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248  10  Highly Toughened Polylactide-Based Materials through Melt-Blending Techniques

                    interpenetrated networks, and the crystallization-induced toughness of PLA-
                    based materials with special emphasis on the literature highlighting key factors
                    affecting their final toughness as well as involved toughening mechanisms within
                    the as-produced PLA-based materials, giving some key examples in this field
                    without being exhaustive.
                    10.2.2
                    Rubber-Toughened Polylactide

                    Intensive studies have been carried out on toughened PLA-based melt blends with
                    biodegradable/renewable or nonbiodegradable polymers as impact modifiers.
                    However, these may result in poor final performances when the morphologies
                    and the interfaces of the blend are not well controlled. In this respect, many
                    researchers have investigated different strategies to impart the desired change
                    in toughness of PLA, including the addition of aliphatic polyesters (e.g., Poly(ϵ-
                    caprolactone) (PCL)), polyhydroxyalkanoates (e.g., poly(3-hydroxybutyrate)
                    (PHB)), aromatic copolyesters (e.g., poly(butylene adipate-co-terephthalate)
                    (PBAT)), elastomers and rubbers (e.g., poly(1,4-cis-isoprene) (PI)), oil derivatives
                    (e.g., soybean oil), and hydrocarbon derivatives (e.g., PE). As of now, three
                    main reviews report the most representative polymeric additives used in the
                    literature as impact modifiers for PLA, which are entitled “Toughening poly-
                    lactide” by Anderson et al. [45], “Research progress in toughening modification
                    of poly(lactic acid)” by Liu and Zhang [41], and “Recent advances in high
                    performance poly(lactide): From green plasticization to super-tough materials
                    via (reactive) compounding,” our newest contribution [47]. However, except for
                    our recent review, only few studies have investigated the origin of the impact
                    modification within rubber-toughened PLA [47]. Therefore, this section will
                    be strictly limited to the literature with the specific purpose of highlighting
                    toughness-dependent factors, underlying toughening mechanisms and origins of
                    toughness improvement in the field of rubber-toughened PLA.
                      Over the past years, PCL-based additives were revealed to be ideal candidates
                    for toughening PLA. Nowadays, the related literature represents the most
                    detailed examples to understand the origin of PLA rubber-toughening as well
                    as toughness-dependent parameters and mechanisms involved. For instance,
                    the existing literature tells us that a simple melt blending between PLA and
                    PCL usually leads to poor improvement in toughness due to the lack of com-
                    patibility between the blend components and related poor interfacial adhesion
                    (Figure 10.11) [70–76]. Broz et al. found that PLA and PCL are not miscible
                    except for some adhesion at the PLA/PCL interface when the major phase is
                    PCL. As a result, no significant improvement in elongation at break is recorded
                    below 60 wt% of PCL [70]. Therefore, the compatibility at the rubber–matrix
                    interface should be properly controlled to address impact modification. In this
                    realm, P[CL-co-LA] [77–80], PCL-b-PLA [78, 81], or PLA-b-PCL-b-PLA [81–83]
                    copolymers as well as other PLA-b-PEO (poly(ethylene oxide)) [83], poly(ethylene
                    glycol) (PEG)-b-poly(propylene glycol) (PPG) [84], or PLA-b-PEG [85] are among
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