Method for realizing base-catalyzed organic oxidation reaction through local pH regulation and control in non-strong alkaline solution

Abstract

The invention discloses a method for realizing base-catalyzed organic oxidation reaction through local pH regulation and control in a non-strong alkaline solution, which comprises the following steps: by taking the non-strong alkaline solution containing organic matters as an electrolyte, applying alternating current to an electrode, periodically switching the polarity of the electrode, and carrying out pH regulation and control on the polarity of the electrode; and the polarity of the same electrode is periodically and alternately converted between a cathode state and an anode state. By adopting the method provided by the invention, the pH value of a non-strong alkaline solution does not need to be adjusted to be strong alkaline, and OH <-> generated by the electrode in a cathode state constructs a strong alkaline environment on the surface of the electrode in situ, so that the base-catalyzed organic oxidation reaction depending on the strong alkaline environment can still be stably supported to be continuously and efficiently carried out under the non-strong alkaline condition of a bulk phase. By regulating and controlling the alternating current period, the local pH of the surface of the electrode can be precisely regulated and controlled, so that the base catalysis organic oxidation reaction is precisely and efficiently catalyzed.

Description

Technical Field

[0001] This invention belongs to the field of electrocatalysis, specifically relating to a method for performing electrocatalytic base-catalyzed organic oxidation reactions in a non-strongly alkaline solution. Background Technology

[0002] Over-reliance on fossil fuels has led to increasingly severe energy shortages and environmental pollution. Hydrogen energy, as a clean energy carrier, is an important alternative to fossil fuels. Although water electrolysis for hydrogen production is clean and efficient, its slow kinetics and high overpotential of the oxygen evolution reaction (OER) at the anolyte limit its economic benefits, severely restricting the development of this technology.

[0003] To improve the energy efficiency and economics of hydrogen electrolysis, researchers have extensively explored replacing OER with more economically viable anodic reactions. Among these, organic oxidation reactions, such as ethylene glycol oxidation (EGOR), urea oxidation (UOR), and hydrazine oxidation (HzOR), have shown significant advantages. From a thermodynamic perspective, the theoretical potential of EGOR is 0.065V, UOR is 0.37V, and HzOR is even lower. These reactions can significantly reduce the actual operating voltage during electrolysis compared to OER, thus reducing energy consumption. From a resource utilization perspective, EGOR can be directionally converted into glycolic acid (a raw material for biodegradable materials, with a market price of approximately RMB 18,000 / ton) and glyoxylic acid (a pharmaceutical intermediate, with a price exceeding RMB 50,000 / ton). Hydrazine oxidation can convert hydrazine in industrial wastewater into harmless N2. Using these organic oxidation reactions to replace OER enables efficient coupling of hydrogen production and the electrosynthesis of high-value chemicals, providing a synergistic solution for clean energy conversion and pollution control, and endowing hydrogen electrolysis technology with both environmental and economic value.

[0004] However, these organic oxidation reactions typically require a strongly alkaline environment to proceed efficiently and stably. In practice, strongly alkaline conditions not only increase the cost of alkali feedstock and the need for replenishment, but also introduce problems such as equipment corrosion, operational safety risks, and wastewater treatment. Therefore, there is an urgent need to develop new electrocatalytic organic oxidation technologies that can operate efficiently and stably under non-strongly alkaline conditions. Achieving this goal will significantly simplify the electrolysis process, reduce material and equipment maintenance costs, improve process safety and environmental compatibility, and have significant scientific and engineering application value for promoting the sustainable development of green hydrogen production and organic electrosynthesis technologies. Summary of the Invention

[0005] In order to at least solve one or more of the technical problems mentioned above, the present invention provides a method for achieving alkaline-catalyzed organic oxidation reaction in a non-strongly alkaline solution by local pH regulation, comprising the steps of: using a non-strongly alkaline solution containing organic matter as an electrolyte, applying alternating current to the electrodes, and periodically switching the polarity of the electrodes so that the polarity of the same electrode periodically alternates between the cathode state and the anode state.

[0006] According to one embodiment of the present invention, before applying alternating current to the electrodes, a pretreatment step is included: immersing the electrodes in a strongly alkaline solution containing organic matter.

[0007] According to one embodiment of the present invention, the electrode is immersed in a strongly alkaline solution containing organic matter for 2-60 seconds.

[0008] According to one embodiment of the present invention, the electrode is selected from any one of a platinum electrode, a platinum-rhodium alloy electrode, a titanium felt coated platinum electrode, a nickel foam electrode, and a titanium electrode. Preferably, the electrode is selected as an electrode that does not react in the electrolyte.

[0009] According to one embodiment of the present invention, the waveform of the alternating current is selected from square wave, sine wave, triangle wave or sawtooth wave.

[0010] According to one embodiment of the present invention, the waveform of the alternating current is selected from a square wave.

[0011] According to one embodiment of the present invention, the voltage of the alternating current is 1-380V.

[0012] According to one embodiment of the present invention, the voltage of the alternating current is 1.2-1.8V.

[0013] According to one embodiment of the present invention, the period of the alternating current is 0.1-60s.

[0014] According to one embodiment of the present invention, the temperature of the electrolyte is 5-95°C.

[0015] According to one embodiment of the present invention, the non-alkaline solution is an aqueous solution with pH < 8.5.

[0016] According to one embodiment of the present invention, the non-alkaline solution is selected from any one or more of the following: natural seawater, river water, and tap water.

[0017] According to one embodiment of the present invention, the alkali-catalyzed organic oxidation reaction is an organic oxidation reaction that depends on a strongly alkaline environment, including methanol oxidation and ethanol oxidation reactions in alcohol oxidation reactions; and formaldehyde oxidation and glucose oxidation reactions in aldehyde oxidation reactions.

[0018] According to one embodiment of the present invention, the alkali-catalyzed organic oxidation reaction is selected from any one of ethylene glycol oxidation reaction, glycerol oxidation reaction, urea oxidation reaction, and hydrazine oxidation reaction.

[0019] According to one embodiment of the present invention, the organic compound is selected from any one of ethylene glycol, glycerol, urea, and hydrazine.

[0020] According to one embodiment of the present invention, the strongly alkaline solution used in the alkaline pretreatment step has a pH > 11 and contains 0.1-10 mol / L of organic matter.

[0021] According to one embodiment of the present invention, the strongly alkaline solution in the alkaline pretreatment step is alkaline seawater containing 2 mol / L ethylene glycol.

[0022] According to one embodiment of the present invention, the electrolyte is natural seawater containing 2 mol / L ethylene glycol.

[0023] According to one embodiment of the present invention, the electrolyte is a non-strongly alkaline solution containing 0.1-10 mol / L of organic matter.

[0024] This invention discloses a method for electrocatalytic base-catalyzed organic oxidation reactions in a non-strongly alkaline solution. The non-strongly alkaline solution is an aqueous solution with a pH < 8.5. Base-catalyzed organic oxidation reactions are organic oxidation reactions that require a strongly alkaline environment to proceed efficiently. A strongly alkaline environment is a chemical environment with a pH > 11. Using a non-strongly alkaline solution containing organic matter as the electrolyte, an alternating current is applied to the electrodes, and the polarity of the electrodes is periodically switched, causing the polarity of the same electrode to alternate periodically between the cathode and anodic states. When the electrode is in the cathode state, a hydrogen evolution reaction occurs, generating hydrogen gas (H2) and hydroxide ions (OH-). - This creates a localized strongly alkaline environment on the electrode surface, allowing the alkali-catalyzed organic oxidation reaction, which can only be efficiently carried out under a strongly alkaline environment, to proceed smoothly when the electrode switches to the anodic state.

[0025] Some organic oxidation reactions coupled with hydrogen evolution reaction (HER) require a strongly alkaline environment to proceed efficiently. However, the use of strongly alkaline solutions not only increases operational complexity and raw material costs but also introduces corrosion and safety risks. Therefore, this invention provides a simple method: by periodically switching electrode polarity, the same electrode alternates between cathode and anodic states. When the electrode is in the cathode state, a hydrogen evolution reaction occurs, generating hydrogen gas (H2) and hydroxide ions (OH-). -This allows for in-situ adjustment of the local pH on the electrode surface, creating a locally strongly alkaline environment. When the electrode is in the anodic state, this locally strongly alkaline environment ensures the continuous and efficient execution of the alkali-catalyzed organic oxidation reaction. Since the electrode surface, acting as the anolyse, is not strongly alkaline at the start of the reaction, the alkali-catalyzed organic oxidation reaction cannot occur. To ensure a smooth start-up, the electrode needs to undergo a simple alkaline pretreatment before the reaction, i.e., immersing the electrode in a strongly alkaline solution containing organic matter (reactants) for several seconds to provide the necessary strongly alkaline environment for the initial alkali-catalyzed organic oxidation reaction.

[0026] Preferably, the non-strongly alkaline solution is an aqueous solution with a pH < 8.5, containing 0.1-10M of an organic compound that requires a base-catalyzed organic oxidation reaction under a strongly alkaline environment. Preferably, the non-strongly alkaline solution is any one or more of natural seawater, river water, and tap water; the organic compound is any one of ethylene glycol, glycerol, urea, and hydrazine. Preferably, the electrolyte is natural seawater containing 2M ethylene glycol.

[0027] Preferably, the solution used for alkaline pretreatment is an alkaline aqueous solution with a pH > 11 containing 0.1-10M organic matter. Preferably, the alkaline aqueous solution can be a 0.1-1M KOH aqueous solution, alkaline seawater, etc.; the organic matter is the same organic matter as in the non-strongly alkaline solution, and can be any one of ethylene glycol, glycerol, urea, and hydrazine. Preferably, the pretreatment solution is alkaline seawater containing 2M ethylene glycol.

[0028] Preferably, the alkaline pretreatment involves immersing the sample in the above-mentioned alkaline pretreatment solution containing organic matter for 2-60 seconds; preferably, the immersion time can be 2 seconds, 5 seconds, 10 seconds, 20 seconds, 30 seconds, 40 seconds, 60 seconds, etc.

[0029] Alkaline seawater is prepared by adding 1 M KOH to natural seawater, allowing it to precipitate completely, and then filtering the resulting solution, which has a pH of 13.2.

[0030] Furthermore, in this invention, when the electrode is in a cathode state, the reaction occurring near the electrode is as follows:

[0031] 2H₂O + 2e - →H2↑+ 2OH -

[0032] When the electrode is in the anodic state, the reaction occurring on the electrode surface can be a base-catalyzed organic oxidation reaction that requires a highly efficient strongly alkaline environment, such as alcohol oxidation, hydrazine oxidation, and urea oxidation. For example, the organic oxidation reaction is an ethylene glycol oxidation reaction, and the reaction equation is:

[0033] (CH2OH)2+5OH − →CH2OHCOO -+4H₂O + 4e −

[0034] Preferably, the waveform of the alternating current is selected from square wave, sine wave, triangle wave or sawtooth wave; preferably square wave.

[0035] Preferably, the voltage of the alternating current is 1-380V; preferably, the voltage of the alternating current is 1V, 2V, 3V, 4V, 10V, 50V, 100V, 150V, 200V, 250V, 300V, 350V, 380V, etc.

[0036] Preferably, the period of the alternating current is 0.1-60s; for example, the period of the alternating current can be 0.1s, 0.2s, 0.5s, 0.8s, 1s, 2s, 5s, 10s, 20s, 30s, 40s, 50s, 60s, etc.

[0037] Preferably, the temperature of the electrolyte is 5-95℃; more preferably, the temperature of the electrolyte is 5℃, 10℃, 15℃, 20℃, 25℃, 30℃, 35℃, 40℃, 45℃, 50℃, 55℃, 60℃, 65℃, 70℃, 75℃, 80℃, 85℃, 90℃, 95℃, etc.

[0038] It should be noted that the present invention does not specifically limit the electrode material. Electrode materials commonly used by those skilled in the art can be used in this method. They can be either loaded electrodes or unloaded electrodes. At the same time, the present invention does not specifically limit the source of the electrode material. It can be a commercially available electrode or an electrode prepared by referring to the disclosed preparation method. Both are within the protection scope of the present invention. For example, the electrode is selected from one of the following: platinum electrode, platinum-rhodium alloy electrode, titanium felt coated platinum electrode, nickel foam electrode, and titanium electrode. Attached Figure Description

[0039] The above and other objects, features, and advantages of exemplary embodiments of the present invention will become readily apparent upon reading the following detailed description with reference to the accompanying drawings. In the drawings, several embodiments of the invention are illustrated by way of example and not limitation, and like or corresponding reference numerals denote like or corresponding parts, wherein:

[0040] Figure 1 This diagram illustrates the principle of the present invention, which involves periodically switching electrode polarity to create a localized alkaline environment in a non-strongly alkaline solution for alkaline-catalyzed organic oxidation reactions.

[0041] Figure 2 A schematic diagram of the square waveform AC input applied in Examples 1-70 is shown.

[0042] Figure 3The current density-time curve of electrolysis using square waveform AC in Example 1 is shown.

[0043] Figure 4 The curves showing the change of current density over time during two cycles in Example 1 are shown.

[0044] Figure 5 The gas chromatogram of the gaseous products obtained by electrolysis using square waveform AC in Example 1 is shown.

[0045] Figure 6 The high-performance liquid chromatography-mass spectra of the liquid products obtained by electrolysis with square waveform AC in Example 1 are shown.

[0046] Figure 7 The current density-time curves of electrolysis using square waveform AC in Examples 1-4 are shown.

[0047] Figure 8 The electrocatalytic oxidation performance of ethylene glycol in natural seawater and alkaline seawater is shown in Comparative Examples 1-2.

[0048] Figure 9 The current density-time curve of electrolysis using direct current is shown in Comparative Example 3.

[0049] Figure 10 The figure shows the current density-time curve of electrolysis using square waveform AC without alkaline pretreatment of the electrodes in Comparative Example 4.

[0050] Figure 11 The curves showing the change of current density over time during two cycles in Comparative Example 4 are shown.

[0051] Figure 12 A schematic diagram of the sinusoidal AC input applied in Example 71 is shown.

[0052] Figure 13 The application shown in Example 71 is applied to Figure 1 The curves showing the voltage of the sinusoidal alternating current on the two electrodes as a function of time (two periods T) are shown, and this data was recorded by an oscilloscope.

[0053] Figure 14 The current density-time curve of electrolysis using sinusoidal alternating current in Example 71 is shown.

[0054] Figure 15 The curves showing the change of current density over time during two cycles in Example 71 are shown.

[0055] Figure 16 A schematic diagram of the triangular waveform AC input applied in Example 72 is shown.

[0056] Figure 17The application shown in Example 72 is applied to Figure 1 The curves showing the voltage of the triangular wave alternating current on the two electrodes as a function of time (two periods T) are shown, and this data was recorded by an oscilloscope.

[0057] Figure 18 The current density-time curve of electrolysis using triangular waveform alternating current in Example 72 is shown.

[0058] Figure 19 The curves showing the change of current density over time during two cycles in Example 72 are shown.

[0059] Figure 20 A schematic diagram of the sawtooth waveform AC input applied in Example 73 is shown.

[0060] Figure 21 The application shown in Example 73 is applied to Figure 1 The curves showing the voltage change over time (two periods T) of the sawtooth alternating current on the two electrodes are shown, and the data was recorded by an oscilloscope.

[0061] Figure 22 The current density-time curve of the electrolysis using sawtooth waveform AC in Example 73 is shown.

[0062] Figure 23 The curves showing the change of current density over time during two cycles in Example 73 are shown. Detailed Implementation

[0063] The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some, not all, of the embodiments of the present invention. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0064] It should be understood that the terms "comprising" and "including" as used in the specification and claims of this invention indicate the presence of the described features, integrals, steps, operations, elements and / or components, but do not exclude the presence or addition of one or more other features, integrals, steps, operations, elements, components and / or collections thereof.

[0065] It should also be understood that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to limit the invention. As used in this specification and claims, the singular forms “a,” “an,” and “the” are intended to include the plural forms unless the context clearly indicates otherwise. It should also be understood that the term “and / or” as used in this specification and claims refers to any combination and all possible combinations of one or more of the associated listed items, and includes such combinations.

[0066] The specific embodiments of the present invention will now be described in detail with reference to the accompanying drawings.

[0067] While numerous embodiments of the invention have been shown and described herein, it will be apparent to those skilled in the art that such embodiments are provided by way of example only. Many modifications, alterations, and alternatives will occur to those skilled in the art without departing from the spirit and essence of the invention. It should be understood that various alternatives to the embodiments of the invention described herein may be employed in the practice of the invention. The appended claims are intended to define the scope of protection of the invention and therefore cover equivalents or alternatives within the scope of these claims.

[0068] In addition, unless otherwise specified, all raw materials used in this invention are commercially available, all methods are general methods, and all equipment is general-purpose equipment that is commercially available. Any range described in this invention includes endpoints, any values ​​between endpoints, and any sub-ranges formed by endpoints or any values ​​between endpoints.

[0069] This invention provides a method for achieving alkaline-catalyzed organic oxidation reaction in a non-strongly alkaline solution through local pH regulation, comprising the steps of: using a non-strongly alkaline solution containing organic matter as an electrolyte, applying alternating current to the electrodes, and periodically switching the polarity of the electrodes so that the polarity of the same electrode periodically alternates between the cathode state and the anode state.

[0070] Preferably, before applying alternating current to the electrodes, a pretreatment step is included: immersing the electrodes in a strongly alkaline solution containing organic matter.

[0071] Preferably, the electrode is immersed in a strongly alkaline solution containing organic matter for 2-60 seconds.

[0072] Preferably, the organic compound is selected from any one of ethylene glycol, glycerol, urea, and hydrazine.

[0073] Preferably, the electrode is selected from any one of platinum electrode, platinum-rhodium alloy electrode, titanium felt coated platinum electrode, nickel foam electrode, and titanium electrode.

[0074] Preferably, the waveform of the alternating current is selected from square wave, sine wave, triangle wave or sawtooth wave.

[0075] Preferably, the waveform of the alternating current is selected from a square wave.

[0076] Preferably, the voltage of the alternating current is 1-380V.

[0077] Preferably, the voltage of the alternating current is 1.2-1.8V.

[0078] Preferably, the period of the alternating current is 0.1-60s.

[0079] Preferably, the temperature of the electrolyte is 5-95℃.

[0080] Preferably, the non-alkaline solution is an aqueous solution with a pH < 8.5.

[0081] Preferably, the non-strongly alkaline solution is selected from any one or more of the following: natural seawater, river water, and tap water.

[0082] When natural seawater, river water, or tap water with a pH less than 8.5 is selected as a non-strongly alkaline solution, the method for achieving alkali-catalyzed organic oxidation reactions in a non-strongly alkaline solution through local pH regulation, as provided in this invention, can be realized. The method of using river water and tap water is the same as that for natural seawater.

[0083] Preferably, the alkali-catalyzed organic oxidation reaction is an organic oxidation reaction that depends on a strongly alkaline environment, including methanol oxidation and ethanol oxidation reactions in alcohol oxidation reactions; and formaldehyde oxidation and glucose oxidation reactions in aldehyde oxidation reactions.

[0084] Preferably, the alkali-catalyzed organic oxidation reaction is selected from any one of ethylene glycol oxidation, glycerol oxidation, urea oxidation, and hydrazine oxidation.

[0085] Preferably, the strongly alkaline solution used in the alkaline pretreatment step has a pH > 11 and contains 0.1-10 mol / L of dissolved organic matter. The organic matter dissolved in the strongly alkaline solution is consistent with the organic matter composition in the electrolyte.

[0086] Preferably, the strongly alkaline solution in the alkaline pretreatment step is alkaline seawater containing 2 mol / L ethylene glycol.

[0087] Preferably, the electrolyte is natural seawater containing 2 mol / L ethylene glycol.

[0088] Preferably, the electrolyte is a non-strongly alkaline solution containing 0.1-10 mol / L of organic matter.

[0089] To address the issue that certain organic oxidation reactions coupled with HER require a strongly alkaline environment for efficient execution, this invention aims to provide a method for the continuous and efficient execution of such organic oxidation reactions under non-strongly alkaline conditions. This method actively regulates the local pH environment on the electrode surface by periodically switching the electrode polarity, thereby stably supporting the continuous and efficient execution of alkaline-catalyzed organic oxidation reactions dependent on a strongly alkaline environment even when the bulk phase is non-alkaline.

[0090] This invention utilizes alternating current as a power source to periodically switch the polarity of electrodes, allowing the same electrode to alternate between cathode and anodic states. For the same electrode, the cathode state refers to its function as a cathode in the hydrogen evolution reaction (HER) at the given voltage, while the anodic state refers to its function as an anode in the oxidation of organic compounds at the same voltage. By adjusting the period, voltage, and waveform of the alternating current, precise control of the pH at the electrode surface can be achieved to meet the different alkaline conditions required for the oxidation of various organic compounds, thereby efficiently realizing electrocatalytic alkaline-catalyzed organic oxidation reactions.

[0091] This invention proposes an innovative technology that constructs a locally strongly alkaline environment in situ by periodically switching electrode polarity, enabling efficient alkaline-catalyzed organic oxidation reactions in non-alkaline solutions. This successfully overcomes the traditional technological limitation that such organic oxidation reactions require strongly alkaline solutions. The technology utilizes the periodic change of alternating current electrode polarity, causing the electrode polarity to periodically alternate between cathode and anodic states. By simply pretreating the electrode with an alkaline solution to initiate the reaction, the OH- produced by the hydrogen evolution reaction can be utilized. - By constructing a strongly alkaline environment in situ on the electrode surface for the alkaline-catalyzed organic oxidation reaction, the reaction can proceed continuously and efficiently. This strategy significantly reduces the cost of hydrogen electrolysis and organic byproduct production, and greatly improves operational safety, providing a more economical, safe, and efficient new approach for the electrocatalytic oxidation of organic compounds.

[0092] Example 1

[0093] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis was performed using a titanium felt-coated platinum electrode as the power source, with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃. Before electrolysis, the two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5s to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, continuous bubble generation was observed on both electrodes, and the current remained stable throughout the process. Figure 3The gas produced was collected by water displacement and analyzed by high-performance gas chromatography. The collected gas was found to be pure hydrogen. Figure 5 ).

[0094] The solutions collected before and after electrolysis were analyzed by high-performance liquid chromatography-mass spectrometry. Glycolic acid was generated after the reaction. Figure 6 ).

[0095] Example 2

[0096] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.0V and -1.0V, respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0097] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds, creating a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, continuous bubble generation was observed on both electrodes, and the current remained stable throughout the process. Figure 7 ).

[0098] Example 3

[0099] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.5V and -1.5V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0100] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds, creating a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, continuous bubble generation was observed on both electrodes, and the current remained stable throughout the process. Figure 7 ).

[0101] Example 4

[0102] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.8V and -1.8V, respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0103] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds, creating a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, continuous bubble generation was observed on both electrodes, and the current remained stable throughout the process. Figure 7 ).

[0104] Comparative Example 1

[0105] Natural seawater containing 2M ethylene glycol was used as the electrolyte. A titanium felt-coated platinum electrode was used as the working electrode, and a platinum sheet and a saturated calomel electrode were used as the counter and reference electrodes, respectively. The electrocatalytic performance of ethylene glycol oxidation was tested using a three-electrode electrochemical system. The tests were conducted at room temperature, and linear sweep voltammetry was used in the range of 0-1.8 V (relative to the reversible hydrogen electrode). The results are as follows: Figure 8 .

[0106] Comparative Example 2

[0107] 1 M KOH was added to natural seawater, and after complete precipitation, the resulting solution was filtered to obtain alkaline seawater with a pH of 13.2. Using alkaline seawater containing 2 M ethylene glycol as the electrolyte, a titanium felt coated platinum electrode as the working electrode, and platinum sheets and mercury / mercury oxide electrodes as the counter and reference electrodes, respectively, a three-electrode electrochemical system was employed to test the electrocatalytic performance of ethylene glycol oxidation. The tests were conducted at room temperature using linear sweep voltammetry in the range of 0–1.8 V (relative to the reversible hydrogen electrode). The results are as follows: Figure 8 .

[0108] Comparative Example 3

[0109] Natural seawater containing 2M ethylene glycol was used as the electrolyte, titanium felt coated with platinum electrodes were used as the two electrodes, and direct current was used as the power source for electrolysis. The constant voltage was 1.2V and the electrolyte temperature was 5℃.

[0110] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. After electrolysis began, bubbles were observed to form on the cathode. After 2 minutes of electrolysis, the current density increased from 31 mA / cm². 2 Decrease to the minimum ( Figure 9 Meanwhile, a white precipitate forms on the electrode surface. This is because the OH- ions on the electrode surface are depleted, making it unable to provide the alkaline environment required for ethylene glycol oxidation.

[0111] Comparative Example 4

[0112] Natural seawater containing 2M ethylene glycol was used as the electrolyte, titanium felt coated with platinum electrodes were used as the two electrodes, and direct current was used as the power source for electrolysis. The constant voltage was 1.2V and the electrolyte temperature was 5℃.

[0113] No pretreatment is performed on the electrodes before electrolysis. After electrolysis begins, the current is mainly contributed by the charging and discharging of the electric double layer, and the stable current density is relatively small. Figure 10 If no bubbles are observed to form, it means that the reaction has not occurred.

[0114] The present invention Figure 1 A schematic diagram illustrating the principle of electrolytic catalytic oxidation of organic matter based on the in-situ construction of a locally strongly alkaline environment using alternating current.

[0115] like Figure 1 As shown, a non-alkaline solution containing organic matter is used as the electrolyte. Alternating current is applied to the electrodes, and by controlling the waveform, voltage, and period of the current, the electrodes periodically alternate between cathode and anodic states. When the electrode is in the cathode state, a hydrogen evolution reaction occurs, generating hydrogen gas (H2) and hydroxide ions (OH-), thereby regulating the local pH of the electrode surface. When the electrode is in the anodic state, the electrode surface becomes locally alkaline due to the accumulation of OH- ions generated by the hydrogen evolution reaction, ensuring the continuous and efficient execution of the alkaline-catalyzed organic oxidation reaction. Figure 1 In the first half-cycle of the alternating current, the white arrow near the left electrode indicates that the electrode is in the anodic state, undergoing a base-catalyzed organic oxidation reaction, with OH- on the electrode surface providing a strongly alkaline environment for the reaction. Simultaneously, the right electrode is in the cathodic state, undergoing a hydrogen evolution reaction to generate OH-, thus maintaining a strongly alkaline environment in situ for the base-catalyzed organic oxidation reaction in the second half-cycle. In the second half-cycle of the alternating current, the black arrow near the left electrode indicates that the electrode is in the cathodic state, undergoing a hydrogen evolution reaction to generate OH-, thus maintaining a strongly alkaline environment in situ for the base-catalyzed organic oxidation reaction in the next cycle. Simultaneously, the right electrode is in the anodic state, undergoing a base-catalyzed organic oxidation reaction (as indicated by the black arrow near the right electrode).

[0116] Figure 2 A schematic diagram of the applied square-wave AC input is shown.

[0117] Figure 3 The current density-time curve of electrolysis using square-wave AC current in Example 1 is shown. Figure 3 The current density-time curve shown has current density on the vertical axis and time on the horizontal axis.

[0118] Figure 4 The curves showing the change of current density over time during two cycles in Example 1 are shown.

[0119] Figure 5 The gas chromatogram of the gaseous product obtained by electrolysis using a square-wave AC current in Example 1 is shown. Figure 5 As shown, the collected gas is pure hydrogen.

[0120] Figure 6 The high-performance liquid chromatography-mass spectra of the liquid product obtained by electrolysis using square waveform AC in Example 1 are shown. Figure 6 The left image in figure a shows the ion flow time spectrum of the 2M ethylene glycol standard sample at a mass-to-charge ratio of 75.0069-75.0089; the right image shows the mass spectrum of the 2M ethylene glycol standard sample at a retention time of 1.23-1.28 min. Figure 6 The left image in b is the ion current-time spectrum of natural seawater containing 2M ethylene glycol before electrolysis at a mass-to-charge ratio of 75.0069-75.0089; the right image is the mass spectrum of natural seawater containing 2M ethylene glycol before electrolysis at a retention time of 1.23-1.28 min. Figure 6 The left image in panel c shows the ion current-time spectrum of electrolyzed natural seawater containing 2M ethylene glycol at a mass-to-charge ratio of 75.0069–75.0089; the right image shows the mass spectrum of electrolyzed natural seawater containing 2M ethylene glycol at a retention time of 1.23–1.28 min. Figure 6 As shown, the generated high-value liquid product is glycolic acid.

[0121] Figure 7 The current density-time curves of electrolysis using square waveform AC in Examples 1-4 are shown.

[0122] Figure 8 The electrocatalytic oxidation performance of ethylene glycol in Comparative Examples 1-2 in natural seawater and alkaline seawater is shown. Ethylene glycol oxidation performs better in alkaline seawater and is extremely weak in natural seawater, indicating that electrocatalytic ethylene glycol oxidation requires a strongly alkaline environment.

[0123] Figure 9 The current density-time curve of electrolysis using direct current in Comparative Example 3 is shown. After 2 minutes of electrolysis, the current density was observed to increase from 31 mA / cm². 2 The concentration drops to a very low level, and a white precipitate forms on the electrode surface. This is because the OH- ions on the electrode surface are depleted, and the strongly alkaline environment required for the oxidation of ethylene glycol can no longer be provided, thus preventing the reaction from proceeding.

[0124] Figure 10 The diagram shows the current density-time curves for electrolysis using square-wave AC current in Comparative Example 4, where no alkaline pretreatment of the electrodes was performed. The current is mainly contributed by the charging and discharging of the electric double layer, resulting in a relatively low stable current density. No bubble formation was observed during the reaction, indicating that the reaction did not occur.

[0125] Figure 11 The curves showing the change of current density over time during two cycles in Comparative Example 4 are shown.

[0126] Example 5

[0127] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2.0V and -2.0V, respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0128] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0129] Example 6

[0130] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 3V and -3V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0131] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0132] Example 7

[0133] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 4V and -4V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0134] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0135] Example 8

[0136] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 5.0V and -5.0V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0137] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0138] Example 9

[0139] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 10V and -10V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0140] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0141] Example 10

[0142] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 50V and -50V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0143] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0144] Example 11

[0145] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 100V and -100V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0146] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0147] Example 12

[0148] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 150V and -150V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0149] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0150] Example 13

[0151] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 200V and -200V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0152] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0153] Example 14

[0154] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 250V and -250V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0155] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0156] Example 15

[0157] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 300V and -300V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0158] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0159] Example 16

[0160] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 350V and -350V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0161] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0162] Example 17

[0163] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A square waveform alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 380V and -380V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0164] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0165] Example 18

[0166] See Figure 1Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0167] Before electrolysis, two platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0168] Example 19

[0169] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and platinum-rhodium alloy electrodes were used as the two electrodes. A square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0170] Before electrolysis, two platinum-rhodium alloy electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0171] Example 20

[0172] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and nickel foam electrodes were used as the two electrodes. A square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.5V and -1.5V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0173] Before electrolysis, two nickel foam electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0174] Example 21

[0175] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, titanium electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.8V and -1.8V, respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0176] Before electrolysis, the two titanium electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0177] Example 22

[0178] See Figure 1 Natural seawater containing 1M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0179] Before electrolysis, two platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0180] Example 23

[0181] See Figure 1 Natural seawater containing 0.1M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0182] Before electrolysis, two platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0183] Example 24

[0184] See Figure 1 Tap water containing 5M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 8V and -8V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0185] Before electrolysis, two platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0186] Example 25

[0187] See Figure 1 Natural seawater containing 10M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0188] Before electrolysis, two platinum electrodes were immersed in alkaline seawater containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0189] Example 26

[0190] See Figure 1 River water containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0191] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0192] Example 27

[0193] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0194] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 0.1M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0195] Example 28

[0196] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0197] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 1M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0198] Example 29

[0199] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0200] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 5M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0201] Example 30

[0202] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0203] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 10M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0204] Example 31

[0205] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0206] Before electrolysis, two platinum electrodes were immersed in a 0.1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0207] Example 32

[0208] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0209] Before electrolysis, two platinum electrodes were immersed in a 0.5M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0210] Example 33

[0211] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0212] Before electrolysis, the two platinum electrodes were immersed in a 0.1M KOH solution containing 2M ethylene glycol for 2 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0213] Example 34

[0214] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0215] Before electrolysis, two platinum electrodes were immersed in a 0.1M KOH solution containing 2M ethylene glycol for 10 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0216] Example 35

[0217] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0218] Before electrolysis, two platinum electrodes were immersed in a 0.1M KOH solution containing 2M ethylene glycol for 20 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0219] Example 36

[0220] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0221] Before electrolysis, two platinum electrodes were immersed in a 0.1M KOH solution containing 2M ethylene glycol for 30 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0222] Example 37

[0223] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0224] Before electrolysis, two platinum electrodes were immersed in a 0.1M KOH solution containing 2M ethylene glycol for 40 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0225] Example 38

[0226] See Figure 1 Natural seawater containing 2M glycerol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0227] Before electrolysis, two platinum electrodes were immersed in a 0.1M KOH solution containing 2M glycerol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0228] Example 39

[0229] See Figure 1 Natural seawater containing 2M urea was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0230] Before electrolysis, two platinum electrodes were immersed in a 0.1M KOH solution containing 2M urea for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0231] Example 40

[0232] See Figure 1 Natural seawater containing 2M hydrazine was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 1s, and an electrolyte temperature of 25℃.

[0233] Before electrolysis, the two platinum electrodes were immersed in a 0.1M KOH solution containing 2M hydrazine for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0234] Example 41

[0235] See Figure 1Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 0.1s, and an electrolyte temperature of 25℃.

[0236] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0237] Example 42

[0238] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V, respectively, a period T of 0.2s, and an electrolyte temperature of 25℃.

[0239] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0240] Example 43

[0241] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 0.5s, and an electrolyte temperature of 25℃.

[0242] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0243] Example 44

[0244] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 0.8s, and an electrolyte temperature of 25℃.

[0245] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0246] Example 45

[0247] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period T of 2s, and an electrolyte temperature of 25℃.

[0248] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0249] Example 46

[0250] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V respectively, a period of 5s, and an electrolyte temperature of 25℃.

[0251] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0252] Example 47

[0253] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V, respectively, a period T of 10s, and an electrolyte temperature of 25℃.

[0254] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0255] Example 48

[0256] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V, respectively, a period T of 20s, and an electrolyte temperature of 25℃.

[0257] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0258] Example 49

[0259] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V, respectively, a period T of 30s, and an electrolyte temperature of 25℃.

[0260] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0261] Example 50

[0262] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V, respectively, a period of 40s, and an electrolyte temperature of 25℃.

[0263] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0264] Example 51

[0265] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V, respectively, a period of 50s, and an electrolyte temperature of 25℃.

[0266] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0267] Example 52

[0268] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 1.2V and -1.2V, respectively, a period of 60s, and an electrolyte temperature of 25℃.

[0269] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 60 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0270] Example 53

[0271] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 5℃.

[0272] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0273] Example 54

[0274] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 10℃.

[0275] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0276] Example 55

[0277] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 15℃.

[0278] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0279] Example 56

[0280] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 20℃.

[0281] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0282] Example 57

[0283] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 30℃.

[0284] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0285] Example 58

[0286] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 35℃.

[0287] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0288] Example 59

[0289] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 40℃.

[0290] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0291] Example 60

[0292] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 45℃.

[0293] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0294] Example 61

[0295] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 50℃.

[0296] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0297] Example 62

[0298] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 55℃.

[0299] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0300] Example 63

[0301] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 60℃.

[0302] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0303] Example 64

[0304] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 65℃.

[0305] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0306] Example 65

[0307] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 70℃.

[0308] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0309] Example 66

[0310] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 75℃.

[0311] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0312] Example 67

[0313] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 80℃.

[0314] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0315] Example 68

[0316] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 85℃.

[0317] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0318] Example 69

[0319] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 90℃.

[0320] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0321] Example 70

[0322] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, platinum electrodes were used as the two electrodes, and a square-wave alternating current was applied. Figure 2 Electrolysis is performed using a power source with voltages Ea (anode voltage) and Ec (cathode voltage) of 2V and -2V respectively, a period T of 1s, and an electrolyte temperature of 95℃.

[0323] Before electrolysis, two platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds to create a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, bubbles were continuously generated on both electrodes, and the current remained stable throughout the process.

[0324] Example 71

[0325] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A sinusoidal alternating current was applied. Figure 12 Electrolysis is performed using it as a power source. Figure 12 The voltage Ea is 1.696V (effective voltage 1.2V), the period T is 1s, and the electrolyte temperature is 5℃.

[0326] Figure 13 Showing the application at Figure 1 The curves showing the voltage of the sinusoidal alternating current on the two electrodes as a function of time (two periods T) are shown, and this data was recorded by an oscilloscope.

[0327] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds, creating a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, continuous bubble generation was observed on both electrodes, and the current remained stable throughout the process. Figure 14 ).

[0328] Figure 15 The curves showing the change of current density over time during two cycles of electrolysis with sinusoidal alternating current are shown.

[0329] Example 72

[0330] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A triangular waveform alternating current was applied. Figure 16 Electrolysis is performed using it as a power source. Figure 16 The voltage Ea is 2.078V (effective voltage 1.2V), the period T is 1s, and the electrolyte temperature is 5℃.

[0331] Figure 17 Showing the application at Figure 1 The curves showing the voltage of the triangular wave alternating current on the two electrodes as a function of time (two periods T) are shown, and this data was recorded by an oscilloscope.

[0332] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds, creating a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, continuous bubble generation was observed on both electrodes, and the current remained stable throughout the process. Figure 18 ).

[0333] Figure 19 The curves showing the change of current density over time during two cycles of electrolysis with triangular waveform alternating current are shown.

[0334] Example 73

[0335] See Figure 1 Natural seawater containing 2M ethylene glycol was used as the electrolyte, and titanium felt coated with platinum electrodes were used as the two electrodes. A sawtooth waveform alternating current was applied. Figure 20 Electrolysis is performed using it as a power source. Figure 20 The voltage Ea is 2.078V (effective voltage 1.2V), the period T is 1s, and the electrolyte temperature is 5℃.

[0336] Figure 21 Showing the application at Figure 1 The curves showing the voltage change over time (two periods T) of the sawtooth alternating current on the two electrodes are shown, and the data was recorded by an oscilloscope.

[0337] Before electrolysis, two titanium felt-coated platinum electrodes were immersed in a 1M KOH solution containing 2M ethylene glycol for 5 seconds, creating a locally strong alkaline environment on the electrode surface to initiate the reaction. During electrolysis, continuous bubble generation was observed on both electrodes, and the current remained stable throughout the process. Figure 22 ).

[0338] Figure 22 When the electrode polarity is anode, the difference between the output frequency of the function signal generator and the acquisition frequency of the electrochemical workstation causes the maximum value of the double layer to exhibit periodic changes during charging and discharging. The electrolytic current remains stable during this process.

[0339] Figure 23 The curves showing the current density versus time during two cycles of electrolysis with sawtooth waveform AC are shown.

[0340] Experiments showed that the electrolysis time for Examples 1-73 could all be sustained for more than 63 hours.

[0341] Obviously, the above embodiments of the present invention are merely examples for clearly illustrating the present invention, and are not intended to limit the implementation of the present invention. For those skilled in the art, other variations or modifications can be made based on the above description. It is impossible to exhaustively list all the implementation methods here. All obvious variations or modifications derived from the technical solutions of the present invention are still within the protection scope of the present invention.

Claims

1. A method for achieving base-catalyzed organic oxidation reactions in a non-strongly alkaline solution through local pH regulation, characterized in that, The steps include: using a non-strongly alkaline solution containing organic matter as the electrolyte, applying alternating current to the electrodes, and periodically switching the polarity of the electrodes so that the polarity of the same electrode alternates periodically between the cathode state and the anode state.

2. The method according to claim 1, characterized in that, Before applying the alternating current to the electrode, an alkaline pretreatment step is included: immersing the electrode in a strongly alkaline solution containing the organic matter.

3. The method according to claim 2, characterized in that, The electrode is immersed in the strongly alkaline solution containing the organic matter for 2-60 seconds.

4. The method according to claim 1, characterized in that, The electrode is selected from any one of the following: platinum electrode, platinum-rhodium alloy electrode, titanium felt coated platinum electrode, nickel foam electrode, and titanium electrode.

5. The method according to claim 1, characterized in that, The waveform of the alternating current is selected from square wave, sine wave, triangle wave or sawtooth wave.

6. The method according to claim 1, characterized in that, The waveform of the alternating current is selected from square waves.

7. The method according to claim 1, characterized in that, The voltage of the alternating current is 1-380V.

8. The method according to claim 7, characterized in that, The voltage of the alternating current is 1.2-1.8V.

9. The method according to claim 1, characterized in that, The period of the alternating current is 0.1-60s.

10. The method according to claim 1, characterized in that, The temperature of the electrolyte is 5-95℃.

11. The method according to claim 1, characterized in that, The non-alkaline solution has a pH < 8.

5.

12. The method according to claim 1, characterized in that, The non-alkaline solution is selected from any one or more of the following: natural seawater, river water, and tap water.

13. The method according to claim 1, characterized in that, The alkali-catalyzed organic oxidation reaction is an organic oxidation reaction that depends on a strongly alkaline environment.

14. The method according to claim 13, characterized in that, The alkali-catalyzed organic oxidation reaction is selected from any one of the following: ethylene glycol oxidation reaction, glycerol oxidation reaction, urea oxidation reaction, and hydrazine oxidation reaction.

15. The method according to claim 2, characterized in that, The strongly alkaline solution used in the alkaline pretreatment step has a pH > 11, and the strongly alkaline solution contains 0.1-10 mol / L of the organic matter.

16. The method according to claim 14, characterized in that, The strongly alkaline solution in the alkaline pretreatment step is alkaline seawater containing 2 mol / L ethylene glycol.

17. The method according to claim 1, characterized in that, The electrolyte is natural seawater containing 2 mol / L ethylene glycol.

18. The method according to any one of claims 1-17, characterized in that, The electrolyte is a non-strongly alkaline solution containing 0.1-10 mol / L of the organic matter.

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