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WO 2007/125039 Al (12) INTERNATIONAL APPLICATION PUBLISHED UNDER THE PATENT COOPERATION TREATY (PCT) (19) World Intellectual Property Organization International Bureau (43) International Publication Date (10) International Publication Number 8 November 2007 (08.11.2007) PCT WO 2007/125039 Al (51) International Patent Classification: (81) Designated States (unless otherwise indicated, for every C08L 67/04 (2006.01) C08L 69/00 (2006.01) kind of national protection available): AE, AG, AL, AM, AT,AU, AZ, BA, BB, BG, BH, BR, BW, BY, BZ, CA, CH, (21) International Application Number: CN, CO, CR, CU, CZ, DE, DK, DM, DZ, EC, EE, EG, ES, PCT/EP2007/053759 FI, GB, GD, GE, GH, GM, GT, HN, HR, HU, ID, IL, IN, IS, JP, KE, KG, KM, KN, KP, KR, KZ, LA, LC, LK, LR, (22) International Filing Date: 18 April 2007 (18.04.2007) LS, LT, LU, LY,MA, MD, MG, MK, MN, MW, MX, MY, MZ, NA, NG, NI, NO, NZ, OM, PG, PH, PL, PT, RO, RS, (25) Filing Language: English RU, SC, SD, SE, SG, SK, SL, SM, SV, SY, TJ, TM, TN, TR, TT, TZ, UA, UG, US, UZ, VC, VN, ZA, ZM, ZW (26) Publication Language: English (84) Designated States (unless otherwise indicated, for every (30) Priority Data: kind of regional protection available): ARIPO (BW, GH, 061 13201.5 27 April 2006 (27.04.2006) EP GM, KE, LS, MW, MZ, NA, SD, SL, SZ, TZ, UG, ZM, 07104484.6 20 March 2007 (20.03.2007) EP ZW), Eurasian (AM, AZ, BY, KG, KZ, MD, RU, TJ, TM), European (AT,BE, BG, CH, CY, CZ, DE, DK, EE, ES, FI, (71) Applicant (for all designated States except US): BASF FR, GB, GR, HU, IE, IS, IT, LT,LU, LV,MC, MT, NL, PL, AKTIENGESELLSCHAFT [DE/DE]; 67056 Lud- PT, RO, SE, SI, SK, TR), OAPI (BF, BJ, CF, CG, CI, CM, wigshafen (DE). GA, GN, GQ, GW, ML, MR, NE, SN, TD, TG). (72) Inventor; and Published: (75) Inventor/Applicant (for US only): LUINSTRA, Gerrit — with international search report [NL/DE]; N3, 11, 68161 Mannheim (DE). For two-letter codes and other abbreviations, refer to the "G uid (74) Common Representative: BASF AKTIENGE¬ ance Notes on Codes and Abbreviations" appearing at the beg in SELLSCHAFT; 67056 Ludwigshafen (DE). ning of each regular issue of the PCT Gazette. (54) Title: TRANSPARENT BLENDS OF POLYPROPYLENE CARBONATE (57) Abstract: This invention is directed to transparent blends of polypropylene carbonate with poly lactide and/or polyhydrox- yalkanoates, to a process for the preparation of said blends as well as the use of said blends. Transparent Blends of Polypropylene carbonate Specification This invention is directed to transparent blends of polypropylene carbonate with poly- lactide and/or polyhydroxyalkanoates, to a process for the preparation of said blends as well as the use of said blends. High molecular weight Polypropylencarbonate (PPC) is a thermoplastic, amorphous (transparent) material with a glass temperature in the range of 25 to 45°C. Latter is depending on the carbonate linkage percentage and the presence and amount of plas- ticizers like cyclic propylene carbonate, which is a typical thermal decomposition prod uct and/or side product of the synthesis. This means that the softening point of the polypropylene carbonate is usually at room or body temperature. This is disadvanta- geous for some applications in for example packaging sector: container prepared from polypropylene carbonate through injection or blow moulding will loose their shape in side a closed car on a sunny day in the sun. In addition, granulate of polypropylene carbonate tend to clog together at ambient temperature. As a consequence, the trans port in form of the usual pellets from manufacturer to costumers may result in a sticky block, which cannot be handled by standard equipment. As a result additional costs arise, for example for necessary milling or melting equipment. The above situation is unfavourable for the application of polypropylene carbonate as a thermoplastic material. An increase in the glass temperature and young modulus of the thermoplastic material would improve the properties with respect to application pur poses and processing. The glass temperature of a polymeric material can for example be increased through the formation of blends with other materials including with other polymers. Blends of polypropylene carbonate are known, however, they are all non-transparent as the result of a non-compatibility. This is expected, since different polymers tend to be immiscible. This has been explained by for example the differences in solubility pa rameter [Van Krevelen, Chapter 7.]: from a theoretical point of view, the solubility pa rameter of two components have to be identical within 0.1 (J/cm 3)/ . This is rarely the case, and it is thus to be expected that polymers in general are immiscible as is o b served for the opaque blends of polypropylene carbonate with SAN, PS, PP, PMMA (see examples). E.g. US 4,912,149 describes non-transparent blends of polypropylene carbonate and PVC. Blends of polyhydroxybutyrate (PHB) or polyhydroxybutyrate-covalerate (PHBV) and polypropylene carbonate are reported in US 6,576,694. The reported blends are, how ever, non transparent as expected on account of the different solubility parameter as explained above. The reported blends consist of 30-70 parts of polypropylene carbon ate respectively 70-30 parts of polyhydroxyalkanoates. Blends like this were also re ported in for example Gaodeng Xuexiao Huaxue Xuebao 2004, 25, 1145 (CA: 141 :350588) or Macromolecular symposia 2004, 210, 241 , J. Appl. Chem. 2004, 92, 2514-21 or ibid 2003, 90, 4054-60. All these reports are concerned about melting be havior of the PHB, but did not find a transparent PPC based material. However, there are good reasons for the use of transparent materials. They provide appealing qualities in form of attractive design options, direct visual contact to pack- aged goods (e.g. vegetables, fruits, meat) or to uniformly dying at low effort and costs. We thus set out to find blend components for polypropylene carbonate to improve the glass temperature and /or young modulus and to keep the excellent transparency in the resulting materials. Surprisingly, it is found that a transparent polypropylene carbonate (PPC) blend is formed by blending it with PLA (polylactid acid) independently of the ratio of the two components (PLA and PPC) in the blend. Yet in another embodiment of this invention, transparent blends of polypropylene car- bonate and PHB(V) are prepared, wherein the maximum amount of PHB(V) is not ex ceeding 15 parts by weight of a total of 100 in the sum with polypropylene carbonate. This is very surprising and favorable for the properties of the blend. In addition, the blends according to the invention have a higher glass temperature than the starting material PPC. Furthermore, we found that the elastic modulus of said blends could be improved without losing the transparency. The resulting blends can be processed using standard methods including injection and blow moulding and are suit able for applications in packaging, play (toys, recreational), hygiene (household) and medical, construction, sporting and art sector. Details The transparent blends of PPC comprise the following components wherein the sum of the parts of PPC and PLA or PHB are 100 parts by weight a) a first embodiment: (i) 1-99 parts by weight of polypropylencarbonate having a molecular weight (Mn) between 30,000 and 5,000,000 Da, (ii) 99-1 parts by weight of polylactid, (iii) 0.1-25 parts of an additional component that is known to function as an antioxidant, a flame retardant, a filler, a (metal) complexing agent, a plasti- cizer or processing aid, pigment, dye, brightener and/or antistatic agent; The first embodiment comprises preferably: (i) 10-90 parts by weight of polypropylencarbonate having a molecular weight (Mn) between 30,000 and 50,000 Da, (ii) 90-1 0 parts by weight of polylactid, (iii) 0.5-1 5 parts of an additional component that is known to function as an antioxidant, a flame retardant, a filler, a (metal) complexing agent, a plasticizer or processing aid, pigment, dye, brightener and/or antistatic agent; or b) a second embodiment: (i) 85-99 parts by weight of polypropylencarbonate having a molecular weight (Mn) between 30,000 and 5,000,000 Da, (ii) 15-1 parts by weight of polyhydroxyalkanoate, (iii) 0.1-25 parts of an additional component that is known to function as an antioxi dant, a flame retardant, a filler, a (metal) complexing agent, a plasticizer or proc essing aid, pigment, dye, brightener or antistatic agent; The second embodiment comprises preferably: (i) 90-98 parts by weight of polypropylencarbonate, (ii) 10-2 parts by weight of polyhydroxybutyrate, (iii) 0.5-1 5 parts of an additional component that is known to function as an an anti oxidant, a flame retardant, a filler, a (metal) complexing agent, a plasticizer or processing aid, pigment, dye, brightener or antistatic agent; or c) a third embodiment comprising mixtures of the first and second embodiments: (i) 5-97 parts by weight of polypropylencarbonate, (iia) 80-2 parts by weight of polylactid, (iib) 15-1 parts by weight of polyhydroxyalkanoate, (iii) 0.5-1 5 parts of an additional component that is known to function as an antioxi- dant, a flame retardant, a filler, a (metal) complexing agent, a plasticizer or proc essing aid, pigment, dye, brightener or antistatic agent; The third embodiment comprises preferably: (i) 30-97 parts by weight of polypropylencarbonate, (iia) 60-2 parts by weight of polylactid, (iib) 10-1 parts by weight of polyhydroxybutyrate, (iii) 0.5-1 5 parts of an additional component that is known to function as an antioxi dant, a flame retardant, a filler, a (metal) complexing agent, a plasticizer or proc essing aid, pigment, dye, brightener or antistatic agent; or d) a fourth embodiment preferably: (i) 20-80 parts by weight of polypropylencarbonate, (ii) 60-15 parts by weight of polylactid, (iii) 0.5-1 5 parts of an additional component that is known to function as an antioxi dant, a flame retardant, a filler, a (metal) complexing agent, a plasticizer or proc essing aid, pigment, dye, brightener or antistatic agent, (iv) 20-5 parts by weight of a biodegradable aliphatic or aliphatic/aromatic polyester.
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