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Dually crosslinked graphene oxide reinforced alginate/polyvinyl alcohol (PVA) double network (DN) hydrogels were prepared via a facile freeze/thaw method followed by soaking in a Ca2+ solution. The morphology and structure of the hydrogels were systematically examined by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), and thermogravimetric analysis (TGA). The effects of pH, dosage of hydrogel, adsorption time, and temperature on the adsorptive property of DN hydrogels towards methylene blue (MB) were also studied. Results indicated that the hydrogels exhibited typical 3D porous structures and had an efficient adsorption effect towards MB due to strong interactions between DN hydrogels and MB molecules. The adsorption isotherm was found to coincide with the Langmuir model with a monolayer adsorption. The highest adsorption capacity of DN hydrogels for MB was examined as 480.76 mg·g−1.

Mesoscaled assemblies are organized in native collagen tissues to achieve remarkable and diverse performance and functions. In this work, a facile, low-cost, and controllable liquid exfoliation method was applied to directly extract these collagen mesostructures from bovine Achilles tendons using a sodium hydroxide (NaOH)/urea aqueous system with freeze−thaw cycles and sonication. A series of collagen fibrils with diameters of 26−230 nm were harvested using this process, and in situ observations under polarizing microscopy (POM) and using molecular dynamics simulations revealed the influence of the NaOH/urea system on the tendon collagen. FTIR and XRD results confirmed that these collagen fibrils preserved typical structural characteristics of type I collagen. These isolated collagen fibrils were then utilized as building blocks to fabricate free-standing collagen membranes, which exhibited good stability in solvents and outstanding mechanical properties and transparency, with potential for utility in optical and electronic sensors. Moreover, in vitro and vivo evaluations demonstrated that these new resulting collagen membranes had good cytocompatibility, biocompatibility, and degradability for potential applications in biomedicine. This work provides a new approach for collagen processing by liquid exfoliation with utility for the formation of robust collagen materials that consist of native collagen mesostructures as building blocks.