Abstract
This study aims to utilize the natural composition of brown seaweed by deriving alginate and cellulose concurrently from the stipe (stem-like) and blade (leaf-like) structures of the seaweed; further, this is followed by fibrillation for the direct and resource-efficient preparation of alginate/cellulose nanofiber (CNF) hybrid inks for three-dimensional (3D) printing of hydrogels. The efficiency of the fibrillation process was evaluated, and the obtained gels were further studied with regard to their rheological behavior. As a proof of concept, the inks were 3D printed into discs, followed by cross-linking with CaCl2 to form biomimetic hydrogels. It was shown that the nanofibrillation process from both seaweed structures is very energy-efficient, with an energy demand lower than 1.5 kW h/kg, and with CNF dimensions below 15 nm. The inks displayed excellent shear-thinning behavior and cytocompatibility and were successfully printed into 3D discs that, after cross-linking, exhibited an interconnected network structure with favorable mechanical properties, and a cell viability of 71%. The designed 3D biomimetic hydrogels offers an environmentally benign, cost-efficient, and biocompatible material platform with a favorable structure for the development of biomedical devices, such as 3D bio printing of soft tissues.
Highlights
Brown seaweed is an encouraging and fascinating natural resource with increasing commercial and ecological importance.[1]
This paper reports on the utilization of the natural composition of brown seaweed to prepare alginate/cellulose nanofiber (CNF) hybrid inks with an excellent shear-thinning behavior suitable for 3D printing
It was found that the natural composition of alginate was beneficial for an energy-efficient nanofibrillation process, resulting in very fine nanofibers on average measured to 6 and 7 (±3) nm for S-A-CNF and B-A-CNF, respectively
Summary
Brown seaweed is an encouraging and fascinating natural resource with increasing commercial and ecological importance.[1] Laminaria digitata is one type of fast-growing and large brown seaweed, which consists of a holdfast (root-like), a stipe (stem-like), and a blade (leaf-like) structure that can grow up to 4 m in length.[2] It grows along the coasts in the relatively cold Northern hemisphere, and its carbohydrate composition varies with season, geographic location, and age,[3] as well as between the different parts of the seaweed (stipe and blade).[4] The polysaccharides in brown seaweed differ considerably from those found in terrestrial plants; cellulose is present in smaller amounts, alginate is the major structural component of the cell wall. Alginate consists of 1,4-glycosidically linked α-L guluronic acid (G) and β-D-mannuronic acid (M). The linear chains are made up of different blocks of guluronic and mannuronic acids, referred to as MM or GG blocks (MG or GM blocks), where the linkage in the block structure results in varying degrees of flexibility or stiffness in the alginates. Several researchers have solved this problem by introducing cellulose nanofibers (CNFs) as a second component to tailor commercial alginate as ink suitable for 3D printing.[7,12]
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