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The manufacture of next-generation 3D-printed foods with personalized requirements can be accelerated by in-depth knowledge of the development of a multifunctional biopolymeric-based ink. As a fat replacer in the food industry, microcrystalline cellulose (MCC) has the potential to address the growing need for sustainable healthy reduced-fat 3D printed foods. The modification of MCC structure by polyphenols gives the way to produce a multifunctional antioxidative Pickering emulsion with improved emulsifying properties. In this study, different types of polyphenols, including gallic acid (GA), tannic acid (TA), and cyanidin-3- O -glucoside (C3G), were individually used to synthesize the grafted MCC- g -polyphenol conjugates by the free-radical grafting method. Then, the antioxidative grafted microconjugates were added to a soy protein-based emulsion gel to partially substitute its oil, and each Pickering emulsion gel variant was printed through an extrusion-based 3D printing system. Emulsifying properties and antioxidant character of MCC were proven to be enhanced after the fabrication of grafted microconjugates. Compared to MCC- g -TA, MCC- g -GA and MCC- g -C3G could efficiently improve the stability of a reduced-fat soy-based emulsion gel upon storage. Moreover, the reduced-fat soy-based emulsion gel containing grafted microconjugates endowed a characteristic shear-thinning behavior with a gel-like structure and superlative thixotropic properties. Following the printing, the antioxidative Pickering emulsion gels containing grafted microconjugates produced well-defined 3D structures with superior lubrication properties. This study demonstrated that the grafting of polyphenols onto MCC could enhance bioactive properties and improve emulsifying performance of MCC, making it a useful component in the development of personalized functional foods.

Three-dimensional (3D) printing is a revolutionary additive manufacturing technique that allows rapid prototyping of objects with intricate architectures. This Review covers the recent state-of-the-art of biopolymers (protein and carbohydrate-based materials) application in pharmaceutical, bioengineering, and food printing and main reinforcement approaches of biomacromolecular structure for the development of 3D constructs. Some perspectives and main important limitations with the biomaterials utilization for advanced 3D printing procedures are also provided. Because of the improved the ink’s flow behavior and enhance the mechanical strength of resulting printed architectures, biopolymers are the most used materials for 3D printing applications. Biobased polymers by taking advantage of modifying the ink viscosity could improve the resolution of deposited layers, printing precision, and consequently, develop well-defined geometries. In this regard, the rheological properties of printable biopolymeric-based inks and factors affecting ink flow behavior related to structural properties of printed constructs are discussed. On the basis of successful applications of biopolymers in 3D printing, it is suggested that other biomacromolecules and nanoparticles combined with the matrix can be introduced into the ink dispersions to enhance the multifunctionality of 3D structures. Furthermore, tuning the biopolymer’s structural properties offers the most common and essential approach to attain the printed architectures with precisely tailored geometry. We finish the Review by giving a viewpoint of the upcoming 3D printing process and recognize some of the existing bottlenecks facing the blossoming 3D pharmaceutical, bioengineering, and food printing applications.

The feasible application of additive manufacturing in the food and pharmaceutical industries strongly depends on the development of highly stable inks with bioactive properties. Surface-modified microcrystalline cellulose (MCC) shows the potential of being a useful particulate ( i.e ., Pickering)-type emulsifier to stabilize emulsions. To attain desired therapeutic properties, MCC can also be tuned with cationic antimicrobial compounds to fabricate an antimicrobial printable ink. However, due to the formation of complex coacervates between the two, the Pickering emulsion is very susceptible to phase separation with an insufficient therapeutic effect. To address this drawback, we reported a green method to produce antioxidant and antimicrobial three-dimensional (3D)-printed objects, illustrated here using a printable ink based on a soy-based particulate-type emulsion gel stabilized by a surface-active MCC conjugate (micro-biosurfactant). A sustainable method for the modification of MCC is investigated by grafting gallic acid onto the MCC backbone, followed by in situ reacting via lauric arginate through Schiff-base formation and/or Michael-type addition. Our results show that the grafted micro-biosurfactant was more efficient in providing the necessary physical stability of soy-based emulsion gel. The grafted micro-biosurfactant produced a multifunctional ink with viscoelastic behavior, thixotropic property, and outstanding bioactivities. Following the 3D printing process, highly porous 3D structures with a more precise geometry were fabricated after addition of the micro-biosurfactant. Dynamic sensory evaluation showed that the micro-biosurfactant has a remarkable ability to improve the temporal perceptions of fibrousness and juiciness in printed meat analogue. The results of this study showed the possibility of the development of a therapeutic 3D-printed meat analogue with desired sensory properties, conceiving it as a promising meat analogue product.

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