Bromide ion electrooxidation electrode and preparation method and application thereof

Abstract

The invention discloses a bromide ion electrooxidation electrode and a preparation method and application thereof. The preparation method comprises the following steps: providing a first deposition solution containing a surfactant, fluoride, a transition metal soluble salt and water; electrifying a first electro-deposition system comprising a first working electrode, a counter electrode and a first deposition solution, and performing first electro-deposition on the first working electrode to form a first electro-deposition layer; providing a second deposition solution comprising a surfactant, a transition metal soluble salt, and water; and electrifying a second electro-deposition system containing a second working electrode, a counter electrode and a second deposition solution, and carrying out second electro-deposition on the second working electrode to form a second electro-deposition layer so as to prepare the bromide ion electro-oxidation electrode. The bromide ion electrooxidation electrode provided by the invention is used for electrocatalytic oxidation of bromide ions, and can realize catalytic oxidation of low-grade bromide ions in brine.

Description

Technical Field

[0001] The invention relates to the technical field of bromine extraction, and in particular to a bromide ion electro-oxidation electrode and a preparation method and application thereof. Background Art

[0002] The main application areas of bromine include fine chemicals, high-end manufacturing, environmental protection, petrochemicals, medicine, energy storage, etc. There are more than 100 related high value-added products, which are necessary resources for a complete industrial system. Bromine production uses brine and seawater as raw materials, and mainly adopts the hydrochloric acid acidification-chlorine oxidation-air blowing (or distillation) method. This method has safety hazards in the storage and transportation of raw chlorine and will produce a large amount of acidic high-salt wastewater. In order to reduce acidic high-salt wastewater, researchers have proposed a method for electrolytic extraction of bromine. For example, the existing patents CN115341229A and CN113789525A both propose a process for generating bromine by electrolytic acidification of sodium bromide, and use titanium plates with precious metal coatings on the surface as electrodes, but the process still requires the addition of 4-10% hydrochloric acid. In addition, brine or concentrated seawater usually contains high concentrations of chloride ions, which will be oxidized to chlorine gas at the same time as the bromide ions are electro-oxidized. The existing patent CN114956264B proposes to separate bromine by electrochemical method, and the electrodes used are metal electrodes such as ruthenium, lead, tin, antimony, and titanium, but this method is suitable for systems with a bromine content of 3-4 g / L. The existing patent CN115074754B proposes a segmented voltage controlled electrolysis method and uses graphite, platinum or silver as electrodes to achieve selective oxidation of bromide ions and avoid the generation of excessive chlorine. This method is also suitable for systems with a bromine content of about 3 g / L.

[0003] At present, the long-term exploitation of underground brine in China has led to a year-on-year decline in bromine resource reserves, and the grade has gradually decreased to about 100 mg / L. Due to the low bromine content in the system, the existing electrochemical method cannot directly extract or the extraction efficiency is low. Therefore, a new method is needed to achieve the catalytic oxidation of low-grade bromide ions in brine and improve the oxidation rate of bromide ions. Summary of the invention

[0004] The main purpose of the present invention is to provide a bromide ion electro-oxidation electrode and a preparation method and application thereof, so as to overcome the deficiencies in the prior art.

[0005] In order to achieve the above-mentioned invention object, the technical solution adopted by the present invention includes: One aspect of the present invention provides a method for preparing a bromide ion electro-oxidation electrode, comprising: providing a first deposition solution comprising a surfactant, a fluoride, a soluble salt of a transition metal, and water; Powering a first electrodeposition system comprising a first working electrode, a counter electrode and a first deposition solution, performing a first electrodeposition on the first working electrode to form a first electrodeposition layer; the first working electrode comprises a porous graphite material; providing a second deposition solution comprising a surfactant, a soluble salt of a transition metal, and water; The second electrodeposition system including the second working electrode, the counter electrode and the second deposition liquid is energized, and the second electrodeposition is performed on the second working electrode to form a second electrodeposition layer to obtain a bromide ion electro-oxidation electrode; the second working electrode includes the first working electrode deposited with the first electrodeposition layer.

[0006] Another aspect of the present invention provides a bromide ion electro-oxidation electrode prepared by the aforementioned preparation method, wherein the bromide ion electro-oxidation electrode comprises a graphite substrate, a first electro-deposited layer and a second electro-deposited layer sequentially stacked on the graphite substrate; the first electro-deposited layer comprises a transition metal oxide, and the second electro-deposited layer comprises a transition metal oxide.

[0007] Another aspect of the present invention also provides the use of the aforementioned bromide ion electro-oxidation electrode in electrocatalytic oxidation of bromide ions.

[0008] Compared with the prior art, the technical solution of the present invention has at least the following advantages: The bromide ion electro-oxidation electrode provided by the present invention is used for electrocatalytic oxidation of bromide ions and is still applicable to systems with a bromide ion concentration lower than 100 mg / L, thereby realizing the catalytic oxidation of low-grade bromide ions in brine, and has a high bromide ion oxidation rate and excellent long-cycle performance, and can extract bromine in a long-term and stable manner. BRIEF DESCRIPTION OF THE DRAWINGS

[0009] In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings required for use in the embodiments or the description of the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments recorded in the present invention. For ordinary technicians in this field, other drawings can be obtained based on these drawings without paying creative work.

[0010] Figure 1 The cross-sectional microscopic morphology of the bromide ion electrooxidation electrode prepared in Example 1 of the present invention; Figure 2 This is a comparison diagram of the oxidation rates of bromide ions at different concentrations on the electrode in Examples 1-3 of the present invention; Figure 3 This is a test diagram of the long cycle performance of the bromide ion electro-oxidation electrode prepared in Example 1 of the present invention for electrocatalytic oxidation of bromide ions; Figure 4This is a capacitance test graph of the first five cycles of 300 cycles of electrocatalytic oxidation of bromide ions by the bromide ion electrooxidation electrode prepared in Example 1 of the present invention; Figure 5 This is a capacitance test graph of the last 5 cycles of 300 cycles of electrocatalytic oxidation of bromide ions by the bromide ion electrooxidation electrode prepared in Example 1 of the present invention. DETAILED DESCRIPTION

[0011] The present invention will be more fully understood by reading the following specific embodiments. However, it should be understood that the specific embodiments disclosed below are only exemplary of the present invention, and the present invention can be embodied in various forms. Therefore, the specific functional details disclosed herein should not be interpreted as limiting, but only as the basis for the claims and as a representative basis for teaching those skilled in the art to adopt the present invention in different ways in any appropriate detailed embodiment.

[0012] As one aspect of the technical solution of the present invention, a method for preparing a bromide ion electro-oxidation electrode involves: providing a first deposition solution comprising a surfactant, a fluoride, a soluble salt of a transition metal, and water; Powering a first electrodeposition system comprising a first working electrode, a counter electrode and a first deposition solution, performing a first electrodeposition on the first working electrode to form a first electrodeposition layer; the first working electrode comprises a porous graphite material; providing a second deposition solution comprising a surfactant, a soluble salt of a transition metal, and water; The second electrodeposition system including the second working electrode, the counter electrode and the second deposition liquid is energized, and the second electrodeposition is performed on the second working electrode to form a second electrodeposition layer to obtain a bromide ion electro-oxidation electrode; the second working electrode includes the first working electrode deposited with the first electrodeposition layer.

[0013] In some embodiments, the surfactant comprises a bromide quaternary ammonium salt surfactant.

[0014] Furthermore, the surfactant includes but is not limited to any one of dodecyltrimethylammonium bromide, tetradecyltrimethylammonium bromide, and hexadecyltrimethylammonium bromide, or a combination of two or more thereof.

[0015] In some embodiments, the fluoride includes but is not limited to any one of sodium fluoride, potassium fluoride, or a combination of both.

[0016] In some embodiments, the transition metal soluble salt includes but is not limited to any one of transition metal nitrates, transition metal sulfates, and transition metal chlorides, or a combination of two or more thereof, and the transition metal contained in the transition metal soluble salt includes cobalt and / or nickel.

[0017] In some embodiments, the concentration of the surfactant in the first deposition liquid or the second deposition liquid is 0.1-0.5 mmol / L.

[0018] In some embodiments, the concentration of fluoride in the first deposition solution is 0.05-0.5 mol / L.

[0019] In some embodiments, the concentration of the soluble transition metal salt in the first deposition solution is 0.05-0.5 mol / L.

[0020] In some embodiments, the concentration of the soluble transition metal salt in the second deposition solution is 0.1-0.5 mol / L.

[0021] In some embodiments, the first electrodeposition time is 0.5 h-5 h.

[0022] In some embodiments, the first electrodeposition process includes: energizing a first electrodeposition system comprising a first working electrode, a counter electrode, and a first deposition solution, and performing the first electrodeposition in a constant current mode.

[0023] In some preferred embodiments, the current value of the constant current in the constant current mode is 5-50 mA / cm 2 .

[0024] In some embodiments, the second electrodeposition process includes: energizing a second electrodeposition system comprising a second working electrode, a counter electrode, and a second deposition solution, and performing the second electrodeposition in a potentiodynamic mode.

[0025] In some preferred embodiments, the potential range of the potentiodynamic mode is -2 to 2 V, the number of scans is 1 to 10, and the scan rate is 1 to 10 mV s -1 .

[0026] In some embodiments, the counter electrode includes, but is not limited to, a titanium sheet.

[0027] In some embodiments, the preparation method further comprises: washing and drying after the first electrodeposition is completed to obtain the first working electrode deposited with the first electrodeposition layer.

[0028] In some embodiments, the preparation method further comprises: washing and drying after the second electrodeposition is completed to obtain the bromide ion electro-oxidation electrode.

[0029] In some specific embodiments, the method for preparing the bromide ion electro-oxidation electrode comprises the following steps: (1) mixing a surfactant, a fluoride, a soluble salt of a transition metal and water to prepare a first deposition solution, wherein the concentration of the surfactant in the first deposition solution is 0.1-0.5 mmol / L, the concentration of the fluoride is 0.05-0.5 mol / L, and the concentration of the soluble salt of the transition metal is 0.05-0.5 mol / L; (2) using a porous graphite sheet as a first working electrode and a titanium sheet as a counter electrode, using the first deposition solution, performing a first electrodeposition in a constant current mode, forming a first electrodeposited layer on the first working electrode, and sequentially washing with water, washing with anhydrous ethanol, and drying at 80° C. for 1 hour to obtain a first working electrode deposited with the first electrodeposited layer; (3) mixing a surfactant, a soluble transition metal salt and water to prepare a second deposition solution, wherein the concentration of the surfactant in the second deposition solution is 0.1-0.5 mmol / L, and the concentration of the soluble transition metal salt is 0.1-0.5 mol / L; (4) The first working electrode deposited with the first electrodeposited layer is used as the second working electrode, and the titanium sheet is used as the counter electrode. The second electrodeposition liquid is used to perform the second electrodeposition in the potentiodynamic mode to form a second electrodeposited layer on the second working electrode. The second electrodeposited layer is washed with water, washed with anhydrous ethanol, and dried at 80° C. for 6 hours to obtain the bromide ion oxidation electrode.

[0030] As another aspect of the technical solution of the present invention, it relates to a bromide ion electro-oxidation electrode prepared by the aforementioned preparation method, wherein the bromide ion electro-oxidation electrode comprises a graphite substrate, a first electro-deposited layer and a second electro-deposited layer sequentially stacked on the graphite substrate; the first electro-deposited layer comprises a transition metal oxide, and the second electro-deposited layer comprises a transition metal oxide.

[0031] In some embodiments, the transition metal oxide includes cobalt oxide and / or nickel oxide.

[0032] As another aspect of the technical solution of the present invention, it also involves the application of the aforementioned bromide ion electro-oxidation electrode in the electrocatalytic oxidation of bromide ions.

[0033] The present invention is further described below by way of examples, but the present invention is not limited to the scope of the examples. The reagents and raw materials used in the following examples are commercially available, and the experimental methods without specific conditions are usually carried out under conventional conditions or under conditions recommended by the manufacturers.

[0034] Example 1 A method for preparing a bromide ion electrooxidation electrode comprises the following steps: (1) mixing hexadecyltrimethylammonium bromide, sodium fluoride, cobalt nitrate and water to prepare a primary sedimentation solution, wherein the concentration of hexadecyltrimethylammonium bromide is 0.1 mmol / L, the concentration of sodium fluoride is 0.5 mol / L, and the concentration of cobalt nitrate is 0.05 mol / L; (2) A porous graphite sheet was used as the working electrode and a titanium sheet was used as the counter electrode. A single deposition solution was used at 10 mA / cm 2 The electrodeposition was carried out in constant current mode for 1 h, followed by washing with water, washing with anhydrous ethanol, and drying at 80°C for 1 h to obtain a deposited electrode.

[0035] (3) Dodecyltrimethylammonium bromide, cobalt chloride and water are mixed to prepare a secondary sedimentation solution, wherein the concentration of dodecyltrimethylammonium bromide is 0.5 mmol / L, and the concentration of cobalt chloride is 0.5 mol / L.

[0036] (4) The primary deposition electrode was used as the working electrode, the titanium sheet was used as the counter electrode, and the secondary deposition solution was used. In the potentiodynamic mode, the potential range was -2 V to 2 V, the number of scans was 10, and the scan rate was 1 mV s -1 The secondary electrodeposition was carried out, and the secondary deposition electrode was obtained by washing with water, washing with anhydrous ethanol, and drying at 80°C for 6 hours, namely, the bromide ion oxidation electrode (denoted as Co@GS). The cross-sectional microstructure is shown in FIG. Figure 1 As shown, it includes a graphite substrate, a first electrodeposited layer and a second electrodeposited layer which are sequentially stacked and deposited on the graphite substrate.

[0037] Using Co@GS electrode material as the working electrode and titanium sheet as the counter electrode, 1.00 mM (80 mg / L) bromide ions were oxidized at a voltage of 1.5 V. The oxidation rate of bromide ions was 97.4% after 12 hours.

[0038] The Co@GS electrode material was subjected to a cycle performance test. The test results are shown in Figure 3 , Figure 4 , Figure 5 , Figure 3 This is a test diagram of the long cycle performance of Co@GS electrode material electrocatalytic oxidation of bromide ions. Figure 4 This is the capacitance test diagram of the first five cycles of the Co@GS electrode material electrocatalytic oxidation of bromide ions in 300 cycles. Figure 5 This is the capacitance test diagram of the Co@GS electrode material after 5 cycles of electrocatalytic oxidation of bromide ions in 300 cycles.

[0039] Example 2 A method for preparing a bromide ion electrooxidation electrode comprises the following steps: (1) Tetradecyltrimethylammonium bromide, potassium fluoride, nickel sulfate and water are mixed to prepare a primary sedimentation solution, wherein the concentration of tetradecyltrimethylammonium bromide is 0.5 mmol / L, the concentration of potassium fluoride is 0.05 mol / L, and the concentration of nickel sulfate is 0.5 mol / L; (2) A porous graphite sheet was used as the working electrode and a titanium sheet was used as the counter electrode. A single deposition solution was used at 50 mA / cm 2 The electrodeposition was carried out in constant current mode for 0.5 h, and then washed with water, washed with anhydrous ethanol, and dried at 80°C for 1 h to obtain a deposited electrode.

[0040] (3) Dodecyltrimethylammonium bromide, cobalt nitrate and water are mixed to prepare a secondary sedimentation solution, wherein the concentration of dodecyltrimethylammonium bromide is 0.1 mmol / L, and the concentration of cobalt nitrate is 0.1 mol / L.

[0041] (4) The primary deposition electrode was used as the working electrode, the titanium sheet was used as the counter electrode, and the secondary deposition solution was used. In the potentiodynamic mode, the potential range was -1.5 V to 1.5 V, the number of scans was 5, and the scan rate was 5 mV s -1 The secondary electrodeposition was carried out, and the secondary deposition electrode was obtained by washing with water, washing with anhydrous ethanol, and drying at 80°C for 6 hours, namely, a bromide ion oxidation electrode (denoted as Ni / Co@GS).

[0042] Using Ni / Co@GS electrode material as the working electrode and titanium sheet as the counter electrode, 0.50 mM (40 mg / L) bromide ions were oxidized at a voltage of 1.75 V. The oxidation rate of bromide ions was 99.1% after 12 hours.

[0043] Example 3 A method for preparing a bromide ion electrooxidation electrode comprises the following steps: (1) mixing hexadecyltrimethylammonium bromide, potassium fluoride, nickel sulfate and water to prepare a primary sedimentation solution, wherein the concentration of hexadecyltrimethylammonium bromide is 0.2 mmol / L, the concentration of potassium fluoride is 0.1 mol / L, and the concentration of nickel sulfate is 0.1 mol / L; (2) A porous graphite sheet was used as the working electrode and a titanium sheet was used as the counter electrode. A single deposition solution was used at 5 mA / cm 2 The electrodeposition was carried out in constant current mode for 5 h, followed by washing with water, washing with anhydrous ethanol, and drying at 80°C for 1 h to obtain a deposited electrode.

[0044] (3) Dodecyltrimethylammonium bromide, nickel nitrate and water are mixed to prepare a secondary deposition solution, wherein the concentration of dodecyltrimethylammonium bromide is 0.5 mmol / L, and the concentration of nickel nitrate is 0.5 mol / L.

[0045] (4) The primary deposition electrode was used as the working electrode, the titanium sheet was used as the counter electrode, and the secondary deposition solution was used. In the potentiodynamic mode, the potential range was -1.2 V to 1.2 V, the number of scans was 1, and the scan rate was 10 mV s -1 The secondary electrodeposition was carried out, and water washing, anhydrous ethanol washing, and drying at 80° C. for 6 hours were performed in sequence to obtain a secondary deposition electrode, namely a bromide ion electrooxidation electrode (denoted as Ni@GS).

[0046] Using Ni@GS electrode material as the working electrode and titanium sheet as the counter electrode, 0.25 mM (20 mg / L) bromide ions were oxidized at a voltage of 2.25 V. The oxidation rate of bromide ions was 92.9% after 12 hours.

[0047] Example 4 A method for preparing a bromide ion electrooxidation electrode comprises the following steps: (1) Tetradecyltrimethylammonium bromide, sodium fluoride, nickel chloride and water are mixed to prepare a primary sedimentation solution, wherein the concentration of tetradecyltrimethylammonium bromide is 0.4 mmol / L, the concentration of sodium fluoride is 0.3 mol / L, and the concentration of nickel chloride is 0.3 mol / L; (2) A porous graphite sheet was used as the working electrode and a titanium sheet was used as the counter electrode. A single deposition solution was used at 10 mA / cm 2 The electrodeposition was carried out in constant current mode for 2 h, followed by washing with water, washing with anhydrous ethanol, and drying at 80°C for 1 h to obtain a deposited electrode.

[0048] (3) Dodecyltrimethylammonium bromide, nickel nitrate and water are mixed to prepare a secondary deposition solution, wherein the concentration of dodecyltrimethylammonium bromide is 0.2 mmol / L, and the concentration of nickel nitrate is 0.3 mol / L.

[0049] (4) The primary deposition electrode was used as the working electrode, the titanium sheet was used as the counter electrode, and the secondary deposition solution was used. In the potentiodynamic mode, the potential range was -2 V to 2 V, the number of scans was 15, and the scan rate was 5 mV s -1 The secondary electrodeposition was carried out, and water washing, anhydrous ethanol washing, and drying at 80° C. for 6 hours were performed in sequence to obtain a secondary deposition electrode, namely a bromide ion electrooxidation electrode (denoted as Ni@GS).

[0050] Using Ni@GS electrode material as the working electrode and titanium sheet as the counter electrode, 1.00 mM bromide ions were oxidized at a voltage of 1.75 V. The oxidation rate of bromide ions was 90.5% after 12 hours.

[0051] Comparative Example 1 A method for preparing an electrode material comprises the following steps: (1) mixing hexadecyltrimethylammonium bromide, sodium fluoride, cobalt nitrate and water to prepare a primary sedimentation solution, wherein the concentration of hexadecyltrimethylammonium bromide is 0.1 mmol / L, the concentration of sodium fluoride is 0.5 mol / L, and the concentration of cobalt nitrate is 0.05 mol / L; (2) A porous graphite sheet was used as the working electrode and a titanium sheet was used as the counter electrode. A single deposition solution was used at 10 mA / cm 2 Electrodeposition was performed in constant current mode for 1 h, followed by washing with water, washing with anhydrous ethanol, and drying at 80°C for 1 h to obtain the electrode material.

[0052] The electrode material obtained in this comparative example was used as the working electrode and the titanium sheet was used as the counter electrode. 1.00 mM bromide ions were oxidized at a voltage of 1.5 V. After 12 hours, the oxidation rate of bromide ions was 64.5%.

[0053] like Figure 2 As shown, Figure 2 This is a comparison diagram of the oxidation rates of bromide ions at different concentrations on the electrode in Examples 1-3 of the present invention. It can be seen that the bromide ion electro-oxidation electrodes of Examples 1-3 of the present invention are used for electrocatalytic oxidation of bromide ions, and are still applicable to systems with bromide ion concentrations lower than 100 mg / L, and the bromide ion oxidation rate is as high as over 90%.

[0054] In summary, the present invention adopts a two-step electrodeposition method to prepare a bromide ion electro-oxidation electrode, which is used as a working electrode for electrocatalytic oxidation of bromide ions. It has high selectivity for bromide ions and good long cycle performance, and can realize the catalytic oxidation of low-grade bromide ions in brine.

[0055] In addition, the inventors of this case also referred to the aforementioned embodiments and conducted experiments with other raw materials, process operations, and process conditions described in this specification, and obtained relatively ideal results.

[0056] The above-mentioned embodiments only express several implementation methods of the present invention, and the descriptions thereof are relatively specific and detailed, but they cannot be understood as limiting the scope of the invention patent. It should be pointed out that, for ordinary technicians in this field, several variations and improvements can be made without departing from the concept of the present invention, and these all belong to the protection scope of the present invention. Therefore, the protection scope of the patent of the present invention shall be subject to the attached claims.

Claims

1. A method for preparing a bromide ion electrooxidation electrode, characterized in that: include: providing a first deposition solution comprising a surfactant, a fluoride, a soluble salt of a transition metal, and water; Powering a first electrodeposition system comprising a first working electrode, a counter electrode and a first deposition solution, performing a first electrodeposition on the first working electrode to form a first electrodeposition layer; the first working electrode comprises a porous graphite material; providing a second deposition solution comprising a surfactant, a soluble transition metal salt, and water; The second electrodeposition system including the second working electrode, the counter electrode and the second deposition liquid is energized, and the second electrodeposition is performed on the second working electrode to form a second electrodeposition layer to obtain a bromide ion electro-oxidation electrode; the second working electrode includes the first working electrode deposited with the first electrodeposition layer.

2. The preparation method according to claim 1, characterized in that: The surfactant includes a bromide ion quaternary ammonium salt surfactant, preferably including any one of dodecyltrimethylammonium bromide, tetradecyltrimethylammonium bromide, and hexadecyltrimethylammonium bromide, or a combination of two or more thereof; And / or, the fluoride comprises any one of sodium fluoride and potassium fluoride or a combination of the two; And / or, the transition metal soluble salt includes any one of transition metal nitrates, transition metal sulfates, and transition metal chlorides, or a combination of two or more thereof, and the transition metal contained in the transition metal soluble salt includes cobalt and / or nickel.

3. The preparation method according to claim 1, characterized in that: The concentration of the surfactant in the first deposition liquid or the second deposition liquid is 0.1-0.5 mmol / L; and / or, the concentration of fluoride in the first deposition solution is 0.05-0.5 mol / L; and / or, the concentration of the soluble transition metal salt in the first deposition solution is 0.05-0.5 mol / L; And / or, the concentration of the soluble transition metal salt in the second deposition solution is 0.1-0.5 mol / L.

4. The preparation method according to claim 1, characterized in that: The first electrodeposition time is 0.5 h-5 h; And / or, the first electrodeposition process comprises: energizing a first electrodeposition system comprising a first working electrode, a counter electrode and a first deposition solution, and performing the first electrodeposition in a constant current mode; Preferably, the current value of the constant current in the constant current mode is 5-50 mA / cm 2 .

5. The preparation method according to claim 1, characterized in that: The second electrodeposition process comprises: energizing a second electrodeposition system comprising a second working electrode, a counter electrode and a second deposition solution, and performing the second electrodeposition in a potentiodynamic mode; Preferably, the potential range of the potentiodynamic mode is -2-2 V, the number of scans is 1-10, and the scan rate is 1-10 mV s -1 .

6. The preparation method according to claim 1, characterized in that: The counter electrode includes a titanium sheet.

7. The preparation method according to claim 1, characterized in that: Also includes: After the first electrodeposition is completed, washing and drying are performed to obtain the first working electrode deposited with the first electrodeposition layer; And / or, the preparation method further comprises: washing and drying after the second electrodeposition is completed to obtain the bromide ion electro-oxidation electrode.

8. The bromide ion oxidation electrode prepared by the preparation method according to any one of claims 1 to 7, characterized in that: The bromide ion electro-oxidation electrode comprises a graphite substrate, a first electrodeposited layer and a second electrodeposited layer which are sequentially stacked on the graphite substrate; the first electrodeposited layer comprises a transition metal oxide, and the second electrodeposited layer comprises a transition metal oxide.

9. The bromide ion electrooxidation electrode according to claim 8, characterized in that: The transition metal oxide includes cobalt oxide and / or nickel oxide.

10. Use of the bromide ion electro-oxidation electrode according to claim 8 or 9 in electrocatalytic oxidation of bromide ions.

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