# US 2017/0283609 A1 · Halogen-free epoxy resin composition, prepreg and laminate using same > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 2017/0283609 A1 - Document ID: US20170283609A1 - Status: Published application - Kind: A1 - Application number: 15/118,204 - Filed: 2015-06-01 - Published: 2017-10-05 - Earliest claimed: 2014-12-26 - Assignees: Shengyi Technology Co., Ltd. - Applicants: Shengyi Technology Co., Ltd. - Inventors: Xianping Zeng; Liexiang He - Web page: https://patentgrep.com/patent/US20170283609A1 ## CPC - C08L 63/04: Epoxynovolacs - C08G 59/4071: {phosphorus containing compounds} - C08G 59/4215: {cycloaliphatic} - C08G 59/4238: {heterocyclic} - C08G 59/4284: {together with other curing agents} - C08G 59/621: {Phenols} - C08G 59/685: {Carboxylates} - C08G 59/686: {containing nitrogen} - C08J 5/043: {with glass fibres} - C08J 5/10: characterised by the additives used in the polymer mixture - C08J 5/244: {using glass fibres} - C08J 5/249: {characterised by the additives used in the prepolymer mixture} - C08L 63/00: Compositions of epoxy resins; Compositions of derivatives of epoxy resins - H05K 1/0373: {containing additives, e.g. fillers (H05K1/036 takes precedence)} - C08J 2363/04: Epoxynovolacs - C08J 2425/08: Copolymers of styrene (C08J2429/08, C08J2435/06, C08J2455/02 take precedence) - C08J 2461/14: Modified phenol-aldehyde condensates - C08L 2201/02: Flame or fire retardant/resistant - C08L 2201/22: Halogen free composition - C08L 2203/20: use in electrical or conductive gadgets - C08L 2205/05: containing polymer components which can react with one another - C08L: COMPOSITIONS OF MACROMOLECULAR COMPOUNDS (compositions based on polymerisable monomers C08F, C08G; artificial filaments or fibres D01F; textile treating compositions D06) - C08G: MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS - C08J: WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H (working, e.g. shaping, of plastics B29) - H05K: PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS ## Abstract Provided in the present invention are a halogen-free epoxy resin composition, prepreg and laminate using the same, the halogen-free epoxy resin composition comprising: (A) a halogen-free epoxy resin; (B) a crosslinking agent; and (C) a phosphorous-containing phenolic resin, the phosphorous-containing phenolic resin being formed by a synthesis of phenol and formaldehyde with dicyclopentadiene phenol, and being substituted by 9,10-dihydro-9-oxa-10-phosphapheanthrene-10-oxide or a derivative thereof. The prepreg and laminate prepared from the halogen-free epoxy resin composition have a high heat resistance, a low dielectric constant, a low dielectric loss factor and a low water absorption rate, and achieve halogen-free flame retardance. ## Claims ### Claim 1 A halogen-free epoxy resin composition, comprising (A) a halogen-free epoxy resin; (B) a crosslinking agent; and (C) a phosphorous-containing novolac resin having the following structure A and A1 are both dependently p, q, m and n represent the numbers of repeating units and are independently integers which are greater than or equal to 1; X is 9,10-dihydro-9-oxa-10-phosphapheanthrene-10-oxide or derivatives thereof; R is selected from the group consisting of hydrogen, aliphatic functional groups or aromatic functional groups. ### Claim 2 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the halogen-free epoxy resin is selected from the group consisting of biphenyl novolac epoxy resin, DCPD novolac epoxy resin, alkylene novolac epoxy resin, bisphenol A novolac epoxy resin, bisphenol F epoxy resin, bisphenol Z epoxy resin, bisphenol AP epoxy resin, bisphenol TMC epoxy resin, biphenyl-containing epoxy resin, tetramethyl biphenyl epoxy resin, phenol novolac epoxy resin, cresol novolac epoxy resin, triphenyl methane epoxy resin, tetraphenyl ethane epoxy resin, dicyclopentadiene-phenol addition reaction epoxy resin, phenol aralkyl epoxy resin, naphthol novolac epoxy resin, naphthol aralkyl epoxy resin, naphthol-phenol co-condensation novolac epoxy resin, naphthol-cresol co-condensation novolac epoxy resin, aromatic hydrocarbon formaldehyde resin-modified novolac epoxy resin, biphenyl-modified novolac epoxy resin or imide-modified epoxy resin, or a mixture of at least two selected therefrom. ### Claim 3 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the halogen-free epoxy resin is selected from the group consisting of biphenyl novolac epoxy resin, DCPD novolac epoxy resin or bisphenol A novolac epoxy resin, or a mixture of at least two selected therefrom. ### Claim 4 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the halogen-free epoxy resin is biphenyl novolac epoxy resin or/and DCPD novolac epoxy resin. ### Claim 5 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the crosslinking agent is selected from the group consisting of active esters, anhydride compounds or novolac resins, or a mixture of at least two selected therefrom. ### Claim 6 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the halogen-free epoxy resin composition further comprises cyanates or prepolymers thereof. ### Claim 7 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the halogen-free epoxy resin composition further comprises a curing accelerator. ### Claim 8 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the halogen-free epoxy resin composition further comprises a flame retardant compound, the flame retardant compound is flame retardant salts. ### Claim 9 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the halogen-free epoxy resin composition further comprises a filler, the filler is organic or/and inorganic fillers. ### Claim 10 (depends on 1) A prepreg comprising a reinforcing material and the halogen-free epoxy resin composition according to claim 1 attached thereon after impregnation and drying. ### Claim 11 (depends on 10) A laminate comprising at least one prepreg according to claim 10. ### Claim 12 (depends on 10) A printed circuit board comprising at least one prepreg according to claim 10. ### Claim 13 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the crosslinking agent is selected from the group consisting of active esters or anhydride compounds. ### Claim 14 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the crosslinking agent is active esters. ### Claim 15 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that the crosslinking agent is selected from the group consisting of active esters having the following structures X is phenyl or naphthyl; j is 0 or 1; k is 0 or 1; n represents the number of repeating unit which is 0.25-1.25. ### Claim 16 (depends on 1) The halogen-free epoxy resin composition according to claim 1, characterized in that based on the addition amount of the halogen-free epoxy resin which is 100 parts by weight, the phosphorous-containing novolac resin is from 30 to 70 parts by weight; the crosslinking agent is from 27 to 58 parts by weight. ### Claim 17 (depends on 6) The halogen-free epoxy resin composition according to claim 6, characterized in that based on the total addition amount of components (A), (B) and (C) which is 100 parts by weight, the cyanates or prepolymers thereof are added in an amount of from 20 to 40 parts by weight. ### Claim 18 (depends on 7) The halogen-free epoxy resin composition according to claim 7, characterized in that based on the total addition amount of components (A), (B) and (C) which is 100 parts by weight, the curing accelerator is added in an amount of from 0.05 to 1 part by weight. ### Claim 19 (depends on 7) The halogen-free epoxy resin composition according to claim 7, characterized in that the curing accelerator is selected from the group consisting of 4-dimethylaminopyridine, 2-methylimidazole, 2-methyl-4-ethylimidazole or 2-phenyl-imidazole, zinc isooctanoate, or a mixture of at least two selected therefrom. ### Claim 20 (depends on 8) The halogen-free epoxy resin composition according to claim 8, characterized in that based on the total addition amount of components (A), (B) and (C) which is 100 parts by weight, the flame retardant compound is added in an amount of from 0 to 50 parts by weight, excluding 0. ### Claim 21 (depends on 9) The halogen-free epoxy resin composition according to claim 9, characterized in that based on the total addition amount of components (A), (B) and (C) which is 100 parts by weight, the filler is added in an amount of from 0 to 100 parts by weight, excluding 0. ### Claim 22 (depends on 9) The halogen-free epoxy resin composition according to claim 9, characterized in that the inorganic filler is selected from the group consisting of molten silica, crystalline silica, spherical silica, hollow silica, aluminium hydroxide, alumina, talc, aluminium nitride, boron nitride, silicon carbide, barium sulfate, barium titanate, strontium titanate, calcium carbonate, calcium silicate, mica or glass fiber powder, or a mixture of at least two selected therefrom. ### Claim 23 (depends on 9) The halogen-free epoxy resin composition according to claim 9, characterized in that the organic filler is selected from the group consisting of polytetrafluoroethylene powder, polyphenylene sulfide or polyether sulfone powder, or a mixture of at least two selected therefrom. ### Claim 24 (depends on 9) The halogen-free epoxy resin composition according to claim 9, characterized in that the filler is silica having a moderate particle size of from 1 to 15 μm.