. The preparation method according to claim 4, characterized in that The pretreatment comprises ultrasonically cleaning the self-supporting substrate in dilute hydrochloric acid, acetone and deionized water respectively; Furthermore, the concentration of the dilute hydrochloric acid is 0.1-2 mol L -1 .

6. The preparation method according to claim 4, characterized in that The alkaline mixed solvent is prepared from deionized water, ethanol and ammonia water.

7. The preparation method according to claim 4, characterized in that The transition metal ion is selected from one or more of Fe, Co, Ni and Cu; Furthermore, the transition metal ions are provided by chlorides, nitrates or hydrates of transition metals such as Fe, Co, Ni or Cu; Furthermore, the dopamine is dopamine hydrochloride.

8. The preparation method according to claim 4, characterized in that The molar ratio of the added transition metal ion to dopamine is 1:2-4; Furthermore, when the transition metal ion includes two different metal ions, the molar ratio of the two metal ions is 1:

1.

9. The preparation method according to claim 4, characterized in that The reaction in step (3) comprises reacting at room temperature for 24-72 hours.

10. Use of the transition metal catalyst electrode for polyethylene glycol reforming to produce hydrogen according to any one of claims 1 to 3 or the transition metal catalyst electrode for polyethylene glycol reforming to produce hydrogen obtained by the preparation method according to any one of claims 4 to 9 in the electrochemical recycling of waste polyethylene glycol; Furthermore, the transition metal catalyst electrode is used to catalyze the reforming of waste polyethylene glycol to produce hydrogen.

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