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Three materials (agar, konjac glucomannan (KGM) and κ-carrageenan) were used to prepare ternary systems, i.e., sol-gels and their dried composites conditioned at varied relative humidity (RH) (33 %, 54 % and 75 %). Combined methods, e.g., scanning electron microscopy, small-angle X-ray scattering, infrared spectroscopy (IR) and X-ray diffraction (XRD), were used to disclose how κ-carrageenan addition tailors the features of agar/KGM/κ-carrageenan ternary system. As affirmed by IR and XRD, the ternary systems with κ-carrageenan below 25 % (agar/KGM/carrageenan, 50:25:25, m/m) displayed proper component interactions, which increased the sol-gel transition temperature and the hardness of obtained gels. For instance, the ternary composites could show hardness about 3 to 4 times higher than that for binary counterpart. These gels were dehydrated to acquire ternary composites. Compared to agar/KGM composite, the ternary composites showed fewer crystallites and nanoscale orders, and newly-formed nanoscale structures from chain assembly. Such multi-scale structures, for composites with κ-carrageenan below 25 %, showed weaker changes with RH, as revealed by especially morphologic and crystalline features. Consequently, the ternary composites with less κ-carrageenan (below 25 %) exhibited stabilized elongation at break and hydrophilicity at different RHs. This hints to us that agar/KGM/κ-carrageenan composite systems can display series applications with improved features, e.g., increased sol-gel transition point.

Granule-bound starch synthase I (GBSSI) and starch-branching enzymes I and II (SBEI and SBEII) are crucial enzymes that biosynthesize starches with varied apparent amylose contents and amylopectin branching structure. With a sweet potato (Ipomoea batatas[L.] Lam. cv. Xushu22), this work shows that downregulating GBSSI (for waxy starch) or SBE (for high-amylose starch) activity allowed the formation of new semicrystalline lamellae (named Type II) in sweet potato starch in addition to the widely reported Type I lamellae. Small-angle X-ray scattering (SAXS) results show that, compared with Type I lamellae, Type II lamellae displayed increased average thickness and thickness-distribution width, with thickened amorphous and crystalline components. The size-exclusion-chromatography (SEC) data revealed mainly two enzyme sets, (i) and (ii), synthesizing amylopectin chains. Reducing the GBSSI or SBE activity increased the amounts of amylopectin long chains (degree of polymerization (DP) ≥ 33). Combined SAXS and SEC analyses indicate that parts of these long chains from enzyme set (i) could be confined to Type II lamellae, followed by DP ≤ 32 short chains in Type I lamellae and the rest of the long chains from enzyme sets (i) and (ii) spanning more than a single lamella.

Biopolymers are widely available, low-/nontoxic, biodegradable, biocompatible, chemically versatile, and inherently functional, making them highly potential for a broad range of applications such as biomedicine, food, textile, and cosmetics. 3D printing (3DP) is capable of fabricating some customized, complex material structures composed of single or multiple material constituents that cannot be achieved by conventional methodologies (e.g. internal structures design); thus, 3DP can greatly expand the application of biopolymer materials. This review presents a comprehensive survey of the latest literature in 3DP technology for materials from biopolymers such as polysaccharides and proteins. The most commonly used 3DP techniques (i.e. inkjet printing, extrusion-based printing, stereolithography, selective laser sintering, and binder jetting) in biomedical and food fields are discussed. Critical factors affecting the quality and accuracy of 3D-printed constructs, including rheological characteristics, printing parameters (e.g. printing rate, and nozzle diameter, movement rate and height), and post-printing processes (e.g. baking, drying, and crosslinking) are analyzed. The properties and the emerging applications of 3D-printed biopolymer materials in biomedical, food, and even wider applications (e.g. wastewater treatment and sensing) are summarized and evaluated. Finally, challenges and future perspectives are discussed. This review can provide insights into the development of new biopolymer-based inks and new biopolymer-based 3D-printed materials with enhanced properties and functionality.