Self-powered electrocatalytic alcoholysis capsule, preparation method and application thereof

Abstract

A self-powered electrocatalytic alcohol solution capsule and a preparation method and application thereof, the alcohol solution capsule comprising a shell, an encapsulation layer arranged in the shell, and an electrochemical unit coated with the encapsulation layer, the electrochemical unit comprising a catalytic electrode, a counter electrode, and an electrolyte layer between the catalytic electrode and the counter electrode, the catalytic electrode comprising a gold foil and a manganese-tannic acid mesocrystal, wherein the manganese-tannic acid mesocrystal is a mesoscopic crystal structure formed by self-assembly of a metal-polyphenol network of a tannic acid and a manganese salt under weak acid conditions on the gold foil. The alcohol solution capsule of the present application adopts a self-generating primary cell structure assembled by edible catalytic electrodes, counter electrodes, electrolyte layers, encapsulation layers, and shells, can efficiently oxidize ethanol in situ in the intestinal tract through electrochemistry, and convert the ethanol into acetic acid, so as to achieve active removal before the ethanol is absorbed into the blood in a large amount, and achieve the purposes of reducing the blood alcohol concentration, reducing alcohol-related organ damage, and improving neurobehavioral impairment.

Description

Technical Field

[0001] This invention relates to the field of functional materials, specifically to a self-powered electrocatalytic hangover detoxification capsule, its preparation method, and its application. Background Technology

[0002] Alcohol poisoning and its resulting multi-organ damage are significant issues in clinical and public health fields. The human body primarily metabolizes ethanol through the alcohol dehydrogenase and aldehyde dehydrogenase systems in the liver. However, this endogenous metabolic process is limited by zero-order kinetics; that is, when alcohol consumption is excessive, the metabolic enzymes quickly reach saturation, and the body cannot synchronously increase its metabolic rate with increasing ethanol intake. Therefore, in cases of acute alcohol exposure, the rate of ethanol absorption often exceeds the rate of elimination by the body, leading to a rapid increase in blood ethanol concentration and further inducing a series of toxic reactions such as liver damage, intestinal barrier disruption, and neurobehavioral abnormalities.

[0003] To overcome the dual bottlenecks of "liver enzyme saturation kinetics" and "rapid gastrointestinal absorption of ethanol" in the clinical management of acute alcohol poisoning, current technologies rely on drug intervention or nutritional supplementation strategies. These strategies use drugs, antidotes, or nutritional supplements to enhance or assist the body's metabolic function. However, these strategies cannot bypass the rate limits of liver metabolic enzymes, making it difficult to achieve rapid and active ethanol clearance in high-dose acute exposure scenarios. Enzyme preparations or enzyme-mimicking detoxification systems can promote alcohol metabolism using exogenous enzymes or biomimetic enzyme nanocomposites. However, these strategies generally suffer from limited enzyme stability, easy inactivation in the gastrointestinal environment, dependence on biological environmental conditions, complex preparation, and high storage requirements. Furthermore, they still belong to "biocatalysis enhancement" systems and have not broken through the host-dependent metabolic framework. In addition, some ingestible electronic devices exist, but they are mainly used for gastrointestinal signal monitoring, environmental sensing, or electrical stimulation regulation and cannot directly act on target metabolites in the gastrointestinal tract. Therefore, they also lack the ability to rapidly and actively clear high-dose ethanol. Summary of the Invention

[0004] One objective of this invention is to provide a self-powered electrocatalytic hangover relief capsule, which employs an edible catalytic electrode, a counter electrode, an electrolyte layer, an encapsulation layer, and a shell to form a self-generating galvanic cell structure. This structure can efficiently perform in-situ electrochemical oxidation of ethanol in the intestines, converting it into acetic acid. This allows for the active clearance of ethanol before it is absorbed into the bloodstream in large quantities, thereby reducing blood alcohol concentration, alleviating alcohol-related organ damage, and improving neurobehavioral impairment.

[0005] This invention is achieved through the following technical solution:

[0006] A self-powered electrocatalytic hangover relief capsule includes a shell with an encapsulation layer inside. The encapsulation layer covers an electrochemical unit, which includes a catalytic electrode, a counter electrode, and an electrolyte layer located between the catalytic electrode and the counter electrode. The catalytic electrode includes a gold foil and a manganese-ellagic acid mesocrystalline structure, wherein the manganese-ellagic acid mesocrystalline structure is a mesoscopic crystal structure formed by ellagic acid and manganese salt forming a metal-polyphenol network under weakly acidic conditions and self-assembling on the gold foil.

[0007] In this technical solution, the hangover relief capsule includes a shell, an encapsulation layer, a catalytic electrode, a counter electrode, and an electrolyte layer. The shell protects the internal encapsulation layer and electrochemical unit, ensuring release at an ideal location, such as through the stomach and then into the intestines, for electrochemical oxidation. This targeted release avoids release in the stomach, effectively improving the reaction effect. In one or more preferred embodiments, the shell can be an existing enteric-coated capsule shell, made of materials such as cellulose acetate phthalate or polyacrylic acid resin. In some preferred embodiments, the enteric-coated capsule shell is configured to release the electrochemical unit before or at the beginning of the intestinal absorption window, thereby reducing the ethanol load entering the circulatory system and alleviating subsequent liver damage, intestinal inflammation, and neurobehavioral abnormalities.

[0008] In this technical solution, the encapsulation layer is used to encapsulate the electrochemical unit to improve its structural stability and biocompatibility, and, together with the outer shell, enhance the intestinal retention capacity of the hangover relief capsule. In some preferred embodiments, the encapsulation layer is a sodium alginate-chitosan composite hydrogel prepared by mixing sodium alginate solution and chitosan solution, and then adding calcium ion crosslinking liquid.

[0009] In this technical solution, the catalytic electrode, counter electrode, and electrolyte layer together constitute the electrochemical unit. The catalytic electrode uses edible gold foil as the conductive substrate, and the amorphous metal polyphenol network formed by manganese salt and ellagic acid self-assembles on the gold foil into a hierarchically ordered mesoscopic crystal structure, namely manganese-ellagic acid mesocrystalline. The manganese-ellagic acid mesocrystalline has abundant redox active sites and continuous electron transport channels, serving as the core functional interface for the electrochemical oxidation reaction of ethanol. The counter electrode can be selected according to actual needs; for example, in some preferred embodiments, edible zinc foil is used as the counter electrode. The counter electrode and the catalytic electrode constitute the two electrodes of the galvanic cell, providing electron flow and potential difference during operation. The electrolyte layer is located between the counter electrode and the catalytic electrode, providing not only an ion conduction pathway but also improving the device's flexibility. In some preferred embodiments, the electrolyte layer is prepared by mixing a gelatin solution and a zinc acetate solution and then cooling to obtain a zinc acetate / gelatin electrolyte layer.

[0010] After entering the digestive system, the hangover relief capsule, protected by the enteric-coated capsule shell, releases its encapsulation layer and electrochemical unit into the intestines. The work function difference between the manganese-ellagic acid mesocrystalline material in the catalytic electrode and the gold foil substrate creates a built-in electric field upon contact, promoting interfacial charge separation and directional electron transfer, thus enhancing the efficiency of the electrochemical oxidation reaction of ethanol. The self-powered galvanic cell system composed of the counter electrode and the catalytic electrode continuously drives the conversion of ethanol to acetic acid in the intestines without external power, thereby actively clearing ethanol before it is absorbed into the bloodstream in large quantities. Furthermore, all components of this hangover relief capsule are made of edible materials or have biomedical compatibility. It is not merely an energy-supplying device or a simple drug / enzyme delivery system, but a metabolic bioelectronic device that combines edibility, self-powering capabilities, in-situ metabolic intervention, and organ protection effects, possessing broad application value.

[0011] Furthermore, the molar ratio of ellagic acid to manganese salt is 1:4 to 4:1. The amount of ellagic acid and manganese salt affects the stability of the metal polyphenol network, thereby affecting the performance of the manganese-ellagic acid mesocrystalline structure and even the catalytic electrode. Excessive metal ions may also pose biosafety risks. Experiments have shown that the preferred molar ratio of ellagic acid to manganese salt is 1:4 to 4:1. In a more preferred embodiment, the amount of manganese salt is greater than the amount of ellagic acid; for example, the molar ratio of ellagic acid to manganese salt is 1:2 to 1:4.

[0012] In a preferred embodiment of the present invention, the manganese salt is manganese acetate.

[0013] Experiments revealed that while most manganese salts can form metal polyphenol networks with ellagic acid, only manganese acetate can form spherical manganese-ellagic acid mesocrystalline crystals on gold foil. These spherical crystals have a larger surface area, significantly improving the reactivity of the hangover relief capsules. Therefore, in a more preferred embodiment, manganese-ellagic acid is prepared based on manganese acetate and ellagic acid.

[0014] Furthermore, the thickness ratio of the encapsulation layer to the electrolyte layer is 2~5:1.

[0015] In this technical solution, setting the thickness of the encapsulation layer to be greater than that of the electrolyte layer enables the hangover relief capsule to possess better mechanical stability, biocompatibility, and structural integrity in the gastrointestinal environment. Simultaneously, a thinner electrolyte layer helps ensure ion transport efficiency and reduces the overall size of the hangover relief capsule. In a more preferred embodiment, the thickness of the encapsulation layer is 0.04~0.10 mm, and the thickness of the electrolyte layer is 0.015~0.03 mm. In actual preparation, the specific amounts of the electrolyte layer and encapsulation layer can be adjusted proportionally according to the cutting dimensions of the catalytic electrode and counter electrode, but it is preferable to meet this thickness ratio to further achieve a balance between energy supply performance, encapsulation stability, and intestinal safety of the hangover relief capsule.

[0016] Another objective of this invention is to provide a method for preparing a self-powered electrocatalytic hangover relief capsule, specifically comprising the following steps:

[0017] Ellagic acid, manganese salt, and solvent are mixed to obtain a first solution. Gold foil is immersed in the first solution and the first solution is adjusted to acidity. The reaction system is sealed and allowed to stand for aging to obtain a catalytic electrode. The catalytic electrode includes gold foil and manganese-ellagic acid mesocrystalline material self-assembled on the gold foil.

[0018] A zinc acetate / gelatin electrolyte layer was prepared by mixing a gelatin solution and a zinc acetate solution.

[0019] A second solution was obtained by mixing sodium alginate solution and chitosan solution. Calcium ion crosslinking liquid was slowly added to the second solution to prepare sodium alginate-chitosan composite hydrogel.

[0020] An electrochemical unit is obtained by stacking a catalytic electrode, which serves as the cathode, and a counter electrode, which is loaded with a zinc acetate / gelatin electrolyte layer, as the anode. The electrochemical unit is then coated with a sodium alginate-chitosan composite hydrogel, and the coated electrochemical unit is then encased in a shell to obtain a self-powered electrocatalytic hangover relief capsule.

[0021] In one or more embodiments, the gold foil is cleaned and then immersed in an aqueous solution of ellagic acid and manganese salt, with acid added to adjust the pH to 4. In some embodiments, the reaction system is aged at 60 °C for 2 days to allow manganese-ellagic acid mesocrystals to grow in situ on the surface of the gold foil.

[0022] Another object of the present invention is to provide the application of any of the aforementioned self-powered electrocatalytic hangover relief capsules, wherein the self-powered electrocatalytic hangover relief capsules are used to prepare drugs for promoting the electrochemical oxidation reaction of ethanol in the intestine, and / or to prepare drugs for improving hippocampal tissue morphological damage caused by ethanol.

[0023] Experiments have shown that the hangover relief capsules not only reduce the ethanol content in the intestines, thus lowering the level of alcohol accumulation in the body, but also, through analysis of hippocampal tissue, can improve intestinal flora imbalance and hippocampal damage caused by acute alcohol exposure, thereby protecting the gut-brain axis homeostasis. Therefore, this hangover relief capsule can be used as a main ingredient, combined with or without other medicinal components, to prepare related drugs, possessing broad application value.

[0024] Compared with the prior art, the present invention has the following advantages and beneficial effects:

[0025] 1. The hangover relief capsule of the present invention adopts a self-generating primary battery structure assembled from an edible catalytic electrode, a counter electrode, an electrolyte layer, an encapsulation layer, and a shell. It can efficiently perform in-situ electrochemical oxidation of ethanol in the intestine, converting it into acetic acid, thereby actively clearing ethanol before it is absorbed into the blood in large quantities, achieving the purpose of reducing blood alcohol concentration, alleviating alcohol-related organ damage, and improving neurobehavioral damage.

[0026] 2. This invention improves the stability of the metal polyphenol network and balances the biocompatibility and reactivity of the hangover relief capsule by designing the ratio of ellagic acid to manganese salt.

[0027] 3. By screening manganese salts, this invention identified manganese-ellagic acid mesocrystalline structures composed of manganese acetate and ellagic acid. The spherical structure of these structures significantly increases the surface area of ​​the manganese-ellagic acid mesocrystalline structures, thereby significantly improving the performance of the hangover relief capsules.

[0028] 4. By designing the thickness of the encapsulation layer and electrolyte layer, this invention can further balance the energy supply performance, encapsulation stability, and intestinal safety of the hangover relief capsule;

[0029] 5. The hangover relief capsule of the present invention can also improve intestinal flora disorder and hippocampal damage caused by acute alcohol exposure, thereby playing a protective role in the brain-gut axis homeostasis. Attached Figure Description

[0030] The accompanying drawings, which are included to provide a further understanding of embodiments of the invention and form part of this application, do not constitute a limitation thereof. In the drawings:

[0031] Figure 1 This is a flowchart illustrating the preparation method of the self-powered electrocatalytic hangover relief capsule in a specific embodiment of the present invention;

[0032] Figure 2 The cross-sectional morphology (a) and elemental distribution (b) of the Mn-EA / Au catalytic electrode prepared in a specific embodiment of the present invention are shown, as well as the morphology (c) and (d) of the spherical Mn-EA mesocrystals.

[0033] Figure 3 This is a schematic diagram of the assembly process of the self-powered electrocatalytic hangover detoxification capsule in a specific embodiment of the present invention;

[0034] Figure 4 This is a schematic diagram of the structure of the self-powered electrocatalytic hangover detoxification capsule in a specific embodiment of the present invention (enteric-coated capsule not shown).

[0035] Figure 5 The structure and mechanism of action of the electrochemical unit of the self-powered electrocatalytic hangover detoxification capsule in a specific embodiment of the present invention are shown;

[0036] Figure 6 The morphology of the plate-like Mn-EA mesocrystalline material prepared in a specific embodiment of the present invention is shown;

[0037] Figure 7 The cyclic reaction activity of the catalytic electrode in a specific embodiment of the present invention is shown (a), and the characteristic peaks of acetic acid and ethanol in the system at different cycles are shown (b).

[0038] Figure 8 The changes in ethanol content (a) and the ethanol consumption rate (b) after the hangover relief capsules were treated with different concentrations of ethanol in a specific embodiment of the present invention are shown.

[0039] Figure 9 The heat generation safety of the hangover relief capsule during the reaction process is shown in a specific embodiment of the present invention;

[0040] Figure 10 The dimensions of the hangover relief capsule used in in vivo testing are shown in a specific embodiment of the present invention;

[0041] Figure 11 This illustrates the retention capacity of the hangover relief capsule in a rat model according to a specific embodiment of the present invention;

[0042] Figure 12 The effect of the hangover relief capsule on lowering blood cholesterol in vivo is shown in a specific embodiment of the present invention;

[0043] Figure 13 The following is an illustration of the treatment process (a) of the acute alcohol poisoning model in a specific embodiment of the present invention, the alcohol tolerance time (b), the recovery time (c), the movement path (d), and the movement distance (e) of the rats;

[0044] Figure 14 The effects of each experimental group on Observed ASVs (a), Simpson index (b), microbial community composition (c), and key indicators of hippocampal tissue (d) are shown in specific embodiments of the present invention. Detailed Implementation

[0045] To make the objectives, technical solutions, and advantages of this invention clearer, the invention will be further described in detail below with reference to the embodiments and accompanying drawings. The illustrative embodiments and descriptions of this invention are only for explaining this invention and are not intended to limit this invention.

[0046] All raw materials used in this invention are not particularly limited in their source; they can be purchased commercially or prepared using conventional methods well-known to those skilled in the art. The purity of all raw materials used in this invention is not particularly limited; however, analytical grade materials are preferred. All raw materials used in this invention have common designations and abbreviations in the art, and each designation and abbreviation is clearly defined within its relevant application. Those skilled in the art can obtain these materials from commercial sources or prepare them using conventional methods based on the designation, abbreviation, and corresponding application.

[0047] The present invention does not impose any particular restrictions on the expression of the substituents, and all expressions are well known to those skilled in the art. Based on common sense, those skilled in the art can correctly understand their meaning according to their expression.

[0048] The terms "first," "second," etc., used in this document (e.g., first solvent, second solution, etc.) are merely for clarity of description and are not intended to restrict any order or emphasize importance. Furthermore, the term "connection" used herein, unless otherwise specified, can refer to a direct connection or an indirect connection via other components.

[0049] I. Preparation of Self-Powered Electrocatalytic Hangover Relief Capsules

[0050]

Example 1

[0051] (A) Edible gold foil was washed sequentially with ethanol and water, then immersed in an aqueous solution consisting of 0.26 mmol of ellagic acid and 0.52 mmol of manganese acetate tetrahydrate, with the pH adjusted to 4 using acetic acid. After sealing, it was aged at 60 °C for 2 days to allow manganese-ellagic acid (Mn-EA) mesocrystalline structures to grow in situ on the gold foil surface. After the reaction was complete, the gold foil was rinsed with water and ethanol and vacuum dried at 40 °C to obtain the Mn-EA / Au catalytic electrode.

[0052] Figure 2 The morphology and elemental distribution of the Mn-EA / Au catalytic electrode and its spherical Mn-EA mesocrystalline structure are shown. As shown in the figure, the Mn-EA / Au catalytic electrode uses gold foil as a conductive substrate, on which spherical Mn-EA mesocrystalline structures are grown in situ.

[0053] (B) Prepare a 10% (w / v) aqueous solution of gelatin, stir at 50 °C until completely dissolved, then slowly add 3 M zinc acetate aqueous solution and mix thoroughly. After cooling to room temperature, a stable Zn(Ac)2 / gelatin quasi-solid electrolyte layer is formed.

[0054] (C) Dissolve sodium alginate in deionized water to prepare a 2% (w / v) solution; separately dissolve chitosan in a 1% (v / v) acetic acid solution to prepare a 1.5% (w / v) solution. Mix the two solutions and stir gently, then add CaCl2 crosslinking solution (100~200 mM) dropwise to induce ionic gelation of sodium alginate. At the same time, an electrostatic complex is formed between chitosan and sodium alginate, thus obtaining a stable sodium alginate-chitosan composite hydrogel.

[0055] (D) such as Figure 3 As shown, a Mn-EA / Au catalytic electrode was used as the cathode, and a zinc foil loaded with Zn(Ac)2 / gelatin quasi-solid electrolyte was used as the anode. The foil was cut to the required size and then stacked and assembled. A compact electrochemical unit was formed by pressing and winding. Subsequently, a sodium alginate-chitosan composite hydrogel was coated onto the outside of the electrochemical unit. Finally, the coated electrochemical unit was encapsulated in an enteric-coated capsule to obtain a self-powered electrocatalytic hangover relief capsule. Figure 4 As shown, during assembly, the thickness of each layer of sodium alginate-chitosan composite hydrogel is 0.05 mm, and the thickness of the Zn(Ac)2 / gelatin quasi-solid electrolyte layer is 0.02 mm.

[0056] like Figure 5 As shown, the self-powered electrocatalytic hangover relief capsule prepared by the above method utilizes the work function difference between the Mn-EA mesocrystalline material and the gold substrate (edible gold foil) to form a built-in electric field upon contact, thereby promoting interfacial charge separation and directional electron transfer, and enhancing the efficiency of the ethanol electro-oxidation reaction. Simultaneously, the Zn negative electrode and the catalytic electrode together form a self-powered battery system, continuously driving the conversion of ethanol to acetic acid without external power supply. Furthermore, the enteric-coated release design of the self-powered electrocatalytic hangover relief capsule ensures that the reaction mainly occurs before or in the early stages of intestinal absorption, thereby reducing the ethanol load entering the circulatory system and alleviating subsequent liver damage, intestinal inflammation, and neurobehavioral abnormalities.

[0057]

Example 2

[0058] In this embodiment, the preparation method of the self-powered electrocatalytic hangover relief capsule is similar to that in Example 1, except that when preparing the Mn-EA / Au catalytic electrode, the aqueous solution contains 0.26 mmol of ellagic acid and 0.26 mmol of manganese acetate tetrahydrate.

[0059]

Example 3

[0060] In this embodiment, the preparation method of the self-powered electrocatalytic hangover relief capsule is similar to that in Example 1, except that when preparing the Mn-EA / Au catalytic electrode, the aqueous solution contains 0.13 mmol of ellagic acid and 0.52 mmol of manganese acetate tetrahydrate.

[0061]

Example 4

[0062] In this embodiment, the preparation method of the self-powered electrocatalytic hangover relief capsule is similar to that in Example 1, except that when preparing the Mn-EA / Au catalytic electrode, the aqueous solution contains 0.52 mmol of ellagic acid and 0.26 mmol of manganese acetate tetrahydrate.

[0063]

Example 5

[0064] In this embodiment, the preparation method of the self-powered electrocatalytic hangover relief capsule is similar to that in Example 1, except that when preparing the Mn-EA / Au catalytic electrode, the aqueous solution contains 0.52 mmol of ellagic acid and 0.13 mmol of manganese acetate tetrahydrate.

[0065]

Example 6

[0066] In this embodiment, the preparation method of the self-powered electrocatalytic hangover relief capsule is similar to that in Example 1, except that manganese nitrate is used instead of manganese acetate when preparing the Mn-EA / Au catalytic electrode.

[0067] In this embodiment, the Mn-EA / Au catalytic electrode prepared based on manganese nitrate has a surface structure of Mn-EA mesomorphs that are not spherical but rather plate-like, such as... Figure 6 As shown, compared to the spherical Mn-EA mesocrystalline material prepared using manganese acetate in Example 1, the surface area will be significantly reduced. Although it can also achieve in-situ electrochemical oxidation of ethanol, the reaction efficiency is not as good as that of the spherical Mn-EA mesocrystalline material.

[0068]

Example 7

[0069] In this embodiment, the preparation method of the self-powered electrocatalytic hangover relief capsule is similar to that in Example 1. The difference is that, during assembly, the thickness of each layer of sodium alginate-chitosan composite hydrogel is 0.10 mm, and the thickness of the Zn(Ac)2 / gelatin quasi-solid electrolyte layer is 0.03 mm.

[0070] II. Performance Testing of Self-Powered Electrocatalytic Hangover Relief Capsules

[0071]

Example 8

[0072] In this embodiment, the electrochemical cycling reaction capability of the electrochemical unit with Mn-EA / Au catalytic electrode prepared in Example 1 was tested.

[0073] Specifically, such as Figure 7 As shown, in a reaction system containing 2 M ZnSO4 and 10 M CH3CH2OH, the catalytic electrode exhibits significant reactivity during cycling and can still maintain a certain level of activity after more than 250 cycles, reflecting that the material can continuously exert a catalytic effect in the ethanol system.

[0074] Furthermore, by analyzing systems with different reaction times... 1 ¹H NMR analysis showed that as the reaction proceeded, the characteristic peak of ethanol gradually weakened, and the characteristic peak of acetic acid was detected, indicating that ethanol underwent oxidative transformation in this system to produce acetic acid. Therefore, the self-powered electrocatalytic hangover detoxification capsule has the function of converting ethanol into acetic acid.

[0075]

Example 9

[0076] In this embodiment, the in vitro ethanol removal capacity and safety of the self-powered electrocatalytic hangover capsule prepared in Example 1 were tested.

[0077] Specifically, the hangover relief capsules were added to ethanol solutions with volume fractions of 5%, 12%, 42%, and 52%, respectively, and treated at 37°C for 6 hours. The changes in ethanol content in the system before and after treatment were measured.

[0078] The test results are as follows Figure 8 As shown, under different initial ethanol concentrations, the ethanol content in the system before treatment increased with increasing ethanol volume fraction. After 6 hours of treatment with the hangover relief capsules, the ethanol content in all groups decreased significantly. Especially in the high-concentration ethanol system, the residual ethanol content remained at a low level after treatment, indicating that the hangover relief capsules have a strong ethanol removal ability over a wide range of ethanol concentrations.

[0079] Furthermore, the ethanol consumption rate for each group was calculated. The results showed that in the 12%, 42%, and 52% ethanol systems, the ethanol consumption rate all reached over 99.4%, with the consumption rate in the 12% and 42% ethanol systems approaching 99.6%; in the 5% ethanol system, the ethanol consumption rate also reached approximately 99.2%. These results indicate that the hangover relief capsules can effectively reduce the ethanol content in systems under different ethanol concentrations, demonstrating excellent ethanol removal effects.

[0080]

Example 10

[0081] In this embodiment, the in vitro thermal safety of the self-powered electrocatalytic hangover detoxification capsule prepared in Example 1 was tested.

[0082] The hangover relief capsules were placed in a 53% ethanol solution, and their surface temperature was monitored using an infrared thermal imager during operation. The temperature distribution at 0 min, 10 min, and 60 min was recorded. The experimental results are as follows: Figure 9 As shown, no significant temperature rise was observed during the reaction process, indicating that the hangover relief capsules have good heat production safety.

[0083]

Example 11

[0084] In this embodiment, the performance of the self-powered electrocatalytic hangover relief capsule prepared in Example 1 was tested in vivo. Specifically, the hangover relief capsule was prepared by cutting it to a length of approximately 5 mm and a width of approximately 3 mm to suit rodents. The hangover relief capsule is as follows... Figure 10 As shown.

[0085] To test the retention behavior of the hangover relief capsules in vivo, Cy7-labeled capsules were administered to rats via gavage. The gastrointestinal tract was then sampled at 2 h, 4 h, and 6 h post-administration for in vitro fluorescence imaging to observe the localization and retention of the hangover relief capsules within the intestines. Figure 11 As shown, hangover relief capsules can remain in the intestines for a long time.

[0086] Furthermore, male SD rats were selected and pretreated for 30 min before being administered ethanol by gavage to establish an acute alcohol poisoning model. An alcohol-relieving capsule group was established, along with a commercially available methadone group and an alcohol group as a control. The alcohol group received no further treatment after gavage administration of alcohol. Blood samples were collected at different time points, and blood ethanol concentrations were measured to evaluate the in vivo ethanol clearance effect of the alcohol-relieving capsules. The experimental results are as follows: Figure 12 As shown, the hangover relief capsules significantly reduced blood alcohol levels within 0.5–6 hours.

[0087] Therefore, it can be seen that hangover relief capsules not only have good and sustained intestinal effects, but also continuously lower blood alcohol levels, thus achieving the effect of relieving hangovers in the body.

[0088] Furthermore, after establishing an acute alcohol poisoning model, we set up an antidote capsule group, a metadoxine group, an empty capsule group, and an alcohol group. The empty capsule group consisted of empty capsules administered by gavage without alcohol treatment, which served as the control group. We recorded the alcohol tolerance time and recovery time of the rats and analyzed the activity patterns of the rats.

[0089] Experimental results are as follows Figure 13As shown, the rats in the hangover relief capsule group had a tolerance time of up to 40 minutes, significantly longer than the metadoxine group and the empty capsule group, indicating that the hangover relief capsules can effectively improve the rats' tolerance to alcohol exposure. Meanwhile, in terms of recovery time, the rats in the hangover relief capsule group recovered to consciousness in approximately 100 minutes, while the recovery time in the metadoxine group and the empty capsule group was 170-190 minutes, indicating that the hangover relief capsules can significantly accelerate the recovery process after intoxication.

[0090] The activity trajectory and path length of the rats showed that the rats in the hangover relief capsule group had a more concentrated movement trajectory and a significantly shorter activity path, which was closer to the normal control state. The effect of the hangover relief capsule on improving abnormal behavior was better than that of the metadoxine group, reflecting that the hangover relief capsule can effectively improve the abnormal behavior of rats after alcohol exposure and promote the recovery of their motor function.

[0091]

Example 12

[0092] In this embodiment, the effect of the self-powered electrocatalytic hangover relief capsule prepared in Example 1 on improving brain-gut axis disorder after acute alcohol exposure was tested.

[0093] Specifically, rat fecal samples were collected from the hangover relief capsule group, metadoxine group, alcohol group, and control group for 16S rRNA gene high-throughput sequencing analysis, and hippocampal tissue was taken for Nissl staining and NeuN and BDNF immunofluorescence detection.

[0094] Experimental results are as follows Figure 14 As shown, after alcohol treatment, the observed ASVs increased and the Simpson index decreased in the alcohol group, indicating a significant disturbance in the gut microbiota structure. Relative abundance analysis at the genus level further indicated that alcohol exposure could cause gut microbiota remodeling. The diversity indicators and gut microbiota composition of the hangover relief capsule group and the metadoxine group showed a trend towards recovery towards the untreated control group, with the hangover relief capsule group exhibiting a superior recovery effect. Analysis of the hippocampus revealed that after alcohol treatment, the hippocampal structure was damaged, NeuN signal distribution was abnormal, and BDNF expression was weakened. After intervention with the hangover relief capsule, hippocampal morphology improved, neuronal-related signals increased, and BDNF expression recovered.

[0095] Therefore, hangover relief capsules can not only reduce the body's alcohol load, but also further improve intestinal flora imbalance and hippocampal damage caused by acute alcohol exposure, thereby playing a protective role in the brain-gut axis homeostasis.

[0096] The specific embodiments described above further illustrate the purpose, technical solution, and beneficial effects of the present invention. It should be understood that the above description is only a specific embodiment of the present invention and is not intended to limit the scope of protection of the present invention. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the scope of protection of the present invention.

Claims

1. A self-powered electrocatalytic hangover relief capsule, comprising a shell, characterized in that, The outer shell is provided with an encapsulation layer, which encapsulates an electrochemical unit. The electrochemical unit includes a catalytic electrode, a counter electrode, and an electrolyte layer located between the catalytic electrode and the counter electrode. The catalytic electrode includes a gold foil and a manganese-ellagic acid mesocrystalline structure, wherein the manganese-ellagic acid mesocrystalline structure is a mesoscopic crystal structure formed by ellagic acid and manganese salt forming a metal-polyphenol network under weak acid conditions and self-assembling on the gold foil.

2. The self-powered electrocatalytic hangover relief capsule according to claim 1, characterized in that, The molar ratio of ellagic acid to manganese salt is 1:4 to 4:

1.

3. The self-powered electrocatalytic hangover relief capsule according to claim 1, characterized in that, The manganese salt is manganese acetate.

4. A self-powered electrocatalytic hangover relief capsule according to any one of claims 1 to 3, characterized in that, The electrolyte layer is prepared by mixing a gelatin solution and a zinc acetate solution and then cooling to obtain a zinc acetate / gelatin electrolyte layer.

5. The self-powered electrocatalytic hangover relief capsule according to claim 4, characterized in that, The encapsulation layer is a sodium alginate-chitosan composite hydrogel prepared by mixing sodium alginate solution and chitosan solution, and then adding calcium ion crosslinking liquid.

6. The self-powered electrocatalytic hangover relief capsule according to claim 4, characterized in that, The thickness ratio of the encapsulation layer to the electrolyte layer is 2~5:

1.

7. A method for preparing a self-powered electrocatalytic hangover relief capsule, characterized in that, Includes the following steps: Ellagic acid, manganese salt, and solvent are mixed to obtain a first solution. Gold foil is immersed in the first solution and the first solution is adjusted to acidity. The reaction system is sealed and allowed to stand for aging to obtain a catalytic electrode. The catalytic electrode includes gold foil and manganese-ellagic acid mesocrystalline material self-assembled on the gold foil. A zinc acetate / gelatin electrolyte layer was prepared by mixing a gelatin solution and a zinc acetate solution. A second solution was obtained by mixing sodium alginate solution and chitosan solution. Calcium ion crosslinking liquid was slowly added to the second solution to prepare sodium alginate-chitosan composite hydrogel. An electrochemical unit is obtained by stacking a catalytic electrode, which serves as the cathode, and a counter electrode, which is loaded with a zinc acetate / gelatin electrolyte layer, as the anode. The electrochemical unit is then coated with a sodium alginate-chitosan composite hydrogel, and the coated electrochemical unit is then encased in a shell to obtain a self-powered electrocatalytic hangover relief capsule.

8. The method for preparing a self-powered electrocatalytic hangover relief capsule according to claim 7, characterized in that, The molar ratio of ellagic acid to manganese salt is 1:4 to 4:

1.

9. The preparation method of a self-powered electrocatalytic hangover relief capsule according to claim 7, characterized in that, The manganese salt is manganese acetate.

10. The application of the self-powered electrocatalytic hangover relief capsule as described in any one of claims 1 to 6, characterized in that, The self-powered electrocatalytic hangover relief capsule is used to prepare a drug for promoting the electrochemical oxidation of ethanol in the intestine, and / or to prepare a drug for improving hippocampal tissue morphological damage caused by ethanol.

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