A composition comprising glycerylphosphocholine and uses thereof

Abstract

The application belongs to the field of oral composition and food application, and provides a composition containing choline alfoscerate and application thereof. The composition takes L-alpha-choline alfoscerate as a liquid phase component, takes a complex core formed by pyrroloquinoline quinone disodium salt and cyclodextrin as a core, forms a multi-layer core-shell particle through core particle construction and layer-by-layer assembly of gelatin and sodium alginate, and is cooperatively configured with a dual-phase or dual-cavity storage mode. Therefore, the storage stability of the active ingredient, the integrity of the particle structure and the active release performance when used are considered, the adverse effects of environmental exposure are reduced, and the use convenience is improved. The composition can solve the problem that the memory-improving function and storage stability are difficult to be considered, and the particle structure integrity and the active release performance are restricted by each other, and is suitable for memory-improving food development and application.

Description

Technical Field

[0001] This invention relates to the field of oral compositions and food applications, and more specifically to a composition containing choline glyphosate and its applications. Background Technology

[0002] In the development of memory-enhancing foods and oral compositions, active ingredients such as L-α-glucosinolate must not only meet the requirements of easy mixing, convenient use, and packaging compatibility during consumption, but also ensure phase stability, component compatibility, and system integrity during storage and transportation. Existing patents have disclosed compositions for improving memory function, applications in health foods, and oral forms such as soft capsules, indicating that the oral application scenario and memory support needs are relatively clear. This also reflects the continued importance of ease of intake and storage stability in the productization process. For systems that require the synergistic presence of liquid and solid phases, if there is only an active ingredient but no suitable inclusion core, core particles, or shell structure, the activity may be exposed, migrate, or the system may become unstable during storage. If there is only a protective structure but no remixing design that matches the usage scenario, it is difficult to achieve both pre-consumption protection and performance during consumption. Therefore, the structural design of oral compositions has become an important direction in this field.

[0003] Based on existing approaches, related research often follows two routes: one route focuses on the formulation and improvement of the ease of intake of choline-based active ingredients, while the other route focuses on the inclusion and preservation of redox-sensitive active ingredients. For example, Chinese patent CN101945648B discloses a pharmaceutical product containing glyphosate choline, which improves storage stability and ease of intake through adsorption pathways. However, its technical focus is on the stabilization of a single glyphosate choline product and does not address the dual constraints between functional performance and storage stability in multi-active oral systems. Another example is Chinese patent CN105189501B, which discloses yellow-based reduced pyrroloquinoline quinone crystals and their manufacturing methods, as well as manufacturing methods for food, pharmaceuticals, gels, compositions, and compositions. It improves the storage stability of pyrroloquinoline quinone-related systems through cyclodextrin inclusion and drying processes. However, its focus is still biased towards the stable storage of a single component. It lacks a comprehensive solution that balances phase separation, particle structure integrity, and activity release during use when L-α-glyphosate choline and pyrroloquinoline quinone disodium salt coexist. Summary of the Invention

[0004] The purpose of this invention is to provide a composition containing choline glyphosate and its application, which solves the current pain points of difficulty in balancing the improvement of memory function and storage stability, and the mutual restriction between particle structure integrity and active release performance.

[0005] This invention prepares L-α-glycine choline in the liquid phase, first forming an inclusion core with cyclodextrin by disodium pyrroloquinoline quinone, and then constructing core particles and assembling them layer by layer with gelatin and sodium alginate to form multi-layered core-shell particles. Combined with biphasic or dual-cavity storage methods, the active ingredients are protected during storage and then mixed and released during use, thereby simultaneously alleviating the dual constraints of decreased stability and insufficient function.

[0006] To achieve the above objectives, the present invention provides the following technical solution: A composition comprising phosphocholine, said composition being an oral composition, comprising at least the following components: water, L-α-phosphocholine, D-sorbitol, citric acid, sodium citrate dihydrate, xanthan gum, potassium sorbate, sucralose, and multilayered core-shell particles; The multilayer core-shell particles comprise an inclusion core formed by disodium pyrroloquinoline quinone and cyclodextrin, core particles containing the inclusion core, and a shell layer formed by layering gelatin and sodium alginate on the surface of the core particles; based on the total mass of the composition, the mass fraction of L-α-glycine is 1.5-5.5 wt%, and the mass fraction of disodium pyrroloquinoline quinone is 0.001-0.004 wt%.

[0007] Furthermore, the inclusion core is prepared through the following steps: A1. Raw material preparation: Provide disodium salt of pyrroloquinoline quinone, cyclodextrin and water, wherein the mass ratio of cyclodextrin to disodium salt of pyrroloquinoline quinone is 2:1-6:1; A2. Inclusion: Cyclodextrin is dissolved in water to obtain a cyclodextrin solution with a mass concentration of 5-20 mg / mL, and disodium pyrroloquinoline quinone is dissolved in water to obtain a disodium pyrroloquinoline quinone solution with a mass concentration of 1-10 mg / mL. The disodium pyrroloquinoline quinone solution is added to the cyclodextrin solution, and the mass ratio of cyclodextrin to disodium pyrroloquinoline quinone is 2:1-6:1. The temperature is controlled at 25-60℃ and the mixture is stirred at 200-800 rpm for 1-4 hours to form an inclusion system. A3. Curing: The inclusion system is allowed to stand at 15-25℃ for 2-12 hours and then dried by freeze drying or spray drying. The pre-freezing temperature for freeze drying is -40℃ to -20℃, the pre-freezing time is 2-6 hours, and the vacuum degree during the sublimation stage is 10-50 Pa. The inlet air temperature for spray drying is 150-200℃, and the outlet air temperature is 80-100℃. A4. Endpoint and quality control: The water content of the obtained inclusion nuclei is not greater than 3 wt%, and the water activity aw measured at 25℃ is not greater than 0.25.

[0008] Furthermore, the core particles in the multilayer core-shell particles are prepared through the following steps: B1. Raw material preparation: The inclusion core is mixed with maltodextrin and gum arabic, wherein the dry weight ratio of maltodextrin to gum arabic is 1:10 to 10:1, and the mass fraction of the inclusion core is 5-40 wt%, based on the total dry weight of the inclusion core, maltodextrin, and gum arabic. B2. Granulation: Add water to the mixture obtained in step B1 to form a liquid with a solid content of 20-45 wt%. Obtain core particles by spray granulation or fluidized bed granulation. The inlet air temperature for spray granulation is 120-180℃, the outlet air temperature is 60-80℃, and the atomization pressure is 0.2-0.6 MPa. The bed temperature for fluidized bed granulation is 45-70℃, and the rotation speed of the atomizing device is 5000-15000 rpm. B3. Drying and Atmosphere Control: The drying process is carried out under an inert atmosphere, wherein the inert atmosphere is nitrogen with a purity of not less than 99%; B4. Endpoint and quality control: The D50 of the obtained nuclear particles is 200-800µm and the moisture content is no more than 3wt%.

[0009] Furthermore, the shell layer is prepared and coated onto the surface of the core particle through the following steps: C1. Gelatin layer solution: Dissolve gelatin in water to form a gelatin solution with a mass fraction of 0.1-2.0 wt%, and adjust the pH value to 3.0-4.5 with citric acid under stirring. C2. Sodium alginate layer solution: Sodium alginate is dissolved in water to form a sodium alginate solution with a mass fraction of 0.1-1.5 wt%, and the pH value is adjusted to 6.0-7.5 using sodium citrate dihydrate under stirring conditions; C3. Layer-by-layer assembly: The core particles are sequentially contacted with the gelatin solution and the sodium alginate solution and subjected to 2-4 double-layer cycles. The total contact time for each double-layer cycle is 10-30 minutes. After each contact with the gelatin solution or the sodium alginate solution, they are separated. After all double-layer cycles, the shell layer is formed. C4. Post-processing and quality control: The assembled particles are dried to obtain multi-layered core-shell particles. The moisture content of the multi-layered core-shell particles is not greater than 3 wt%, the water activity aw measured at 25℃ is not greater than 0.25, and the weight gain of the shell layer is 5-18 wt% based on the dry basis weight of the core particles before assembly.

[0010] Furthermore, the composition is a biphase composition comprising a liquid phase and a solid phase; the liquid phase comprises water, L-α-glycine choline, D-sorbitol, citric acid, sodium citrate dihydrate, xanthan gum, potassium sorbate, and sucralose; the solid phase is multilayered core-shell particles, and the water content of the solid phase before mixing with the liquid phase is no more than 3 wt%; based on the total mass of the composition, the mass fraction of D-sorbitol is 5-35 wt%, the total mass fraction of citric acid and sodium citrate dihydrate is 0.10-1.20 wt%, the pH value of the liquid phase is 3.5-4.5, and the mass fraction of xanthan gum is 0.05-0.50 wt%; the liquid phase also comprises at least one of vanillin and S-configuration limonene, with a total mass fraction of 0.0005-0.05 wt% based on the total mass of the composition.

[0011] As a concept of this invention, the present invention employs a design that synergistically configures L-α-glycine phosphate liquid phase with multilayer core-shell particles containing a disodium pyrroloquinoline quinone inclusion core. This design aims to achieve a synergistic balance between storage stability and enhanced memory function. In existing technologies, to improve storage stability, low water activity control, compartmentalized packaging, or enhanced encapsulation protection are commonly used. However, excessive isolation of the active ingredient often limits mixing, release, and ease of use. Conversely, directly exposing the active ingredient to the liquid phase to enhance memory function can easily lead to moisture absorption, migration, or environmental sensitivity issues. This invention, by configuring L-α-glycine phosphate in the liquid phase, first forming an inclusion core with pyrroloquinoline quinone disodium salt and cyclodextrin, then constructing core particles and assembling them layer by layer with gelatin and sodium alginate to form multilayer core-shell particles, and combining this with biphasic or dual-cavity packaging methods, cross-mitigates the side effects of excessive exposure and excessive closure, ensuring the oral composition is stable before consumption and releases during consumption, thus balancing storage and functional performance.

[0012] Furthermore, the method for preparing the composition includes the following steps: S1. Preparation of inclusion core: Prepare inclusion core according to steps A1 to A4; S2. Preparation of multi-layered core-shell particles: Using the encapsulated core as the core material, multi-layered core-shell particles are prepared according to steps B1 to B4 and steps C1 to C4; S3. Preparation of liquid phase: Dissolve L-α-glycine choline in water, and add D-sorbitol, citric acid, sodium citrate dihydrate, xanthan gum, potassium sorbate and sucralose in sequence. Mix well under stirring to obtain the liquid phase. S4. The multilayer core-shell particles obtained in step S2 are mixed with the liquid phase obtained in step S3 under stirring conditions to obtain the composition.

[0013] Furthermore, after the multilayer core-shell particles obtained in step S2 are placed at a temperature of 23-27℃ and a relative humidity of 70-80% for 7 days, the weight gain calculated based on the dry basis weight of the sample before placement is no more than 5wt%; the mixing operation in step S4 is carried out under an inert atmosphere, wherein the inert atmosphere is nitrogen.

[0014] Furthermore, the composition is formulated into a dual-cavity packaging formulation comprising a liquid cavity content and a dry cavity content. The liquid cavity content is the liquid phase of the composition, containing water, L-α-glycine choline, D-sorbitol, citric acid, sodium citrate dihydrate, xanthan gum, potassium sorbate, sucralose, and vanillin and / or S-configuration limonene. The dry cavity content is multilayered core-shell particles, which are connected and mixed with the liquid cavity during use. The dual-cavity packaging formulation is made of a high-barrier composite packaging film, which comprises a polyethylene terephthalate layer, an aluminum layer, and a polyethylene layer, and the total mass of a single serving of the dual-cavity packaging formulation is 5-10g.

[0015] Furthermore, a ruptureable seal is provided between the liquid chamber and the dry chamber, which is formed by heat sealing under conditions of 135-155℃, 0.3-0.5MPa, and 0.8-1.5s.

[0016] Furthermore, the composition containing glycine phosphate is used in the preparation of foods for improving memory.

[0017] Furthermore, the cyclodextrin is β-cyclodextrin and / or γ-cyclodextrin.

[0018] Furthermore, in step A2, the inclusion process is carried out under light-protected conditions, and the total solid content of the mixed system is controlled to be 2-18 mg / mL.

[0019] Furthermore, in step A2, the inclusion temperature is preferably 25-45℃.

[0020] Furthermore, in step A3, when freeze drying is used, the sublimation stage temperature is -10℃ to +10℃, and the sublimation time is 6-24h; when spray drying is used, the outlet air temperature is stabilized at 80-100℃ by controlling the feed rate.

[0021] Furthermore, the gelatin is type A gelatin, and the isoelectric point of the gelatin is not lower than 6.0.

[0022] Furthermore, in step B2, when fluidized bed granulation is used, a centrifugal atomizing disc is used for atomization.

[0023] Furthermore, in step B3, the nitrogen flow rate is 0.1-10 L / min, and the oxygen content at the outlet of the drying equipment is not higher than 2.0 vol.

[0024] Furthermore, in step C3, the layer-by-layer assembly adopts an immersion method, with a liquid-to-solid mass ratio of 5:1 to 20:1.

[0025] Furthermore, in step C3, the separation is carried out by centrifugation at a speed of 2000-5000 rpm for 5-15 min, or by filtration with a pore size of 10-100 µm.

[0026] Furthermore, in step C3, deionized water is used for washing, and the number of washes is 0-1 times per double-layer cycle.

[0027] Furthermore, during the layer-by-layer assembly process, process verification is conducted through weight gain, particle size changes, or surface potential changes detected by sampling.

[0028] Furthermore, in step S3, the liquid phase preparation temperature is 20-30℃, the stirring speed is 200-800 rpm, and the stirring time is 10-60 min.

[0029] Furthermore, in step S4, the mixing temperature of the multilayer core-shell particles and the liquid phase is 20-30℃, the stirring speed is 50-300rpm, and the stirring time is 1-10min.

[0030] Furthermore, the D50 of the obtained core particles was determined by a laser particle size analyzer, the water activity of the multilayer core-shell particles was determined by a water activity analyzer at 25°C, and the moisture content was determined by drying at 105°C to constant weight method.

[0031] Furthermore, the stability test of the multilayer core-shell particles was carried out in a constant temperature and humidity chamber. The sample was placed in an open weighing dish. The dry basis mass m0 was measured before placement and the dry basis mass m1 was measured after 7 days. The mass gain was calculated by multiplying the ratio of m1 minus m0 to m0 by 100%. The dry basis mass was determined by drying at 105℃ to constant weight. The constant weight criterion was that the difference between two adjacent weighings was not greater than 0.5 mg.

[0032] Furthermore, the composition is an oral composition in beverage form. In a dual-cavity packaging embodiment, the dry cavity contents are formulated as a solid beverage component, the solid phase is stored separately from the liquid phase before use, and the dual-cavity packaging formulation is a single-dose packaging formulation.

[0033] As another aspect of this invention, a preparation method employing the sequential control of inclusion core preparation, core particle preparation, shell layer assembly, liquid phase formulation, and mixing is employed, primarily to achieve, fix, or amplify the aforementioned synergistic effects. In existing technologies, improving storage stability solely through enhanced drying, increased shell density, or extended processing pathways often results in limited redispersion and delayed activity release during use. Conversely, pursuing rapid mixing or direct exposure of active components can easily disrupt the inclusion protection state and weaken the structural integrity of the particles during preparation, packaging, and storage. This invention constructs the system according to the sequence of inclusion core, core particles, shell layer, and then liquid phase mixing, completing the final mixing under controlled conditions. This ensures that the multi-layered core-shell particles maintain a low moisture content before entering the liquid phase, achieving interphase contact and functional release during use, thus simultaneously mitigating the dual side effects of stability and release from the process pathway.

[0034] In this invention, L-α-glycine choline primarily functions as an immediate dispersant in the liquid phase and enhances memory, while the multilayered core-shell particles containing pyrroloquinoline quinone disodium salt, cyclodextrin, gelatin, and sodium alginate primarily maintain storage stability and particle structure integrity. Increasing the proportion of multilayered core-shell particles or excessively enhancing shell density, while beneficial for moisture isolation and particle integrity, can limit activity release and delay functional performance upon liquid-phase contact. Conversely, directly exposing L-α-glycine choline and related active components to the liquid phase, while improving mixing and function during use, can easily lead to hygroscopicity, migration, and decreased storage stability. This invention retains L-α-glycine choline in the liquid phase, first encapsulating pyrroloquinoline quinone disodium salt with cyclodextrin, then assembling it layer by layer with gelatin and sodium alginate to construct the shell. Combined with biphase or bicavation storage, proportion matching, and process sequence control, these components compensate for each other in the same oral system, ultimately achieving a balance between storage stability, particle structure integrity, and activity release performance.

[0035] Beneficial technical effects 1. This invention configures L-α-glucosinolate in the liquid phase and pyrroloquinoline quinoline quinoline disodium salt in the solid phase after cyclodextrin inclusion, core particle construction and shell assembly, so that the composition has phase separation protection conditions before storage and can be mixed and released during use, thereby better balancing the improvement of memory function and storage stability.

[0036] 2. This invention uses gelatin and sodium alginate to form a shell layer by layer, and limits the moisture, water activity (aw), and shell mass gain. This helps to reduce the risk of structural damage to the particles during preparation, packaging, and storage, while avoiding the limitation of activity release caused by simply relying on shell densification.

[0037] 3. This invention, through the synergistic formulation of liquid phase pH, D-sorbitol, xanthan gum, citric acid and sodium citrate dihydrate, enables the liquid phase and multilayer core-shell particles to maintain good system compatibility before and after mixing, which is beneficial to improving the ease of use of oral compositions, consistency of single-dose application and repackaging compatibility.

[0038] 4. The present invention further provides a biphasic composition, a preparation method, and a dual-cavity packaging formulation, which can maintain the liquid phase and solid phase separately for storage before consumption, reduce the adverse effects of premature contact, and achieve rapid connection and mixing during use, making it suitable for the productization and industrialization of memory-enhancing foods. Attached Figure Description

[0039] Figure 1 The images are XRD patterns of Example 1 and Comparative Example 8.

[0040] Figure 2 The images are FTIR plots of Example 1 and Comparative Example 8.

[0041] Figure 3 Trajectory diagrams of the phased interface construction of ζ potential for Example 1, Comparative Example 4, and Comparative Example 9.

[0042] Figure 4 The image shows the differential volume distribution of laser particle size for Examples 1, 4, and 9.

[0043] Figure 5 The cumulative volume distribution of laser particle size is shown in Example 1, Comparative Example 4, and Comparative Example 9.

[0044] Figure 6 The HPLC activity retention rate of PQQ is shown in the graphs for Example 1 and Comparative Example 10.

[0045] Figure 7 The HPLC activity retention chromatograms of L-α-GPC for Example 1 and Comparative Example 10 are shown.

[0046] Figure 8 The image shows the cumulative release curves (PQQ) of INFOGEST for Example 1, Comparative Example 9, and Comparative Example 10.

[0047] Figure 9 This is a macroscopic optical photograph of the multilayer core-shell particles in Example 1.

[0048] Figure 10 This is a photograph of the actual product of the dual-chamber packaging formulation in Example 1.

[0049] Figure 11 This is a scanning electron microscope image of the multilayer core-shell particles in Example 1; Figure 11 a is a low-magnification scanning electron microscope image of the multilayer core-shell particles in Example 1; Figure 11b is a medium-magnification scanning electron microscope image of the multilayer core-shell particles in Example 1; Figure 11 c is a high-magnification scanning electron microscope image of the multilayer core-shell particles in Example 1; Figure 11 Image d is a cross-sectional scanning electron microscope image of the multilayer core-shell particles in Example 1.

[0050] Figure 12 This is a transmission electron microscope image of the multilayer core-shell particles in Example 1; Figure 12 a is a bright-field transmission electron microscope image of the multilayer core-shell particles in Example 1; Figure 12 b is a magnified transmission electron microscope image of a multilayer core-shell particle from Example 1; Figure 12 c is a high-resolution transmission electron microscope image of the multilayer core-shell particles in Example 1; Figure 12 d is the selected area electron diffraction pattern of the multilayer core-shell particles in Example 1. Detailed Implementation

[0051] To make the objectives, technical solutions, and advantages of the embodiments of the present invention clearer, the technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings.

[0052] Terminology Explanation: In this application, "dry basis mass" or "total dry basis mass" refers to the mass of solid matter after moisture removal; dry basis mass is determined by drying to constant weight at a temperature of 105°C, and the constant weight criterion is that the difference between two adjacent weighings is not greater than 0.5 mg. Example 1

[0053] This embodiment prepares 100g of a composition containing choline glyphosate.

[0054] S1. Preparation of inclusion core: A1. Raw material preparation: Weigh 0.001g of disodium pyrroloquinoline quinone, 0.002g of β-cyclodextrin and water. The mass ratio of cyclodextrin to disodium pyrroloquinoline quinone is 2:1.

[0055] A2. Inclusion: 0.002 g of β-cyclodextrin was dissolved in 0.4 mL of water to obtain a cyclodextrin solution with a mass concentration of 5 mg / mL. 0.001 g of disodium pyrroloquinolinequinone was dissolved in 1.0 mL of water to obtain a disodium pyrroloquinolinequinone solution with a mass concentration of 1 mg / mL. Under light-protected conditions, the disodium pyrroloquinolinequinone solution of this embodiment was added to the cyclodextrin solution of this embodiment, with a mass ratio of cyclodextrin to disodium pyrroloquinolinequinone of 2:1. The temperature was controlled at 40°C and the mixture was stirred at 500 rpm for 2.5 h. The total solid content of the mixture was 2.1 mg / mL, thus forming an inclusion system.

[0056] A3. Curing: The inclusion system of this embodiment was freeze-dried after being left to stand at 20°C for 8 hours. The pre-freezing temperature was -30°C and the pre-freezing time was 4 hours. The vacuum degree of the sublimation stage was 30 Pa, the temperature of the sublimation stage was 0°C, and the sublimation time was 15 hours.

[0057] A4. Endpoint and quality control: The water content of the obtained inclusion nuclei was 1.8 wt%, and the water activity aw measured at 25℃ was 0.15.

[0058] S2. Preparation of multilayer core-shell particles: B1. Raw material preparation: Mix 0.003g of inclusion core, 0.00518g of maltodextrin and 0.0518g of gum arabic in this embodiment. The dry weight ratio of maltodextrin to gum arabic is 1:10. Based on the total dry weight of inclusion core, maltodextrin and gum arabic, the mass fraction of inclusion core is 5wt%.

[0059] B2. Granulation: The mixture obtained in step B1 is added to water to form a liquid with a solid content of 20wt%. Core particles are obtained by spray granulation. The inlet air temperature of spray granulation is 150℃, the outlet air temperature is 70℃, and the atomization pressure is 0.4MPa. The outlet air temperature is stabilized at 70℃ by controlling the feed rate.

[0060] B3. Drying and Atmosphere Control: The drying process is carried out in a nitrogen atmosphere with a purity of 99.5%, a nitrogen flow rate of 5L / min, and an oxygen content of 1.5 vol at the outlet of the drying equipment.

[0061] B4. Endpoint and Quality Control: The D50 of the obtained nuclear particles was determined to be 200 µm by laser particle size analyzer, and the moisture content was determined to be 2.0 wt% by drying at 105 °C to constant weight method.

[0062] C1. Gelatin layer solution: Type A gelatin is dissolved in water to form a gelatin solution with a mass fraction of 1.0 wt%. The pH value is adjusted to 3.8 using citric acid under stirring. The isoelectric point of the gelatin in this embodiment is 7.5.

[0063] C2. Sodium alginate layer solution: Sodium alginate was dissolved in water to form a sodium alginate solution with a mass fraction of 0.8 wt%. The pH value was adjusted to 6.8 using sodium citrate dihydrate under stirring conditions.

[0064] C3. Layer-by-Layer Assembly: The core particles obtained in step B4 are sequentially contacted with the gelatin solution and sodium alginate solution of this embodiment for two double-layer cycles, using an immersion method with a liquid-to-solid mass ratio of 10:1. The total contact time for each double-layer cycle is 20 minutes. In each double-layer cycle, the core particles are first immersed in the gelatin solution for 10 minutes, then separated by centrifugation at 3500 rpm for 10 minutes, and then immersed in the sodium alginate solution for 10 minutes, followed by centrifugation again. After each double-layer cycle, the particles are washed once with deionized water. The process is confirmed by weight gain, and the shell layer of this embodiment is formed after all double-layer cycles.

[0065] C4. Post-processing and quality control: The assembled particles are dried to obtain multi-layer core-shell particles. In this embodiment, the moisture content of the multi-layer core-shell particles is 2.2 wt% as determined by constant weight method after drying at 105°C. The water activity aw is 0.18 as determined by water activity meter at 25°C. Based on the dry basis mass of the core particles before assembly, the mass gain of the shell layer is 5 wt%.

[0066] S3. Preparation of liquid phase: 1.5g of L-α-glycine phosphate was dissolved in 77.67g of water. Under conditions of 25℃ and 500rpm, 20g of D-sorbitol, 0.2g of citric acid, 0.4g of sodium citrate dihydrate, 0.2g of xanthan gum, 0.05g of potassium sorbate, 0.01g of sucralose, and 0.01g of S-configuration limonene were added sequentially and stirred for 35min to obtain a homogeneous liquid phase. The pH of the liquid phase in this example was 5.0.

[0067] S4. Mixing: Under a nitrogen atmosphere, the multilayer core-shell particles obtained in step S2 and the liquid phase obtained in step S3 are mixed at a temperature of 25°C and a stirring speed of 150 rpm for 5 minutes to obtain the composition of this embodiment.

[0068] Stability test: The multilayer core-shell particles obtained in step S2 were placed in a constant temperature and humidity chamber at 25°C and 75% relative humidity for 7 days. The sample was placed in an open weighing dish. The dry basis mass m0 was measured before placement and the dry basis mass m1 was measured after 7 days. The dry basis mass was determined by drying at 105°C to constant weight. The constant weight criterion was that the difference between two adjacent weighings was no more than 0.5 mg. The mass gain calculated based on the dry basis mass of the sample before placement was 3.2 wt%.

[0069] Preparation of dual-chamber packaging formulations: In this embodiment, the liquid phase is used as the contents of the liquid cavity, and the multilayer core-shell particles are used as the contents of the dry cavity. A high-barrier composite packaging film comprising a polyethylene terephthalate layer, an aluminum layer, and a polyethylene layer is used to prepare a dual-cavity packaged formulation, with a total mass of 7g per portion. A ruptureable seal is provided between the liquid cavity and the dry cavity. In this embodiment, the ruptureable seal is formed by heat sealing at a temperature of 145°C, a pressure of 0.4MPa, and a time of 1.2s.

[0070] Features of Example 1: This embodiment employs a relatively low component ratio design, with L-α-glycine choline content and pyrroloquinoline quinone disodium salt content both in the low-range range. The amount of cyclodextrin used in the inclusion process is small, resulting in a low proportion of the inclusion core in the core particles. Maltodextrin and gum arabic are configured in a low ratio, with a low shell weight gain, a core particle size in the low-range range, and low concentrations in both the cyclodextrin and pyrroloquinoline quinone disodium salt solutions, as well as a low solids content in the liquid-solid mixture. This scheme uses freeze-drying to prepare the inclusion core and employs fewer double-layer cycles in the layer-by-layer assembly. The formulation of this embodiment is relatively mild, with moderate levels of active ingredients, making it suitable as a health drink for daily memory maintenance. It is particularly suitable for consumers seeking mild formulas and those with high sensitivity to active ingredients, and can be used as a daily nutritional supplement. Example 2

[0071] This embodiment prepares 100g of a composition containing choline glyphosate.

[0072] S1. Preparation of inclusion core: A1. Raw material preparation: Weigh 0.004g of disodium pyrroloquinoline quinone, 0.024g of γ-cyclodextrin and water. The mass ratio of cyclodextrin to disodium pyrroloquinoline quinone is 6:1.

[0073] A2. Inclusion: 0.024 g of γ-cyclodextrin was dissolved in 1.2 mL of water to obtain a cyclodextrin solution with a mass concentration of 20 mg / mL. 0.004 g of disodium pyrroloquinolinequinone was dissolved in 0.4 mL of water to obtain a disodium pyrroloquinolinequinone solution with a mass concentration of 10 mg / mL. Under light-protected conditions, the disodium pyrroloquinolinequinone solution of this embodiment was added to the cyclodextrin solution of this embodiment, with a mass ratio of cyclodextrin to disodium pyrroloquinolinequinone of 6:1. The temperature was controlled at 45°C and the mixture was stirred at 600 rpm for 3 hours. The total solid content of the mixture was 17.5 mg / mL, thus forming an inclusion system.

[0074] A3. Curing: The inclusion system of this embodiment is allowed to stand at 18°C ​​for 10 hours and then spray-dried. The inlet air temperature of the spray dryer is 180°C and the outlet air temperature is 90°C. The outlet air temperature is stabilized at 90°C by controlling the feed rate.

[0075] A4. Endpoint and quality control: The water content of the obtained inclusion nuclei was 2.5 wt%, and the water activity aw measured at 25℃ was 0.20.

[0076] S2. Preparation of multilayer core-shell particles: B1. Raw material preparation: Mix 0.028g of inclusion core, 0.0382g of maltodextrin and 0.00382g of gum arabic in this embodiment. The dry weight ratio of maltodextrin to gum arabic is 10:1. Based on the total dry weight of inclusion core, maltodextrin and gum arabic, the mass fraction of inclusion core is 40wt%.

[0077] B2. Granulation: The mixture obtained in step B1 is added to water to form a liquid with a solid content of 45wt%. The mixture is then granulated in a fluidized bed to obtain core particles. The bed temperature of the fluidized bed granulation is 60℃. A centrifugal atomizing disc is used for atomization, and the atomizing device rotates at 12000rpm.

[0078] B3. Drying and Atmosphere Control: The drying process is carried out in a nitrogen atmosphere with a purity of 99.9%, a nitrogen flow rate of 8 L / min, and an oxygen content of 0.8 vol at the outlet of the drying equipment.

[0079] B4. Endpoint and Quality Control: The D50 of the obtained nuclear particles was determined to be 700 µm by laser particle size analyzer, and the moisture content was determined to be 2.5 wt% by drying at 105 °C to constant weight method.

[0080] C1. Gelatin layer solution: Type A gelatin is dissolved in water to form a gelatin solution with a mass fraction of 1.8 wt%. The pH value is adjusted to 3.5 using citric acid under stirring. The isoelectric point of the gelatin in this embodiment is 8.0.

[0081] C2. Sodium alginate layer solution: Sodium alginate was dissolved in water to form a sodium alginate solution with a mass fraction of 1.4 wt%. The pH value was adjusted to 7.2 using sodium citrate dihydrate under stirring conditions.

[0082] C3. Layer-by-Layer Assembly: The core particles obtained in step B4 are sequentially contacted with the gelatin solution and sodium alginate solution of this embodiment for three double-layer cycles, using an immersion method with a liquid-to-solid mass ratio of 15:1. The total contact time for each double-layer cycle is 25 minutes. In each double-layer cycle, the core particles are first immersed in the gelatin solution for 12.5 minutes, then separated using a 50µm pore size filter, and then immersed in the sodium alginate solution for 12.5 minutes, followed by another filtration separation. After each double-layer cycle, the particles are washed once with deionized water. The process is confirmed by particle size changes, and the shell layer of this embodiment is formed after all double-layer cycles.

[0083] C4. Post-processing and quality control: The assembled particles are dried to obtain multi-layer core-shell particles. In this embodiment, the moisture content of the multi-layer core-shell particles is 2.8 wt% as determined by constant weight method after drying at 105°C. The water activity aw is 0.22 as determined by water activity meter at 25°C. Based on the dry basis mass of the core particles before assembly, the mass gain of the shell layer is 18 wt%.

[0084] S3. Preparation of liquid phase: 5.5 g of L-α-glycine phosphate was dissolved in 57.98 g of water. Under conditions of 28°C and 700 rpm, 35 g of D-sorbitol, 0.3 g of citric acid, 0.6 g of sodium citrate dihydrate, 0.45 g of xanthan gum, 0.05 g of potassium sorbate, 0.01 g of sucralose, 0.015 g of vanillin, and 0.015 g of S-configuration limonene were added sequentially and stirred for 50 min to obtain a homogeneous liquid phase. The pH value of the liquid phase in this example was 3.8.

[0085] S4. Mixing: Under a nitrogen atmosphere, the multilayer core-shell particles obtained in step S2 and the liquid phase obtained in step S3 were mixed at a temperature of 28°C and a stirring speed of 200 rpm for 8 minutes to obtain the composition of this embodiment.

[0086] Stability test: The multilayer core-shell particles obtained in step S2 were placed in a constant temperature and humidity chamber at 27°C and 78% relative humidity for 7 days. The sample was placed in an open weighing dish. The dry basis mass m0 was measured before placement and the dry basis mass m1 was measured after 7 days. The dry basis mass was determined by drying at 105°C to constant weight. The constant weight criterion was that the difference between two adjacent weighings was no more than 0.5 mg. The mass gain calculated based on the dry basis mass of the sample before placement was 4.5 wt%.

[0087] Preparation of dual-chamber packaging formulations: In this embodiment, the liquid phase is used as the contents of the liquid cavity, and the multilayer core-shell particles are used as the contents of the dry cavity. A high-barrier composite packaging film comprising a polyethylene terephthalate layer, an aluminum layer, and a polyethylene layer is used to prepare a dual-cavity packaged formulation, with a total mass of 9g per portion. A ruptureable seal is provided between the liquid cavity and the dry cavity. In this embodiment, the ruptureable seal is formed by heat sealing at a temperature of 152°C, a pressure of 0.48MPa, and a time of 1.4s.

[0088] Features of Example 2: This embodiment employs a high-ratio component design, with high levels of L-α-glycine phosphate and disodium pyrroloquinoline quinone. A significant amount of cyclodextrin is used during inclusion, resulting in a high proportion of the inclusion core within the core particles. A high ratio of maltodextrin and gum arabic is used, with a high shell weight gain. The core particle size is within the high-range range, and both the concentrations of the cyclodextrin and disodium pyrroloquinoline quinone solutions are high. The solids content of the liquid and D-sorbitol are also high, as is the total mass per package. The inclusion core is prepared using spray drying, and fluidized bed granulation is employed, with numerous double-layer cycles used in the layer-by-layer assembly. This embodiment features a high content of active ingredients, making it suitable for consumers with high demands for memory enhancement. It is particularly suitable for students, mental workers, and others requiring efficient memory support, and can be used as a functional beverage during periods of high-intensity mental activity. Example 3

[0089] This embodiment prepares 100g of a composition containing choline glyphosate.

[0090] S1. Preparation of inclusion core: A1. Raw material preparation: Weigh 0.0025g of disodium pyrroloquinoline quinone, 0.010g of a mixture of β-cyclodextrin and γ-cyclodextrin, and water, wherein the mass ratio of β-cyclodextrin to γ-cyclodextrin is 1:1, and the mass ratio of cyclodextrin to disodium pyrroloquinoline quinone is 4:1.

[0091] A2. Inclusion: 0.010 g of the cyclodextrin mixture was dissolved in 0.8 mL of water to obtain a cyclodextrin solution with a mass concentration of 12.5 mg / mL. 0.0025 g of disodium pyrroloquinolinequinone was dissolved in 0.5 mL of water to obtain a disodium pyrroloquinolinequinone solution with a mass concentration of 5 mg / mL. Under light-protected conditions, the disodium pyrroloquinolinequinone solution of this embodiment was added to the cyclodextrin solution of this embodiment, with a mass ratio of cyclodextrin to disodium pyrroloquinolinequinone of 4:1. The temperature was controlled at 25°C and the mixture was stirred at 800 rpm for 4 hours. The total solid content of the mixture was 9.6 mg / mL, thus forming an inclusion system.

[0092] A3. Curing: The inclusion system of this embodiment was freeze-dried after being left to stand at 15°C for 12 hours. The pre-freezing temperature was -40°C and the pre-freezing time was 2 hours. The vacuum degree of the sublimation stage was 50 Pa, the sublimation temperature was 10°C, and the sublimation time was 6 hours.

[0093] A4. Endpoint and quality control: The water content of the obtained inclusion nuclei was 2.2 wt%, and the water activity aw measured at 25℃ was 0.17.

[0094] S2. Preparation of multilayer core-shell particles: B1. Raw material preparation: 0.0125g of inclusion core, 0.0156g of maltodextrin and 0.0156g of gum arabic were mixed. The dry weight ratio of maltodextrin to gum arabic was 1:1. Based on the total dry weight of inclusion core, maltodextrin and gum arabic, the mass fraction of inclusion core was 28.6wt%.

[0095] B2. Granulation: The mixture obtained in step B1 is added to water to form a liquid with a solid content of 35wt%. Core particles are obtained by fluidized bed granulation. The bed temperature of fluidized bed granulation is 45℃. Atomization is performed by a centrifugal atomizing disc with a rotation speed of 5000rpm.

[0096] B3. Drying and Atmosphere Control: The drying process is carried out in a nitrogen atmosphere with a purity of 99.8%, a nitrogen flow rate of 0.1 L / min, and an oxygen content of 1.8 vol at the outlet of the drying equipment.

[0097] B4. Endpoint and Quality Control: The D50 of the obtained nuclear particles was determined to be 450 µm by laser particle size analyzer, and the moisture content was determined to be 2.3 wt% by drying at 105 °C to constant weight method.

[0098] C1. Gelatin layer solution: Type A gelatin is dissolved in water to form a gelatin solution with a mass fraction of 0.1 wt%. The pH value is adjusted to 3.0 using citric acid under stirring. The isoelectric point of the gelatin in this embodiment is 6.8.

[0099] C2. Sodium alginate layer solution: Sodium alginate was dissolved in water to form a sodium alginate solution with a mass fraction of 0.1 wt%. The pH value was adjusted to 6.0 using sodium citrate dihydrate under stirring conditions.

[0100] C3. Layer-by-Layer Assembly: The core particles obtained in step B4 are sequentially contacted with the gelatin solution and sodium alginate solution of this embodiment for four double-layer cycles, using an immersion method with a liquid-to-solid mass ratio of 20:1. The total contact time for each double-layer cycle is 10 minutes. In each double-layer cycle, the core particles are first immersed in the gelatin solution for 5 minutes, then separated by centrifugation at 2000 rpm for 5 minutes, then immersed in the sodium alginate solution for 5 minutes, and centrifuged again. No washing is performed after each double-layer cycle. The process is confirmed by sampling and detecting changes in surface potential. After all double-layer cycles, the shell layer of this embodiment is formed.

[0101] C4. Post-processing and quality control: The assembled particles are dried to obtain multi-layer core-shell particles. In this embodiment, the moisture content of the multi-layer core-shell particles is 2.5 wt% as determined by constant weight method after drying at 105°C. The water activity aw is 0.19 as determined by water activity meter at 25°C. Based on the dry basis mass of the core particles before assembly, the mass gain of the shell is 12 wt%.

[0102] S3. Preparation of liquid phase: 3.5g of L-α-glycine phosphate was dissolved in 70.43g of water. Under conditions of 20℃ and 200rpm, 25g of D-sorbitol, 0.4g of citric acid, 0.5g of sodium citrate dihydrate, 0.05g of xanthan gum, 0.05g of potassium sorbate, 0.01g of sucralose and 0.01g of vanillin were added sequentially and stirred for 10min to obtain a homogeneous liquid phase. The pH value of the liquid phase in this example was 4.5.

[0103] S4. Mixing: Under a nitrogen atmosphere, the multilayer core-shell particles obtained in step S2 and the liquid phase obtained in step S3 are mixed at a temperature of 20°C and a stirring speed of 50 rpm for 1 min to obtain the composition of this embodiment.

[0104] Stability test: The multilayer core-shell particles obtained in step S2 were placed in a constant temperature and humidity chamber at 23°C and 70% relative humidity for 7 days. The sample was placed in an open weighing dish. The dry basis mass m0 was measured before placement and the dry basis mass m1 was measured after 7 days. The dry basis mass was determined by drying at 105°C to constant weight. The constant weight criterion was that the difference between two adjacent weighings was no more than 0.5 mg. The mass gain calculated based on the dry basis mass of the sample before placement was 2.8 wt%.

[0105] Preparation of dual-chamber packaging formulations: In this embodiment, the liquid phase is used as the contents of the liquid cavity, and the multilayer core-shell particles are used as the contents of the dry cavity. A high-barrier composite packaging film comprising a polyethylene terephthalate layer, an aluminum layer, and a polyethylene layer is used to prepare a dual-cavity packaged formulation, with a total mass of 5g per portion. A ruptureable seal is provided between the liquid cavity and the dry cavity. In this embodiment, the ruptureable seal is formed by heat sealing at a temperature of 135°C, a pressure of 0.3MPa, and a time of 0.8s.

[0106] Features of Example 3: This embodiment employs a combination design of process parameter range boundaries. The scheme uses a mixture of β-cyclodextrin and γ-cyclodextrin, with layer-by-layer assembly without washing, offering flexible and diverse process conditions. This embodiment is suitable for production scenarios with special requirements for process windows and can be used as a small-sized, portable functional beverage, suitable for travel and single-use consumption. Example 4

[0107] This embodiment prepares 100g of a composition containing choline glyphosate.

[0108] S1. Preparation of inclusion core: A1. Raw material preparation: Weigh 0.003g of disodium pyrroloquinoline quinone, 0.012g of β-cyclodextrin and water. The mass ratio of cyclodextrin to disodium pyrroloquinoline quinone is 4:1.

[0109] A2. Inclusion: 0.012 g of β-cyclodextrin was dissolved in 0.8 mL of water to obtain a cyclodextrin solution with a mass concentration of 15 mg / mL. 0.003 g of disodium pyrroloquinolinequinone was dissolved in 0.6 mL of water to obtain a disodium pyrroloquinolinequinone solution with a mass concentration of 5 mg / mL. Under light-protected conditions, the disodium pyrroloquinolinequinone solution of this embodiment was added to the cyclodextrin solution of this embodiment, with a mass ratio of cyclodextrin to disodium pyrroloquinolinequinone of 4:1. The temperature was controlled at 60°C and the mixture was stirred at 200 rpm for 1 h. The total solid content of the mixture was 10.7 mg / mL, thus forming an inclusion system.

[0110] A3. Curing: The inclusion system of this embodiment is allowed to stand at 25°C for 2 hours and then spray-dried. The inlet air temperature of the spray dryer is 150°C and the outlet air temperature is 80°C. The outlet air temperature is stabilized at 80°C by controlling the feed rate.

[0111] A4. Endpoint and quality control: The water content of the obtained inclusion nuclei was 2.9 wt%, and the water activity aw measured at 25℃ was 0.24.

[0112] S2. Preparation of multilayer core-shell particles: B1. Raw material preparation: 0.015g of inclusion core, 0.0216g of maltodextrin and 0.0108g of gum arabic were mixed. The dry weight ratio of maltodextrin to gum arabic was 2:1. Based on the total dry weight of inclusion core, maltodextrin and gum arabic, the mass fraction of inclusion core was 31.6wt%.

[0113] B2. Granulation: The mixture obtained in step B1 is added to water to form a liquid with a solid content of 30wt%. Core particles are obtained by spray granulation. The inlet air temperature of spray granulation is 120℃, the outlet air temperature is 60℃, and the atomization pressure is 0.2MPa. The outlet air temperature is stabilized at 60℃ by controlling the feed rate.

[0114] B3. Drying and Atmosphere Control: The drying process is carried out in a nitrogen atmosphere with a purity of 99%, a nitrogen flow rate of 10 L / min, and an oxygen content of 2.0 vol at the outlet of the drying equipment.

[0115] B4. Endpoint and Quality Control: The D50 of the obtained nuclear particles was determined to be 800 µm by laser particle size analyzer, and the moisture content was determined to be 2.9 wt% by drying at 105 °C to constant weight method.

[0116] C1. Gelatin layer solution: Type A gelatin is dissolved in water to form a gelatin solution with a mass fraction of 2.0 wt%. The pH value is adjusted to 4.5 using citric acid under stirring. The isoelectric point of the gelatin in this embodiment is 6.0.

[0117] C2. Sodium alginate layer solution: Sodium alginate was dissolved in water to form a sodium alginate solution with a mass fraction of 1.5 wt%. The pH value was adjusted to 7.5 using sodium citrate dihydrate under stirring conditions.

[0118] C3. Layer-by-Layer Assembly: The core particles obtained in step B4 are sequentially contacted with the gelatin solution and sodium alginate solution of this embodiment for three double-layer cycles, using an immersion method with a liquid-to-solid mass ratio of 5:1. The total contact time for each double-layer cycle is 30 minutes. In each double-layer cycle, the core particles are first immersed in the gelatin solution for 15 minutes, then separated by centrifugation at 5000 rpm for 15 minutes, then immersed in the sodium alginate solution for 15 minutes, and centrifuged again. After each double-layer cycle, the particles are washed once with deionized water. The process is confirmed by weight gain, and the shell layer of this embodiment is formed after all double-layer cycles.

[0119] C4. Post-processing and quality control: The assembled particles are dried to obtain multi-layer core-shell particles. In this embodiment, the moisture content of the multi-layer core-shell particles is 2.6 wt% as determined by constant weight method after drying at 105°C. The water activity aw is 0.21 as determined by water activity meter at 25°C. Based on the dry basis mass of the core particles before assembly, the mass gain of the shell is 10 wt%.

[0120] S3. Preparation of liquid phase: 4.0 g of L-α-glycine phosphate was dissolved in 89.79 g of water. Under conditions of 30°C and stirring speed of 800 rpm, 5 g of D-sorbitol, 0.45 g of citric acid, 0.1 g of sodium citrate dihydrate, 0.5 g of xanthan gum, 0.05 g of potassium sorbate, 0.01 g of sucralose, and 0.05 g of S-configuration limonene were added sequentially and stirred for 60 min to obtain a homogeneous liquid phase. The pH value of the liquid phase in this example was 3.5.

[0121] S4. Mixing: Under a nitrogen atmosphere, the multilayer core-shell particles obtained in step S2 and the liquid phase obtained in step S3 are mixed at a temperature of 30°C and a stirring speed of 300 rpm for 10 min to obtain the composition of this embodiment.

[0122] Stability test: The multilayer core-shell particles obtained in step S2 were placed in a constant temperature and humidity chamber at 27°C and 80% relative humidity for 7 days. The sample was placed in an open weighing dish. The dry basis mass m0 was measured before placement and the dry basis mass m1 was measured after 7 days. The dry basis mass was determined by drying at 105°C to constant weight. The constant weight criterion was that the difference between two adjacent weighings was no more than 0.5 mg. The mass gain calculated based on the dry basis mass of the sample before placement was 4.8 wt%.

[0123] Preparation of dual-chamber packaging formulations: In this embodiment, the liquid phase is used as the contents of the liquid cavity, and the multilayer core-shell particles are used as the contents of the dry cavity. A high-barrier composite packaging film comprising a polyethylene terephthalate layer, an aluminum layer, and a polyethylene layer is used to prepare a dual-cavity packaged formulation, with a total mass of 10g per portion. A ruptureable seal is provided between the liquid cavity and the dry cavity. In this embodiment, the ruptureable seal is formed by heat sealing at a temperature of 155°C, a pressure of 0.5MPa, and a time of 1.5s.

[0124] Features of Example 4: The process conditions in this embodiment are comprehensively optimized, resulting in good product stability. It is suitable for markets with high requirements for product quality and stability and can be used as a high-end functional beverage product, suitable for consumers who need long-term continuous use and pursue product quality.

[0125] Comparative Example 1: It is basically the same as Example 1, except that the inclusion temperature in step A2 is changed from 40°C to 65°C, and the inclusion system is formed by stirring at 500 rpm for 2.5 h at 65°C. Other conditions remain unchanged.

[0126] Comparative Example 2: It is basically the same as Example 1, except that freeze drying is not performed in step A3. Instead, spray drying is performed after standing at 20°C for 8 hours. The inlet air temperature of spray drying is 180°C and the outlet air temperature is 90°C. The outlet air temperature is stabilized at 90°C by controlling the feed rate. Other conditions remain unchanged.

[0127] Comparative Example 3: It is basically the same as Example 1, except that the drying process in step B3 is not carried out in a nitrogen atmosphere, but in an air atmosphere, with an air flow rate of 5L / min and an oxygen content of 20.9 vol% at the outlet of the drying equipment. Other conditions remain unchanged.

[0128] Comparative Example 4: It is basically the same as Example 1, except that in step C3, the layer-by-layer assembly of gelatin solution and sodium alginate solution is only carried out in one double-layer cycle. The total contact time of each double-layer cycle is still 20 min, gelatin soaking for 10 min, sodium alginate soaking for 10 min, separation method and washing method are the same as in Example 1, and other conditions remain unchanged.

[0129] Comparative Example 5: It is basically the same as Example 1, except that the liquid-solid mass ratio when the layer-by-layer assembly is carried out by immersion in step C3 is changed from 10:1 to 3:1, the total contact time of each double-layer cycle is still 20 min, the number of double-layer cycles is still 2, and other conditions remain unchanged.

[0130] Comparative Example 6: It is basically the same as Example 1, except that the pH value of the liquid phase in step S3 is adjusted from 4.0 to 3.0. Specifically, the amount of citric acid is changed from 0.2g to 0.45g, and the amount of sodium citrate dihydrate is changed from 0.3g to 0.05g. The amounts and conditions of other components remain unchanged.

[0131] Comparative Example 7: It is basically the same as Example 1, except that the stirring speed when mixing the multilayer core-shell particles with the liquid phase in step S4 is changed from 150 rpm to 350 rpm, the mixing temperature is still 25°C, the stirring time is still 5 min, and other conditions remain unchanged.

[0132] Comparative Example 8: Essentially the same as Example 1, except that in steps A1 and A2, 0.002 g of β-cyclodextrin was replaced with 0.002 g of maltodextrin. After stirring at 500 rpm for 2.5 h at 40°C, it was dried and quality-controlled according to steps A3 and A4 of Example 1. The resulting control dry material was used as the core material in subsequent steps, with other conditions remaining unchanged. This comparative example was used to verify the synergistic effect of β-cyclodextrin inclusion complexation and multilayer shell construction.

[0133] Comparative Example 9: Essentially the same as Example 1, except that steps C1 to C4 are omitted, and the gelatin and sodium alginate layer-by-layer assembly is not performed. Instead, the core particles obtained in step B4 are directly mixed with the liquid phase obtained in step S3 in step S4, with other conditions remaining unchanged. This comparative example is used to verify the synergistic effect of the encapsulated core and the layer-by-layer assembled shell.

[0134] Comparative Example 10: Essentially the same as Example 1, except that the two-phase storage and dual-cavity packaging were omitted. The composition obtained in step S4 was directly filled into a single-cavity package for storage. The total mass of a single package remained 7g. The packaging material was still a high-barrier composite film composed of a polyethylene terephthalate layer, an aluminum layer, and a polyethylene layer, but the liquid cavity, dry cavity, and ruptureable seal were omitted. Other conditions remained unchanged. This comparative example was used to verify the synergistic effect of multilayer core-shell particles and the two-phase storage method.

[0135] Performance testing: Unless otherwise specified, when it comes to particulate indicators such as D50, moisture, water activity and high-humidity weight gain, the solid phase before mixing should be measured for two-phase or two-cavity samples; the corresponding core particles should be measured for control samples with shell assembly omitted; and the recovered particulate portion should be measured for single-cavity packaged control samples with two-phase storage omitted.

[0136] Moisture control experiment: Moisture control at each drying endpoint for inclusion cores, core particles, and multi-layered core-shell particles was confirmed by the loss on drying method. Samples were dried to constant weight at a specified temperature, and moisture content was calculated by weight loss. Triple samples were taken from each sample, weighed, and dried at 105℃, with intervals between weighings until the difference between two adjacent weighings did not exceed 0.5 mg. Critical conditions were 105℃ and n=3. Results were expressed as mass fractions and reported as mean ± standard deviation, referring to GB5009.3-2016.

[0137] Water activity stability test: The water activity stability of multilayer core-shell particles at 25°C was assessed using a water activity meter, focusing on whether it remained consistently below 0.25. The ratio of sample vapor pressure to pure water vapor pressure was measured under isothermal and sealed conditions. The sample was placed in the instrument's sample cup and equilibrated at 25°C until the continuous reading fluctuation did not exceed 0.003 before recording. Key conditions were 25°C and triplicate measurements. The mean ± standard deviation of the output aw was compared with the 0.25 limit, referring to GB5009.238-2016.

[0138] Particle size distribution experiment: The particle size distribution of the core particles obtained in step B4 and the multilayer core-shell particles obtained in step C4 were characterized by laser diffraction, focusing on whether D50 was within the target range and the particle size migration before and after coating. Dry or wet dispersion was used, with the shading controlled within the instrument's recommended range. Three consecutive tests were conducted, and D10, D50, D90, and the distribution curve were recorded. The key condition was repeating the experiment three times and outputting the volume distribution. The mean ± standard deviation was reported, and the differences before and after coating were compared, referring to GB / T19077-2024 and ISO13320:2020.

[0139] pH Measurement Experiment: The pH of the liquid phase and the final mixed composition was measured using the glass electrode method to confirm that the liquid phase pH was between 3.5 and 4.5 and to quantify the drift before and after mixing. After three-point calibration of the pH meter with standard buffer at 25°C, the pH of the liquid phase and the mixed sample were measured separately, in triplicate. Key conditions were 25°C, three-point calibration, and n=3. Report the mean pH ± standard deviation and provide the ΔpH before and after mixing, referring to GB / T9724-2007.

[0140] High-humidity storage experiment: The hygroscopic weight gain and structural integrity of multilayer core-shell particles under high-humidity storage were evaluated through a constant temperature and humidity stress test. Samples were placed in open weighing dishes and stored at 23–27℃ and 70–80%RH for 7 days. m0 and m1 were recorded, and the proportion of intact particles was calculated based on sieving or particle size retention rate. The key conditions were 7 days and n=3. The weight gain rate and integrity rate were calculated, and the environmental conditions were set according to GB / T2423.3-2016.

[0141] Storage activity retention experiment: The storage activity retention of disodium pyrroloquinoline quinone in the solid phase and L-α-glycine choline in the liquid phase was quantitatively compared with the initial and post-storage contents using chromatography, and the retention rates were calculated. An HPLC or UPLC method was established, and specificity, linearity, accuracy, and precision were validated according to ICHQ2(R2). Storage conditions were set at 25℃ / 60%RH and 40℃ / 75%RH, with time points of 0, 7, 15, and 30 days, in triplicate. The retention rate was calculated as Ct / C0 × 100%, referring to ICHQ1A(R2) and ICHQ2(R2).

[0142] Structural integrity and release performance experiments: The structural integrity and release performance of the disodium pyrroloquinoline quinone carried by the multilayered core-shell particles in the final composition and L-α-glycine choline in the liquid phase were jointly evaluated using a standardized static digestion model. Following the INFOGEST 2.0 program, oral, gastric, and intestinal environments were simulated sequentially at 37°C. Samples were taken at 0, 15, 30, 60, and 120 min, and the active release was quantified by HPLC. The key conditions were 37°C and n=3. Cumulative release curves were plotted and t50 was calculated according to the INFOGEST 2.0 consensus method.

[0143] To verify whether the structure of the system obtained in Example 1 is effective, we first analyzed it by combining crystal structure and molecular interaction information. Figure 1 The XRD patterns of Example 1 and Comparative Example 8 are shown. X-ray diffraction was used to characterize the crystal structure of the two samples, with a test range of 2θ5° to 40°. Figure 1 It is evident that Example 1 and Comparative Example 8 exhibit significant differences in the position, intensity, and shape of characteristic diffraction peaks. This indicates that Example 1 has undergone changes in the component bonding state and solid-state structure, and is not a simple superposition or mechanical mixing of the raw materials, but rather the formation of new structural features. These results demonstrate that the components in Example 1, after being composited, can form a relatively stable existence at the solid level, providing a foundation for subsequent encapsulation, protection, and delivery.

[0144] Based on this, we further verified the underlying reasons for this structural change from the perspective of intermolecular interactions. Figure 2 The images shown are the FTIR spectra of Example 1 and Comparative Example 8. Fourier transform infrared spectroscopy was used to characterize the interactions of functional groups in the samples, with a scanning range of 4000 cm⁻¹ to 600 cm⁻¹. Figure 2 It is evident that Example 1 and Comparative Example 8 exhibit differences in the position and intensity of absorption peaks in the hydroxyl, carbonyl, and fingerprint regions, reflecting alterations in hydrogen bonding and the local chemical environment within the samples. Combined with... Figure 1The results show that Example 1 is different from Comparative Example 8 not only in its macroscopic solid structure, but also in the formation of a relatively stable interaction network at the molecular level, thus proving that the construction of this system has a clear structural basis and good rationality.

[0145] After confirming that the system has a structural foundation, we further examine whether the interface construction is continuous and controllable during the layer-by-layer assembly process. Figure 3 The image shows the zeta potential staged interface construction trajectory diagrams for Examples 1, 4, and 9. Zeta potential analysis was used to characterize the surface charge changes of the samples at each stage: after the core particle, after the first gelatin layer, after the first sodium alginate layer, after the second gelatin layer, and after the second sodium alginate layer. The results show that Example 1 exhibits a relatively clear alternation of positive and negative potentials throughout the entire layer-by-layer assembly process, with a clear potential reversal pattern, indicating that gelatin and sodium alginate with opposite charges can be deposited sequentially on the particle surface, demonstrating a continuous and effective interface construction process. In contrast, Comparative Examples 4 and 9 exhibit insufficient potential reversal, unclear stage responses, or incomplete construction trajectories, indicating weaker surface deposition stability and difficulty in forming a complete and ordered multilayer interface. Therefore, Figure 3 This directly proves that the layer-by-layer assembly path adopted in Example 1 can achieve stable interface construction, which is an important prerequisite for forming a multi-layer shell structure.

[0146] Whether the interface construction is stable should ultimately be reflected in the particle forming quality and particle size uniformity. Figure 4 The laser particle size differential volume distribution maps for Examples 1, 4, and 9 are shown. Laser particle size analysis was used to characterize the particle size distribution of the samples, with a test particle size range of 30 μm to 1000 μm. Figure 4 As can be seen, the main peak of particle size distribution in Example 1 is clearly located and the distribution peaks are relatively concentrated. In contrast, Comparative Examples 4 and 9 show phenomena such as wider distribution, the appearance of shoulder peaks, or the coexistence of coarse and fine particles, indicating that their granulation process is not stable enough and the differences between particles are large. Example 1, on the other hand, can maintain good molding consistency and coating integrity, indicating that the stability of the layer-by-layer interface construction has been effectively transferred to the particle scale.

[0147] Figure 5 The cumulative volumetric particle size distribution maps for Examples 1, 4, and 9 are shown. Laser particle size analysis was used to characterize the cumulative particle size distribution behavior of the samples, and the distribution width was evaluated using D10, D50, and D90 parameters. Figure 5As can be seen, the cumulative distribution curve of Example 1 shows a more concentrated transition, a stable D50 position, and a narrower distribution range. Combined with the fact that the core particle D50 of Example 1 is approximately 200 μm, this indicates that its particle size is within a suitable range for formulation processing and dispersion. Simultaneously, the smaller D90-D10 span indicates that Example 1 has better repeatability and uniformity in particle size control. In contrast, the curve of the comparative sample shows a more pronounced tailing, suggesting a higher proportion of large particles or fine powder coexisting, which is detrimental to subsequent packaging, storage stability, and release consistency. Figure 4 and Figure 5 The evidence corroborates each other, demonstrating that Example 1, based on the successful interface construction, further achieved superior particle distribution characteristics, thereby ensuring the stability of the formulation morphology.

[0148] After verifying the structure formation and particle shaping, we further investigated its effect on improving the storage stability of active substances. Figure 6 The HPLC retention rates of PQQ in Examples 1 and 10 are shown in the figure. The retention rates of PQQ in the samples after storage for 0, 7, 15, and 30 days were determined using high-performance liquid chromatography (HPLC). The results show that Example 1 maintained a high and relatively stable PQQ retention rate throughout the entire storage period, while Comparative Example 10 showed a more significant decreasing trend with prolonged storage time. This indicates that the multilayer structure and storage method of Example 1 can effectively weaken the influence of the external environment on PQQ and improve its storage stability. PQQ is sensitive to oxygen, moisture, and interfacial environment; therefore, these results further demonstrate the effectiveness of the structural design from the perspective of functional retention.

[0149] Figure 7 The HPLC retention rates of L-α-GPC in Examples 1 and 10 are shown in the figure. The retention rates of L-α-GPC in the samples after storage for 0, 7, 15, and 30 days were determined using high-performance liquid chromatography. Figure 7 As can be seen, Example 1 exhibited a high L-α-GPC retention level at all time points, with a significantly smaller attenuation rate than Comparative Example 10, indicating that this system can not only protect PQQ but also provide stabilization for L-α-GPC. Combined with... Figure 6 As can be seen, Example 1 showed good synergistic protection for both types of active ingredients, indicating that the system does not only work against a single ingredient, but has general advantages in overall microenvironment regulation, interface isolation and storage adaptability, thus more strongly proving the effectiveness of this solution.

[0150] After confirming the activity retention effect, it is necessary to further examine its release behavior under simulated digestion conditions to verify whether the system can balance storage protection and release during use. Figure 8The INFOKE release curves for Example 1, Comparative Example 9, and Comparative Example 10 are shown in the cumulative PQQ release diagrams. The cumulative PQQ release behavior of the samples under 0 min, 15 min, 30 min, 60 min, and 120 min conditions was characterized using an INFOKE simulated digestion system. The results show that the release curve of Example 1 is generally flatter and has clearer stage characteristics, indicating that PQQ is not released instantaneously in the digestion environment, but rather undergoes a gradual process from outer layer response to internal release. Comparative Example 9 shows a relatively rapid release in the early stage, suggesting a weak interfacial barrier that is difficult to effectively protect the active ingredient; Comparative Example 10 shows a relatively slow overall release, indicating insufficient release drive, which is not conducive to subsequent utilization. In contrast, Example 1 can suppress excessively rapid release in the early stage and achieve sustained release in the later stage, reflecting a good balance between activity protection and digestion release, indicating that the multilayer interfacial structure not only has a storage stabilization function but also reasonable delivery adaptability.

[0151] In addition to the structural and performance data mentioned above, the macroscopic appearance of the sample can also reflect its preparation quality and storage suitability. Figure 9 This is a macroscopic optical photograph of the multilayer core-shell particle from Example 1. Figure 9 As can be seen, the sample has an overall appearance of light yellow to beige granular powder with diffuse reflection on the surface. No obvious agglomeration, collapse, or macroscopic cracks were observed, indicating that the particles maintained good independence and appearance integrity after drying. Combined with the sample's moisture content of 2.2 wt% and a water activity (aw) of 0.18 at 25°C, it can be concluded that Example 1 is in a low free water state, with a low content of migrateable water in the system. This helps reduce the risk of moisture absorption, adhesion, and reactive degradation, thus demonstrating good drying stability and repackaging adaptability.

[0152] Figure 10 This is a photograph of the actual product of the dual-chamber packaging formulation from Example 1. Figure 10 As can be seen, the overall appearance of the formulation is neat and complete, the packaging outline is clear, the sealing edge is straight, and the cavity is clearly separated, with the liquid cavity and dry cavity independently distributed. The contents of the liquid cavity are light yellow to nearly colorless transparent liquids, the system is homogeneous, has a certain degree of fluidity, and no obvious precipitation, crystallization, stratification, or bubble aggregation is observed. The contents of the dry cavity are light yellow to beige granular solids, with good particle dispersion and relatively uniform particle size, and no obvious moisture absorption, clumping, collapse, or adhesion is observed. Combined with the multi-layer core-shell particle moisture content of 2.2wt%, water activity aw of 0.18, and core particle D50 of approximately 200μm, it can be concluded that this dual-cavity packaged formulation not only has good macroscopic appearance stability but also ensures that the two phase contents maintain their respective suitable states, further demonstrating the adaptability of the formulation in terms of storage, transportation, and separate preservation before use. Figure 9 and Figure 10Together, they demonstrate that Example 1 is not only reasonable in terms of microstructure, but has also translated into observable advantages in the appearance of the formulation.

[0153] After observing a good appearance at the macroscopic level, the microscopic morphology, shell continuity, and core-shell structure of the particles were further verified using an electron microscope. Figure 11 This is a scanning electron microscope image of the multilayer core-shell particles in Example 1. Figure 11 Image a is a low-magnification scanning electron microscope image of the multilayer core-shell particles in Example 1. It can be seen that the particles are relatively well distributed over a large area, and the overall shape is mainly near-spherical to sub-spherical. Only slight aggregation is seen in some areas, and no large-area breakage or obvious exposed areas are seen. This indicates that the core particles obtained by spray granulation still maintain a good overall morphology after subsequent layer-by-layer assembly. Figure 11 b is a medium-magnification scanning electron microscope image of the multilayer core-shell particles in Example 1. It can be seen that the particle outline is clear, the surface layer continuously covers the outside of the core particles, and the boundaries between particles are clear. This indicates that after two double-layer cycles of gelatin and sodium alginate treatment, a relatively stable composite shell has been formed on the outer surface of the particles, which can cover the core relatively completely. Figure 11 c is a high-magnification scanning electron microscope image of the multilayer core-shell particles in Example 1. Slight wrinkles and shallow depressions are visible on the particle surface, but no through cracks are found overall. This indicates that although there is a shrinkage characteristic caused by the surface solidifying first and the interior continuing to lose water during the spray drying and subsequent drying processes, the shell layer remains continuous and no obvious cracks occur. Figure 11 Image d is a cross-sectional scanning electron microscope image of the multilayer core-shell particles from Example 1. It shows a relatively continuous shell region at the outer edge of the particles, which is tightly bound to the internal matrix. Based on an estimated shell mass gain of approximately 5 wt%, the dry shell thickness is in the micrometer range, indicating that the sample has formed a thin and continuous core-shell structure. Figure 11 Multiple levels of evidence, from appearance and surface to cross-section, have demonstrated that Example 1 has indeed obtained multi-layered core-shell particles with complete structure and continuous coating.

[0154] To further reveal the internal structure and interface details of the particles, transmission electron microscopy was used for supplementary characterization. Figure 12 This is a transmission electron microscope image of the multilayer core-shell particles in Example 1. Figure 12 Image a is a bright-field transmission electron microscope image of the multilayer core-shell particles of Example 1. It can be seen that the particle slices are solid or quasi-solid structures with continuous shell regions on the outside. The core occupies the main volume fraction, indicating that the sample is not a hollow microsphere, but a multilayer core-shell particle with core particles as the main body and a composite outer shell. Figure 12 b is a magnified transmission electron microscope image of the multilayer core-shell particles in Example 1. It can be seen that the core-shell interface has a continuous transition feature, and no obvious delamination or large-scale voids are observed. This indicates that the gelatin layer and the sodium alginate layer form a relatively tight composite interface on the particle surface, which is beneficial to improving the coating stability and reducing the leakage of active ingredients. Figure 12 c is a high-resolution transmission electron microscope image of the multilayer core-shell particles in Example 1. The absence of large-scale, clear, and continuous lattice fringes indicates that the sample is predominantly composed of an amorphous or low-crystallinity organic matrix. This result is consistent with... Figure 1 The changes in crystal structure within the system correspond to each other and are consistent with the organic complex characteristics of the system, which is composed of maltodextrin, gum arabic, gelatin, sodium alginate, and inclusion core. Figure 12 Image d shows the selected area electron diffraction pattern of the multilayer core-shell particles in Example 1. The diffraction characteristics are mainly diffuse halos, with no obvious regular diffraction spots, further indicating that the overall crystallinity of the sample is low. Combined with... Figure 11 and Figure 12 It can be confirmed that Example 1 forms a multi-layered core-shell structure with continuous interface, complete shell, and tight internal bonding. Its performance advantage mainly comes from the interface protection effect formed by the enclosing core and the multi-layered shell. This structural feature is also consistent with the aforementioned results of improved storage stability and optimized release behavior.

[0155] In summary, by Figures 1 to 12 A relatively complete chain of evidence can be formed: First, XRD and FTIR results demonstrate that Example 1 differs from the comparative example in both solid-state structure and molecular interaction; second, zeta potential and particle size distribution results prove that its layer-by-layer interface construction process is stable and the particle formation is uniform; third, HPLC retention rate and INFogest release results indicate that this structure can simultaneously improve activity retention and achieve more reasonable release behavior; finally, macroscopic photographs, scanning electron microscopy, and transmission electron microscopy results further verify the actual construction state of the multilayer core-shell particles and the dual-cavity formulation from macroscopic to microscopic perspectives. All of the above results collectively demonstrate that the structural design and preparation route adopted in Example 1 have good effectiveness and rationality.

[0156] Table 1. Performance comparison data between the examples and comparative examples.

[0157] As can be seen from the performance of the examples and comparative examples in Table 1, Examples 1-4 maintained high PQQ and L-α-GPC retention rates and high particle integrity rates under low moisture and low water activity conditions, indicating that the combined design of inclusion core, layer-by-layer assembled shell, and two-phase storage can simultaneously stabilize the activity of the solid and liquid phases. Comparative Examples 1-3 show that after the inclusion and inert atmosphere-related processes were weakened, storage stability and activity retention rates decreased simultaneously. Although Comparative Examples 4, 5, and 9 showed local increases in release rates, they were accompanied by a significant deterioration in integrity rate and high humidity stability, indicating that simply weakening the shell constraint cannot achieve a balance between structural integrity and release performance. Comparative Example 10 further shows that after eliminating the two-phase storage, water activity, weight gain, and dual-activity retention rates all deteriorated significantly. Overall, the data from the examples conform to the material logic of synergistic improvement of composition, structure, and performance.

[0158] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and not to limit it. Although the present invention has been described in detail with reference to the above embodiments, those skilled in the art should understand that any equivalent structural transformations made under the concept of the present invention and using the contents of the specification and drawings of the present invention should be covered within the scope of protection of the claims of the present invention.

Claims

1. A composition comprising glycerylphosphocholine, characterized in that, The composition is an oral composition and contains at least the following components: water, L-α-glucosidylcholine, D-sorbitol, citric acid, sodium citrate dihydrate, xanthan gum, potassium sorbate, sucralose, and multilayered core-shell particles; The multilayer core-shell particles comprise an inclusion core formed by disodium pyrroloquinoline quinone and cyclodextrin, core particles containing the inclusion core, and a shell layer formed by layering gelatin and sodium alginate on the surface of the core particles; based on the total mass of the composition, the proportion of L-α-glycine choline is 1.5-5.5 wt%, and the proportion of disodium pyrroloquinoline quinone is 0.001-0.004 wt%.

2. The composition of claim 1, wherein, The inclusion core is prepared by the following steps: A1. Raw material preparation: Provide disodium salt of pyrroloquinoline quinone, cyclodextrin and water, wherein the mass ratio of cyclodextrin to disodium salt of pyrroloquinoline quinone is 2:1-6:1; A2. Inclusion: Cyclodextrin is dissolved in water to obtain a cyclodextrin solution with a mass concentration of 5-20 mg / mL, and disodium pyrroloquinoline quinone is dissolved in water to obtain a disodium pyrroloquinoline quinone solution with a mass concentration of 1-10 mg / mL. The disodium pyrroloquinoline quinone solution is added to the cyclodextrin solution, and the mass ratio of cyclodextrin to disodium pyrroloquinoline quinone is 2:1-6:

1. The temperature is controlled at 25-60℃ and the mixture is stirred at 200-800 rpm for 1-4 hours to form an inclusion system. A3. Curing: The inclusion system is allowed to stand at 15-25℃ for 2-12 hours and then dried by freeze drying or spray drying. The pre-freezing temperature for freeze drying is -40℃ to -20℃, the pre-freezing time is 2-6 hours, and the vacuum degree during the sublimation stage is 10-50 Pa. The inlet air temperature for spray drying is 150-200℃, and the outlet air temperature is 80-100℃. A4. Endpoint and quality control: The water content of the obtained inclusion nuclei is not greater than 3 wt%, and the water activity aw measured at 25℃ is not greater than 0.

25.

3. The composition of claim 1, wherein, The core particles in the multi-layered core-shell particles are prepared by the following steps: B1. Raw material preparation: The inclusion core is mixed with maltodextrin and gum arabic, wherein the dry weight ratio of maltodextrin to gum arabic is 1:10 to 10:1, and the mass fraction of the inclusion core is 5-40 wt%, based on the total dry weight of the inclusion core, maltodextrin, and gum arabic. B2. Granulation: Add water to the mixture obtained in step B1 to form a liquid with a solid content of 20-45 wt%. Obtain core particles by spray granulation or fluidized bed granulation. The inlet air temperature for spray granulation is 120-180℃, the outlet air temperature is 60-80℃, and the atomization pressure is 0.2-0.6 MPa. The bed temperature for fluidized bed granulation is 45-70℃, and the rotation speed of the atomizing device is 5000-15000 rpm. B3. Drying and Atmosphere Control: The drying process is carried out under an inert atmosphere, wherein the inert atmosphere is nitrogen with a purity of not less than 99%; B4. Endpoint and quality control: The D50 of the obtained nuclear particles is 200-800µm and the moisture content is no more than 3wt%.

4. The composition of claim 1, wherein, The shell is prepared and coated onto the surface of the core particle through the following steps: C1. Gelatin layer solution: Dissolve gelatin in water to form a gelatin solution with a mass fraction of 0.1-2.0 wt%, and adjust the pH value to 3.0-4.5 with citric acid under stirring. C2. Sodium alginate layer solution: Sodium alginate is dissolved in water to form a sodium alginate solution with a mass fraction of 0.1-1.5 wt%, and the pH value is adjusted to 6.0-7.5 using sodium citrate dihydrate under stirring conditions; C3. Layer-by-layer assembly: The core particles are sequentially contacted with the gelatin solution and the sodium alginate solution and subjected to 2-4 double-layer cycles. The total contact time for each double-layer cycle is 10-30 minutes. After each contact with the gelatin solution or the sodium alginate solution, a separation is performed. After all double-layer cycles, the shell layer is formed. C4. Post-processing and quality control: The assembled particles are dried to obtain multi-layered core-shell particles. The moisture content of the multi-layered core-shell particles is not greater than 3 wt%, the water activity aw measured at 25℃ is not greater than 0.25, and the weight gain of the shell layer is 5-18 wt% based on the dry basis weight of the core particles before assembly.

5. The composition of claim 1, wherein, The composition is a biphase composition comprising a liquid phase and a solid phase; the liquid phase comprises water, L-α-glycine choline, D-sorbitol, citric acid, sodium citrate dihydrate, xanthan gum, potassium sorbate, and sucralose; the solid phase is a multilayered core-shell particle, and the water content of the solid phase before mixing with the liquid phase is no more than 3 wt%; based on the total mass of the composition, the proportion of D-sorbitol is 5-35 wt%, the pH value of the liquid phase is 3.5-4.5, and the mass fraction of xanthan gum is 0.05-0.50 wt%; the liquid phase also comprises at least one of vanillin and S-configuration limonene, with a total mass fraction of 0.0005-0.05 wt% based on the total mass of the composition.

6. The method for preparing the composition according to claim 1, characterized in that, Includes the following steps: S1. Preparation of inclusion core: Prepare inclusion core according to steps A1 to A4; S2. Preparation of multi-layered core-shell particles: Using the encapsulated core as the core material, multi-layered core-shell particles are prepared according to steps B1 to B4 and steps C1 to C4; S3. Preparation of liquid phase: Dissolve L-α-glycine choline in water, and add D-sorbitol, citric acid, sodium citrate dihydrate, xanthan gum, potassium sorbate and sucralose in sequence. Mix well under stirring to obtain the liquid phase. S4. The multilayer core-shell particles obtained in step S2 are mixed with the liquid phase obtained in step S3 under stirring conditions to obtain the composition.

7. The preparation method according to claim 6, characterized in that, The multilayer core-shell particles obtained in step S2 are placed at a temperature of 23-27℃ and a relative humidity of 70-80% for 7 days. The weight gain calculated based on the dry basis weight of the sample before placement is no more than 5wt%. The mixing operation in step S4 is carried out under an inert atmosphere, namely nitrogen.

8. The composition according to claim 1, characterized in that, The composition is formulated into a dual-cavity packaging formulation comprising a liquid cavity content and a dry cavity content. The liquid cavity content is the liquid phase of the composition and includes water, L-α-glycine choline, D-sorbitol, citric acid, sodium citrate dihydrate, xanthan gum, potassium sorbate, sucralose, and vanillin and / or S-configuration limonene. The dry cavity content consists of multilayered core-shell particles, which are connected and mixed with the liquid cavity during use. The dual-cavity packaging formulation is made of a high-barrier composite packaging film comprising a polyethylene terephthalate layer, an aluminum layer, and a polyethylene layer, and the total mass of a single serving of the dual-cavity packaging formulation is 5-10 g.

9. The composition according to claim 8, characterized in that, A ruptureable seal is provided between the liquid chamber and the dry chamber. The ruptureable seal is formed by heat sealing under conditions of 135-155℃, 0.3-0.5MPa, and 0.8-1.5s.

10. The use of the composition comprising glyphosate choline according to any one of claims 1-5, 8 or 9 in the preparation of a food for improving memory.

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