Graphene aerogel-based water electrolysis hydrogen production electrode and preparation method thereof

Abstract

The application belongs to the technical field of electrocatalytic material preparation, and particularly relates to a graphene aerogel-based water electrolysis hydrogen production electrode and a preparation method thereof. The anode electrode comprises an anode catalytic layer, an anode carrier layer and a substrate layer which are sequentially stacked, and the cathode electrode comprises a cathode catalytic layer, a cathode carrier layer and a substrate layer which are sequentially stacked. The anode catalytic layer is a nano nickel-iron alloy, the anode carrier layer is nano carbon tube and spinel powder loaded with graphene aerogel, and the cathode catalytic layer is a carbon-titanium alloy. The spinel powder loaded with graphene aerogel is arranged in the anode electrode, and the nano cuprous oxide powder loaded with graphene aerogel is arranged in the cathode electrode, so that the graphene aerogel can correlate the active sites on the electrode surface, thereby enhancing short-layer electron conduction, increasing the electrolysis effect of the electrode, and the carrier layer is selected from nano carbon tube and graphene aerogel microporous structure, thereby improving the catalytic efficiency and electrolysis efficiency.

Description

TECHNICAL FIELD

[0001] The application belongs to the technical field of electrocatalytic material preparation, and particularly relates to a graphene aerogel-based water electrolysis hydrogen production electrode and a preparation method thereof. BACKGROUND

[0002] Hydrogen energy, as a clean energy, can replace fossil fuels to the greatest extent to weaken the greenhouse gas effect of carbon dioxide. Water electrolysis hydrogen production is a relatively convenient method for producing hydrogen. In an electrolytic cell filled with electrolyte, direct current is introduced, and water molecules are electrochemically reacted on the electrode to decompose into hydrogen and oxygen.

[0003] In a large-scale water electrolysis electrolytic cell, in order to save costs, a catalyst is generally sprayed only on the cathode (HER) side, and a nickel mesh is still used on the anode (OER) side. Hydrogen is generated on the cathode, and oxygen is generated on the anode during the water electrolysis process. Since the anode involves a complex reaction process of four electron transfers, the anode reaction needs a higher overpotential than the cathode reaction under the same current density, and is the rate-controlling step of the water electrolysis reaction, so the development of anode catalysts has attracted more attention from researchers. At present, commercial catalysts are all noble metal-based catalysts, such as ruthenium, iridium, nickel, etc. Although they have good performance, their reserves on the earth are very limited, and they are expensive and have poor stability, so it is difficult for them to maintain the original performance under high current density. Therefore, it is very important to develop a cheap and efficient catalytic material. SUMMARY

[0004] The purpose of the present application is to provide a graphene aerogel-based water electrolysis hydrogen production electrode and a preparation method thereof, which solves the technical problems in the prior art that the anode overpotential is high, the energy consumption is high, the anode catalyst loss rate is accelerated, and it is difficult to control the water electrolysis reaction rate.

[0005] The application achieves the above-mentioned purpose by the following technical solutions:

[0006] A graphene aerogel-based water electrolysis hydrogen production electrode, the anode electrode comprises an anode catalytic layer, an anode carrier layer and a substrate layer which are sequentially stacked, and the cathode electrode comprises a cathode catalytic layer, a cathode carrier layer and a substrate layer which are sequentially stacked; wherein:

[0007] The anode catalytic layer is a nano nickel-iron alloy;

[0008] The anode carrier layer is a nano carbon tube and a spinel powder on which graphene aerogel is loaded;

[0009] The cathode catalytic layer is a carbon-titanium alloy;

[0010] The cathode carrier layer is a nano carbon tube and a nano cuprous oxide powder on which graphene aerogel is loaded;

[0011] The base layer is a nickel alloy.

[0012] As a further optimization scheme of the present application, the loading amount of the spinel powder is 7-15 mg / cm 2 .

[0013] As a further optimization scheme of the present application, the loading amount of the nano cuprous oxide is 1.3-5.2 mg / cm 2 .

[0014] As a further optimization scheme of the present application, the spinel powder is selected from one or both of copper ferrite spinel powder and hercynite powder.

[0015] A preparation method of a graphene aerogel-based water electrolysis hydrogen production electrode according to any one of the above, comprising the following steps:

[0016] S1: taking nickel alloy particles for ball milling treatment, uniformly mixing after adding a binder to obtain a pre-mixture, molding the pre-mixture by molding, calcining the nickel alloy electrode in an inert gas to obtain a Raney nickel alloy electrode base layer, and performing alkaline washing on the nickel alloy electrode to obtain a porous Raney nickel alloy electrode base layer;

[0017] S2: ultrasonic vibration dispersing the spinel powder in graphene aerogel, then performing precipitation and drying to obtain an anode intermediate carrier, mixing the nanometer carbon tube and the obtained anode intermediate carrier, and obtaining an anode carrier layer in the form of a dispersion suspension after the mixing is completed;

[0018] S3: performing one-time spraying of the anode carrier layer on the base layer, dispersing nanometer nickel-iron alloy in an organic solvent, uniformly mixing after the mixing, and performing two-time spraying of the base layer, and obtaining an anode after solidification;

[0019] S4: ultrasonic vibration dispersing the nano cuprous oxide powder in graphene aerogel, then performing precipitation and drying to obtain a cathode intermediate carrier, mixing the nanometer carbon tube and the obtained cathode intermediate carrier, and obtaining a cathode carrier layer in the form of a dispersion suspension after the mixing is completed;

[0020] S5: performing one-time spraying of the cathode carrier layer on the base layer, dispersing carbon-titanium alloy powder in an organic solvent, uniformly mixing after the mixing, and performing two-time spraying of the base layer, and obtaining a cathode after solidification.

[0021] As a further optimization scheme of the present application, in the step S1, the nickel alloy electrode is soaked in an alkaline solution for 8-15 h, cleaned with deionized water and dried to obtain a Raney nickel electrode; the alkaline solution is a 25-40 wt% KOH or NaOH solution.

[0022] As a further optimization scheme of the present application, the graphene aerogel in the step S2 and the step S4 is in powder form, wherein the mass ratio of the graphene aerogel to the spinel powder in the step S2 is 3:1-15; the mass ratio of the graphene aerogel to the nano-cuprous oxide powder in the step S4 is 1:1-9.

[0023] As a further optimization scheme of the present application, the mass concentration of the nano-carbon tube in the anode carrier layer in the step S2 is 4%-15%.

[0024] As a further optimization scheme of the present application, the mass concentration of the nano-carbon tube in the cathode carrier layer in the step S4 is 12-21%.

[0025] The present application has the following beneficial effects:

[0026] 1) The present application sets the spinel powder loaded with graphene aerogel in the anode and the nano-cuprous oxide powder loaded with graphene aerogel in the cathode, so that the graphene aerogel can correlate the active sites on the electrode surface, thereby enhancing the short-layer electron conduction, increasing the electrolysis effect of the electrode, and the carrier layer selects the microporous structure such as nano-carbon tube and graphene aerogel, thereby improving the catalytic efficiency and electrolysis efficiency.

[0027] 2) In the present application, the anode directly uses the nickel mesh in the prior art, and obviously, the nickel alloy is selected as the base layer, the nano-microporous structure containing the spinel powder is selected as the carrier layer, and the design of the nano-nickel-iron alloy catalytic layer is obviously lower in cost, forms the nickel particles loaded on the spinel surface, is beneficial to the adsorption and dissociation of H2 on the surface of the catalytic layer, the spinel carrier has the porous topography, is beneficial to the loading of nickel, thereby stabilizing the active sites of the catalyst, and can enhance the adsorption of the key intermediate product in the reaction, thereby improving the catalytic efficiency.

[0028] 3) In the present application, the cathode selects the nickel alloy as the base layer, the nano-microporous structure containing cuprous oxide as the carrier layer, and the design of the carbon-titanium alloy catalytic layer, since the cathode does not need to bear a high overpotential, obviously, cuprous oxide as the carrier layer is lower in cost; and the aggregation tendency of cuprous oxide is small, thereby improving the stability of the catalytic layer. DETAILED DESCRIPTION

[0029] The present application is described in further detail below, and it is necessary to point out here that the following detailed description is only used to further illustrate the present application, and cannot be understood as limiting the protection scope of the present application, and the skilled in the art can make some non-essential improvements and adjustments to the present application according to the above application content.

[0030] Example 1

[0031] The embodiment provides a graphene aerogel-based water electrolysis hydrogen production electrode, a positive electrode comprises a positive electrode catalytic layer, a positive electrode carrier layer and a substrate layer which are sequentially stacked, and a negative electrode comprises a negative electrode catalytic layer, a negative electrode carrier layer and a substrate layer which are sequentially stacked.

[0032] The positive electrode catalytic layer is a nano nickel-iron alloy.

[0033] The positive electrode carrier layer is a nano carbon tube and spinel powder on which graphene aerogel is loaded, the loading amount of the spinel powder is 7 mg / cm 2 The spinel powder is copper ferrite spinel powder.

[0034] The negative electrode catalytic layer is a carbon-titanium alloy.

[0035] The negative electrode carrier layer is a nano carbon tube and nano cuprous oxide powder on which graphene aerogel is loaded, the loading amount of the nano cuprous oxide is 1.3 mg / cm 2 .

[0036] The substrate layer is a nickel alloy.

[0037] A preparation method of the graphene aerogel-based water electrolysis hydrogen production electrode according to any one of the above, steps are as follows:

[0038] S1: take nickel alloy particles and perform ball milling treatment, add polyvinylidene fluoride and uniformly mix to obtain a preparation, perform mold pressing forming on the preparation, calcine in an inert gas to obtain a nickel alloy electrode, perform alkali washing on the nickel alloy electrode to obtain a porous Raney nickel alloy electrode substrate layer.

[0039] In the alkali washing step, the nickel alloy electrode is soaked in an alkali solution for 8 h, washed with deionized water and dried to obtain a Raney nickel electrode; the alkali solution is a 25wt% NaOH solution.

[0040] S2: ultrasonic vibration dispersion of copper ferrite spinel powder in graphene aerogel powder, then perform precipitation and drying to obtain an anode intermediate carrier, mix the nano carbon tube and the obtained anode intermediate carrier, and obtain the anode carrier layer in the form of a dispersion suspension, the mass concentration of the nano carbon tube in the anode carrier layer is 4%;

[0041] In the alkali washing step, the nickel alloy electrode is soaked in an alkali solution for 8 h, washed with deionized water and dried to obtain a Raney nickel electrode; the alkali solution is a 25wt% NaOH solution.

[0042] S3: perform first spraying of the anode carrier layer on the substrate layer, disperse the nano nickel-iron alloy in an organic solvent, uniformly mix and perform second spraying on the substrate layer, and obtain the anode after solidification.

[0043] S4: ultrasonic vibration dispersion of nano-cuprous oxide powder in graphene aerogel, then precipitation and drying to obtain a cathode intermediate carrier, mixing nano-carbon tubes and the obtained cathode intermediate carrier to obtain a cathode carrier layer in the form of a dispersion suspension, the mass concentration of nano-carbon tubes in the cathode carrier layer being 12%;

[0044] The mass ratio of the graphene aerogel to the nano-cuprous oxide powder is 1:1.

[0045] S5: one-time spraying of the cathode carrier layer onto the substrate layer, dispersing carbon-titanium alloy powder into an organic solvent, uniformly mixing and then second-time spraying onto the substrate layer, and obtaining a cathode after solidification.

[0046] Example 2

[0047] The embodiment provides a graphene aerogel-based water electrolysis hydrogen production electrode, a positive electrode comprising an anode catalytic layer, an anode carrier layer and a substrate layer which are sequentially stacked, and a negative electrode comprising a cathode catalytic layer, a cathode carrier layer and a substrate layer which are sequentially stacked; wherein:

[0048] The anode catalytic layer is nano-nickel-iron alloy.

[0049] The anode carrier layer is nano-carbon tubes and spinel powder on the surface of which graphene aerogel is loaded, the loading amount of the spinel powder being 10 mg / cm 2 , and the spinel powder being selected from iron-aluminum spinel powder.

[0050] The cathode catalytic layer is carbon-titanium alloy.

[0051] The cathode carrier layer is nano-carbon tubes and nano-cuprous oxide powder on the surface of which graphene aerogel is loaded, the loading amount of the nano-cuprous oxide being 3.5 mg / cm 2 .

[0052] The substrate layer is nickel alloy.

[0053] A preparation method of a graphene aerogel-based water electrolysis hydrogen production electrode according to any one of the above, comprising the following steps:

[0054] S1: taking nickel alloy particles to perform ball milling treatment, adding polyvinylidene fluoride to uniformly mix to obtain a pre-mixture, performing die forming on the pre-mixture, calcining in an inert gas to obtain a nickel alloy electrode, performing alkali washing on the nickel alloy electrode to obtain a porous Raney nickel alloy electrode substrate layer.

[0055] The alkali washing step is that the nickel alloy electrode is soaked in an alkali solution for 10 h, washed with deionized water and dried to obtain a Raney nickel electrode; and the alkali solution is a 30wt% KOH solution.

[0056] S2: ultrasonic vibration dispersion of the hercynite powder in the graphene aerogel powder, then precipitation and drying to obtain an anode intermediate carrier, mixing the nanometer carbon tube and the obtained anode intermediate carrier to obtain an anode carrier layer in the form of a dispersion suspension, the mass concentration of the nanometer carbon tube in the anode carrier layer being 10%;

[0057] The mass ratio of the graphene aerogel to the hercynite powder is 3:5.

[0058] S3: one-time spraying of the anode carrier layer onto the base layer, then dispersing the nanometer nickel-iron alloy into an organic solvent, uniformly mixing and then two-time spraying onto the base layer, and then solidification to obtain an anode.

[0059] S4: ultrasonic vibration dispersion of the nanometer cuprous oxide powder in the graphene aerogel, then precipitation and drying to obtain a cathode intermediate carrier, mixing the nanometer carbon tube and the obtained cathode intermediate carrier to obtain a cathode carrier layer in the form of a dispersion suspension, the mass concentration of the nanometer carbon tube in the cathode carrier layer being 18%.

[0060] The mass ratio of the graphene aerogel to the nanometer cuprous oxide powder is 1:5.

[0061] S5: one-time spraying of the cathode carrier layer onto the base layer, then dispersing the carbon-titanium alloy powder into an organic solvent, uniformly mixing and then two-time spraying onto the base layer, and then solidification to obtain a cathode.

[0062] Example 3

[0063] The embodiment provides an electrolytic water hydrogen production electrode based on graphene aerogel, wherein the anode electrode comprises an anode catalytic layer, an anode carrier layer and a base layer which are sequentially stacked, and the cathode electrode comprises a cathode catalytic layer, a cathode carrier layer and a base layer which are sequentially stacked.

[0064] The anode catalytic layer is a nanometer nickel-iron alloy.

[0065] The anode carrier layer is a nanometer carbon tube and hercynite powder on which graphene aerogel is loaded, the loading amount of the hercynite powder being 15 mg / cm 2 , and the hercynite powder is copper ferrite hercynite powder.

[0066] The cathode catalytic layer is a carbon-titanium alloy.

[0067] The cathode carrier layer is a nanometer carbon tube and nanometer cuprous oxide powder on which graphene aerogel is loaded, the loading amount of the nanometer cuprous oxide being 5.2 mg / cm 2 .

[0068] The base layer is a nickel alloy.

[0069] A method for preparing a graphene aerogel-based water electrolysis hydrogen production electrode according to any one of the above, the steps are as follows:

[0070] S1: Take the nickel alloy particles for ball milling treatment, add polyvinylidene fluoride after mixing uniformly to obtain a pre-mixture, the pre-mixture is molded, calcined in an inert gas to obtain a nickel alloy electrode, the nickel alloy electrode is alkali washed to obtain a porous Raney nickel alloy electrode substrate layer;

[0071] The alkali washing step is to immerse the nickel alloy electrode in an alkali solution for 15 h, wash with deionized water and dry to obtain a Raney nickel electrode; the alkali solution is a 40wt% NaOH solution

[0072] S2: ultrasonic vibration dispersion of copper ferrite spinel powder in graphene aerogel powder, then precipitation, drying to obtain an anode intermediate carrier, mixing nano carbon tubes and the obtained anode intermediate carrier, mixing to obtain an anode carrier layer in the form of a dispersion suspension, the mass concentration of nano carbon tubes in the anode carrier layer is 15%;

[0073] The mass ratio of graphene aerogel to spinel powder is 3:15.

[0074] S3: one-time spraying of the anode carrier layer onto the substrate layer, dispersing nano nickel-iron alloy into an organic solvent, mixing uniformly, and then two-time spraying onto the substrate layer, and after solidification, an anode is obtained.

[0075] S4: ultrasonic vibration dispersion of nano cuprous oxide powder in graphene aerogel, then precipitation, drying to obtain a cathode intermediate carrier, mixing nano carbon tubes and the obtained cathode intermediate carrier, mixing to obtain a cathode carrier layer in the form of a dispersion suspension, the mass concentration of nano carbon tubes in the cathode carrier layer is 21%;

[0076] The mass ratio of graphene aerogel to nano cuprous oxide powder is 1:9.

[0077] S5: one-time spraying of the cathode carrier layer onto the substrate layer, dispersing carbon-titanium alloy powder into an organic solvent, mixing uniformly, and then two-time spraying onto the substrate layer, and after solidification, a cathode is obtained.

[0078] Comparative Example 1

[0079] The main difference between this comparative example and the above examples 1-3 is that the spinel powder is not used in the anode, and cuprous oxide is used in the cathode.

[0080] Specifically provided is a graphene aerogel-based water electrolysis hydrogen production electrode, the anode electrode includes an anode catalytic layer, an anode carrier layer and a substrate layer which are stacked in sequence, and the cathode electrode includes a cathode catalytic layer, a cathode carrier layer and a substrate layer which are stacked in sequence; wherein:

[0081] The anode catalytic layer is a nano nickel-iron alloy;

[0082] The anode carrier layer is a nano carbon tube and graphene aerogel,

[0083] The cathode catalytic layer is a carbon-titanium alloy;

[0084] The cathode carrier layer is a nano carbon tube and graphene aerogel;

[0085] The substrate layer is a nickel alloy.

[0086] A preparation method of a graphene aerogel-based water electrolysis hydrogen production electrode according to any one of the above, the steps are as follows:

[0087] S1: Take the nickel alloy particles and perform ball milling treatment, add polyvinylidene fluoride and mix uniformly to obtain a pre-mixture, perform mold forming on the pre-mixture, calcine in an inert gas to obtain a nickel alloy electrode, perform alkali washing on the nickel alloy electrode to obtain a Raney nickel alloy electrode substrate layer with a porous structure;

[0088] The alkali washing step is to immerse the nickel alloy electrode in an alkali solution for 8h, wash with deionized water and dry to obtain a Raney nickel electrode; the alkali solution is a 25wt% NaOH solution.

[0089] S2: Spray the graphene aerogel onto the substrate layer once, disperse the nano nickel-iron alloy in an organic solvent, mix uniformly, and then spray the mixture onto the substrate layer again, and obtain the anode after solidification;

[0090] S4: Mix the nano carbon tube and graphene aerogel, and obtain the cathode carrier layer in the form of a dispersion suspension after mixing, the mass concentration of the nano carbon tube in the cathode carrier layer is 12%;

[0091] S5: Spray the cathode carrier layer onto the substrate layer once, disperse the carbon-titanium alloy powder in an organic solvent, mix uniformly, and then spray the mixture onto the substrate layer again, and obtain the cathode after solidification.

[0092] Comparative Example 2

[0093] The main difference between the present comparative example and the above-mentioned Examples 1-3 is that the loading amount of spinel powder is increased in the anode electrode material, and the loading amount of nano cuprous oxide is increased in the cathode electrode.

[0094] Specifically provided is a graphene aerogel-based water electrolysis hydrogen production electrode, the anode electrode includes an anode catalytic layer, an anode carrier layer and a substrate layer which are sequentially stacked, and the cathode electrode includes a cathode catalytic layer, a cathode carrier layer and a substrate layer which are sequentially stacked; wherein:

[0095] The anode catalytic layer is a nano nickel-iron alloy;

[0096] The anode carrier layer is nanometer carbon tube and spinel powder with graphene aerogel on the surface, and the loading amount of the spinel powder is 30 mg / cm 2 The spinel powder is selected from hercynite powder.

[0097] The cathode catalytic layer is carbon-titanium alloy.

[0098] The cathode carrier layer is nanometer cuprous oxide powder with graphene aerogel on the surface, and the loading amount of the nanometer cuprous oxide is 10 mg / cm 2 .

[0099] The base layer is nickel alloy.

[0100] A preparation method of a graphene aerogel-based water electrolysis hydrogen electrode according to any one of the above, comprising the following steps:

[0101] S1: taking nickel alloy particles for ball milling treatment, adding polyvinylidene fluoride and mixing uniformly to obtain a pre-mixture, performing mold pressing on the pre-mixture, calcining in an inert gas to obtain a nickel alloy electrode, performing alkali washing on the nickel alloy electrode to obtain a Raney nickel alloy electrode base layer with a porous structure;

[0102] In the alkali washing step, the nickel alloy electrode is soaked in an alkali solution for 10 h, washed with deionized water and dried to obtain a Raney nickel electrode. The alkali solution is a 30wt% KOH solution.

[0103] S2: ultrasonic vibration dispersion of hercynite powder in graphene aerogel powder, followed by precipitation and drying to obtain an anode intermediate carrier, mixing nanometer carbon tube and the obtained anode intermediate carrier, and obtaining an anode carrier layer in the form of a dispersion suspension after complete mixing, and the mass concentration of nanometer carbon tube in the anode carrier layer is 10%;

[0104] The mass ratio of graphene aerogel to spinel powder is 3:5.

[0105] S3: one-time spraying of the anode carrier layer on the base layer, dispersing nanometer nickel-iron alloy in an organic solvent, mixing uniformly, and two-time spraying on the base layer, and obtaining an anode after solidification.

[0106] S4: ultrasonic vibration dispersion of nanometer cuprous oxide powder in graphene aerogel, followed by precipitation and drying to obtain a cathode intermediate carrier, mixing nanometer carbon tube and the obtained cathode intermediate carrier, and obtaining a cathode carrier layer in the form of a dispersion suspension after complete mixing, and the mass concentration of nanometer carbon tube in the cathode carrier layer is 18%;

[0107] The mass ratio of graphene aerogel to nanometer cuprous oxide powder is 1:5.

[0108] S5: Spraying the cathode carrier layer onto the substrate layer for the first time, dispersing the carbon-titanium alloy powder into an organic solvent, mixing uniformly, and spraying onto the substrate layer for the second time, and obtaining the cathode after solidification.

[0109] Comparative Example 3

[0110] The conventional metal nickel mesh in the prior art is directly used as the water electrolysis anode, and the cathode uses a platinum mesh.

[0111] The electrode materials prepared in the above examples and comparative examples are subjected to performance tests in combination with experiments as follows:

[0112] 1. Based on the three-electrode system in electrochemistry, the linear voltammetry scanning method is used to test the oxygen evolution performance of the anode, and the test results are shown in Table 1. The silver / silver chloride is used as the reference electrode, the platinum mesh electrode is used as the counter electrode, the electrolyte is 1 mol / l potassium hydroxide solution, the scanning rate of the linear voltammetry scanning method is 5 mv / s, and the scanning range is 0-1 v. In the table, J is the current density, unit: mA / cm-2; E is the potential difference, unit: v.

[0113] Table 1:

[0114] ;

[0115] 2. The cyclic stability test is tested by chronopotentiometry. The two-electrode system is used, the two electrodes are the anode and the cathode respectively, the electrolyte used is 1 mol / l potassium hydroxide solution, the constant current density is 100 mA / cm -2 , the test time is 24 h, and the test results are shown in Table 2. In the table, Time is the electrolysis time, unit: h.

[0116] Table 2:

[0117] ;

[0118] As can be seen from the results of Table 1 and Table 2, the comparative example 3 is a conventional electrode material in the electrolytic cell in the prior art, and compared with the experimental examples 1-3, it can be seen that the electrode prepared in the experimental examples 1-3 based on graphene aerogel has excellent water electrolysis performance, the overpotential control of the anode is relatively stable, and the structural stability is good; while in the comparative example 1, the removal of the spinel powder in the anode and the removal of the cuprous oxide in the cathode in the preparation process of the electrode material leads to a great reduction of the overall electrolysis efficiency, which can also be seen from the data of the current density in Table 1, and the overpotential control of the anode is poor, which leads to a fast consumption of the anode, thus it can be obtained that the increase of the spinel powder in the anode and the increase of the cuprous oxide in the cathode can increase the overall electrolysis performance of the electrode. While in the comparative example 2, the loadings of the spinel powder in the anode material and the nano cuprous oxide in the cathode are increased in the preparation process of the electrode material, and as can be obtained from Table 1, although the current density is improved compared with the comparative example 1, the anode potential difference is still at a high position, and it can be obtained that the use of the spinel powder and the cuprous oxide needs to be strictly controlled in order to achieve the optimal electrolysis performance and the control of the overpotential of the anode.

[0119] The above embodiments only express several embodiments of the present application, and the description is more specific and detailed, but it should not be understood as a limitation on the scope of the patent of the present application. It should be pointed out that for ordinary skilled in the art, without departing from the concept of the present application, a number of modifications and improvements can be made, which are all within the protection scope of the present application.

Claims

1. A graphene aerogel-based electrode for hydrogen production by water electrolysis, characterized by: The positive electrode comprises a positive anode catalytic layer, a positive anode carrier layer and a substrate layer which are sequentially stacked, and the negative electrode comprises a negative cathode catalytic layer, a negative cathode carrier layer and a substrate layer which are sequentially stacked; wherein: The positive anode catalytic layer is a nano nickel-iron alloy; The positive anode carrier layer is a nano carbon tube and spinel powder with graphene aerogel loaded on the surface; The negative cathode catalytic layer is a carbon-titanium alloy; The negative cathode carrier layer is a nano carbon tube and nano cuprous oxide powder with graphene aerogel loaded on the surface; The substrate layer is a nickel alloy; The loading of the spinel powder is 7-15 mg / cm 2 ; The loading of the nano-cuprous oxide is 1.3-5.2 mg / cm 2 ; The spinel powder is selected from one or both of copper ferrite spinel powder and iron aluminum spinel powder.

2. A method for preparing a graphene aerogel-based water electrolysis hydrogen electrode according to claim 1, characterized by: The steps are as follows: S1: Take the nickel alloy particles for ball milling treatment, mix uniformly after adding the binder to obtain a pre-mixture, form the pre-mixture by molding, calcine in an inert gas to obtain a nickel alloy electrode, alkali wash the nickel alloy electrode to obtain a porous Raney nickel alloy electrode substrate layer; S2: Ultrasonic vibration disperse the spinel powder in graphene aerogel, then perform precipitation and drying to obtain an anode intermediate carrier, mix the nano carbon tube and the obtained anode intermediate carrier to obtain an anode carrier layer in the form of a dispersion suspension; S3: Perform first spraying of the anode carrier layer on the substrate layer, disperse the nano nickel-iron alloy in an organic solvent, mix uniformly and then perform second spraying on the substrate layer, and obtain an anode after solidification; S4: Ultrasonic vibration disperse the nano cuprous oxide powder in graphene aerogel, then perform precipitation and drying to obtain a cathode intermediate carrier, mix the nano carbon tube and the obtained cathode intermediate carrier to obtain a cathode carrier layer in the form of a dispersion suspension; S5: Perform first spraying of the cathode carrier layer on the substrate layer, disperse the carbon-titanium alloy powder in an organic solvent, mix uniformly and then perform second spraying on the substrate layer, and obtain a cathode after solidification.

3. The method for preparing a water electrolysis hydrogen production electrode based on graphene aerogel according to claim 2, characterized in that: In the step S1, immerse the nickel alloy electrode in an alkali solution for 8-15 h, clean with deionized water and dry to obtain a Raney nickel electrode; the alkali solution is a 25-40 wt% KOH or NaOH solution.

4. The method according to claim 2, wherein the method is characterized by: In the step S2 and the step S4, the graphene aerogel is in the form of powder, wherein the mass ratio of the graphene aerogel to the spinel powder in the step S2 is 3:1-15, and the mass ratio of the graphene aerogel to the nano cuprous oxide powder in the step S4 is 1:1-9.

5. The method according to claim 2, wherein the method is characterized by: In the step S2, the mass concentration of the nano carbon tube in the anode carrier layer is 4%-15%.

6. The method according to claim 2, wherein the method is characterized by: In the step S4, the mass concentration of the nano carbon tube in the cathode carrier layer is 12-21%.