Starch-based composites with different modified starches were prepared by combining starches with sisal fibers to investigate the effects of single-modification/cross-modification of starch on the mechanical properties of new biodegradable composites. Mechanical test results showed that cross-modification of starch improved the toughness of the composites, whereas single-modification improved the tensile strength. The oxidized esterified starch-based composite (OESC) exhibited the best toughness, with improved elongation at break and Young's modulus by 136.1% and 54.3%, respectively, compared with a native starch-based composite. Meanwhile, the tensile strength of the esterified starch-based composite (ESC) improved by 61.6%. The hydrogen bonds, crystallinity, and micro-structure of the composites were investigated to reveal the inherent mechanism of the changes in performance. Fourier transform infrared spectroscopy showed that modification of starch changed the functional groups of starch. Thus, the ESC formed the strongest hydrogen bonds. X-ray diffraction analysis showed that the crystallinity decreased after the starches were modified. The OESC exhibited the lowest crystallinity, with a severely damaged structure. Many starch branches were combined with sisal fibers so that the composite was not easily pulled off. Scanning electron microscopy images showed that the OESC formed good cell structures internally when starch uniformly attached to the surface of the fibers.
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