# US 7,741,397 B2 · Filled polymer compositions made from interpolymers of ethylene/α-olefins and uses thereof > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 7,741,397 B2 - Document ID: US7741397B2 - Status: Granted - Kind: B2 - Application number: 11/376,833 - Filed: 2006-03-15 - Published: 2006-09-07 - Granted: 2010-06-22 - Earliest claimed: 2004-03-17 - Assignees: Dow Global Technologies LLC - Inventors: Wenbin Liang; Yunwa W. Cheung; Charles F. Diehl; Kyle G. Kummer - Web page: https://patentgrep.com/patent/US7741397B2 ## CPC - C08K 3/013: Fillers, pigments or reinforcing additives - C08K: Use of inorganic or non-macromolecular organic substances as compounding ingredients (paints, inks, varnishes, dyes, polishes, adhesives C09) ## Abstract A filled polymer composition comprises (i) an ethylene/α-olefin interpolymer, and (ii) a filler. The ethylene/α-olefin interpolymer is a block copolymer having at least a hard block and at least a soft block. The soft block comprises a higher amount of comonomers than the hard block. The block interpolymer has a number of unique characteristics disclosed here. The filled polymer compositions provided herein, in certain embodiments, have relatively higher heat resistance and improved noise, vibration and harshness properties and can be used in automotive floorings, roofings, wire and cable coating applications. ## Claims ### Claim 1 A filled polymer composition comprising: (i) a polymer and (ii) a filler, wherein the polymer comprises an ethylene/α-olefin multi-block interpolymer comprising at least 50 mole percent ethylene that (a) has a Mw/Mn from about 1.7 to about 3.5, at least one melting point, Tm, in degrees Celsius, and a density, d, in grams/cubic centimeter, wherein the numerical values of Tm and d correspond to the relationship: Tm>−2002.9+4538.5(d)−2422.2(d)2; or (b) has a Mw/Mn from about 1.7 to about 3.5, and is characterized by a heat of fusion, ΔH in J/g, and a delta quantity, ΔT, in degrees Celsius defined as the temperature difference between the tallest DSC peak and the tallest CRYSTAF peak, wherein the numerical values of ΔT and ΔH have the following relationships: ΔT>−0.1299(ΔH)+62.81 for ΔH greater than zero and up to 130 J/g, ΔT≧48° C. for ΔH greater than 130 J/g, wherein the CRYSTAF peak is determined using at least 5 percent of the cumulative polymer, and if less than 5 percent of the polymer has an identifiable CRYSTAF peak, then the CRYSTAF temperature is 30° C.; or (c) is characterized by an elastic recovery, Re, in percent at 300 percent strain and 1 cycle measured with a compression-molded film of the ethylene/α-olefin interpolymer, and has a density, d, in grams/cubic centimeter, wherein the numerical values of Re and d satisfy the following relationship when the ethylene/α-olefin interpolymer is substantially free of a cross-linked phase: Re>1481−1629(d); or (d) has a molecular fraction which elutes between 40° C. and 130° C. when fractionated using TREF, characterized in that the fraction has a molar comonomer content of at least 5 percent higher than that of a comparable random ethylene interpolymer fraction eluting between the same temperatures, wherein said comparable random ethylene interpolymer has the same comonomer(s) and has a melt index, density, and molar comonomer content (based on the whole polymer) within 10 percent of that of the ethylene/α-olefin interpolymer; or (e) is characterized by a storage modulus at 25° C., G′(25° C.), and a storage modulus at 100° C., G′(100° C.), wherein the ratio of G′(25° C.) to G′(100° C.) is from about 1:1 to about 10:1. ### Claim 2 (depends on 1) The filled polymer composition of claim 1, wherein the ethylene/α-olefin interpolymer has a Mw/Mn from about 1.7 to about 3.5, at least one melting point, Tm, in degrees Celsius, and a density, d, in grams/cubic centimeter, wherein the numerical values of Tm and d correspond to the relationship: Tm≧858.91−1825.3(d)+1112.8(d)2. ### Claim 3 (depends on 1) The filled polymer composition of claim 1, wherein the ethylene/α-olefin interpolymer has a Mw/Mn from about 1.7 to about 3.5 and is characterized by a heat of fusion, ΔH in J/g, and a delta quantity, AT, in degrees Celsius defined as the temperature difference between the tallest DSC peak and the tallest CRYSTAF peak, wherein the numerical values of ΔT and ΔH have the following relationships: ΔT>−0.1299(ΔH)+62.81 for ΔH greater than zero and up to 130 J/g, ΔT≧48° C. for ΔH greater than 130 J/g, wherein the CRYSTAF peak is determined using at least 5 percent of the cumulative polymer, and if less than 5 percent of the polymer has an identitiable CRYSTAF peak, then the CRYSTAF temperature is 30° C. ### Claim 4 (depends on 1) The filled polymer composition of claim 1, wherein the ethylene/α-olefin interpolymer is characterized by an elastic recovery, Re, in percent at 300 percent strain and 1 cycle measured with a compression-molded film of the ethylene/α-olefin interpolymer, and has a density, d, in grams/cubic centimeter, wherein the numerical values of Re and d satisfy the following relationship when the ethylene/α-olefin interpolymer is substantially free of a cross-linked phase: Re>1481−1629(d). ### Claim 5 (depends on 1) The filled polymer composition of claim 1, wherein the numerical values of Re and d satisfy the following relationship: Re>1491−1629(d). ### Claim 6 (depends on 1) The filled polymer composition of claim 1, wherein the numerical values of Re and d satisfy the following relationship: Re>1501−1629(d). ### Claim 7 (depends on 1) The filled polymer composition of claim 1, wherein the numerical values of Re and d satisfy the following relationship: Re>1511−1629(d). ### Claim 8 (depends on 1) The filled polymer composition of claim 1, wherein the ethylene/α-olefin interpolymer has a molecular fraction which elutes between 40° C. and 130° C. when fractionated using TREF, characterized in that the fraction has a molar comonomer content of at least 5 percent higher than that of a comparable random ethylene interpolymer fraction eluting between the same temperatures, wherein said comparable random ethylene interpolymer has the same comonomer(s) and has a melt index, density, and molar comonomer content (based on the whole polymer) within 10 percent of that of the ethylene/α-olefin interpolymer. ### Claim 9 (depends on 1) The filled polymer composition of claim 1, wherein the ethylene/α-olefin interpolymer is characterized by a storage modulus at 25° C., G′(25° C.), and a storage modulus at 100° C., G′(100° C.), wherein the ratio of G′(25° C.) to G′(100° C.) is from about 1:1 to about 10:1. ### Claim 10 (depends on 1) The filled polymer composition of claim 1, wherein the α-olefin is propylene, 1-butene, 1-pentene, 1-hexene, 1-octene or a combination thereof. ### Claim 11 (depends on 1) The filled polymer composition of claim 1, wherein the ethylene/α-olefin interpolymer is present in a range from about 5% to about 70% by total weight of the composition. ### Claim 12 (depends on 1) The filled polymer composition of claim 1, wherein the filler is selected from calcium carbonate, barium sulfate, aluminum hydroxide, magnesium hydroxide, glass fibers, nano-clays, talc, carbon black or graphite, flyash, cement dust, clay, feldspar, nepheline, silica or glass, fumed silica, alumina, magnesium oxide, zinc oxide, aluminum silicate, calcium silicate, titanium dioxide, titanates, glass microspheres and chalk. ### Claim 13 (depends on 12) The filled polymer composition of claim 12, wherein the filler is selected from calcium carbonate and barium sulfate. ### Claim 14 (depends on 13) The filled polymer composition of claim 13, wherein the filler is calcium carbonate. ### Claim 15 (depends on 12) The filled polymer composition of claim 12, wherein the filler is present in a range from about 30% to about 95%. ### Claim 16 (depends on 1) The filled polymer composition of claim 1, wherein the polymer further comprises a second polymer. ### Claim 17 (depends on 16) The filled polymer composition of claim 16, wherein the second polymer is selected from polyethylene, a polypropylene, a polyvinyl chloride, ethylene-propylene copolymer, a (ethylene-co-vinyl acetate), a terpolymer of ethylene, propylene, a nonconjugated diene, a mixed polymer of ethylene and vinyl acetate, a styrene-butadiene mixed polymers and a combination thereof. ### Claim 18 A filled polymer composition comprising: (i) a polymer (ii) a filler. wherein the polymer comprises an ethylene/α-olefin interpolymer that (a) has a Mw/Mn from about 1.7 to about 3.5. at least one melting point, Tm, in degrees Celsius, and a density, d, in grams/cubic centimeter, wherein the numerical values of Tm and d correspond to the relationship: Tm>−2002.9+4538.5(d)−2422.2(d)2; or (b) has a Mw/Mn from about 1.7 to about 3.5, and is characterized by a heat of fusion, ΔH in J/g, and a delta quantity, ΔT. in degrees Celsius defined as the temperature difference between the tallest DSC peak and the tallest CRYSTAF peak, wherein the numerical values of ΔT and ΔH have the following relationships: ΔT>−0.1299(ΔH)+62.81 for ΔH greater than zero and up to 130 J/g. ΔT≧48° C. for ΔH greater than 130 J/g, wherein the CRYSTAF peak is determined using at least 5 percent of the cumulative polymer, and if less than 5 percent of the polymer has an identifiable CRYSTAF peak, then the CRYSTAF temperature is 30° C. or (c) is characterized by an elastic recovery, Re, in percent at 300 percent strain and 1 cycle measured with a compression-molded film of the ethylene/α-olefin interpolymer, and has a density, d. in grams/cubic centimeter, wherein the numerical values of Re and d satisfy the following relationship when the ethylene/α-olefin interpolymer is substantially free of a cross-linked phase: Re>1481−1629(d); or (d) has a molecular fraction which elutes between 40° C. and 130° C. when fractionated using TREF, characterized in that the fraction has a molar comonomer content of at least 5 percent higher than that of a comparable random ethylene interpolymer fraction eluting between the same temperatures, wherein said comparable random ethylene interpolymer has the same comonomer(s) and has a melt index, density, and molar comonomer content (based on the whole polymer) within 10 percent of that of the ethylene/α-olefin interpolymer; or (e) is characterized by a storage modulus at 25° C., G′(25° C.), and a storage modulus at 100° C., G′(100° C.), wherein the ratio of G′(25° C.) to G′(100° C.) is from about 1:1 to about 10:1; and (iii) a plasticizer. ### Claim 19 (depends on 18) The filled polymer composition of claim 18, wherein the plasticizer comprises a processing oil, an epoxidized oil, a polyester, a polyether, a polyether ester or a combination thereof. ### Claim 20 (depends on 19) The filled polymer composition of claim 19, wherein the plasticizer comprises paraffinic processing oil and stearic acid. ### Claim 21 (depends on 18) The filled polymer composition of claim 18, wherein the plasticizer is a present in an amount from about 1% up to about 15%. ### Claim 22 (depends on 18) The filled polymer composition of claim 18, wherein the filler is selected from aluminum hydroxide and magnesium hydroxide. ### Claim 23 (depends on 1) The filled polymer composition of claim 1, wherein the polymer is a blend of ethylene/α-olefin copolymers. ### Claim 24 (depends on 1) A sound deadening article comprising the filled polymer composition of claim 1. ### Claim 25 (depends on 1) An automotive carpet comprising the filled polymer composition of claim 1. ### Claim 26 (depends on 1) A roofing material comprising the filled polymer composition of claim 1. ### Claim 27 (depends on 1) A wire or cable coating comprising the filled polymer composition of claim 1. ### Claim 28 (depends on 1) A floor tile comprising the filled polymer composition of claim 1. ### Claim 29 (depends on 1) A floor sheet comprising the filled polymer composition of claim 1. ### Claim 30 (depends on 1) A profile comprising the filled polymer composition of claim 1. ### Claim 31 (depends on 1) A gasket comprising the filled polymer composition of claim 1. ### Claim 32 (depends on 1) A floor mat comprising the filled polymer composition of claim 1. ### Claim 33 A filled polymer composition comprising: (i) a polymer and (ii) a filler, wherein the polymer comprises an ethylene/α-olefin multi-block interpolymer comprising at least 50 mole percent ethylene that has (a) at least a molecular fraction which elutes between 40° C. and 130° C. when fractionated using TREF, characterized in that the fraction has a block index of at least 0.5 and up to about 1 or (b) an average block index greater than zero and up to about 1.0 and a molecular weight distribution, Mw/Mn, greater than about 1.3. ### Claim 34 (depends on 33) The filled polymer composition of claim 33, wherein the ethylene/α-olefin interpolymer has at least a molecular fraction which elutes between 40° C. and 130° C. when fractionated using TREF, characterized in that the fraction has a block index of at least 0.5 and up to about 1. ### Claim 35 (depends on 33) The filled polymer composition of claim 33, wherein the ethylene/α-olefin interpolymer has an average block index greater than zero and up to about 1.0 and a molecular weight distribution, Mw/Mn, greater than about 1.3. ### Claim 36 (depends on 33) The filled polymer composition of claim 33, wherein the α-olefin is propylene, 1-butene, 1-pentene, I -hexene, 1-octene or a combination thereof. ### Claim 37 (depends on 33) The filled polymer composition of claim 33, wherein the ethylene/α-olefin interpolymer is present in a range from about 5% to about 70% by total weight of the composition. ### Claim 38 (depends on 33) The filled polymer composition of claim 33, wherein the filler is selected from calcium carbonate, barium sulfate, aluminum hydroxide, magnesium hydroxide, glass fibers, nano-clays, talc, carbon black or graphite, flyash, cement dust, clay, feldspar, nepheline, silica or glass, fumed silica, alumina, magnesium oxide, zinc oxide, aluminum silicate, calcium silicate, titanium dioxide, titanates, glass microspheres and chalk. ### Claim 39 (depends on 38) The filled polymer composition of claim 38, wherein the filler is calcium carbonate. ### Claim 40 (depends on 33) The filled polymer composition of claim 33, wherein the filler is present in a range from about 30% to about 95%. ### Claim 41 (depends on 33) The filled polymer composition of claim 33, wherein the polymer further comprises a second polymer. ### Claim 42 (depends on 41) The filled polymer composition of claim 41, wherein the second polymer is selected from polyethylene, a polypropylene, a polyvinyl chloride, ethylene-propylene copolymer, a (ethylene-co-vinyl acetate), a terpolymer of ethylene, propylene, a nonconjugated diene, a mixed polymer of ethylene and vinyl acetate, a styrene-butadiene mixed polymers and a combination thereof. ### Claim 43 (depends on 33) The filled polymer composition of claim 33, wherein the composition further comprises at least a plasticizer. ### Claim 44 (depends on 43) The filled polymer composition of claim 43, wherein the plasticizer comprises a processing oil, an epoxidized oil, a polyester, a polyether, a polyether ester or a combination thereof. ### Claim 45 (depends on 44) The filled polymer composition of claim 44, wherein the plasticizer comprises paraffinic processing oil and stearic acid. ### Claim 46 (depends on 43) The filled polymer composition of claim 43, wherein the plasticizer is a present in an amount from about 1% up to about 15%. ### Claim 47 (depends on 33) The filled polymer composition of claim 33, wherein the polymer is a blend of ethylene/α-olefin copolymers. ### Claim 48 (depends on 33) A sound deadening article comprising the filled polymer composition of claim 33. ### Claim 49 (depends on 33) An automotive carpet comprising the filled polymer composition of claim 33. ### Claim 50 (depends on 33) A roofing material comprising the filled polymer composition of claim 33. ### Claim 51 (depends on 33) A wire or cable coating comprising the filled polymer composition of claim 33. ### Claim 52 (depends on 33) A floor tile comprising the filled polymer composition of claim 33. ### Claim 53 (depends on 33) A floor sheet comprising the filled polymer composition of claim 33. ### Claim 54 (depends on 33) A profile comprising the filled polymer composition of claim 33. ### Claim 55 (depends on 33) A gasket comprising the filled polymer composition of claim 33. ### Claim 56 (depends on 33) A floor mat comprising the filled polymer composition of claim 33. ### Claim 57 (depends on 18) The filled polymer composition of claim 18, wherein the filler is selected from calcium carbonate, barium sulfate, aluminum hydroxide, magnesium hydroxide, glass fibers, nano-clays, talc, carbon black or graphite, flyash, cement dust, clay, feldspar, nepheline, silica or glass, fumed silica, alumina, magnesium oxide, zinc oxide, aluminum silicate, calcium silicate, titanium dioxide, titanates, glass microspheres and chalk. ### Claim 58 (depends on 18) The filled polymer composition of claim 18, wherein the filler is selected from calcium carbonate and barium sulfate.