A high-entropy layered double hydroxide electrode material, a preparation method and application thereof

Abstract

This invention relates to the field of electrode materials technology, specifically to a high-entropy layered double hydroxide electrode material, its preparation method, and its application. The electrode material includes a metal substrate and a layered double hydroxide with a high-entropy structure grown in situ on the surface of the metal substrate. The layered double hydroxide consists of a main layer and intercalated anions filling the spaces between the main layers. The main layers include Ni, Co, Fe, Cu, and Al elements, and the intercalated anions are any one of phosphate, carbonate, or dodecyl sulfate. The high-entropy layered double hydroxide electrode material of this invention uses phosphate, carbonate, or dodecyl sulfate intercalation to adjust the interlayer structure, effectively expanding the interlayer spacing of the high-entropy layered double hydroxide to form an interlayer microenvironment more conducive to ion migration and interfacial reactions during electrochemical hydrodechlorination.

Description

Technical Field

[0001] This invention relates to the field of electrode materials technology, specifically to a high-entropy layered double hydroxide electrode material, its preparation method, and its application. Background Technology

[0002] Chlorinated organic pollutants are widely found in wastewater from industries such as chemical, petrochemical, and pharmaceutical, as well as in extracts from contaminated site remediation. They are characterized by high toxicity, strong chemical stability, and difficulty in biodegradation. Therefore, efficient dechlorination and harmless disposal are crucial for water environment management and risk reduction. Electrochemical hydrodechlorination is a water treatment technology that utilizes electrocatalytic reactions to convert chlorinated organic pollutants into non-toxic or low-toxic products on the cathode surface. It offers advantages such as ambient temperature and pressure, controllable process parameters, and easy integration with water treatment units.

[0003] However, existing cathode materials used in electrochemical hydrodechlorination mainly include noble metal systems and non-noble metal systems. Noble metals (such as Pd and Pt) and their supported materials can improve the kinetics of dechlorination reactions, but their high raw material costs and significant resource constraints limit the economic viability of large-scale applications. Non-noble metal materials have a cost advantage, but they generally face problems such as high competition from hydrogen evolution reactions and insufficient electron / proton utilization in the dechlorination pathway, making it difficult to balance energy efficiency and selectivity.

[0004] To address the aforementioned contradictions, many related patents in recent years have proposed using high-entropy layered double hydroxides (HE-LDH) as electrocatalytic materials. For example, Chinese invention patent CN120485852A discloses a method for constructing "high-valence metal-doped high-entropy LDH / MOF composite materials" on three-dimensional current collectors such as nickel foam, mainly targeting water electrolysis or urea electrolysis systems, with the goal of improving HER / OER / UOR activity and overall electrolysis performance. Chinese invention patent CN119461517A proposes a pentagonal high-entropy layered double hydroxide for activating persulfate and degrading tetracycline in advanced oxidation scenarios, focusing on the mechanism regulation of the oxidation process. Chinese invention patent CN120646922A discloses a composite material of high-entropy layered double hydroxides and aerogel systems for electromagnetic wave absorption or infrared stealth applications. However, the technical objectives of the aforementioned patents differ significantly from the key requirements of electrochemical hydrodechlorination. Existing similar high-entropy double hydroxide routes generally focus more on improving the performance of electrolytic reactions or the application of oxidative / functional materials, and have not yet formed a specialized material system and electrode construction path for "improving the effective utilization of electrons / protons in the dechlorination path and suppressing side reactions of hydrogen evolution reaction" on the cathode side of electrochemical hydrodechlorination.

[0005] Furthermore, interlayer anions have a significant impact on the interlayer spacing, ion migration channels, and interfacial reaction microenvironment, which in turn affect the performance of high-entropy layered double hydroxides. In multi-metal coprecipitation systems, the hydrolysis / precipitation kinetics of different metal ions differ significantly. Without a holistic process design for "controlled nucleation - uniform growth - subsequent aging and stabilization," insufficient consistency in composition and structure can easily occur. Summary of the Invention

[0006] To address the aforementioned problems, this invention provides a high-entropy layered double hydroxide electrode material, its preparation method, and its applications.

[0007] The technical solution of the present invention is: a high-entropy layered double hydroxide electrode material, comprising a metal substrate and a layered double hydroxide with a high-entropy structure grown in situ on the surface of the metal substrate; the layered double hydroxide is composed of a main layer and intercalated anions filling the spaces between the main layers, wherein the main layer comprises Ni, Co, Fe, Cu and Al elements, and the intercalated anions are any one of phosphate, carbonate or dodecyl sulfate.

[0008] Note: This invention uses phosphate, carbonate or dodecyl sulfate intercalation to adjust the interlayer structure, thereby effectively expanding the interlayer spacing of high-entropy layered double hydroxides to form an interlayer microenvironment that is more conducive to ion migration and interfacial reactions during electrochemical hydrodechlorination.

[0009] Furthermore, the layered double hydroxide has a three-dimensional nanosheet structure, which is distributed in an array on the surface of the metal substrate.

[0010] Note: The layered double hydroxides with the above structure can be directly bonded to the metal substrate, and the mass transfer and adsorption efficiency of hydrogen ions can be improved through the numerous micropores in the three-dimensional nanosheet structure.

[0011] Furthermore, the metal substrate is nickel foam or nickel mesh.

[0012] Note: The above-mentioned metal substrate has a huge specific surface area and open pores, which can be fully wetted by the metal salt solution to grow layered double hydroxides in situ on the metal substrate.

[0013] On the other hand, the present invention also provides a method for preparing the above-mentioned high-entropy layered double hydroxide electrode material, comprising the following steps: S1. Dissolve nickel nitrate, cobalt nitrate, ferric nitrate, copper nitrate, and aluminum nitrate separately in deionized water to prepare salt solutions of 0.08~0.12 mol / L. Then, take each salt solution to prepare a mother liquor and dilute the mother liquor 7~9 times with deionized water to obtain a mixed solution. S2. Immerse the metal substrate in the mixture and stir at room temperature for 25-35 minutes. Then, adjust the pH of the mixture to 9-11 using a sodium hydroxide solution with a molar concentration of 2-6 mol / L, and continue stirring at room temperature for 50-70 minutes to obtain an alkalized mixture. The mass ratio of the metal substrate to the mixture is 1:7-9. S3. Transfer the alkalization mixture to the reaction vessel, add the intercalated anion source to the alkalization mixture, and perform a hydrothermal reaction at 55~65℃ for 11~13h. Then, remove the metal substrate and perform post-processing to obtain a high-entropy layered double hydroxide electrode material. The molar concentration of the intercalated anion source in the alkalization mixture is 0.1~0.2mol / L.

[0014] Note: The above preparation method involves in-situ nucleation / growth of various water-soluble metal nitrates through alkalization co-precipitation in the presence of nickel foam substrate, and subsequent hydrothermal process to achieve intercalation and aging coupled treatment, so as to achieve specific anion intercalation simultaneously during aging, thereby obtaining an integrated high-entropy layered double hydroxide composite material that can be directly used as a cathode. Moreover, the preparation process path is clear, highly controllable, and suitable for large-scale implementation.

[0015] Furthermore, the molar ratio of Ni, Co, Fe, Cu and Al elements in the mother liquor is 2.5~3.5:1.5~2.5:0.5~1.5:1.5~2.5:1.5~2.5.

[0016] Note: The above molar ratio ensures good bonding between the layered double hydroxide and the metal substrate, thus guaranteeing the stability of the electrode material.

[0017] Furthermore, in step S2, after immersing the metal substrate in the mixture, nitrogen gas is continuously introduced into the mixture at a rate of 1~1.5 L / min.

[0018] Note: Introducing nitrogen can reduce the interference of carbon dioxide in the air on the composition of intercalated anions and improve the consistency of the material structure.

[0019] Furthermore, when adjusting the pH value, the sodium hydroxide solution is added dropwise, and the addition of sodium hydroxide solution is completed within 25~35 minutes. During the pH adjustment, for every 1 increase in the pH of the mixture, the nitrogen gas introduction rate increases by 0.4~0.6 L / min.

[0020] Explanation: By controlling the nitrogen gas introduction rate and pH adjustment rate, impurities in the layered double hydroxide can be reduced. At the same time, the nitrogen gas introduction rate gradually increases with the increase of pH value, which can effectively prevent carbon dioxide from dissolving into the alkaline mixture, allowing the metal salt to fully precipitate and form a porous three-dimensional nanosheet structure on the metal substrate.

[0021] Furthermore, in step S3, the intercalation anion source is any one of phosphate, carbonate, and dodecyl sulfate.

[0022] Note: The above-mentioned anion source can effectively expand the interlayer spacing of layered double hydroxides, change the interlayer microenvironment, and improve the conductivity, activity, and stability of electrode materials.

[0023] Furthermore, the post-processing method is as follows: first wash with anhydrous ethanol, then rinse with deionized water, and then freeze-dry.

[0024] Note: The above post-treatment method can effectively remove the salt solution remaining in the layered double hydroxide and avoid clogging of the micropores inside the layered double hydroxide.

[0025] On the other hand, the present invention also provides the application of the above-mentioned high-entropy layered double hydroxide electrode material in electrochemical hydrogenation dechlorination.

[0026] Note: The above-mentioned high-entropy layered double hydroxide electrode material constructs multi-metal synergistic active sites adapted to electrochemical hydrodechlorination in a non-noble metal system, and achieves structural regulation and interfacial consolidation through a controllable anion system and a mild aging process, thereby realizing efficient electrochemical hydrodechlorination.

[0027] The beneficial effects of this invention are: (1) The high-entropy layered double hydroxide electrode material of the present invention uses phosphate, carbonate or dodecyl sulfate intercalation to adjust the interlayer structure, thereby effectively expanding the interlayer spacing of the high-entropy layered double hydroxide to form an interlayer microenvironment that is more conducive to ion migration and interfacial reaction during electrochemical hydrogenation and dechlorination.

[0028] (2) The preparation method of the present invention uses a variety of water-soluble metal nitrates to carry out in-situ nucleation / growth through alkalization co-precipitation in the presence of nickel foam substrate, and realizes intercalation and aging coupling treatment in subsequent hydrothermal process, thereby obtaining an integrated high-entropy layered double hydroxide composite material that can be directly used as a cathode. The preparation process path is clear, highly controllable and suitable for large-scale implementation.

[0029] (3) The high-entropy layered double hydroxide electrode material prepared by the present invention constructs multi-metal synergistic active sites adapted to electrochemical hydrogen dechlorination in a non-noble metal system, and achieves structural regulation and interface consolidation through a controllable anion system and a mild aging process, thereby achieving efficient electrochemical hydrogen dechlorination. Attached Figure Description

[0030] Figure 1 This is the XRD diffraction pattern of Experimental Example 1 of this invention; Figure 2 This is a graph showing the degradation performance of the electrode material of Experimental Example 1 of the present invention on chloramphenicol; Figure 3 This is a graph showing the degradation performance of the electrode material of Experimental Example 2 of the present invention on chloramphenicol; Figure 4 This is a graph showing the degradation performance of the electrode material of Experimental Example 3 of the present invention on chloramphenicol; Figure 5 This is a graph showing the degradation performance of the electrode material for chloramphenicol in Experimental Example 4 of this invention; Figure 6 This is a graph showing the degradation performance of the electrode material of Experimental Example 5 of the present invention on chloramphenicol; Figure 7 This is a graph showing the degradation performance of the electrode material of Experimental Example 6 of the present invention on chloramphenicol; Figure 8 This is a graph showing the degradation performance of the electrode material of Experimental Example 7 of the present invention on chloramphenicol; Figure 9 This is a graph showing the degradation performance of the electrode material of Experimental Example 8 of the present invention on chloramphenicol. Detailed Implementation

[0031] To further illustrate the methods and effects of this invention, the technical solution of this invention will be clearly and completely described below in conjunction with experiments.

[0032] Example 1: A high-entropy layered double hydroxide electrode material, comprising a metal substrate and a layered double hydroxide with a high-entropy structure grown in situ on the surface of the metal substrate; the layered double hydroxide is composed of a main layer and intercalated anions filling the spaces between the main layers, wherein the main layer comprises Ni, Co, Fe, Cu and Al elements, and the intercalated anions are phosphate groups; The layered double hydroxide has a three-dimensional nanosheet structure, which is distributed in an array on the surface of the metal substrate; the metal substrate is nickel foam. The preparation method of the above-mentioned high-entropy layered double hydroxide electrode material includes the following steps: S1. Dissolve nickel nitrate, cobalt nitrate, ferric nitrate, copper nitrate, and aluminum nitrate separately in deionized water to prepare salt solutions with a molar concentration of 0.1 mol / L. Then, take each salt solution by molar ratio to prepare 10 ml of stock solution. Dilute the stock solution 8 times with deionized water to obtain a mixed solution. The molar ratio of Ni, Co, Fe, Cu, and Al in the stock solution is 3:2:1:2:2. The size of the metal substrate is 2×2 cm. S2. Immerse the metal substrate in the mixture, continuously introduce nitrogen gas into the mixture at a rate of 1.25 L / min, and stir at room temperature for 30 min. Adjust the pH of the mixture to 10 using a 4 mol / L sodium hydroxide solution, and continue stirring at room temperature for 60 min to obtain an alkalized mixture; wherein the mass ratio of the metal substrate to the mixture is 1:8. S3. The alkalization mixture was transferred to a reaction vessel. An intercalated anion source was added to the alkalization mixture, and the mixture was subjected to hydrothermal reaction at 60°C for 12 hours. The metal substrate was then removed and post-treated to obtain a high-entropy layered double hydroxide electrode material. The molar concentration of the intercalated anion source in the alkalization mixture was 0.15 mol / L. The intercalated anion source was trisodium phosphate. The post-treatment method was as follows: first, washing with anhydrous ethanol, then rinsing with deionized water, followed by freeze-drying. The freeze-drying temperature was -18°C, and the time was 24 hours.

[0033] Example 2: This example is basically the same as Example 1, except that the intercalation anion source is sodium dodecyl sulfate; Example 3: This example is basically the same as Example 1, except that the intercalation anion source is sodium carbonate.

[0034] Example 4: This example is basically the same as Example 1, except that the molar ratio of Ni, Co, Fe, Cu and Al in the mother liquor is 2.5:1.5:0.5:1.5:1.5.

[0035] Example 5: This example is basically the same as Example 1, except that the molar ratio of Ni, Co, Fe, Cu and Al in the mother liquor is 3.5:2.5:1.5:2.5:2.5.

[0036] Example 6: This example is basically the same as Example 1, except that the pH value of the mixture is adjusted to 9 using a sodium hydroxide solution with a molar concentration of 4 mol / L.

[0037] Example 7: This example is basically the same as Example 1, except that the pH value of the mixture is adjusted to 11 using a sodium hydroxide solution with a molar concentration of 4 mol / L.

[0038] Example 8: This example is basically the same as Example 1, except that after adding the intercalated anion source to the alkalized mixture, the mixture is subjected to hydrothermal reaction at 55°C for 11 hours.

[0039] Example 9: This example is basically the same as Example 1, except that after adding the intercalated anion source to the alkalized mixture, the mixture is subjected to hydrothermal reaction at 65°C for 13 hours.

[0040] Example 10: This example is basically the same as Example 1, except that the molar concentration of the intercalated anion source in the alkaline mixture is 0.1 mol / L.

[0041] Example 11: This example is basically the same as Example 1, except that the molar concentration of the intercalated anion source in the alkaline mixture is 0.2 mol / L.

[0042] Example 12: This example is basically the same as Example 1, except that in step S2, the sodium hydroxide solution is added dropwise when adjusting the pH value, and the dropwise addition is completed within 30 minutes. During the pH adjustment, for every 1 increase in the pH of the mixture, the nitrogen gas introduction rate increases by 0.5 L / min.

[0043] Example 13: This example is basically the same as Example 14, except that the sodium hydroxide solution is added dropwise within 25 minutes.

[0044] Example 14: This example is basically the same as Example 14, except that the sodium hydroxide solution is added dropwise within 35 minutes.

[0045] Example 15: This example is basically the same as Example 14, except that the nitrogen introduction rate increases by 0.4 L / min for every 1 increase in pH of the mixture during pH adjustment.

[0046] Example 16: This example is basically the same as Example 14, except that the nitrogen introduction rate increases by 0.6 L / min for every 1 increase in pH of the mixture during pH adjustment.

[0047] Comparative Example 1: Referring to Example 1, in step S2, the metal substrate and the intercalated anion source were added together into the mixture.

[0048] Experimental Example: To investigate the performance of the electrode materials in each embodiment and comparative example, a 0.1 mol / L Na₂SO₄ solution was prepared at room temperature, and chloramphenicol (30 mg / L) was added to the Na₂SO₄ solution to obtain simulated wastewater. The simulated wastewater was placed in the cathode chamber of an electrochemical reactor (H-type electrolytic cell). Separately, a 0.1 mol / L Na₂SO₄ solution without chloramphenicol was prepared and added to the anode chamber of the electrochemical reactor (H-type electrolytic cell) to construct an electrochemical reaction system. The electrode materials prepared in each embodiment and comparative example were used as cathodes for electrochemical hydrogenation and dechlorination reactions. Samples were taken periodically during the reaction, and high-performance liquid chromatography (HPLC) was used to determine the change in chloramphenicol concentration to calculate the removal effect. The specific investigation is as follows: Experiment Example 1: Investigating the Influence of Intercalated Anion Types on Electrode Material Properties like Figure 1As shown, a comparison of the XRD diffraction patterns of Examples 1, 2, 3 and Comparative Example 1 reveals that, compared to the electrode material of Example 3, the peak at ~10° in the electrode materials of Examples 1 and 2 shifted to the left, and the electrode material of Example 1 exhibited the strongest peak broadening phenomenon. This indicates that the interlayer spacing of the high-entropy layered double hydroxide with phosphate intercalation was effectively expanded, accompanied by severe lattice distortion, forming an interlayer microenvironment more conducive to the proton coupling electron transfer process and interfacial reaction during electrochemical hydrodechlorination, and providing more active sites for the catalytic reaction. No obvious diffraction peaks were observed in Comparative Example 1, possibly because phosphate ions have a strong tendency to coordinate with various metal cations. During coprecipitation, metal ions that should have gradually assembled into layers through hydroxyl bridging were preferentially removed by phosphate ions, resulting in the inhibition or interruption of nucleation and crystallization of the layered double hydroxide layers.

[0049] like Figure 2 As shown, a comparison of Examples 1, 2, and 3 reveals that the electrode material of Example 1 achieved a degradation rate of over 96% for chloramphenicol within 60 minutes and over 99% within 120 minutes. This indicates that the electrode material of Example 1 exhibits the highest efficiency in the hydrogenation dechlorination reaction. This may be because the interlayer spacing of the phosphate-intercalated layered double hydroxide is larger, resulting in better structural stability. Therefore, the intercalated anion source selected in Example 1 is superior.

[0050] Experiment Example 2: Investigating the effect of mother liquor ratio on electrode material performance like Figure 3 As shown in the comparison of Examples 1, 4, and 5, it can be seen that the electrode material of Example 1 has the highest degradation rate and the fastest degradation rate for chloramphenicol, indicating that the electrode material of Example 1 has the best performance. This may be because the main plate structure is the most stable and the electron transport efficiency is higher under the mother liquor ratio of Example 1. Therefore, the mother liquor ratio selected in Example 1 is better.

[0051] Experiment Example 3: Investigating the effect of pH value of the mixed solution on the performance of electrode materials. like Figure 4 As shown in the comparison of Examples 1, 6, and 7, it can be seen that the electrode material of Example 1 has the highest degradation rate and the fastest degradation rate for chloramphenicol, indicating that the electrode material of Example 1 has the best performance. This may be because the metal ions in the mixed solution can be fully precipitated onto the metal substrate at the pH value of the mixed solution in Example 1. Therefore, the pH value of the mixed solution selected in Example 1 is the best.

[0052] Experiment Example 4: Investigating the Influence of Hydrothermal Reaction Parameters on Electrode Material Properties like Figure 5As shown in the comparison of Examples 1, 8, and 9, it can be seen that the electrode material of Example 1 has the highest degradation rate and the fastest degradation rate for chloramphenicol, indicating that the electrode material of Example 1 has the best performance. This may be because the anion source can be fully intercalated at the hydrothermal reaction temperature and time of Example 1, so the hydrothermal reaction parameters selected in Example 1 are optimal.

[0053] Experiment Example 5: Investigating the effect of intercalation anion source concentration on electrode material properties like Figure 6 As shown in the comparison of Examples 1, 10, and 11, it can be seen that the electrode material of Example 1 has the highest degradation rate and the fastest degradation rate for chloramphenicol, indicating that the electrode material of Example 1 has the best performance. This may be because the interlayer spacing of the layered double hydroxide is larger at the intercalation anion source concentration of Example 1. Therefore, the intercalation anion source concentration selected in Example 1 is the optimal one.

[0054] Experiment Example 6: Investigating the effect of nitrogen introduction method on electrode material properties like Figure 7 As shown, a comparison between Examples 1 and 12 reveals that the electrode material of Example 12 exhibits a faster degradation rate of chloramphenicol within 60 minutes, with a degradation rate exceeding 98%. This may be because the nitrogen introduction method in Example 12 allows for the full discharge of carbon dioxide, preventing a large amount of carbon dioxide from dissolving into the alkalization mixture, thereby reducing side reaction products and ensuring sufficient precipitation of metal ions. Therefore, the nitrogen introduction method selected in Example 12 is the optimal one.

[0055] Experiment Example 7: Investigating the effect of sodium hydroxide solution addition time on electrode material performance. like Figure 8 As shown in the comparison of Examples 12, 13, and 14, it can be seen that the electrode material of Example 12 exhibits a faster degradation rate and the highest degradation rate of chloramphenicol within 60 minutes. This may be because the addition time of the nitrogen-containing sodium hydroxide solution selected in Example 12 results in the fewest side reaction products in the mixed solution and the most stable electrode material structure. Therefore, the sodium hydroxide solution addition time selected in Example 12 is optimal.

[0056] Experiment Example 8: Investigating the effect of increasing nitrogen gas introduction rate on electrode material properties. like Figure 9 As shown in the comparison of Examples 12, 15, and 16, it can be seen that the electrode material of Example 12 exhibits a faster degradation rate and the highest degradation rate of chloramphenicol within 60 minutes. This may be because the increase in nitrogen gas introduction rate selected in Example 12 results in the fewest side reactions. Therefore, the increase in nitrogen gas introduction rate selected in Example 12 is the optimal one.

Claims

1. A high-entropy layered double hydroxide electrode material, characterized in that, The invention includes a metal substrate and a layered double hydroxide with a high-entropy structure grown in situ on the surface of the metal substrate; the layered double hydroxide consists of a main layer and intercalated anions filling the space between the main layers, wherein the main layer includes elements of Ni, Co, Fe, Cu and Al, and the intercalated anions are any one of phosphate, carbonate or dodecyl sulfate.

2. The high-entropy layered double hydroxide electrode material according to claim 1, characterized in that, The layered double hydroxide has a three-dimensional nanosheet structure, which is distributed in an array on the surface of the metal substrate.

3. The high-entropy layered double hydroxide electrode material according to claim 1, characterized in that, The metal substrate is nickel foam or nickel mesh.

4. A method for preparing a high-entropy layered double hydroxide electrode material according to any one of claims 1 to 3, characterized in that, Includes the following steps: S1. Dissolve nickel nitrate, cobalt nitrate, ferric nitrate, copper nitrate, and aluminum nitrate separately in deionized water to prepare salt solutions of 0.08~0.12 mol / L. Then, take each salt solution to prepare a mother liquor and dilute the mother liquor 7~9 times with deionized water to obtain a mixed solution. S2. Immerse the metal substrate in the mixture and stir at room temperature for 25-35 minutes. Then, adjust the pH of the mixture to 9-11 using a sodium hydroxide solution with a molar concentration of 2-6 mol / L, and continue stirring at room temperature for 50-70 minutes to obtain an alkalized mixture. The mass ratio of the metal substrate to the mixture is 1:7-9. S3. Transfer the alkalization mixture to the reaction vessel, add the intercalated anion source to the alkalization mixture, and perform a hydrothermal reaction at 55~65℃ for 11~13h. Then, remove the metal substrate and perform post-processing to obtain a high-entropy layered double hydroxide electrode material. The molar concentration of the intercalated anion source in the alkalization mixture is 0.1~0.2mol / L.

5. The method for preparing a high-entropy layered double hydroxide electrode material according to claim 4, characterized in that, The molar ratio of Ni, Co, Fe, Cu and Al in the mother liquor is 2.5~3.5:1.5~2.5:0.5~1.5:1.5~2.5:1.5~2.

5.

6. The method for preparing a high-entropy layered double hydroxide electrode material according to claim 4, characterized in that, In step S2, after immersing the metal substrate in the mixture, nitrogen gas is continuously introduced into the mixture at a rate of 1~1.5 L / min.

7. The method for preparing a high-entropy layered double hydroxide electrode material according to claim 6, characterized in that, In step S2, sodium hydroxide solution is added dropwise when adjusting the pH value, and the addition of sodium hydroxide solution is completed within 25~35 minutes. During the pH adjustment, for every 1 increase in the pH of the mixture, the nitrogen gas introduction rate increases by 0.4~0.6 L / min.

8. The method for preparing a high-entropy layered double hydroxide electrode material according to claim 4, characterized in that, In step S3, the intercalation anion source is any one of phosphate, carbonate, and dodecyl sulfate.

9. The method for preparing a high-entropy layered double hydroxide electrode material according to claim 4, characterized in that, The post-processing method is as follows: first wash with anhydrous ethanol, then rinse with deionized water, and then freeze-dry.

10. The application of a high-entropy layered double hydroxide electrode material according to any one of claims 1 to 3 in electrochemical hydrogenation dechlorination.

Images