Additive manufacturing of smart materials that can be dynamically programmed with external stimuli is known as 4D printing. Among the 4D printable materials, hydrogels are the most extensively studied materials in various biomedical areas because of their hierarchical structure, similarity to native human tissues, and supreme bioactivity. However, conventional smart hydrogels suffer from poor mechanical properties, slow actuation speed, and instability of actuated shape. Herein, we present 4D-printed hydrogels based on poly(acrylic acid) that can concurrently possess shape-memory and self-healing properties. The printing of the hydrogels is achieved by solvent-free copolymerization of the hydrophilic acrylic acid (AAc) and hydrophobic hexadecyl acrylate (C16A) monomers in the presence of TPO photoinitiator using a stereolithography-based commercial resin printer followed by swelling in water. The printed hydrogels undergo a reversible strong-to-weak gel transition below and above human body temperature due to the melting and crystallization of the hydrophobic C16A domains. In this way, the shape-memory and self-healing properties of the hydrogels can be magically actuated near the body temperature by adjusting the molar ratio of the monomers. Furthermore, the printed hydrogels display a high Young’s modulus (up to ∼215 MPa) and high toughness (up to ∼7 MJ/m3), and their mechanical properties can be tuned from brittle to ductile by reducing the molar fraction of C16A, or the deformation speed. Overall, the developed 4D printable hydrogels have great potential for various biomedical applications.

Three-dimensional (3D) printing is one of the most futuristic manufacturing technologies, allowing on-demand manufacturing of products with highly complex geometries and tunable material properties. Among the different 3D-printing technologies, fused deposition modeling (FDM) is the most popular one due to its affordability, adaptability, and pertinency in many areas, including the biomedical field. Yet, only limited amounts of materials are commercially available for FDM, which hampers their application potential. Polybutylene succinate (PBS) is one of the biocompatible and biodegradable thermoplastics that could be subjected to FDM printing for healthcare applications. However, microbial contamination and the formation of biofilms is a critical issue during direct usage of thermoplastics, including PBS. Herein, we developed a composite filament containing polybutylene succinate (PBS) and lignin for FDM printing. Compared to pure PBS, the PBS/lignin composite with 2.5~3.5% lignin showed better printability and antioxidant and antimicrobial properties. We further coated silver/zinc oxide on the printed graft to enhance their antimicrobial performance and obtain the strain-specific antimicrobial activity. We expect that the developed approach can be used in biomedical applications such as patient-specific orthoses.

There is a need to develop the next generation of medical products that require biomaterials with improved properties. The versatility of various gels has pushed them to the forefront of biomaterials research. Cryogels, a type of gel scaffold made by controlled crosslinking under subzero or freezing temperatures, have great potential to address many current challenges. Unlike their hydrogel counterparts, which are also able to hold large amounts of biologically relevant fluids such as water, cryogels are often characterized by highly dense and crosslinked polymer walls, macroporous structures, and often improved properties. Recently, one biomaterial that has garnered a lot of interest for cryogel fabrication is silk and its derivatives. In this review, we provide a brief overview of silk-based biomaterials and how cryogelation can be used for novel scaffold design. We discuss how various parameters and fabrication strategies can be used to tune the properties of silk-based biomaterials. Finally, we discuss specific biomedical applications of silk-based biomaterials. Ultimately, we aim to demonstrate how the latest advances in silk-based cryogel scaffolds can be used to address challenges in numerous bioengineering disciplines.

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There is a need to develop circular and sustainable economies by utilizing sustainable, green, and renewable resources in high-tech industrial fields especially in the pharmaceutical industry. In the last decade, many derivatives of food and agricultural waste have gained considerable attention due to their abundance, renewability, biocompatibility, environmental amiability, and remarkable biological features. Particularly, lignin, which has been used as a low-grade burning fuel in the past, recently attracted a lot of attention for biomedical applications because of its antioxidant, anti-UV, and antimicrobial properties. Moreover, lignin has abundant phenolic, aliphatic hydroxyl groups, and other chemically reactive sites, making it a desirable biomaterial for drug delivery applications. In this review, we provide an overview of designing different forms of lignin-based biomaterials, including hydrogels, cryogels, electrospun scaffolds, and three-dimensional (3D) printed structures and how they have been used for bioactive compound delivery. We highlight various design criteria and parameters that influence the properties of each type of lignin-based biomaterial and corelate them to various drug delivery applications. In addition, we provide a critical analysis, including the advantages and challenges encountered by each biomaterial fabrication strategy. Finally, we highlight the prospects and future directions associated with the application of lignin-based biomaterials in the pharmaceutical field. We expect that this review will cover the most recent and important developments in this field and serve as a steppingstone for the next generation of pharmaceutical research.