COPOLYCARBONATE COMPOSITIONS WITH IMPROVED PROCESSING BEHAVIOUR CONTAINING PE-WAX

Abstract

The invention relates to copolycarbonate compositions containing oxidized, acid-modified polyethylene wax, to their use for producing blends and moldings and to moldings obtained therewith. Said copolycarbonate compositions have an improved processing behaviour.

Claims

1.-15. (canceled)

16. A composition comprising A) 67.0 to 99.95 wt % of one or more copolycarbonates comprising monomer units selected from the group consisting of the structural units of general formulae (1a), (1b), (1c) and (1d) ##STR00015## in which R.sup.1 represents hydrogen or C.sub.1-C.sub.4-alkyl, R2 represents C1-C4-alkyl, n represents 0, 1, 2 or 3 and R.sup.3 represents C.sub.1-C.sub.4-alkyl, aralkyl or aryl, or 67.0 to 99.95 wt % of a blend of the one or more copolycarbonates and at least one further homo- or copolycarbonate comprising one or more monomer units of general formula (2): ##STR00016## in which R.sup.4 represents H, linear or branched C.sub.1-C.sub.10(alkyl and R.sup.5 represents linear or branched C.sub.1-C.sub.10alkyl; wherein the optionally present further homo- or copolycarbonate has no monomer units of formulae (1a), (1b), (1c) and (1d); B) 0.05 to 10.0 wt % of at least one oxidized acid-modified polyethylene wax; and C) optionally one or more additives and/or fillers in a total amount of up to 30.0 wt %.

17. The composition as claimed in claim 16, wherein the oxidation index of the oxidized acid-modified polyethylene wax is greater than 8.

18. The composition as claimed in claim 16, wherein the oxidized acid-modified polyethylene wax has an acid number between 0.5 and 20 mg KOH/g, a crystallinity of not less than 60% and not more than 90% and a melting temperature between 90° C. and 130° C.

19. The composition as claimed in claim 16, wherein the oxidized acid-modified polyethylene wax has a melt viscosity, determined as per ISO 11443, between 70 mPa.Math.s and 800 mPa.Math.s.

20. The composition as claimed in claim 16, wherein the amount of oxidized acid-modified polyethylene wax is 0.10 to 5.0 wt %.

21. The composition as claimed in claim 16, wherein the total proportion of the monomer units of formulae (1a), (1 b), (1c) and (1d) in the copolycarbonate is 0.1-88 mol % (based on the sum of the diphenol monomer units present therein).

22. The composition as claimed in claim 16, wherein the composition comprises the one or more copolycarbonates comprising one or more monomer units of formulae (1a), (1b), (1c) and/or (1d) in an amount of at least 60 wt %.

23. The composition as claimed in claim 16, wherein the copolycarbonate comprising the monomer units of formulae (1a), (1b), (1c) and/or (1d) further comprises monomer units of formula (3) ##STR00017## in which R.sup.6 and R.sup.7 independently of one another represent H, C.sub.1-C.sub.18-alkyl-, C.sub.1-C.sub.18-alkoxy, halogen such as Cl or Br or respectively optionally substituted aryl or aralkyl and Y represents a single bond, —SO.sub.2—, —CO—, —O—, —S—, C.sub.1-C.sub.6-alkylene or C.sub.2-C.sub.5-alkylidene, furthermore C.sub.6-C.sub.12-arylene, which may optionally be fused with further heteroatom-comprising aromatic rings.

24. The composition as claimed in claim 16, wherein the copolycarbonate comprises monomer units derived from compounds of general formulae (1a″), (1b′), (1c′) and/or (1d′) in combination with monomer units derived from compounds of general formula (3c), ##STR00018## wherein R.sup.3 is methyl or phenyl.

25. The composition as claimed in claim 16, wherein the composition comprises as component A) a blend of the copolycarbonate and the further homo- or copolycarbonate comprising one or more monomer units of general formula (2), wherein R.sup.4 represents H and R.sup.5 represents linear or branched C.sub.1-C.sub.6 alkyl.

26. The composition as claimed in claim 16, wherein the composition comprises one or more additives selected from the group consisting of thermal stabilizers, demolding agents and UV stabilizers.

27. The composition according to claim 16, wherein the composition comprises an inorganic filler.

28. The composition as claimed in claim 16, wherein the composition comprises 0.002 to 0.2 wt % of thelinal stabilizer, 0.01 wt % to 1.00 wt % of UV stabilizer and 0.05 wt % to 2.00 wt % of demolding agent.

29. A blend, molding, extrudate, film or film laminate obtainable from copolycarbonate compositions as claimed in claim 16 or else a molding, extrudate or film comprising coextrusion layers obtainable from copolycarbonate compositions as claimed in claim 16.

30. A method comprising utilizing oxidized acid-modified polyethylene waxes for improving the flowability of compositions comprising a copolycarbonate as claimed in claim 16 or a blend of the copolycarbonate and a further homo- or copolycarbonate as claimed in claim 16.

Description

EXAMPLES

[0167] Raw Materials Used: [0168] Component A is a blend of PC1 and PC2 (examples 1-4), copolycarbonate PC3 or PC4(examples 5 to 12) or one of copolycarbonates PC5 to PC11 (see table 7, examples 13-40). [0169] PC 1 is a commercially available copolycarbonate based on bisphenol A and bisphenol TMC having an MVR of 18 cm.sup.3/10 min (330° C./2.16 kg) and a softening temperature (VST/B 120) of 183° C. (Apec 1895 from Bayer MaterialScience AG). [0170] PC 2 is a polycarbonate powder based on bisphenol A having an MVR of 6 cm.sup.3/10 min (300° C./1.2 kg). It serves to improve incorporation (metering) of the PE wax. [0171] PC 3 Lexan XHT2141; high heat copolycarbonate based on bisphenol A and the bisphenol of formula)(Ib′) where R.sup.3 =phenyl from Sabic Innovative Plastics having an MVR of 43 cm.sup.3/10 min (330° C., 2.16 kg) [0172] PC 4 Lexan XHT4143; UV stabilized high heat copolycarbonate based on bisphenol A and the bisphenol of formula (Ib′) where R.sup.3 phenyl from Sabic Innovative Plastics [0173] Component B (PE wax): Oxidized acid-modified polyethylene wax having a molecular weight of 4000 g/mol, an acid number of 1 mg KOH/g, a degree of crystallization of 80% and a melting point (DSC) of 121° C. and also a melt viscosity (at 140° C.) of 650 mPa*s. Hi-Wax 405MP from Mitsui Chemicals Inc. was used. The oxidation index OI as determined by IR spectroscopy was 55.4. The determination was effected with a commercially available FT IR spectrometer, for example Nicolet 5700 or Thermo Fisher Scientific 20DX FT IR instrument. The ratio of the area of the peak between 1750 cm.sup.−1 and 1680 cm.sup.−1 (carbonyl) to the area of the peak between 1400 cm.sup.−1 and 1330 cm.sup.−1 (aliphatics CHx) was established. The calculation was as follows: C═O area/aliphatics area*100.

Synthesis of the bisphenol of Formula (Ib′) where R.SUP.3.=methyl:

[0174] ##STR00014##

[0175] A flange reactor is initially charged with a solution of 2 kg (20.2 mol) of N-methylpyrrolidone (NMP) and 1273.3 g (4 mol) of phenolphthalein. 2 liters of water and then 18 mol of a 40% aqueous methylamine solution are added with stirring. The reaction solution turns violet upon addition of the methylamine. The mixture is then stirred for a further 8 hours at 82° C. utilizing a dry ice cooler. This causes the coloring of the reaction batch to change to dark yellowish. Once the reaction has ended the reaction batch is precipitated by means of a dropping funnel with stirring into a reservoir of water acidified with hydrochloric acid.

[0176] The precipitated white reaction product is slurried with 2 liters of water and then suctioned off using a G3 frit. The crude product obtained is redissolved in 3.5 liters of a dilute sodium hydroxide solution (16 mol) and in turn precipitated in a reservoir of water acidified with hydrochloric acid. The reprecipitated crude product is repeatedly slurried with 2 liters of water and then suctioned off each time. This washing procedure is repeated until the conductivity of the washing water is less than 15 μS.

[0177] The thus obtained product is dried to constant mass in a vacuum drying cabinet at 90° C.,

[0178] After 4-fold performance of the experiment the following yields were obtained in each case: [0179] 1a) 950 g of a white solid [0180] 1b) 890 g of a white solid [0181] 1c) 1120 g of a white solid [0182] 1d) 1050 g of a white solid [0183] (melting point 264° C.)

[0184] Characterization of the obtained bisphenol was effected by .sup.1H-NMR spectroscopy.

Synthesis of copolycarbonate based on a bisphenol of formula (1b′) where R.SUP.3.=methyl and bisphenol A:

[0185] To a nitrogen-inertized solution of 532.01 g (1.6055 mol) of bisphenol A (BPA), 2601.36 g (11.39 mol) of bisphenol from example 1, 93.74 g (0.624 mol, 4.8 mol % based on diphenols) of p-tert-butylphenol (BUP) as chain terminator and 1196 g (29.9 mol) sodium hydroxide in 25.9 liters of water are added 11.79 liters of methylene chloride and 14.1 liters of chlorobenzene. At a pH of 12.5-13.5 and 20° C., 2.057 kg (20.8 mol) of phosgene are introduced. In order to prevent the pH from falling below 12.5, 30% sodium hydroxide was added during the phosgenation. Once phosgenation is complete and after purging with nitrogen the mixture is stirred for a further 30 minutes, 14.7 g (0.13 mol, 1 mol % based on diphenols) of N-ethylpiperidine are added as catalyst and the mixture is stirred for a further 1 hour. After removal of the aqueous phase and acidification with phosphoric acid the organic phase is washed several times with water using a separator until salt-free. The organic phase is separated off and subjected to a solvent exchange in which methylene chloride is replaced with chlorobenzene. The concentrated copolycarbonate solution in chlorobenzene is then freed of solvent using a vented extruder. The obtained polycarbonate melt extrudates are cooled in a water bath, drawn off and finally palletized. Transparent polycarbonate pellets are obtained.

Synthesis of copolycarbonates PC5 to PC11

[0186] Copolycarbonates PC-5 to PC-11 were produced as per the preceding procedure for producing copolycarbonate based on a bisphenol of formula (Ib′) where R.sup.3=methyl and bisphenol A (see table 7 for stoichiometry).

Synthesis of the copolycarbonate Compositions of Examples 1-4

[0187] The copolycarbonate compositions of examples 1-4 based on raw materials PC1 and PC2 and also component B are mixed according to the formulations reported in table 1 in a twin-screw extruder at 300° C. The thus-obtained polymer compositions are pelletized and are ready for polymer-physical characterization.

Synthesis of the copolycarbonate Compositions of Examples 1-4

[0188] The polycarbonate compositions of examples 5 to 40 are produced in a DSM Miniextruder based on the raw materials stated. The melt temperature was 330° C. The thus-obtained polymer compositions are pelletized and are ready for polymer physical characterization.

[0189] Characterization of the Molding Materials According to the Invention (Test Methods)

[0190] Characterization of the molding materials according to the invention (test methods): Melt volume flow rate (MVR) was determined in accordance with ISO 1133 (at a test temperature of 330° C., mass 2.16 kg) using a Zwick 4106 instrument from Roell.

[0191] Vicat softening temperature VST/B120 was determined as a measure of heat distortion resistance in accordance with ISO 306 on test specimens measuring 80 mm×10 mm×4 mm with a 50 N ram loading and a heating rate of 50° C./h or of 120° C./h with a Coesfeld Eco 2920 instrument from Coesfeld Materialtest.

[0192] Modulus of elasticity was measured according to ISO 527 on single side injection-molded shoulder bars having a core measuring 80×10×4 mm.

[0193] Spiral flow: Either a defined length is set or a defined pressure is specified. The test specimen geometry is 8×2 mm, the flow length is obtained from the test.

[0194] The comparative value is set to a defined flow length. The samples to be measured are characterized under identical conditions. Larger numerical values indicate improved flowability (longer flow length).

[0195] The rheological tests were performed with an MCR 301 cone-and-plate rheometer with a CP 25 measuring cone and the conditions reported below: [0196] Test method: Oscillation—cone and plate [0197] Frequency: 75 to 0.08 Hz=angular frequency of 471 to 0.5 [1/s] [0198] Deformation: 10% -20 measurement points [0199] Temperatures: 300° C., 280° C. and 260° C., +−0.3° C.

TABLE-US-00001 TABLE 1 Compositions and experimental data for examples 1-4 Examples: 1 (comparison) 2 3 4 PC-1 % 93   93 93 93 PC-2 % 7  5.5 4 2.5 PE wax % 1.5 3 4.5 MVR ml/10 min 15.8 17.0 18.1 21.0 330° C./ 2.16 kg Vicat VSTB ° C. 181.4  180.0 178.9 178.4 120 Modulus of N/mm.sup.2 2524    2500 2454 2410 elasticity Spiral flow cm 25*  26.5 34 56 The % values are wt % values in each case.

[0200] It is clearly apparent that the MVR is significantly increased due to the addition of the PE wax, i.e. the melt viscosity is reduced and the flowability is thus increased. The Vicat temperature is only slightly reduced by addition of the PE wax but remains a high range even at large amount. The tensile modulus is only slightly reduced by addition of the PE wax but remains a high range even at large amount. It is apparent from the spiral flow values that addition of the oxidized polyethylene wax achieves a marked improvement in flowability.

TABLE-US-00002 TABLE 2 Melt viscosities of the compositions of examples 1-4 The values in the following table are each reported together with the shear rates in [1/sec]. Examples 1 (comparison) 2 3 4 Melt visc. at 300° C. eta 50 Pa .Math. s 1683 948 617 410 eta 100 Pa .Math. s 1506 813 525 295 eta 200 Pa .Math. s 1268 676 447 219 eta 500 Pa .Math. s 851 537 332 139 eta 1000 Pa .Math. s 608 424 275 96 eta 1500 Pa .Math. s 483 376 234 82 eta 5000 Pa .Math. s 223 196 138 43 Melt visc. at 320° C. eta 50 Pa .Math. s 919 646 449 282 eta 100 Pa .Math. s 861 540 372 217 eta 200 Pa .Math. s 784 457 309 148 eta 500 Pa .Math. s 607 339 222 105 eta 1000 Pa .Math. s 440 262 176 72 eta 1500 Pa .Math. s 347 233 150 59 eta 5000 Pa .Math. s 157 139 81 33 Melt visc. at 330° C. eta 50 Pa .Math. s 604 490 331 257 eta 100 Pa .Math. s 593 437 288 180 eta 200 Pa .Math. s 556 368 229 135 eta 500 Pa .Math. s 457 281 180 96 eta 1000 Pa .Math. s 352 217 142 68 eta 1500 Pa .Math. s 286 186 118 54 eta 5000 Pa .Math. s 135 114 63 29 Melt visc. at 340° C. eta 50 Pa .Math. s 439 347 269 219 eta 100 Pa .Math. s 429 316 229 167 eta 200 Pa .Math. s 410 267 195 123 eta 500 Pa .Math. s 347 209 146 86 eta 1000 Pa .Math. s 280 168 117 65 eta 1500 Pa .Math. s 234 148 99 50 eta 5000 Pa .Math. s 116 93 53 26 Melt visc. at 360° C. eta 50 Pa .Math. s 215 198 190 135 eta 100 Pa .Math. s 214 186 170 107 eta 200 Pa .Math. s 213 166 140 80 eta 500 Pa .Math. s 193 127 105 56 eta 1000 Pa .Math. s 166 102 78 44 eta 1500 Pa .Math. s 148 91 67 36 eta 5000 Pa .Math. s 85 61 40 18

[0201] It is apparent from the melt viscosities that a marked improvement in flowability is achieved through addition of the oxidized polyethylene wax for all temperatures of the processing-relevant range and over all shear rates.

TABLE-US-00003 TABLE 3 Composition of the compounds of examples 5-12 Example 5 (com- 9 (com- parison) 6 7 8 parison) 10 11 12 PC-3 % 100 99.5 99.0 98.0 PC-4 % 100 99.5 99.0 98.0 PE Wax % 0.5 1.0 2.0 0.5 1.0 2.0 Tg [° C.] 164.1 165.0 164.9 164.7 183.9 183.4 183.8 184.3 The % values are wt % values in each case.

TABLE-US-00004 TABLE 4 Melt viscosity at angular frequency of 471 to 0.503 [Hz] Example Cone/plate 5 9 rheology (comp.) 6 7 8 (comp.) 10 11 12 Melt visc. at 260° C. [Hz] 471 Pa .Math. s 1260 1310 1310 1240 2080 2080 1940 1450 329 Pa .Math. s 1520 1580 1570 1480 2570 2600 2430 1960 229 Pa .Math. s 1780 1860 1840 1730 3120 3170 3030 2340 160 Pa .Math. s 2050 2140 2120 1990 3720 3790 3680 2980 112 Pa .Math. s 2320 2430 2410 2260 4370 4470 4400 3810 77.8 Pa .Math. s 2580 2700 2680 2520 5160 5290 5250 4780 54.3 Pa .Math. s 2830 2950 2940 2760 6030 6180 6180 5730 37.9 Pa .Math. s 3050 3180 3170 2970 6930 7100 7160 6620 26.4 Pa .Math. s 3230 3380 3360 3160 7850 8040 8160 7560 18.4 Pa .Math. s 3390 3540 3530 3310 8770 8980 9180 8520 12.9 Pa .Math. s 3510 3670 3660 3430 9670 9950 10200 9640 8.97 Pa .Math. s 3600 3760 3760 3530 10600 10900 11200 10500 6.25 Pa .Math. s 3660 3840 3840 3610 11500 11800 12100 11200 4.36 Pa .Math. s 3710 3890 3900 3670 12300 12500 12900 11800 3.04 Pa .Math. s 3750 3940 3950 3730 12900 13000 13400 12300 2.12 Pa .Math. s 3770 3960 3990 3770 13300 13400 13800 12600 1.48 Pa .Math. s 3790 3990 4020 3820 13600 13700 14200 12900 1.03 Pa .Math. s 3800 4010 4050 3860 13800 13900 14400 13200 0.721 Pa .Math. s 3810 4020 4070 3890 14000 14100 14700 13400 0.503 Pa .Math. s 3810 4030 4080 3910 14100 14200 14800 13500 Melt visc. at 280° C. [Hz] 471 Pa .Math. s 570 621 613 594 815 934 840 866 329 Pa .Math. s 695 710 696 675 1060 1130 1070 1090 229 Pa .Math. s 800 794 776 751 1320 1340 1300 1310 160 Pa .Math. s 892 871 850 823 1590 1560 1530 1540 112 Pa .Math. s 967 940 917 887 1860 1770 1750 1760 77.8 Pa .Math. s 1030 1000 975 943 2100 1980 1960 1970 54.3 Pa .Math. s 1080 1050 1020 991 2310 2180 2140 2160 37.9 Pa .Math. s 1130 1090 1060 1030 2490 2350 2300 2330 26.4 Pa .Math. s 1160 1120 1090 1060 2650 2500 2440 2480 18.4 Pa .Math. s 1180 1150 1120 1080 2790 2620 2560 2600 12.9 Pa .Math. s 1200 1160 1130 1100 2890 2710 2650 2700 8.97 Pa .Math. s 1210 1180 1150 1110 2970 2780 2720 2780 6.25 Pa .Math. s 1220 1180 1160 1130 3030 2840 2770 2840 4.36 Pa .Math. s 1220 1190 1170 1140 3070 2870 2810 2880 3.04 Pa .Math. s 1230 1200 1180 1160 3090 2900 2850 2930 2.12 Pa .Math. s 1230 1200 1180 1170 3110 2920 2870 2960 1.48 Pa .Math. s 1230 1200 1190 1180 3120 2940 2890 3000 1.03 Pa .Math. s 1230 1200 1190 1180 3120 2950 2910 3030 0.721 Pa .Math. s 1230 1200 1200 1190 3120 2950 2920 3050 0.503 Pa .Math. s 1230 1200 1190 1190 3120 2950 2910 3070 Melt visc. at 300° C. [Hz] 471 Pa .Math. s 366 334 344 327 558 545 510 526 329 Pa .Math. s 399 362 374 355 648 625 577 599 229 Pa .Math. s 430 387 401 380 731 698 641 668 160 Pa .Math. s 457 408 424 401 804 765 700 730 112 Pa .Math. s 479 426 442 418 868 825 752 785 77.8 Pa .Math. s 496 439 457 431 923 876 796 832 54.3 Pa .Math. s 510 449 469 441 967 918 832 869 37.9 Pa .Math. s 520 457 478 449 1000 951 861 899 26.4 Pa .Math. s 528 462 484 456 1030 977 882 922 18.4 Pa .Math. s 533 466 490 461 1050 995 899 940 12.9 Pa .Math. s 536 469 494 466 1060 1010 911 954 8.97 Pa .Math. s 538 471 498 471 1070 1020 920 965 6.25 Pa .Math. s 540 472 501 476 1070 1020 927 975 4.36 Pa .Math. s 542 473 503 481 1070 1030 933 985 3.04 Pa .Math. s 543 474 506 485 1080 1030 938 995 2.12 Pa .Math. s 544 474 507 488 1080 1030 941 1000 1.48 Pa .Math. s 545 475 509 491 1070 1030 943 1010 1.03 Pa .Math. s 547 476 511 493 1070 1030 944 1010 0.721 Pa .Math. s 549 477 514 495 1070 1030 944 1020 0.503 Pa .Math. s 552 478 515 494 1070 1030 939 1010

[0202] Table 4 shows that compared to the inventive examples 6, 7, 8 and 10, 11, 12, the comparative examples 5 and 9 which do not comprise the flow assistant exhibit higher melt viscosities and thus have poorer flowability at the three measurement temperatures.

TABLE-US-00005 TABLE 5 Composition of the copolycarbonates PC-5 to PC-11 Copolycarbonate no. based on: PC-5 PC-6 PC-7 PC-8 PC-9 PC-10 PC-11 Bisphenol according to formula (1b′) where R.sup.3 = methyl [mol %] 77.93 78.5 77.5 76.5 80 80 80 [wt %] 70.9 71.6 70.4 69.2 73.4 73.4 73.4 Bisphenol A (BPA) [mol %] 22.07 21.5 22.5 23.5 20 20 20 [wt %] 29.1 28.4 29.6 30.8 26.6 26.6 26.6 Glass transition temper- ature Tg [° C.] 179.4 179.6 179.6 182.3 175.3 176.1 173.9 η.sub.rel — 1.234 1.225 1.237 1.216 1.228 1.218

TABLE-US-00006 TABLE 6 Composition of the compounds of examples 13-40 PE PC-9 PC-10 PC-11 PC-6 PC-7 PC-8 PC-5 wax Tg Example % % % % % % % % ° C. 13 100 176.7 (comparative) 14 99.5 0.5 175.5 15 99.0 1 175.3 16 98.0 2 175.3 17 100 177.1 (comparative) 18 99.5 0.5 176.2 19 99.0 1 174.8 20 98.0 2 175.0 21 100 173.4 (comparative) 22 99.5 0.5 173.6 23 99.0 1 172.7 24 98.0 2 172.9 25 100 179.0 (comparative) 26 99.5 0.5 177.7 27 99.0 1 176.4 28 98.0 2 176.2 29 100 180.1 (comparative) 30 99.5 0.5 179.5 31 99.0 1 178.7 32 98.0 2 178.5 33 100 184.3 (comparative) 34 99.5 0.5 183.2 35 99.0 1 184.8 36 98.0 2 183.2 37 100 180.3 (comparative) 38 99.5 0.5 179.3 39 99.0 1 178.9 40 98.0 2 178.3 The % values are wt % values in each case.

TABLE-US-00007 TABLE 7 Melt viscosity at angular frequency of 471 to 0.503 [Hz]: Example Cone/plate 13 (com- 17 (com- rheology parison) 14 15 16 parison) 18 19 20 Melt visc. at 260° C. [Hz] 471 Pa .Math. s 366 346 327 323 259 207 170 157 329 Pa .Math. s 399 377 356 350 280 221 180 165 229 Pa .Math. s 429 407 383 376 299 234 189 172 160 Pa .Math. s 456 433 406 398 315 244 196 178 112 Pa .Math. s 479 456 425 417 330 253 203 183 77.8 Pa .Math. s 497 475 441 432 341 261 208 188 54.3 Pa .Math. s 511 490 453 445 351 268 212 192 37.9 Pa .Math. s 521 501 463 454 359 273 216 198 26.4 Pa .Math. s 529 510 471 463 365 278 221 207 18.4 Pa .Math. s 533 516 476 469 369 282 224 217 12.9 Pa .Math. s 535 520 479 474 373 285 228 231 8.97 Pa .Math. s 536 523 482 479 377 290 232 252 6.25 Pa .Math. s 536 524 484 484 380 294 237 283 4.36 Pa .Math. s 535 525 485 488 383 298 241 329 3.04 Pa .Math. s 534 526 485 491 386 303 246 398 2.12 Pa .Math. s 531 525 484 492 390 309 252 505 1.48 Pa .Math. s 529 525 483 493 395 316 259 659 1.03 Pa .Math. s 527 527 482 492 401 325 267 888 0.721 Pa .Math. s 524 529 481 490 409 335 276 1230 0.503 Pa .Math. s 519 531 485 419 346 286 1700 Melt visc. at 280° C. [Hz] 471 Pa .Math. s 111 86 87 76 414 358 263 201 329 Pa .Math. s 184 82 73 75 458 393 285 216 229 Pa .Math. s 832 69 95 55 502 427 305 231 160 Pa .Math. s 929 93 94 75 542 457 323 243 112 Pa .Math. s 1020 945 865 854 577 484 338 254 77.8 Pa .Math. s 1100 1020 928 914 608 507 350 263 54.3 Pa .Math. s 1170 1080 983 966 635 526 360 271 37.9 Pa .Math. s 1230 1130 1030 1010 656 541 368 278 26.4 Pa .Math. s 1280 1170 1070 1050 674 554 374 286 18.4 Pa .Math. s 1330 1200 1100 1080 686 563 380 290 12.9 Pa .Math. s 1350 1230 1120 1100 696 570 385 296 8.97 Pa .Math. s 1370 1250 1140 1120 703 576 390 302 6.25 Pa .Math. s 1390 1260 1150 1130 708 580 395 309 4.36 Pa .Math. s 1400 1270 1160 1150 712 584 400 317 3.04 Pa .Math. s 1410 1280 1170 1160 716 588 405 325 2.12 Pa .Math. s 1410 1280 1180 1170 718 592 410 333 1.48 Pa .Math. s 1410 1290 1180 1180 722 597 416 343 1.03 Pa .Math. s 1410 1290 1180 1180 725 603 424 353 0.721 Pa .Math. s 1410 1280 1180 1190 729 612 434 365 0.503 Pa .Math. s 1410 1280 1170 1180 733 624 446 379 Melt visc. at 300° C. [Hz] 471 Pa .Math. s 860 1040 880 1010 970 674 729 741 329 Pa .Math. s 1150 1420 1290 1400 1200 906 835 879 229 Pa .Math. s 1480 1820 1640 1800 1410 1120 945 1010 160 Pa .Math. s 1910 2300 2160 2230 1610 1290 1050 1130 112 Pa .Math. s 2400 2740 2660 2620 1790 1440 1150 1250 77.8 Pa .Math. s 2850 3130 3070 2980 1970 1570 1230 1350 54.3 Pa .Math. s 3200 3500 3430 3320 2140 1690 1310 1440 37.9 Pa .Math. s 3530 3850 3760 3650 2280 1790 1370 1520 26.4 Pa .Math. s 3830 4170 4070 3940 2410 1870 1420 1590 18.4 Pa .Math. s 4100 4450 4340 4200 2510 1940 1470 1640 12.9 Pa .Math. s 4340 4700 4580 4430 2600 2000 1500 1690 8.97 Pa .Math. s 4540 4900 4770 4620 2660 2040 1520 1720 6.25 Pa .Math. s 4700 5070 4930 4780 2710 2070 1540 1750 4.36 Pa .Math. s 4830 5200 5060 4910 2750 2100 1560 1780 3.04 Pa .Math. s 4940 5300 5160 5020 2770 2110 1570 1810 2.12 Pa .Math. s 5020 5380 5240 5110 2790 2120 1580 1850 1.48 Pa .Math. s 5080 5430 5300 5180 2800 2130 1600 1890 1.03 Pa .Math. s 5110 5460 5340 5250 2810 2140 1610 1930 0.721 Pa .Math. s 5130 5470 5370 5290 2810 2150 1620 1970 0.503 Pa .Math. s 5130 5460 5360 5310 2800 2140 1630 2050 Example Cone/plate 21 (com- 25 (com- rheology parison) 22 23 24 parison) 26 27 28 Melt visc. at 260° C. [Hz] 471 132 85 71 71 296 221 182 133 329 Pa .Math. s 140 89 73 73 322 238 194 140 229 Pa .Math. s 146 92 75 75 348 254 204 146 160 Pa .Math. s 152 95 76 76 371 268 211 150 112 Pa .Math. s 157 96 77 76 390 279 217 154 77.8 Pa .Math. s 160 98 77 77 407 289 222 156 54.3 Pa .Math. s 164 99 78 77 420 296 225 158 37.9 Pa .Math. s 167 100 78 78 431 301 227 159 26.4 Pa .Math. s 171 102 79 79 439 305 229 161 18.4 Pa .Math. s 173 102 79 79 444 307 230 162 12.9 Pa .Math. s 176 103 80 80 448 308 231 163 8.97 Pa .Math. s 180 104 80 80 451 309 231 165 6.25 Pa .Math. s 186 105 81 81 452 309 231 166 4.36 Pa .Math. s 194 108 82 82 454 309 231 167 3.04 Pa .Math. s 206 111 83 84 455 309 231 169 2.12 Pa .Math. s 222 116 85 86 456 309 231 171 1.48 Pa .Math. s 244 123 89 89 458 310 233 173 1.03 Pa .Math. s 272 133 93 93 461 311 235 177 0.721 Pa .Math. s 307 147 98 99 466 314 238 183 0.503 Pa .Math. s 354 167 105 105 472 317 244 191 Melt visc. at 280° C. 471 321 259 225 206 751 619 489 480 329 Pa .Math. s 343 277 240 218 860 705 582 542 229 Pa .Math. s 362 294 253 229 970 788 656 599 160 Pa .Math. s 379 308 264 238 1080 865 718 649 112 Pa .Math. s 392 320 273 244 1170 935 770 693 77.8 Pa .Math. s 401 329 280 250 1260 996 814 731 54.3 Pa .Math. s 407 336 286 253 1340 1050 849 761 37.9 Pa .Math. s 411 341 290 257 1400 1090 877 786 26.4 Pa .Math. s 414 346 294 259 1450 1120 898 806 18.4 Pa .Math. s 415 349 297 262 1490 1140 915 821 12.9 Pa .Math. s 415 352 300 265 1520 1160 928 834 8.97 Pa .Math. s 416 355 303 268 1540 1170 937 846 6.25 Pa .Math. s 416 357 306 272 1550 1180 945 857 4.36 Pa .Math. s 416 359 309 275 1560 1190 952 868 3.04 Pa .Math. s 417 363 313 278 1570 1190 958 881 2.12 Pa .Math. s 418 366 316 281 1570 1190 960 891 1.48 Pa .Math. s 421 370 321 285 1570 1200 963 901 1.03 Pa .Math. s 425 377 327 289 1570 1200 967 910 0.721 Pa .Math. s 431 385 336 295 1570 1200 967 917 0.503 Pa .Math. s 439 395 346 303 1570 1190 965 922 Melt visc. at 300° C. 471 Pa .Math. s 648 533 507 489 913 1150 749 841 329 Pa .Math. s 741 603 567 545 1260 1380 1030 985 229 Pa .Math. s 831 669 623 598 1610 1630 1310 1140 160 Pa .Math. s 917 730 675 648 2050 1890 1560 1290 112 Pa .Math. s 997 784 720 691 2480 2160 1790 1450 77.8 Pa .Math. s 1070 832 758 728 2850 2430 1980 1590 54.3 Pa .Math. s 1130 871 788 758 3200 2700 2160 1720 37.9 Pa .Math. s 1180 903 813 782 3520 2940 2320 1830 26.4 Pa .Math. s 1220 928 831 800 3810 3150 2460 1920 18.4 Pa .Math. s 1250 947 845 814 4070 3340 2570 1990 12.9 Pa .Math. s 1270 962 856 826 4280 3490 2660 2050 8.97 Pa .Math. s 1290 973 864 836 4460 3610 2730 2100 6.25 Pa .Math. s 1300 984 871 845 4590 3700 2780 2130 4.36 Pa .Math. s 1310 990 878 855 4690 3760 2820 2160 3.04 Pa .Math. s 1320 996 885 866 4770 3820 2860 2190 2.12 Pa .Math. s 1320 1000 890 876 4810 3850 2880 2210 1.48 Pa .Math. s 1320 1010 895 887 4860 3880 2910 2240 1.03 Pa .Math. s 1330 1010 900 895 4880 3910 2920 2260 0.721 Pa .Math. s 1330 1020 903 901 4890 3920 2930 2280 0.503 Pa .Math. s 1330 1030 904 903 4880 3910 2930 2290 Example Cone/plate 29 33 rheology (comp.) 30 31 32 (comp.) 34 35 36 Melt visc. at 260° C. [Hz] 471 Pa .Math. s 268 188 187 162 333 403 302 294 329 Pa .Math. s 292 203 198 171 369 442 328 319 229 Pa .Math. s 317 218 208 179 404 478 352 342 160 Pa .Math. s 339 230 216 185 438 510 372 362 112 Pa .Math. s 358 241 222 190 468 538 389 379 77.8 Pa .Math. s 375 250 226 193 495 560 403 392 54.3 Pa .Math. s 388 257 229 196 517 578 413 402 37.9 Pa .Math. s 400 262 231 198 536 592 421 410 26.4 Pa .Math. s 413 266 233 199 557 603 428 417 18.4 Pa .Math. s 418 270 233 201 566 611 433 422 12.9 Pa .Math. s 426 272 234 202 575 616 437 428 8.97 Pa .Math. s 433 274 235 203 583 620 441 433 6.25 Pa .Math. s 441 275 235 204 590 624 445 439 4.36 Pa .Math. s 451 276 235 205 597 626 448 444 3.04 Pa .Math. s 464 278 236 206 604 628 451 449 2.12 Pa .Math. s 482 281 236 206 613 629 454 454 1.48 Pa .Math. s 509 285 236 207 627 630 457 458 1.03 Pa .Math. s 547 292 237 209 648 631 460 462 0.721 Pa .Math. s 599 303 239 212 680 631 465 466 0.503 Pa .Math. s 673 319 240 216 734 631 471 472 Melt visc. at 280° C. [Hz] 471 Pa .Math. s 642 556 513 468 630 693 627 588 329 Pa .Math. s 748 647 583 521 818 805 714 667 229 Pa .Math. s 846 727 647 570 1010 918 804 748 160 Pa .Math. s 934 798 704 614 1190 1030 889 825 112 Pa .Math. s 1020 862 754 652 1330 1130 967 896 77.8 Pa .Math. s 1090 917 796 683 1450 1230 1040 959 54.3 Pa .Math. s 1150 964 831 707 1570 1310 1100 1010 37.9 Pa .Math. s 1200 1000 858 725 1660 1380 1150 1060 26.4 Pa .Math. s 1240 1030 879 739 1750 1440 1190 1090 18.4 Pa .Math. s 1270 1050 895 750 1810 1480 1220 1120 12.9 Pa .Math. s 1290 1070 907 758 1860 1520 1240 1140 8.97 Pa .Math. s 1300 1080 917 764 1900 1540 1260 1160 6.25 Pa .Math. s 1310 1090 925 771 1930 1560 1270 1180 4.36 Pa .Math. s 1320 1100 931 778 1950 1580 1280 1190 3.04 Pa .Math. s 1320 1100 937 785 1960 1590 1290 1210 2.12 Pa .Math. s 1320 1110 941 789 1970 1590 1300 1220 1.48 Pa .Math. s 1330 1110 945 794 1970 1600 1310 1230 1.03 Pa .Math. s 1330 1120 949 798 1980 1600 1310 1240 0.721 Pa .Math. s 1330 1120 952 801 1980 1600 1320 1250 0.503 Pa .Math. s 1330 1120 953 801 1980 1600 1310 1250 Melt visc. at 300° C. [Hz] 471 Pa .Math. s 862 1100 787 826 993 1000 1080 997 329 Pa .Math. s 1210 1300 1090 1100 1450 1420 1480 1280 229 Pa .Math. s 1560 1520 1390 1350 1880 1870 1850 1540 160 Pa .Math. s 1960 1750 1690 1570 2540 2390 2210 1810 112 Pa .Math. s 2330 1990 1960 1780 3190 2860 2560 2080 77.8 Pa .Math. s 2660 2230 2190 1970 3770 3300 2920 2350 54.3 Pa .Math. s 2960 2450 2390 2150 4290 3720 3260 2620 37.9 Pa .Math. s 3230 2650 2580 2310 4810 4130 3590 2880 26.4 Pa .Math. s 3480 2820 2740 2450 5310 4510 3880 3110 18.4 Pa .Math. s 3700 2970 2870 2560 5770 4850 4150 3310 12.9 Pa .Math. s 3880 3090 2980 2650 6180 5150 4370 3490 8.97 Pa .Math. s 4020 3180 3070 2730 6540 5410 4550 3620 6.25 Pa .Math. s 4130 3250 3140 2790 6830 5610 4700 3730 4.36 Pa .Math. s 4210 3300 3190 2830 7060 5780 4820 3810 3.04 Pa .Math. s 4270 3340 3230 2880 7240 5900 4910 3880 2.12 Pa .Math. s 4310 3370 3260 2910 7380 6000 4980 3940 1.48 Pa .Math. s 4350 3390 3290 2940 7480 6080 5040 3990 1.03 Pa .Math. s 4360 3410 3310 2980 7550 6130 5090 4040 0.721 Pa .Math. s 4380 3420 3330 3010 7590 6170 5130 4070 0.503 Pa .Math. s 4370 3410 3330 3020 7600 6180 5140 4100 Example Cone/plate 37 rheology (comp.) 38 39 40 Melt viscosity at 260° C. [Hz] 471 Pas 391 344 285 250 329 Pas 430 375 308 270 229 Pas 467 404 329 288 160 Pas 500 429 347 302 112 Pas 528 450 362 314 77.8 Pas 552 468 374 324 54.3 Pas 570 481 382 331 37.9 Pas 584 491 389 337 26.4 Pas 595 498 394 341 18.4 Pas 601 502 397 345 12.9 Pas 604 505 399 348 8.97 Pas 606 507 401 351 6.25 Pas 607 507 402 354 4.36 Pas 606 507 403 357 3.04 Pas 606 508 403 360 2.12 Pas 603 506 403 362 1.48 Pas 602 505 403 363 1.03 Pas 601 505 403 365 0.721 Pas 599 504 403 368 0.503 Pas 595 501 403 371 Melt viscosity at 280° C. [Hz] 471 Pas 657 670 534 588 329 Pas 838 768 653 681 229 Pas 1010 868 758 767 160 Pas 1160 965 850 848 112 Pas 1300 1060 927 921 77.8 Pas 1420 1140 995 985 54.3 Pas 1530 1220 1050 1040 37.9 Pas 1620 1280 1100 1090 26.4 Pas 1700 1330 1140 1130 18.4 Pas 1770 1380 1180 1160 12.9 Pas 1820 1410 1200 1180 8.97 Pas 1860 1440 1220 1200 6.25 Pas 1890 1450 1230 1210 4.36 Pas 1910 1470 1240 1230 3.04 Pas 1920 1480 1250 1240 2.12 Pas 1930 1480 1260 1250 1.48 Pas 1930 1480 1260 1260 1.03 Pas 1930 1480 1260 1270 0.721 Pas 1930 1480 1260 1270 0.503 Pas 1920 1470 1250 1270 Melt viscosity at 300° C. [Hz] 471 Pas 999 1340 1060 880 329 Pas 1430 1610 1330 1220 229 Pas 1870 1920 1590 1520 160 Pas 2360 2260 1870 1820 112 Pas 2820 2610 2160 2100 77.8 Pas 3260 2980 2450 2370 54.3 Pas 3700 3340 2730 2620 37.9 Pas 4130 3690 2990 2860 26.4 Pas 4540 4010 3230 3070 18.4 Pas 4920 4300 3450 3250 12.9 Pas 5270 4560 3630 3400 8.97 Pas 5570 4770 3790 3530 6.25 Pas 5830 4950 3910 3640 4.36 Pas 6030 5090 4000 3720 3.04 Pas 6200 5210 4080 3800 2.12 Pas 6320 5290 4140 3850 1.48 Pas 6420 5350 4180 3900 1.03 Pas 6480 5400 4210 3940 0.721 Pas 6510 5420 4230 3980 0.503 Pas 6520 5420 4230 4010

[0203] Table 7 shows that compared to the inventive examples in the table, the comparative examples 13, 17, 21, 25, 29, 33 and 37 which do not comprise the PE wax exhibit higher melt viscosities and thus have poorer flowability at the three measurement temperatures.