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Decoupling Formulation and Processing Effects in Thermoplastic Starch Through a Data-Driven Structure–Property Framework
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DOI：10.1002/pen.70687.png)
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Abstract
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Thermoplastic starch (TPS) is a melt-processable biopolymer whose properties depend strongly on formulation and processing. This work analyzes the combined influence of starch origin (corn, potato, rice), plasticizer system (glycerol, glycerol–triethyl citrate), and processing temperature (125°C–135°C) on the microstructure, mechanical, water-interaction, thermal and rheological behavior of extruded and injection-molded TPS. Potato TPS forms the strongest matrices (≈2.0–3.4 MPa), corn TPS attains an intermediate strength level (≈1.3–1.5 MPa), and rice TPS becomes highly ductile but less strong when plasticized with Gly–TEC (elongation ≈58%–82%, strength ≈0.5–0.8 MPa). Replacing glycerol with Gly–TEC increases ductility in all starches while shifting water uptake within a 32–59 wt.% window, decreasing it in corn and potato TPS and increasing it in rice TPS. All formulations exhibit pronounced shear-thinning, and Gly–TEC lowers melt viscosity and enhances processability. Principal component analysis and random forest modeling reveal a hierarchy among the governing parameters, decoupling formulation and processing contributions within a structure–property framework: starch origin defines the intrinsic property baseline, plasticizer composition controls the mechanical–hydrophilic response, and processing temperature fine-tunes ductility, while the model's accuracy (R2 ≈ 0.94 for strength, 0.90 for elongation) confirms reliable TPS property prediction.
Keywords:
plasticizer type
predictive modeling
processing temperature
starch origin
thermoplastic starch
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