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聚（L-丙交酯）和聚（丁二酸丁二醇酯）对热塑性淀粉的原位化学改性以制备有效互溶的三元共混物

In Situ Chemical Modification of Thermoplastic Starch with Poly(L-lactide) and Poly(butylene succinate) for an Effectively Miscible Ternary Blend.

作者信息

Jariyasakoolroj Piyawanee, Chirachanchai Suwabun

机构信息

Department of Packaging and Materials Technology, Faculty of Agro-Industry, Kasetsart University, Bangkok 10900, Thailand.

Center for Advanced Studies for Agriculture and Food (CASAF), KU Institute for Advanced Studies, Kasetsart University, Bangkok 10900, Thailand.

出版信息

Polymers (Basel). 2022 Feb 21;14(4):825. doi: 10.3390/polym14040825.

DOI:10.3390/polym14040825
PMID:35215738
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8880544/
Abstract

Thermoplastic starch (TPS) is in situ ring-opening polymerized with L-lactide (L-LA) and directly condensed with a poly(butylene succinate) (PBS) prepolymer in an extruder using two different production pathways to demonstrate the concept "like dissolves like" in a miscible poly(lactide)/TPS/PBS (PLA/TPS/PBS) ternary blend. The TPS crystalline pattern changes from a V-type to an E-type after TPS modification with a hydrophobic-PLLA segment. Heteronuclear multiple-bond correlation confirmed the successful formation of PLLA-TPS-PBS copolymers via two different in situ chemical modification pathways (i.e., (I) step-by-step modification and (II) one-pot reaction). All obtained PLLA-TPS-PBS copolymers functioned as the miscible phase, enhancing PLA/PLLA-TPS-PBS/PBS ternary blend miscibility, especially the random structural PLLA-TPS-PBS-II copolymers created in an in situ one-pot reaction. However, the PLLA-TPS-PBS-I copolymers can enhance PBS crystallization only. While the random PLLA-TPS-PBS-II copolymers exhibit a homogeneous multi-phase dispersion and crystallization acceleration in both the PLA and PBS chains. Moreover, the storage modulus level of the PLA/PLLA-TPS-PBS-II/PBS ternary blend remains high with a downward temperature shift in the glass transition region, indicating a stronger and more flexible system. The practical achievement of in situ modified TPS and, consequently, a miscible PLA/PLLA-TPS-PBS/PBS ternary blend with favorable physical properties, reveal its potential application in both compostable and food contact packaging.

摘要

热塑性淀粉（TPS）与L-丙交酯（L-LA）进行原位开环聚合，并在挤出机中使用两种不同的生产途径与聚丁二酸丁二醇酯（PBS）预聚物直接缩合，以证明在可混溶的聚丙交酯/TPS/PBS（PLA/TPS/PBS）三元共混物中“相似相溶”的概念。用疏水性聚L-丙交酯（PLLA）链段对TPS进行改性后，TPS的结晶模式从V型变为E型。异核多键相关证实了通过两种不同的原位化学改性途径（即（I）分步改性和（II）一锅法反应）成功形成了PLLA-TPS-PBS共聚物。所有得到的PLLA-TPS-PBS共聚物均作为可混溶相，提高了PLA/PLLA-TPS-PBS/PBS三元共混物的混溶性，尤其是通过原位一锅法反应制备的无规结构PLLA-TPS-PBS-II共聚物。然而，PLLA-TPS-PBS-I共聚物仅能促进PBS的结晶。而无规PLLA-TPS-PBS-II共聚物在PLA和PBS链中均表现出均匀的多相分散和结晶加速。此外，PLA/PLLA-TPS-PBS-II/PBS三元共混物的储能模量水平在玻璃化转变区域随温度下降仍保持较高，表明该体系更强且更具柔韧性。原位改性TPS的实际成果以及由此得到的具有良好物理性能的可混溶PLA/PLLA-TPS-PBS/PBS三元共混物，揭示了其在可堆肥和食品接触包装方面的潜在应用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/c2bc348c1ce2/polymers-14-00825-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/220fff63ef4c/polymers-14-00825-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/7d4be42f1222/polymers-14-00825-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/c870c0c16056/polymers-14-00825-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/fd91ff848609/polymers-14-00825-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/c0a9a53b610c/polymers-14-00825-g003a.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/f2ac0fc02516/polymers-14-00825-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/eb7de9a705eb/polymers-14-00825-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/45f8ccd1ab05/polymers-14-00825-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/9390258a632e/polymers-14-00825-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/c2bc348c1ce2/polymers-14-00825-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/220fff63ef4c/polymers-14-00825-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/7d4be42f1222/polymers-14-00825-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/c870c0c16056/polymers-14-00825-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/fd91ff848609/polymers-14-00825-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/c0a9a53b610c/polymers-14-00825-g003a.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/f2ac0fc02516/polymers-14-00825-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/eb7de9a705eb/polymers-14-00825-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/45f8ccd1ab05/polymers-14-00825-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/9390258a632e/polymers-14-00825-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/295e/8880544/c2bc348c1ce2/polymers-14-00825-g008.jpg

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