Phosphorus-containing carboxyl-terminated hyperbranched polyester, preparation method thereof, phosphorus-containing hyperbranched epoxy resin, and preparation method and application of phosphorus-containing hyperbranched epoxy resin
A hyperbranched polyester and epoxy resin technology, applied in the field of materials, can solve the problems of reducing the heat resistance and modulus of the resin, reducing the mechanical properties and hygroscopicity of the resin system, and the brittleness of the cured product.
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[0029] The structural formula of the phosphorus-containing carboxyl-terminated hyperbranched polyester described in this application is shown in formula (I), wherein P is a hyperbranched structure. In some specific embodiments, the phosphorus-containing carboxyl-terminated hyperbranched polyester is marked as HPAC-n; n=1, m can correspond to 6, representing the first-generation carboxyl-terminated hyperbranched polymer; n=2, m can correspond to 12, representing the second-generation carboxyl-terminated hyperbranched polymer; n=3, m can correspond to 24, which represents the third-generation carboxyl-terminated hyperbranched polymer; n=4, and m can correspond to 48, which represents the fourth-generation carboxyl-terminated hyperbranched polymer. Specifically, when the molar ratio of tricarboxyethylphosphine and glycol is about 4:3, HPAC-1 can be obtained; when the molar ratio of tricarboxyethylphosphine and glycol is about 10:9 , HPAC-2 can be obtained; when the mol ratio of t...
Embodiment 1
[0060] 1) Add 1mol of tricarboxyethylphosphine (TCEPO), 0.9mol of diethylene glycol (DEG), 1.73g of p-toluenesulfonic acid, and 300ml of xylene to the three ports of the water separator, condenser tube, thermometer and agitator In the flask, the temperature was raised to 155°C under the protection of nitrogen, and the reaction was carried out for 6 hours. After the reaction, the xylene was removed to obtain the second-generation phosphorus-containing flame-retardant carboxyl-terminated hyperbranched polyester;
[0061] 2) Add 0.1 mol of the phosphorus-containing flame-retardant carboxyl-terminated hyperbranched polyester prepared above and 3.6 mol of epichlorohydrin (ECH) into a three-necked reaction flask, react at 100-115°C for 2 hours, and evaporate Excessive ECH; add organic solvent to fully dissolve, slowly add 4.8 mol concentration of 40wt% sodium hydroxide aqueous solution dropwise at room temperature, react for 5 hours, wash with water three times after the reaction, an...
Embodiment 2
[0064] 1) Add 2.2mol tricarboxyethylphosphine (TCEPO), 2.1mol diethylene glycol (DEG), 3.86g p-toluenesulfonic acid, and 400ml xylene to the water separator, condenser tube, thermometer and stirrer In a three-necked flask, the temperature was raised to 160° C. under the protection of nitrogen, and the reaction was carried out for 6 hours. After the reaction, the xylene was removed to obtain the third-generation phosphorus-containing flame-retardant carboxyl-terminated hyperbranched polyester;
[0065] 2) Add 0.1mol of the third-generation phosphorus-containing flame-retardant carboxyl-terminated hyperbranched polyester prepared above and 4.8mol of epichlorohydrin (ECH) into a three-necked reaction flask, and react at 100-115°C for 2 hours. Finish steaming off excess ECH; add an organic solvent to fully dissolve, slowly add 5.2 mol concentration of 45wt% sodium hydroxide aqueous solution dropwise at room temperature, react for 5 hours, wash with water three times after the react...
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