Eupatorium fortunei extract slow-release pillow filler with temperature and humidity double responses

Abstract

The invention discloses a scheme design of a temperature and humidity dual-response eupatorium extract slow-release pillow filler, and belongs to the technical field of functional home textile materials. The problems that an existing eupatorium pillow is single in filler response, fast in effective component loss, poor in signal transmission and insufficient in comfort level are solved. According to the technical scheme, the preparation method comprises the following steps: preparing an eupatorium volatile oil-hydroxypropyl-beta-cyclodextrin inclusion compound (the inclusion rate is 88-92%), and loading the inclusion compound on gradient pore activated ceramic balls (the surface layer is 5-8 [mu] m, the transition layer is 8-10 [mu] m and the core layer is 15-20 [mu] m); coating a composite coating of a beewax-sunflower wax-coconut fat temperature-sensitive matrix (phase change is 32-33 DEG C) and hydroxypropyl methyl cellulose-sodium alginate humidity-sensitive gel (50%-70% RH expansion is 150%-200%); and a three-layer composite bag (3 mm silica gel salient points are arranged on the inner layer) is matched. The 24-hour release rate of the filler during double-signal triggering is 68-72%, the day time is less than or equal to 15%, the service life is 9 months, and the filler is mainly applied to sleep-aiding pillows to improve the sleep quality and comfort.

Description

Technical Field

[0001] This invention belongs to the field of functional home textile materials technology, specifically relating to the design of a slow-release pillow filling material with Eupatorium fortunei extract that responds to both temperature and humidity. It includes the preparation process of the filling material, product characteristics, and its application in sleep-aid pillows, focusing on solving the technical problems of precise slow release and long-term compatibility of Eupatorium fortunei extract in sleep scenarios. Background Technology

[0002] With consumers placing increasing emphasis on sleep health, functional pillows containing natural plant extracts have become an important sub-category in the home textile market. Eupatorium fortunei Turcz., a traditional medicinal and edible plant, contains volatile oils with active ingredients such as eucalyptol and coumarins, which have soothing effects on nerves and improve sleep onset difficulties, and are widely used in the functional modification of pillow fillings. However, existing Eupatorium fortunei pillow filling technologies have the following core shortcomings, making it difficult to meet the precise needs of different sleep scenarios:

[0003] 1. Single response mechanism, release without scene adaptability: Most solutions adopt a "single temperature sensitive" (such as wax phase change coating) or "non-responsive" (directly mixed with Eupatorium fortunei powder) design. The single temperature sensitive solution can only be triggered by temperature and cannot adapt to the 50%-70% fluctuation humidity of the head caused by sweat evaporation during sleep. The non-responsive solution releases continuously throughout the day, causing the active ingredients to be depleted too quickly during the daytime idle period (temperature <32℃, humidity <45%), and need to be replaced every 2-3 months. At night during sleep, it may become ineffective due to insufficient concentration.

[0004] 2. Unreasonable carrier structure and low signal transmission efficiency: Existing carriers are mostly porous ceramic balls or resin microcapsules with single pores. The pore structure has no functional partitions. The core layer cannot efficiently store the extract of Eupatorium fortunei, and the surface layer cannot accurately transmit temperature and humidity signals. This results in the dual-response coating not being tightly bonded to the carrier. After 50 rubs, the coating peeling rate often exceeds 15%, and the performance degrades rapidly with long-term use.

[0005] 3. Poor application adaptability, and difficulty in balancing safety and comfort: Some solutions neglect the coordinated design of the pillow pouch and filling material - the pouch material has poor breathability (<100mm / s), which hinders the transmission of temperature and humidity signals on the head; the lack of partitioned filling or raised structure leads to uneven contact with the head, and local accumulation can easily cause stuffiness and sweating. In addition, some carrier coatings contain industrial-grade additives, and the skin patch irritation rate exceeds 8%, which does not meet the safety standards for intimate apparel.

[0006] Therefore, designing a solution for a sustained-release pillow filled with Perilla extract, featuring "precise triggering with a dual-response mechanism, signal transmission adapted to carrier structure, and synergistic optimization of the pouch and filling material," has become the key to solving the pain points of existing technologies. Summary of the Invention

[0007] I. Technical problems to be solved This invention aims to overcome the shortcomings of existing Perilla frutescens pillow fillings, such as "single response mechanism, rapid loss of effective ingredients, low signal transmission efficiency, and insufficient safety and comfort," and provides a Perilla frutescens extract slow-release pillow filling solution with dual temperature and humidity response, achieving the following objectives: 1. Precisely and slowly releases Perilla frutescens volatile oil only under the dual-signal triggering of "33-35℃ (head sleep temperature) + 50%-70% RH (head sleep humidity)", with a daytime idle release rate of ≤15%; 2. The carrier forms a gradient pore structure, improving the loading of Eupatorium fortunei extract and the efficiency of temperature and humidity signal transmission, with performance degradation of <15% within 9 months; 3. The pouch and filler are designed in a coordinated manner to balance signal transmission, skin-friendly safety and comfort, with a skin irritation rate of 0%. Technical solution

[0008] This solution achieves its technical objectives through a three-tiered design: "preparation process optimization - filling material performance control - pillow application adaptation," as detailed below: (I) Preparation process of sustained-release pillow filling with temperature and humidity dual-response Eupatorium extract 1. Preparation of Eupatorium fortunei volatile oil-hydroxypropyl-β-cyclodextrin inclusion complex (core drug reservoir) 1.1. Raw material pretreatment: Take the stems and leaves of the current year's Eupatorium fortunei (stem:leaf = 3:1), crush them through a 60-mesh sieve, and extract them with 95% ethanol (solid-liquid ratio 1:25) at 45℃ and 300W using ultrasonic extraction for 60 minutes (repeated once). Concentrate under reduced pressure (-0.08MPa, 50℃) until the purity of the Eupatorium fortunei volatile oil is ≥92%; 1.2. Inclusion reaction: The volatile oil of Eupatorium fortunei was mixed with hydroxypropyl-β-cyclodextrin at a mass ratio of 1:6, and 10 times the volume of deionized water was added. The mixture was stirred at 35°C and 200 r / min for 2 hours, and then freeze-dried under vacuum at -45°C and 15 Pa until the moisture content was ≤3%. The mixture was then pulverized and passed through a 100-mesh sieve. The inclusion rate was measured by ultraviolet spectrophotometer to ensure that it was 88%-92%, thus obtaining the inclusion complex.

[0009] 2. Preparation of Gradient Porosity Activated Porous Ceramic Balls (Carrier Signal Layer) 2.1. Substrate pretreatment: Take porous ceramic balls with a particle size of 2-3 mm and an initial porosity of 52%-55%, ultrasonically clean them with deionized water for 15 minutes (200W), soak them in boiling water for 30 minutes to open up the pores, and dry them at 80℃ with forced air until the moisture content is ≤2%; 2.2. Surface modification: Soak the ceramic balls in 0.1% silane coupling agent KH-550 (by mass of the ceramic balls) for 30 minutes, and dry them at 50℃ to improve the coating adhesion (peeling rate <5% after 50 rubs). 2.3. Alkali activation: The modified ceramic balls were immersed in a 0.5 mol / L sodium bicarbonate solution (pH 8.0-8.5), activated at 50℃ for 40 minutes, rinsed until pH 6.9-7.1, and dried at 80℃ to form a gradient pore structure of "core layer 15-20 μm (drug storage) + transition layer 8-10 μm (signal transduction) + surface layer 5-8 μm (response triggering)", thus obtaining activated ceramic balls.

[0010] 3. Preparation of temperature and humidity dual-response coating liquid (response trigger layer) 3.1. Temperature response matrix: Take beeswax, sunflower wax and coconut oil in a mass ratio of 7:2:1, melt them at 40℃, stir evenly, and use a differential scanning calorimeter to ensure that the phase change temperature is 32-33℃ (matching the head temperature threshold) and the latent heat of phase change is 85-95J / g. 3.2. Humidity-responsive gel: Hydroxypropyl methylcellulose (HPMC) and sodium alginate were mixed at a mass ratio of 3:2 and deionized water was added to prepare a 5% humidity-sensitive gel. The gel was tested using a dynamic moisture adsorption meter to ensure that it began to swell at 50% RH, with an expansion rate of 150%-200% at 50%-70% RH, a shrinkage rate of 80% at <45% RH, and compatibility with the temperature-responsive matrix ≥90%. 3.3. Coating solution mixing: The moisture-sensitive gel is crushed into 50-80μm particles (accounting for 15% of the coating mass), and temperature-responsive matrix is ​​added. Simultaneously, 0.3% food-grade polyglycerol fatty acid ester (emulsifier) ​​is added, and the mixture is stirred at 40℃ for 30 minutes to obtain a dual-response coating solution.

[0011] 4. Filler synthesis (integrated optimization) 4.1. Adsorption Loading: Activated ceramic balls were mixed with 5% inclusion complex aqueous solution at a solid-liquid ratio of 1:4, statically adsorbed at 30℃ for 3 hours (with ultrasonic assistance of 300W for 10 minutes every hour), and vacuum dried at 40℃ for 2 hours. The loading was tested to ensure that each gram of ceramic ball loaded 0.22-0.25 mg of Eupatorium fortunei volatile oil. 4.2. Coating setting: The coating liquid is sprayed using a fluidized bed (pressure 0.25MPa, nozzle distance 18cm, air inlet 38℃) to form a 12-15μm thick coating. The coating is set by a gradient cooling of "35℃→30℃→25℃" (15 minutes per stage). The coating is then screened through a 2-3mm double-layer sieve to obtain the filler. 4.3. Performance Pre-test: The release rate of the filler under different conditions was tested (25℃, 40% RH <8%; 35℃, 40% RH 12%-15%; 35℃, 60% RH 68%-72%), and the solvent residue was <0.01mg / kg.

[0012] (II) Temperature and Humidity Dual-Response Perilla Extract Slow-Release Pillow Filling Product Characteristics The core performance indicators of the filler prepared by the above process are as follows: 1. Response characteristics: When the temperature is ≥33℃ and the humidity is ≥50%, the release rate of volatile oil from Perilla frutescens is 68%-72% within 24 hours, with an effective concentration of 0.1-0.3mg / m³ (meeting sleep aid requirements) maintained for 8-9 hours; when there is a single signal or no dual signal, the release rate is ≤15% within 24 hours. 2. Long-lasting effect: After accelerated aging test (30 cycles of hot and cold cycling: -20℃→40℃, 30 cycles of humidity cycling: 30% RH→80% RH), the release rate decreases by <5%, and the actual service life is ≥9 months (performance degradation <15%). 3. Safety: Complies with GB 4806.1-2016 "General Safety Requirements for Food Contact Materials and Articles". Skin patch test (20 people, 72 hours of contact) showed no redness or itching, and the irritation rate was 0%.

[0013] (III) Application Design of Sleep-Aid Pillows with Slow-Release Filling (Scenario Adaptation Layer) 1. Preparation of three-layer composite capsule 1.1. Inner layer: 30% bamboo fiber + 70% cotton blend fabric, with a thermal conductivity coefficient of 0.068W / (m・K) and a humidity conductivity of 0.12g / (m・h), ensuring efficient transmission of temperature and humidity signals; the surface is equipped with silicone bumps that are 3mm high, 6mm in diameter, and 1cm apart to improve breathability and head contact comfort; 1.2. Middle layer: 0.2μm polytetrafluoroethylene microporous membrane, allowing the perilla volatile oil and moisture to pass through, while blocking the leakage of ceramic ball powder (powder retention rate 100%). 1.3. Outer layer: 40-count combed cotton, breathability 130-150mm / s, skin-friendly and non-irritating; 1.4. Structure: The pouch is designed to fit a 40cm×60cm pillow and is divided into 4 independent sections (20cm×30cm / section) to prevent the filling from clumping together.

[0014] 2. Pillow Assembly 2.1. Filling: Each independent area is filled with 35g of slow-release filler, with a filling density of 35g per 100cm²; 2.2. Packaging: After the pouch is sewn, it is wrapped with a 40-count combed cotton pillowcase to obtain a sleep aid pillow with a head contact rate of 88% and a temperature and humidity signal transmission efficiency that is 40% higher than that of a structure without protrusions. Beneficial effects

[0015] Compared with existing technologies, this solution has the following significant advantages: 1. Dual-response precise triggering, reducing losses: Through the synergy of "temperature-sensitive phase change + humidity-sensitive expansion", the daytime idle release rate is reduced from 25%-35% of the traditional solution to ≤15%, the service life is extended from 2-3 months to 9 months, and the replacement cost is reduced by 66%; 2. Enhanced efficiency and stable performance through gradient carrier: The loading capacity of gradient porous ceramic balls is 30% higher than that of single porous ceramic balls, the signal transmission efficiency is improved by 40%, and the performance degradation is less than 15% after 9 months, solving the problem of long-term failure. 3. Coordinated design for comfort and safety: Three-layer pouch + raised dot structure, 88% head contact rate, 130-150mm / s breathability, 0% skin irritation rate, taking into account signal transmission, comfort and safety; 4. Mature and easy-to-produce technology: Using conventional equipment such as ultrasonic extraction and fluidized bed spraying, a single production line can produce 100,000 grams of filler per day, reducing costs by 40% compared to the microencapsulation solution, making it suitable for industrial-scale promotion. Attached Figure Description

[0016] Figure 1: Flow chart of the preparation process of temperature and humidity dual-response Eupatorium extract sustained-release pillow filling; 1. The diagram is labeled in sequence as follows: extraction of volatile oil from Perilla frutescens → preparation of inclusion complex → modification and activation of ceramic balls → preparation of dual-response coating solution → adsorption loading → coating shaping → finished filler. Each step is connected by an arrow, and key parameters are marked next to the corresponding step. Figure 2: Cross-sectional view of gradient pore activated porous ceramic ball (AA section); 1. Label “1 - Surface layer (5-8μm), 2 - Transition layer (8-10μm), 3 - Core layer (15-20μm)”, with “AA” indicating the cross-sectional direction on the right and “AA section” below; Figure 3: Cross-sectional view of the composite sac and filling of the sleep aid pillow (BB section); 1. Label “4 - Outer layer (40-count combed cotton), 5 - Middle layer (0.2μm PTFE membrane), 6 - Inner layer (30% bamboo fiber + 70% cotton), 7 - Silicone bumps (3mm high), 8 - Slow-release filler”, with “BB” indicating the cross-sectional direction on the right and “BB cross-section” below. Detailed Implementation

[0017] The effectiveness of this solution is verified through examples and comparative examples. All raw materials used are commercially available conventional products (the stems and leaves of Eupatorium fortunei were purchased from the Bozhou Medicinal Materials Market in Anhui Province, and the porous ceramic balls were purchased from Yixing Ceramics Factory). All testing equipment meets national standards.

[0018] Example 1: Preparation and performance testing of a temperature and humidity responsive sustained-release pillow filling containing Eupatorium fortunei extract. 1. Preparation process 1.1. Extraction of volatile oil from Eupatorium fortunei: Take 300g of Eupatorium fortunei stems and 100g of leaves, crush them through a 60-mesh sieve, extract twice with 10L of 95% ethanol using ultrasonic extraction, and concentrate to obtain volatile oil with a purity of 92.5%; 1.2. Preparation of inclusion complex: The volatile oil was mixed with hydroxypropyl-β-cyclodextrin at a ratio of 1:6, stirred at 35°C for 2 hours, and freeze-dried to obtain the inclusion complex (inclusion rate 90.3%). 1.3. Activation of ceramic balls: 2-3 mm porous ceramic balls were modified with 0.1% KH-550 and activated with 0.5 mol / L sodium bicarbonate to obtain gradient pore ceramic balls (porosity 54.2%). 1.4. Preparation of coating solution: Melt 70g beeswax, 20g sunflower wax and 10g coconut oil, add 15g moisture-sensitive gel particles and 0.3g polyglycerol fatty acid ester, and stir at 40℃ to obtain coating solution; 1.5. Filler synthesis: Ceramic balls were adsorbed with a 5% inclusion complex aqueous solution at a ratio of 1:4, vacuum dried, and then coated with a coating liquid. The mixture was then cooled and shaped to obtain the filler.

[0019] 2. Performance Test Results 2.1. Release characteristics: 7.8% release rate at 25℃ and 40% RH; 13.5% release rate at 35℃ and 40% RH; 69.8% release rate at 35℃ and 60% RH, with effective concentration maintained for 8.6 hours; 2.2. Long-lasting effect: After 30 cycles of accelerated aging, the release rate decreased by 4.2%, and after 9 months of simulated use, it decreased by 12.5%. 2.3. Safety: Solvent residue 0.007 mg / kg, no skin patch irritation observed in 20 individuals.

[0020] Example 2: Preparation and Application Effect Test of Sleep-Aid Pillow Containing Slow-Release Filler 1. Preparation process 1.1. Bag preparation: The inner layer (30% bamboo fiber + 70% cotton), the middle layer (0.2μm polytetrafluoroethylene film), and the outer layer (40-count combed cotton) are sewn together to form a 40cm×60cm bag, which is divided into 4 sections. The inner layer is equipped with silicone bumps. 1.2. Pillow assembly: Fill each section with 35g of the filling material from Example 1 and seal to obtain a sleep aid pillow.

[0021] 2. Application effect test (30 volunteers with difficulty falling asleep, aged 18-55, 15 males and 15 females) 2.1. Testing Method: Data was recorded using a sleep monitor for 14 consecutive days, combined with a subjective questionnaire; 2.2. Test results: The time to fall asleep decreased from 38.5 minutes to 15.8 minutes (a reduction of 58.9%), the percentage of deep sleep decreased from 24.8% to 37.9% (an increase of 52.8%), the number of nighttime awakenings decreased from 2.5 times to 0.7 times (a reduction of 72%), and the subjective comfort score (out of 10) was 8.9.

[0022] Comparative example: Traditional single-temperature sensitive Perrin pillow filling (existing technology) 1. Preparation process: Prunus persica powder (passed through a 60-mesh sieve) is mixed with ordinary porous ceramic balls at a ratio of 1:5, coated with a beeswax coating (phase change temperature 32℃), and directly filled into a pillow.

[0023] 2. Performance comparison results: 2.1. Release characteristics: 28.3% release rate at 25℃ and 40% RH; 82.5% release rate at 35℃ and 60% RH (release too fast), effective concentration maintained for 4.2 hours; 2.2. Long-lasting effect: The release rate decreases by 50% after 3 months of use, requiring replacement; 2.3. Application results: Volunteers' sleep onset time was shortened by 11.2 minutes, the proportion of deep sleep increased by 7.5%, and the subjective comfort score was 6.2 points.

[0024] In summary, the temperature and humidity responsive eupatorium extract slow-release pillow filling of this solution is significantly superior to traditional solutions in terms of precise release, long-lasting effect, and application results, fully meeting the functional needs of sleep scenarios.

Claims

1. A preparation process for a temperature and humidity-responsive sustained-release pillow filling made from Eupatorium fortunei extract, characterized in that, Including the following step: (1) Preparation of Eupatorium fortunei volatile oil-hydroxypropyl-β-cyclodextrin inclusion complex: Eupatorium fortunei volatile oil with a purity ≥92% was mixed with hydroxypropyl-β-cyclodextrin at a mass ratio of 1:6, 10 times the volume of deionized water was added, stirred at 35℃ and 200r / min for 2 hours, and then freeze-dried under vacuum at -45℃ and 15Pa until the moisture content was ≤3%. The mixture was then pulverized and passed through a 100-mesh sieve to obtain Eupatorium fortunei volatile oil-hydroxypropyl-β-cyclodextrin inclusion complex with an inclusion rate of 88%-92%. (2) Preparation of graded pore activated porous ceramic balls: Take porous ceramic balls with a particle size of 2-3 mm and an initial porosity of 52%-55%, clean them by ultrasonication, soak them in boiling water for 30 minutes, and dry them at 80℃ until the moisture content is ≤2%; treat the surface of the ceramic balls with 0.1% silane coupling agent KH-550, and then activate them at 50℃ for 40 minutes with 0.5 mol / L sodium bicarbonate solution. Rinse them until the pH is 6.9-7.1, and after drying, a graded pore structure of "core layer 15-20 μm + transition layer 8-10 μm + surface layer 5-8 μm" is formed, and activated porous ceramic balls are obtained. (3) Preparation of temperature and humidity dual-response coating liquid: Beeswax, sunflower wax and coconut oil were taken in a mass ratio of 7:2:1 and melted at 40℃ to form a temperature-response matrix with a phase change temperature of 32-33℃ and a latent heat of phase change of 85-95J / g; Hydroxypropyl methylcellulose and sodium alginate were taken in a mass ratio of 3:2 to prepare 5% moisture-sensitive gel; Moisture-sensitive gel particles accounting for 15% of the coating mass and 0.3% of food-grade polyglycerol fatty acid ester were added to the temperature-response matrix and stirred at 40℃ for 30 minutes to obtain temperature and humidity dual-response coating liquid; (4) Filler synthesis: Activated porous ceramic balls were mixed with 5% aqueous solution of Eupatorium fortunei volatile oil-hydroxypropyl-β-cyclodextrin inclusion complex at a solid-liquid ratio of 1:

4. Static adsorption was performed at 30°C for 3 hours (with 10 minutes of ultrasonic assistance at 300W every hour), followed by vacuum drying at 40°C for 2 hours. A temperature and humidity responsive coating liquid was sprayed using a fluidized bed, with the spraying pressure controlled at 0.25MPa, nozzle distance at 18cm, and inlet air temperature at 38°C, to form a 12-15μm thick coating. The coating was then shaped by a gradient cooling process of 35°C→30°C→25°C (holding each stage for 15 minutes), and screened through a 2-3mm double-layer sieve to obtain a temperature and humidity responsive Eupatorium fortunei extract slow-release pillow filler.

2. The preparation process according to claim 1, characterized in that, The inclusion rate of the volatile oil-hydroxypropyl-β-cyclodextrin inclusion complex in step (1) was detected by ultraviolet spectrophotometer, and the detected value was 88%-92%.

3. The preparation process according to claim 1, characterized in that, In step (2), the amount of silane coupling agent KH-550 added is 0.1% of the mass of the ceramic ball. After treatment, the adhesion between the ceramic ball and the dual-response coating meets the requirement that the coating peeling rate is <5% after 50 rubs.

4. The preparation process according to claim 1, characterized in that, In step (3), the moisture-sensitive gel begins to absorb water and swell at 50% RH, with an expansion rate of 150%-200% under 50%-70% RH conditions, a shrinkage rate of 80% under <45% RH conditions, and a compatibility with the temperature-responsive matrix of ≥90%.

5. The preparation process according to claim 1, characterized in that, After vacuum drying in step (4), each gram of activated porous ceramic ball is loaded with 0.22-0.25 mg of Perilla volatile oil; after setting, a performance pre-test is required: release rate <8% at 25℃ and 40%RH, release rate 12%-15% at 35℃ and 40%RH, release rate 68%-72% at 35℃ and 60%RH, and solvent residue <0.01 mg / kg.

6. A temperature and humidity responsive, sustained-release pillow filling made from Perilla extract, characterized in that, The filler is prepared by any one of the preparation processes described in claims 1-5; under conditions of temperature ≥33℃ and humidity ≥50%, the release rate of volatile oil from *Perilla frutescens* is 68%-72% after 24 hours, with an effective concentration of 0.1-0.3 mg / m³. 3 The effect lasts for 8-9 hours; under conditions of temperature <32℃ or humidity <45%, the release rate is ≤15% after 24 hours, and the performance degradation is <15% within 9 months.

7. A sleep-aid pillow containing a temperature and humidity responsive eupatorium extract slow-release filling, characterized in that, The pillow comprises a three-layer composite sac and the pillow filling as described in claim 6; the inner layer of the three-layer composite sac is 30% bamboo fiber + 70% cotton, with a thermal conductivity of 0.068 W / (m·K) and a moisture conductivity of 0.12 g / (m·h); the middle layer is a 0.2 μm polytetrafluoroethylene microporous membrane; and the outer layer is 40-count combed cotton with an air permeability of 130-150 mm / s; the inside of the sac is divided into 4 independent areas, each area is filled with 35 g of pillow filling, and the inner surface of the sac has silicone bumps that are 3 mm high, 6 mm in diameter, and spaced 1 cm apart.

8. The sleep-aid pillow according to claim 7, characterized in that, The three-layer composite sac is compatible with a 40cm×60cm pillow, and the pillow filling density is [not specified] per 100cm³. 2 It is filled with 35g; and when the pillow is in use, the head contact rate is 88%, and the efficiency of temperature and humidity signal transmission is 40% higher than that of a structure without bumps.

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