Zhang Zhen, Quinn Ethan C, Olmedo-Martínez Jorge L, Caputo Maria Rosaria, Franklin Kevin A, Müller Alejandro J, Chen Eugene Y-X
Department of Chemistry, Colorado State University, Fort Collins, CO 80523-1872, USA.
POLYMAT and Department of Polymers and Advanced Materials: Physics, Chemistry and Technology, Faculty of Chemistry, University of the Basque Country UPV/EHU, Paseo Manuel de Lardizábal 3, 20018, Donostia-San Sebastián, Spain.
Angew Chem Int Ed Engl. 2023 Dec 4;62(49):e202311264. doi: 10.1002/anie.202311264. Epub 2023 Nov 7.
Poly(3-hydroxybutyrate) (P3HB), a biologically produced, biodegradable natural polyester, exhibits excellent thermal and barrier properties but suffers from mechanical brittleness, largely limiting its applications. Here we report a mono-material product design strategy to toughen stereoperfect, brittle bio or synthetic P3HB by blending it with stereomicrostructurally engineered P3HB. Through tacticity ([mm] from 0 to 100 %) and molecular weight (M to 788 kDa) tuning, high-performance synthetic P3HB materials with tensile strength to ≈30 MPa, fracture strain to ≈800 %, and toughness to 126 MJ m (>110× tougher than bio-P3HB) have been produced. Physical blending of the brittle P3HB with such P3HB in 10 to 90 wt % dramatically enhances its ductility from ≈5 % to 95-450 % and optical clarity from 19 % to 85 % visible light transmittance while maintaining desirably high elastic modulus (>1 GPa), tensile strength (>35 MPa), and melting temperature (160-170 °C). This P3HB-toughening-P3HB methodology departs from the traditional approach of incorporating chemically distinct components to toughen P3HB, which hinders chemical or mechanical recycling, highlighting the potential of the mono-material product design solely based on biodegradable P3HB to deliver P3HB materials with diverse performance properties.
聚（3-羟基丁酸酯）（P3HB）是一种生物合成的可生物降解天然聚酯，具有优异的热性能和阻隔性能，但存在机械脆性问题，这在很大程度上限制了其应用。在此，我们报告了一种单材料产品设计策略，通过将立体完美、脆性的生物或合成P3HB与立体微结构工程化的P3HB共混来增韧。通过调节立构规整度（[mm]从0到100%）和分子量（M至788 kDa），制备出了具有约30 MPa的拉伸强度、约800%的断裂应变和约126 MJ·m的韧性（比生物P3HB韧110倍以上）的高性能合成P3HB材料。将脆性P3HB与这种P3HB以10至90 wt%的比例进行物理共混，可显著提高其延展性，从约5%提高到95 - 450%，同时将光学透明度从19%提高到85%的可见光透过率，同时保持理想的高弹性模量（>1 GPa）、拉伸强度（>35 MPa）和熔点（160 - 170°C）。这种P3HB增韧P3HB的方法不同于传统的通过加入化学性质不同的组分来增韧P3HB的方法，后者会阻碍化学或机械回收利用，突出了仅基于可生物降解P3HB的单材料产品设计在提供具有多种性能的P3HB材料方面的潜力。
