Tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate
The excessive use and disposal of plastic products have become a severe threat to the environment, animal welfare, and human health. Naturally synthesized, marine-degradable polyhydroxybutyrate (PHB) represents a viable green substitute for conventional plastics. However, the inherent brittleness of...
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sg-ntu-dr.10356-1640452023-01-03T06:41:14Z Tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate Hou, Xunan Sun, Wen Liu, Zhibang Liu, Siqi Yeo, Jayven Chee Chuan Lu, Xuehong He, Chaobin School of Materials Science and Engineering Engineering::Materials Blends Polyhydroxyalkanoates The excessive use and disposal of plastic products have become a severe threat to the environment, animal welfare, and human health. Naturally synthesized, marine-degradable polyhydroxybutyrate (PHB) represents a viable green substitute for conventional plastics. However, the inherent brittleness of PHB remains a major challenge due to undesirable large spherulites and secondary crystallization. Herein, we report PHB-based (up to 70 wt %) ductile and flexible materials by facile physical blending with edible poly(vinyl acetate) (PVAc). Theoretical and experimental analyses show that entropy rather than enthalpy drives the high miscibility between two polymers. Entropic mixing turns fragile PHB spherulitic crystals (>70 μm) into myriads of ultrafine domains (<2 μm). Interfacial entanglements between PVAc and PHB further prevent secondary crystal formation of the rigid amorphous phase. The resultant biopolymer blends demonstrate mechanical properties similar to commercial polyethylene plastics, such as high ductility (elongation >500%), toughness (∼62 MJ m-3), flexibility, and shape recovery under repeated bending (180°) or twisting (360°). Under controlled composting conditions, the food-safe bioblends exhibit ∼2.4 times weight loss of virgin PHB. The proposed strategy proves applicable to other crystalline/amorphous polymeric mixtures. This discovery sheds new light on the rational design of green plastics for future sustainable electronics, agriculture, and biomedicine. X.H. would like to thank the National University of Singapore (NUS) for providing NUS Research Scholarship. 2023-01-03T06:41:14Z 2023-01-03T06:41:14Z 2022 Journal Article Hou, X., Sun, W., Liu, Z., Liu, S., Yeo, J. C. C., Lu, X. & He, C. (2022). Tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate. Macromolecules, 55(13), 5527-5534. https://dx.doi.org/10.1021/acs.macromol.2c00832 0024-9297 https://hdl.handle.net/10356/164045 10.1021/acs.macromol.2c00832 2-s2.0-85134514570 13 55 5527 5534 en Macromolecules © 2022 American Chemical Society. All rights reserved. |
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Engineering::Materials Blends Polyhydroxyalkanoates Hou, Xunan Sun, Wen Liu, Zhibang Liu, Siqi Yeo, Jayven Chee Chuan Lu, Xuehong He, Chaobin Tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate |
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The excessive use and disposal of plastic products have become a severe threat to the environment, animal welfare, and human health. Naturally synthesized, marine-degradable polyhydroxybutyrate (PHB) represents a viable green substitute for conventional plastics. However, the inherent brittleness of PHB remains a major challenge due to undesirable large spherulites and secondary crystallization. Herein, we report PHB-based (up to 70 wt %) ductile and flexible materials by facile physical blending with edible poly(vinyl acetate) (PVAc). Theoretical and experimental analyses show that entropy rather than enthalpy drives the high miscibility between two polymers. Entropic mixing turns fragile PHB spherulitic crystals (>70 μm) into myriads of ultrafine domains (<2 μm). Interfacial entanglements between PVAc and PHB further prevent secondary crystal formation of the rigid amorphous phase. The resultant biopolymer blends demonstrate mechanical properties similar to commercial polyethylene plastics, such as high ductility (elongation >500%), toughness (∼62 MJ m-3), flexibility, and shape recovery under repeated bending (180°) or twisting (360°). Under controlled composting conditions, the food-safe bioblends exhibit ∼2.4 times weight loss of virgin PHB. The proposed strategy proves applicable to other crystalline/amorphous polymeric mixtures. This discovery sheds new light on the rational design of green plastics for future sustainable electronics, agriculture, and biomedicine. |
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School of Materials Science and Engineering |
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School of Materials Science and Engineering Hou, Xunan Sun, Wen Liu, Zhibang Liu, Siqi Yeo, Jayven Chee Chuan Lu, Xuehong He, Chaobin |
format |
Article |
author |
Hou, Xunan Sun, Wen Liu, Zhibang Liu, Siqi Yeo, Jayven Chee Chuan Lu, Xuehong He, Chaobin |
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Hou, Xunan |
title |
Tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate |
title_short |
Tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate |
title_full |
Tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate |
title_fullStr |
Tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate |
title_full_unstemmed |
Tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate |
title_sort |
tailoring crystalline morphology via entropy-driven miscibility: toward ultratough, biodegradable, and durable polyhydroxybutyrate |
publishDate |
2023 |
url |
https://hdl.handle.net/10356/164045 |
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1754611261307355136 |