Enhanced hydrogel composition, and preparation method therefor and use thereof

Abstract

An enhanced hydrogel composition, and a preparation method therefor and the use thereof. According to the composition, a hydrogel is formed by means of a physical cross-linking mechanism using the chelation between calcium ions and an alginic acid raw material, with the assistance of a carboxymethyl cellulose raw material to reduce the sensitivity of the chelation. The hydrogel retains a high water absorption rate of media; meanwhile, the elastic modulus of the hydrogel is significantly enhanced by means of the introduction of silicon dioxide. The method for preparing the composition comprises: dispersing the carboxymethyl cellulose raw material, the alginic acid raw material, and the silicon dioxide in a solution, mixing same uniformly, drying the mixture to obtain a material A, and then mixing the material A with a calcium source to obtain the composition. Further provided is the use of the composition in the preparation of a space-occupying product in the digestive tract.

Description

Enhanced hydrogel composition, preparation method and application thereof

[0001] Cross-reference to related applications

[0002] The present disclosure claims priority to the application No. 2024108373441, filed on June 26, 2024, with the China Patent Office, and entitled "Enhanced hydrogel composition, preparation method and application thereof", the entire content of which is incorporated herein by reference. TECHNICAL FIELD

[0003] The present disclosure relates to the field of food technology, in particular, to an enhanced hydrogel composition, a preparation method and application thereof. BACKGROUND

[0004] With the development of society and the improvement of living standards, obesity and diabetes have become a serious global health problem. At present, the treatment methods for weight loss and diabetes mainly include drug treatment, diet control and surgery, etc. Among them, surgery is an effective treatment method, but the risk of surgery is large and the recovery time is long; and in the process of weight loss by drug treatment, there is often the problem of weight rebound after drug withdrawal, or the drug itself has some side effects; diet control is a safe and effective non-surgical treatment for weight loss, but weight lossers need to have strong self-control, so it is often difficult to achieve long-term and effective weight loss. In order to assist weight lossers in controlling their diet, weight lossers are usually asked to eat some products with strong satiety, so it is of great significance to develop a safe and effective product to assist people in losing weight.

[0005] The prior art proposes some space-occupying gels in the digestive tract to increase satiety and achieve the purpose of weight loss. However, the current space-occupying gels in the digestive tract can only provide good space-occupying effect in the stomach, and when the space-occupying gel reaches the intestine, the intestinal fluid pH value and the intestinal pressure in the intestine destroy the structure of the space-occupying gel, resulting in inconsistent satiety duration of people, making it difficult to achieve the purpose of sustained weight loss and sugar control.

[0006] In view of this, the present disclosure is proposed. SUMMARY

[0007] The purpose of the present disclosure is to provide an enhanced hydrogel composition, a preparation method and application thereof.

[0008] The present disclosure is implemented as follows:

[0009] In a first aspect, the present disclosure provides an enhanced hydrogel composition, raw materials including carboxymethyl cellulose raw materials, alginic acid raw materials, a calcium source and silicon dioxide, and the mass relationship of each component in the raw materials satisfies:

[0010] W1 = m2 / (m1+m2) x 100%, and 10%≤W1≤70%;

[0011] W2 = m5 / (m1+m2+m5) x 100%, and 5%≤W2≤40%;

[0012] f = m4 / m3, and 0.09≤f≤3.00;

[0013] wherein, m1 is the mass of the carboxymethyl cellulose raw material, m2 is the mass of the alginic acid raw material, m3 is the mass of the carboxyl in the alginic acid raw material, m4 is the mass of Ca 2+ in the calcium source, and m5 is the mass of the silicon dioxide.

[0014] In a second aspect, the present disclosure provides a preparation method of the composition according to any one of the preceding embodiments, comprising dispersing the carboxymethyl cellulose raw material, the alginic acid raw material and the silicon dioxide in a solution, mixing uniformly and then drying to obtain A material, and then mixing the A material with the calcium source to obtain the composition.

[0015] In a third aspect, the present disclosure provides use of the composition according to any one of the preceding embodiments in preparation of a product for occupying space in the digestive tract.

[0016] The present disclosure has the following beneficial effects:

[0017] The present disclosure provides an enhanced hydrogel composition and a preparation method and use thereof, which can quickly form a hydrogel in water, wherein the alginic acid raw material is physically cross-linked with calcium ions, and the carboxymethyl cellulose raw material can reduce the sensitivity of the alginic acid raw material to calcium ions, so that the prepared hydrogel greatly improves the medium water absorption rate while retaining a certain elastic modulus of the hydrogel, and the addition of silicon dioxide enhances the strength of the hydrogel. The process of forming a hydrogel by the composition of the present disclosure is a physical cross-linking method, and no chemical reaction occurs. The hydrogel prepared from the composition has high strength, high elastic modulus and excellent water absorption performance. After entering the digestive tract, the hydrogel can occupy the gastric volume in the stomach, thereby reducing food intake and achieving the purposes of weight loss and blood sugar control. When the hydrogel reaches the small intestine, in the high-pH environment of the small intestine, the hydrogel swells again, and the hydroxide at high pH reacts with the silicon dioxide to locally form a microgel to enhance the elastic modulus at high pH, thereby occupying the volume of the small intestine and / or exerting pressure on the small intestine wall to continuously produce a feeling of satiety, so as to be more conducive to the management of body weight and blood sugar. BRIEF DESCRIPTION OF DRAWINGS

[0018] In order to more clearly illustrate the technical solutions of the embodiments of the present disclosure, the following will briefly introduce the drawings needed to be used in the embodiments. It should be understood that the following drawings only show some of the embodiments of the present disclosure, and therefore should not be considered as limiting the scope, and for those skilled in the art, other related drawings can also be obtained without creative labor.

[0019] Figure 1 is a weight loss effect broken line graph provided by the test example 2 of the present disclosure. DETAILED DESCRIPTION

[0020] The embodiments of the present disclosure will be described in detail below with reference to the embodiments, but those skilled in the art will understand that the following embodiments are only used to illustrate the present disclosure and should not be considered as limiting the scope of the present disclosure. The specific conditions are not specified in the embodiments, and the conventional conditions or the conditions recommended by the manufacturer are used. The reagents or instruments used are not specified by the manufacturer, and are conventional products that can be purchased on the market.

[0021] The endpoints of the ranges and any values disclosed in the present disclosure are not limited to the precise values stated. The ranges or values should be construed to include values approximately around the ranges or values. For numerical ranges, the endpoints of each range are included, the endpoints of each range and the individual points are included, and the individual points are included, and one or more new numerical ranges can be formed by combining the endpoints of each range, the endpoints of each range and the individual points, and the individual points, which should be considered as specifically disclosed herein.

[0022] The prior art uses chemical cross-linking of low molecular weight carboxymethyl cellulose sodium to obtain a hydrogel with certain strength and water absorption performance, which can increase satiety in the stomach and achieve the purpose of weight loss. However, the preparation process of the hydrogel uses chemical cross-linking, which uses the hydroxyl groups in carboxymethyl cellulose sodium to react to form ester bonds, thereby realizing the connection between molecules to obtain a hydrogel product. The preparation process is complex, the yield is low, and the cost is high.

[0023] Based on the existing chemical cross-linking method for preparing the gastric volume-occupying hydrogel, the inventors found that there is a key problem in the actual application of the hydrogel, that is, the medium water absorption rate and the elastic modulus of the hydrogel are often contradictory. Generally speaking, when the medium water absorption rate of the hydrogel increases, the hydrogel is softer, the corresponding elastic modulus of the hydrogel is lower, and the mechanical properties are also poor, and the satiety is easy to fail under the peristalsis and pressure of the digestive tract; when the medium water absorption rate of the hydrogel decreases, the hydrogel is harder, the corresponding elastic modulus of the hydrogel is higher, and the hydrogel has good mechanical properties, but the decrease in water absorption rate leads to a smaller volume of the hydrogel, which also reduces the satiety of the hydrogel.

[0024] In addition, the existing hydrogel can only provide good space-occupying effect in the stomach. When the hydrogel reaches the intestine, the high pH value of the intestinal fluid in the intestine will make the gel further swell and lose a large part of the gel strength, and cannot generate pressure on the intestine, ultimately leading to a shortened duration of satiety.

[0025] Therefore, the present disclosure not only needs to develop a simple process, but also needs to improve the medium water absorption rate and elastic modulus of the hydrogel, and improve the resistance of the hydrogel under different pH and pressure. Based on this, the inventors propose the following solutions.

[0026] In a first aspect, the present disclosure provides an enhanced hydrogel composition, the raw materials including carboxymethyl cellulose raw materials, alginic acid raw materials, a calcium source and silicon dioxide, and the mass relationship of each component in the raw materials satisfies:

[0027] W1 = m2 / (m1+m2) x 100%, and 10%≤W1≤70%;

[0028] W2 = m5 / (m1+m2+m5) x 100%, and 5%≤W2≤40%;

[0029] f = m4 / m3, and 0.09≤f≤3.00;

[0030] Wherein, m1 is the mass of the carboxymethyl cellulose raw material, m2 is the mass of the alginic acid raw material, m3 is the mass of the carboxyl in the alginic acid raw material, m4 is the mass of Ca 2+ in the calcium source, and m5 is the mass of silicon dioxide. The units of m1, m2, m3, m4 and m5 are the same, for example, they can be g or kg.

[0031] The composition of the present disclosure is dispersed in water, and the composition can gel to form a hydrogel. Specifically, the alginic acid raw material in the composition can chelate with calcium ions in a solution state to form a hydrogel and undergo physical crosslinking. However, due to the high sensitivity of the alginic acid raw material to calcium ions, directly mixing the alginic acid raw material and the calcium source can cause the alginic acid raw material to rapidly chelate with calcium ions in a solution state, resulting in a hydrogel with high strength and poor water absorption capacity, which cannot meet the requirements of a space-occupying gel in the digestive tract.

[0032] Therefore, the applicant proposes adding carboxymethyl cellulose raw materials to the system of alginic acid raw materials and calcium sources. The carboxymethyl cellulose raw materials can reduce the sensitivity of the alginic acid raw materials to calcium ions, and achieve controllable adjustment of the water absorption capacity and elastic modulus during the gelation process of the composition. By controlling the values of W1 and f, the hydrogel formed by the composition provided by the present disclosure not only has good water absorption capacity, but also has high elastic modulus. The addition of silicon dioxide to the composition system enables the hydrogel formed by the composition of the present disclosure to have high strength.

[0033] Further, the composition of the present disclosure does not undergo chemical reactions during preparation, and is a physical cross-linking process. The main molecular chain is formed by chelation of alginic acid raw materials and calcium sources. Compared with the chemical cross-linking process, the water absorption capacity and elastic modulus of the hydrogel can be controlled by strictly controlling the molecular weight of the cross-linked molecules. The composition provided by the present disclosure is more convenient to prepare, has higher yield, and has lower development cost.

[0034] When the composition of the present disclosure is dispersed in water, the composition rapidly absorbs water and swells to form a gel-like hydrogel. After swallowing the hydrogel, the hydrogel enters the stomach through the esophagus. Because the hydrogel prepared from the composition of the present disclosure has high strength, high elastic modulus, and excellent water absorption performance, it can occupy the volume of the stomach contents in the stomach, thereby reducing food intake to achieve the purpose of weight loss and blood glucose control. When the hydrogel reaches the small intestine, the hydrogel swells again in the high-pH environment of the small intestine, and the hydroxide ions at high pH react with the silicon dioxide to form a microgel locally, thereby enhancing the elastic modulus at high pH and occupying the volume of the small intestine and / or exerting pressure on the small intestine wall to continuously produce a feeling of satiety, thereby facilitating weight management.

[0035] To further optimize the strength, water absorption, and elastic modulus of the hydrogel formed after the composition provided by the present disclosure is gelled, the parameter ranges of W1, W2, and f can be further controlled.

[0036] Specifically, W1 satisfies: 10%≤W1≤70%, W2 satisfies: 10%≤W2≤30%, and f satisfies: 0.2≤f≤3.00.

[0037] More preferably, W1 satisfies: 12%≤W1≤22%, W2 satisfies: 10%≤W2≤25%, and f satisfies: 0.2≤f≤2.00.

[0038] For example, W1 can be 10%, 20%, 30%, 40%, 50%, 60%, or 70%, and a range value between any two of the above values. W2 can be 10%, 15%, 20%, 25%, or 30%, and a range value between any two of the above values. f can be 0.2, 0.50, 1.00, 1.50, or 2.00, and a range value between any two of the above values.

[0039] In an optional embodiment, the composition forms a hydrogel after absorbing water, and the medium water absorption rate of the composition is ≥40 times, i.e., the enhanced hydrogel composition provided by the present disclosure can absorb a medium aqueous solution of 40 times or more than the dry base mass thereof; in simulated gastric juice, the elastic modulus of the hydrogel is ≥600 Pa; and in simulated intestinal juice, the elastic modulus of the hydrogel is ≥400 Pa.

[0040] The simulated gastric fluid is an artificial gastric fluid, which is a liquid with the performance of gastric fluid configured artificially. The simulated gastric fluid in the present disclosure is an artificial gastric fluid configured according to the fourth part of the Pharmacopoeia of the People's Republic of China 2020, and then diluted by 8 times to simulate the state of the human gastric fluid half an hour before a meal.

[0041] Similarly, the simulated intestinal fluid is an artificial intestinal fluid, which is a liquid with the performance of intestinal fluid configured artificially. The simulated intestinal fluid in the present disclosure is an artificial intestinal fluid configured according to the fourth part of the Pharmacopoeia of the People's Republic of China 2020.

[0042] By controlling the selection and ratio of each component of the composition in the present disclosure, the composition provided by the present disclosure has a good medium water absorption rate (the water absorption capacity can reach more than 40 times the dry base mass of the composition) after forming a hydrogel, and has a high elastic modulus in the simulated gastric fluid and the simulated intestinal fluid, which can realize the effect of occupying the digestive tract and producing satiety of the hydrogel, and can assist in achieving the effect of weight loss.

[0043] Further, the selection of the source of the raw material is another factor for improving the performance of the hydrogel formed by the composition. For example, some literature reports that sodium alginate can form a gel in the stomach at pH to prolong the emptying time of the stomach, thereby reducing food intake and preventing obesity. However, due to the limitations of different sources, molecular weights and molecular structures (the ratio between mannuronic acid and guluronic acid) of alginate, the weight loss effect varies greatly in different literature reports, which greatly limits the application of alginate in the field of weight loss.

[0044] In order to further improve the performance of the hydrogel, in an optional embodiment, the viscosity of the sodium alginate raw material in the solution is ≥4000 mPa·S when the concentration of the sodium alginate raw material in the solution is 2%; preferably, the viscosity of the sodium alginate raw material in the solution is ≥5000 mPa·S when the concentration of the sodium alginate raw material in the solution is 2%; more preferably, the viscosity of the sodium alginate raw material in the solution is 5500-20000 mPa·S when the concentration of the sodium alginate raw material in the solution is 2%.

[0045] The viscosity of the carboxymethyl cellulose raw material in the solution is ≥4000 mPa·S when the concentration of the carboxymethyl cellulose raw material in the solution is 2%; preferably, the viscosity of the carboxymethyl cellulose raw material in the solution is ≥5000 mPa·S when the concentration of the carboxymethyl cellulose raw material in the solution is 2%; more preferably, the viscosity of the carboxymethyl cellulose raw material in the solution is 6000-20000 mPa·S when the concentration of the carboxymethyl cellulose raw material in the solution is 2%.

[0046] Since the molecular weight and molecular structure of the carboxymethyl cellulose raw material and the sodium alginate raw material will exhibit different performances, the present disclosure controls the viscosity range of the carboxymethyl cellulose raw material and the sodium alginate raw material, thereby controlling the molecular weight and molecular structure of the carboxymethyl cellulose raw material and the sodium alginate raw material, and further improving the water absorption and elastic modulus of the hydrogel formed by the composition.

[0047] Preferably, the carboxymethyl cellulose raw material includes, but is not limited to, carboxymethyl cellulose and its salts, the salts of carboxymethyl cellulose include any one of sodium carboxymethyl cellulose, potassium carboxymethyl cellulose and ammonium carboxymethyl cellulose, and any raw material having the structure of carboxymethyl cellulose can be used as a raw material for reducing the sensitivity of sodium alginate and calcium source.

[0048] Preferably, the alginate raw material includes, but is not limited to, alginate and its salts, the salts of alginate include any one of sodium alginate, potassium alginate and ammonium alginate, and any raw material having the structure of alginate and its carboxyl group can be used as a raw material for chelating with calcium source and physical cross-linking.

[0049] Preferably, the calcium source includes, but is not limited to, at least one of calcium carbonate, calcium chloride, calcium citrate, calcium lactate, calcium gluconate, calcium acetate or calcium phosphate; all products capable of providing calcium source can be used as the calcium source of the present disclosure. More preferably, the calcium source is a low solubility calcium source; more preferably, the low solubility calcium source is one of calcium lactate, calcium carbonate and calcium phosphate.

[0050] It should be noted that since the composition provided by the present disclosure needs to enter the digestive tract after forming a hydrogel to achieve the digestive tract occupation, thereby providing satiety and achieving the effect of weight loss, it can be understood that each component in the raw material of the composition of the present disclosure is a food-grade component to ensure that the hydrogel formed by the composition is edible.

[0051] The applicant further found that in the process of forming a hydrogel, the hydrogel composition can be directly added to water, or the different components in the hydrogel composition can be added to water separately.

[0052] In an optional embodiment, when the different components in the hydrogel composition are added to water separately, the present disclosure can also package the raw materials of the composition separately to facilitate the indication of the mixing order of the composition.

[0053] In an optional embodiment, the raw materials of the hydrogel composition include separately packaged A material and B material, the A material is a mixture of carboxymethyl cellulose raw material, alginate raw material and silicon dioxide, and the B material is a calcium source. The A material is configured to be mixed with the solution first, and the B material is configured to be added to the solution after the A material is dispersed to avoid the calcium source reacting rapidly with the alginate raw material, resulting in a decrease in the water absorption performance of the hydrogel.

[0054] Preferably, in order to ensure that the A material can be dispersed rapidly in the solution to form a colloidal suspension, the particle size of the A material is 0.1 mm to 2 mm, more preferably 0.3 mm to 2 mm, and more preferably 0.3 mm to 1 mm.

[0055] In a second aspect, the present disclosure provides a method for preparing the hydrogel composition according to any one of the preceding embodiments, comprising dispersing the carboxymethyl cellulose raw material, the alginic acid raw material and the silicon dioxide in a solution, drying the mixture to obtain A material, and then mixing the A material with a calcium source to obtain the hydrogel composition.

[0056] Preferably, the concentration of the polymers in the solution is 1% to 10% and the drying temperature is 70°C to 140°C during the preparation of the A material.

[0057] Preferably, the concentration of the polymers in the solution is 1% to 10% and the drying temperature is 70°C to 140°C during the preparation of the A material.

[0058] The hydrogel composition provided by the present disclosure is in a solid state before gelation, and can quickly gelate to obtain a hydrogel after being added into water. After the hydrogel is consumed, the hydrogel can occupy the digestive tract and provide a feeling of satiety, thereby reducing the frequency and amount of eating and achieving weight loss and improving the symptoms of diabetes.

[0059] In a third aspect, the present disclosure provides a use of the composition according to any one of the preceding embodiments in the preparation of a digestive tract occupying product.

[0060] In an optional embodiment, the method for using the hydrogel composition provided by the present disclosure comprises adding the entire solid composition into water and stirring, or adding the mixture of the carboxymethyl cellulose raw material, the alginic acid raw material and the silicon dioxide into water and stirring to obtain a pre-gel suspension, and then adding the calcium source into the pre-gel suspension and stirring to obtain the hydrogel.

[0061] That is, when the composition is packaged as A material and B material, the A material is first added into water and stirred to obtain a pre-gel suspension, and then the B material is added into water and stirred to obtain the hydrogel.

[0062] In an optional embodiment, in order to ensure that the components in the raw materials are uniformly mixed, the stirring time of each stirring is 2 to 5 minutes, and in order to obtain a hydrogel with complete morphology, it is necessary to ensure that the liquid does not generate vortex during the stirring process.

[0063] Example 1

[0064] The present embodiment provides an enhanced hydrogel composition, which is composed of A material and B material. The A material is sodium carboxymethyl cellulose, sodium alginate and silicon dioxide, and the B material is calcium lactate.

[0065] The mass of the sodium carboxymethyl cellulose is 20.0 g, and the viscosity is 8000 mPa·S when the concentration in the solution is 2%.

[0066] The mass of the sodium alginate is 4.0 g, and the viscosity is 5800 mPa·S when the concentration in the solution is 2%.

[0067] The mass of the silicon dioxide is 2.5 g.

[0068] The embodiment also provides a preparation method of the composition, comprising the following steps:

[0069] The 4.0 g of sodium alginate is stirred and dispersed in 500 mL of water, and then 4.0 g of silicon dioxide is stirred and dispersed in the water. After that, 20.0 g of sodium carboxymethyl cellulose is added. The sodium alginate, the sodium carboxymethyl cellulose, the silicon dioxide and the water are mixed under mechanical stirring at 1000 rpm to form a uniform suspension. The suspension is transferred to a metal tray, and the thickness of the suspension in the metal tray is controlled to be less than 1 cm. Then, the metal tray is placed in an oven at 70°C for drying for 24 h to obtain solid A material. The solid A material is crushed in a crusher and sieved through 10-mesh and 120-mesh screens to obtain granular A material with a particle size of 0.1-2 mm, which is packaged for use.

[0070] The calcium lactate is packaged as B material. The mass of the calcium lactate in the B material and the mass of the sodium alginate in the A material satisfy f = 0.61.

[0071] Embodiment 2

[0072] The embodiment provides an enhanced hydrogel composition, which is composed of A material and B material. The A material is sodium carboxymethyl cellulose, sodium alginate and silicon dioxide. The B material is calcium lactate.

[0073] The mass of the sodium carboxymethyl cellulose is 20.0 g, and the viscosity is 8000 mPa·S when the concentration in the solution is 2%.

[0074] The mass of the sodium alginate is 5.0 g, and the viscosity is 5800 mPa·S when the concentration in the solution is 2%.

[0075] The mass of the silicon dioxide is 4.0 g.

[0076] The embodiment also provides a preparation method of the composition, comprising the following steps:

[0077] The 5.0 g of sodium alginate is stirred and dispersed in 500 mL of water, and then 4.0 g of silicon dioxide is stirred and dispersed in the water. After that, 20.0 g of sodium carboxymethyl cellulose is added. The sodium alginate, the sodium carboxymethyl cellulose, the silicon dioxide and the water are mixed under mechanical stirring at 1000 rpm to form a uniform suspension. The suspension is transferred to a metal tray, and the thickness of the suspension in the metal tray is controlled to be less than 1 cm. Then, the metal tray is placed in an oven at 70°C for drying for 24 h to obtain solid A material. The solid A material is crushed in a crusher and sieved through 10-mesh and 120-mesh screens to obtain granular A material with a particle size of 0.1-2 mm, which is packaged for use.

[0078] The calcium lactate is encapsulated as the B material, and the mass of the calcium lactate in the B material and the mass of the sodium alginate in the A material satisfy f = 0.42.

[0079] Embodiment 3

[0080] The embodiment provides an enhanced hydrogel composition, which is composed of A material and B material, the A material being sodium carboxymethyl cellulose, sodium alginate and silicon dioxide, and the B material being calcium lactate.

[0081] The mass of the sodium carboxymethyl cellulose is 20.0 g, and the viscosity is 8000 mPa·S when the concentration in the solution is 2%.

[0082] The mass of the sodium alginate is 5.0 g, and the viscosity is 5800 mPa·S when the concentration in the solution is 2%.

[0083] The mass of the silicon dioxide is 2.8 g.

[0084] The embodiment also provides a preparation method of the composition, which comprises the following steps.

[0085] The 5.0 g of sodium alginate is added into 500 mL of water and stirred and dispersed, then 2.8 g of silicon dioxide is added into the water and stirred and dispersed, and then 20.0 g of sodium carboxymethyl cellulose is added, and the sodium alginate, the sodium carboxymethyl cellulose, the silicon dioxide and the water are mixed under mechanical stirring at 1000 rpm to form a uniform suspension. The suspension is transferred into a metal tray, the thickness of the suspension in the metal tray is controlled to be below 1 cm, and then the metal tray is placed in an oven at 70 DEG C and dried for 24 h to obtain solid A material. The solid A material is crushed in a crusher, and then sieved through 10-mesh and 120-mesh sieves to obtain granular A material with a particle size of 0.1-1 mm, which is encapsulated and ready for use.

[0086] The calcium lactate is encapsulated as the B material, and the mass of the calcium lactate in the B material and the mass of the sodium alginate in the A material satisfy f = 0.76.

[0087] Embodiment 4

[0088] The embodiment provides an enhanced hydrogel composition, which is composed of A material and B material, the A material being sodium carboxymethyl cellulose, sodium alginate and silicon dioxide, and the B material being calcium lactate.

[0089] The mass of the sodium carboxymethyl cellulose is 20.0 g, and the viscosity is 8000 mPa·S when the concentration in the solution is 2%.

[0090] The mass of the sodium alginate is 5.0 g, and the viscosity is 5800 mPa·S when the concentration in the solution is 2%.

[0091] The mass of the silicon dioxide is 2.8 g.

[0092] The present embodiment also provides a preparation method of the above-mentioned composition, comprising the following steps:

[0093] 5.0 g of sodium alginate was added into 500 mL of water and stirred to disperse, then 2.8 g of silicon dioxide was added into the water and stirred to disperse, and then 20.0 g of sodium carboxymethyl cellulose was added, and the sodium alginate, sodium carboxymethyl cellulose, silicon dioxide and water were mixed under mechanical stirring at 1000 rpm to form a uniform suspension. The suspension was transferred into a metal tray, the thickness of the suspension in the metal tray was controlled to be below 1 cm, and then the metal tray was placed in an oven at 70°C for drying for 24 h to obtain solid A material. The solid A material was crushed in a crusher, and sieved through 10 mesh and 120 mesh sieves to obtain granular A material with a particle size of 0.1-2 mm, which was packaged for use.

[0094] The calcium lactate was packaged as B material, and the mass of calcium lactate in the B material and the mass of sodium alginate in the A material satisfied f = 1.68.

[0095] Example 5

[0096] The present embodiment provides a reinforced hydrogel composition, which is basically the same as that of Example 4, except that the viscosity of sodium carboxymethyl cellulose in the solution is 13000 mPa·S when the concentration of sodium carboxymethyl cellulose in the solution is 2%.

[0097] Example 6

[0098] The present embodiment provides a reinforced hydrogel composition, which is composed of A material and B material, the A material is sodium carboxymethyl cellulose, sodium alginate and silicon dioxide, and the B material is calcium lactate. The preparation method of the A material is the same as that of Example 3, and the f value is 0.76. The only difference is that the A material and the B material are directly mixed according to the f value and packaged for use.

[0099] Comparative Example 1

[0100] The present comparative example provides a hydrogel composition, the raw material composition and the preparation method of which are similar to those of Example 3, except that no silicon dioxide is added in the A material.

[0101] Comparative Example 2

[0102] The present comparative example provides a hydrogel composition, the raw material composition and the preparation method of which are similar to those of Example 3, except that no silicon dioxide is added in the A material, and f = 1.51.

[0103] Comparative Example 3

[0104] The present comparative example provides a hydrogel composition, the raw material composition and the preparation method of which are similar to those of Example 3, except that the content of silicon dioxide in the A material is 0.3 g.

[0105] Comparative Example 4

[0106] This comparative example provides a hydrogel composition, similar to Example 3, with the only difference that the A material includes only 27.8 g of sodium alginate, and f = 1.68.

[0107] Comparative Example 5

[0108] This comparative example provides a hydrogel composition, similar to Example 3, with the only difference that the A material includes pectin instead of sodium carboxymethyl cellulose, and does not include silicon dioxide.

[0109] Comparative Example 6

[0110] This comparative example provides a hydrogel composition, similar to Example 3, with the only difference that the A material includes sodium carboxymethyl cellulose with a viscosity of 1000 mPa·S in a 2% aqueous solution.

[0111] Experimental Example 1

[0112] 1) Detection in simulated gastric juice:

[0113] According to the fourth part of the Pharmacopoeia of the People's Republic of China 2020, artificial gastric juice is prepared, then diluted 8 times, and the pH is adjusted to 2.1, as simulated artificial gastric juice half an hour before a meal (hereinafter referred to as simulated gastric juice).

[0114] 60 mL of simulated gastric juice is stirred on a magnetic stirrer, the stirring speed is 100 rpm, 0.6 g of A material of Examples 1-6 and Comparative Examples 1-6 is weighed and slowly added to the above simulated gastric juice, after stirring for 5 min, B material is slowly added to the above simulated gastric juice according to the f value of Examples 1-6 and Comparative Examples 1-6, and stirring is continued for 5 min, which is used for the treatment process of simulated gastric juice.

[0115] A piece of 150-mesh gauze is weighed and recorded as g1, then the above stirred mixture is filtered with 150-mesh gauze to remove the unabsorbed simulated gastric juice (when filtering, pay attention to scraping the liquid on the surface of the gauze with your hand gently until no liquid is visible on your hand, then stop), weigh the mixture and gauze together and record as g2, and observe the state of the hydrogel obtained after filtration.

[0116] The medium water absorption rate MUR1 of the composition in the simulated gastric juice is calculated = (g2-g1) / 0.6. The elastic modulus G1' of the filtered hydrogel is determined by a rheometer (the value at a uniform angular frequency of 10 rad / s is taken), and the results are shown in Table 1.

[0117] 2) Detection in simulated intestinal juice:

[0118] According to the fourth part of the Pharmacopoeia of the People's Republic of China 2020, artificial intestinal juice is prepared, as simulated small intestinal juice (hereinafter referred to as simulated intestinal juice).

[0119] The hydrogel after the detection in the simulated gastric fluid is weighed and recorded as g0, and then the hydrogel is added to a 200 mL beaker of simulated intestinal fluid, and the beaker is transferred to a shaker for treatment in simulated intestinal fluid at 37°C and 60 rpm / min for 120 min.

[0120] A piece of 150-mesh gauze is weighed and recorded as g3, and then the mixture after the treatment is filtered with 150-mesh gauze to remove the unabsorbed simulated intestinal fluid (when filtering, attention is paid to gently scraping the liquid on the surface of the gauze with the hand until no liquid is visible to the naked eye, and then the mixture and the gauze are weighed and recorded as g4, and the state of the hydrogel obtained after the filtration is observed.

[0121] The medium water absorption rate MUR2 of the hydrogel in the simulated intestinal fluid is calculated as (g4-g3) / (g0*MUR1). The elastic modulus G2' of the hydrogel after the filtration is determined by a rheometer (the value at a uniform angular frequency of 10 rad / s is taken), and the results are shown in Table 1.

[0122] Table 1 Composition and properties of hydrogel

[0123] As can be seen from Table 1, the composition provided by the embodiments of the present disclosure can have a medium water absorption rate of up to 78.63 times the original weight after becoming a hydrogel, and still has a high elastic modulus (greater than 700 Pa) after absorbing water in the simulated gastric fluid. At the same time, according to the experimental results of Examples 1-6 and Comparative Examples 1-6 in Table 1, it can be seen that: for Comparative Examples 1-3 without adding silica or with a small amount of silica, the elastic modulus significantly decreases after reaching the intestinal pH, and is less than 400 Pa; for Examples 1-6 containing silica, the elastic modulus is greater than 600 Pa at the intestinal pH; for Comparative Example 4 without adding carboxymethyl cellulose raw materials, we found that its water absorption performance is poor but the elastic modulus is extremely large, which is due to the high sensitivity of pure sodium alginate to calcium ions; for Comparative Examples 5 and 6 with different carboxymethyl cellulose raw materials, it is not difficult to find that they cannot obtain a composition that takes into account both medium water absorption and elastic modulus. In summary, Examples 1-6 of the present disclosure reduce the sensitivity of calcium ion cross-linked sodium alginate by adding carboxymethyl cellulose raw materials, and when reaching the intestine, the hydroxide at high pH reacts with silica to form a local microgel, which enhances the elastic modulus at high pH, thereby occupying the volume of the small intestine and / or exerting pressure on the small intestine wall to continuously produce satiety, which is more conducive to weight management.

[0124] Experimental Example 2

[0125] Twenty volunteers were recruited and randomly divided into two groups, the control group was given the same amount of sucrose, and the experimental group was given 3g of the enhanced hydrogel composition of Example 4 for two meals a day, and the hydrogel was prepared according to the method of Example 6 for 20 volunteers to try. The drinking time is 30 minutes before meals, twice a day, at noon and dinner in the afternoon. At the same time, the volunteers were given nutritional intervention, and the daily caloric intake was reduced by 300kcal. The body weight of the volunteers was recorded every 4 weeks for 24 weeks, and the body weight loss rate TWL = (initial body weight - follow-up body weight) / initial body weight was calculated, and the results are shown in Figure 1.

[0126] As can be seen from Figure 1, through the use of the composition provided by the present disclosure and the nutritional intervention, a good weight loss effect is achieved, the body weight loss rate is between 8-10% within 24 weeks, and the weight loss effect is significantly, while the weight loss effect of the control group is less than 3%. It shows that the hydrogel composition provided by the present disclosure has a good weight loss effect.

[0127] The enhanced hydrogel composition provided by the present disclosure and its preparation method and application have at least the following advantages:

[0128] 1) The composition provided by the present disclosure is prepared by physical action of food-grade raw materials, and can be directly used as food.

[0129] 2) The present disclosure uses alginic acid raw materials and calcium source to prepare the composition and form hydrogel by physical cross-linking, compared with the hydrogel prepared by chemical cross-linking method, the preparation process is simpler, and the yield is higher, which is conducive to large-scale production.

[0130] 3) In the chelation system of alginic acid raw materials and calcium source, carboxymethyl cellulose raw materials are added, which can reduce the sensitivity of alginic acid raw materials to calcium ions, and realize the controllable adjustment of water absorption capacity and elastic modulus in the process of gelation of the composition. By controlling the values of W1 and f, the hydrogel formed by the composition provided by the present disclosure not only has good water absorption capacity, but also has high elastic modulus. The addition of silicon dioxide in the composition system makes the hydrogel formed by the composition of the present disclosure have high strength.

[0131] 4) When the composition of the present disclosure is dispersed in water and rapidly absorbs water to swell and form a hydrogel, the hydrogel prepared by the composition of the present disclosure has high elastic modulus and excellent water absorption performance, which can occupy the gastric volume in the stomach to reduce food intake, thereby achieving the purpose of weight loss and blood glucose control. When the hydrogel reaches the small intestine, in the high pH environment of the small intestine, the hydrogel swells again, and the hydroxide with high pH reacts with silicon dioxide to form a microgel locally, which maintains the elastic modulus of the hydrogel in the intestinal tract, thereby occupying the volume of the small intestine and / or exerting pressure on the small intestine wall to produce satiety, so as to be more conducive to weight management. Industrial applicability

[0132] The present disclosure provides an enhanced hydrogel composition and its method of preparation and use, which is capable of occupying the volume of the stomach and / or occupying the volume of the small intestine and / or exerting pressure on the wall of the small intestine in the form of a hydrogel in the gastrointestinal tract to continuously produce satiety, which is beneficial for the management of body weight and blood glucose.

Claims

1. A reinforced hydrogel composition, characterized in that, The raw materials include carboxymethyl cellulose, alginate, calcium, and silicon dioxide, and the mass relationships of the components in the raw materials satisfy the following: W1 = m2 / (m1+m2)×100%, and 10%≤W1≤70%; W2 = m5 / (m1+m2+m5)×100%, and 5%≤W2≤40%; f = m4 / m3, and 0.09≤f≤3.00; Where m1 is the mass of carboxymethyl cellulose raw material, m2 is the mass of alginic acid raw material, m3 is the mass of carboxyl groups in alginic acid raw material, and m4 is the mass of Ca in calcium source. 2+ The mass of m5 is the mass of silicon dioxide.

2. The composition according to claim 1, characterized in that, The following conditions must be met: W1 satisfies: 10% ≤ W1 ≤ 70%; W2 satisfies: 10% ≤ W2 ≤ 30%; and f satisfies: 0.2 ≤ f ≤ 3.

00. More preferably, W1 satisfies: 12% ≤ W1 ≤ 22%, W2 satisfies: 10% ≤ W2 ≤ 25%, and f satisfies: 0.2 ≤ f ≤ 2.

00.

3. The composition according to claim 1 or 2, characterized in that, The composition forms a hydrogel after absorbing water, and the medium water absorption rate of the composition is ≥40 times; in simulated gastric fluid, the elastic modulus of the hydrogel is ≥600 Pa; in simulated intestinal fluid, the elastic modulus of the hydrogel is ≥400 Pa.

4. The composition according to claim 1, characterized in that, The carboxymethyl cellulose raw material has a viscosity ≥ 4000 mPa·s when the concentration in the solution is 2%; Preferably, the carboxymethyl cellulose raw material includes carboxymethyl cellulose and its salts, wherein the carboxymethyl cellulose salts include any one of sodium carboxymethyl cellulose, potassium carboxymethyl cellulose, and ammonium carboxymethyl cellulose.

5. The composition according to claim 1, characterized in that, The alginate raw material has a viscosity ≥ 4000 mPa·s when the concentration of the solution is 2%; Preferably, the alginate raw material includes alginate and its salts, wherein the alginate salts include any one of sodium alginate, potassium alginate, and ammonium alginate.

6. The composition according to claim 1, characterized in that, The calcium source includes at least one of calcium carbonate, calcium chloride, calcium citrate, calcium lactate, calcium gluconate, calcium acetate, or calcium phosphate; more preferably, the calcium source is a calcium source with low solubility; even more preferably, the calcium source with low solubility is one of calcium lactate, calcium carbonate, and calcium phosphate.

7. The composition according to claim 1, characterized in that, The particle size of the composition is 0.1 mm to 2 mm, more preferably 0.3 mm to 2 mm, and even more preferably 0.3 mm to 1 mm.

8. A method for preparing the composition according to any one of claims 1 to 7, characterized in that, The process involves dispersing carboxymethyl cellulose raw materials, alginate raw materials, and silica in a solution, mixing them evenly, and then drying them to obtain material A. Material A is then mixed with a calcium source to obtain the final product.

9. The preparation method according to claim 8, characterized in that, During the preparation of material A, the polymer concentration in the solution is 1% to 10%, and the drying temperature is 70°C to 140°C; preferably, the drying temperature is 70°C to 90°C.

10. The use of the composition according to any one of claims 1 to 7 in the preparation of a digestive tract occupant product.

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