We demonstrate that surface modified nanocellulose fibers (NCFs) can be used as substrates to synthesize supercapacitor electrodes with the highest full electrode-normalized gravimetric (127 F g(-1)) and volumetric (122 F cm(-3)) capacitances at high current densities (300 mA cm(-2) ≈ 33 A g(-1)) until date reported for conducting polymer-based electrodes with active mass loadings as high as 9 mg cm(-2). By introducing quaternary amine groups on the surface of NCFs prior to polypyrrole (PPy) polymerization, the macropore volume of the formed PPy-NCF composites can be minimized while maintaining the volume of the micro- and mesopores at the same level as when unmodified or carboxylate groups functionalized NCFs are employed as polymerization substrates. Symmetric, aqueous electrolyte-based, devices comprising these porosity-optimized electrodes exhibit device-specific volumetric energy and power densities of 3.1 mWh cm(-3) and 3 W cm(-3) respectively; which are among the highest values reported for conducting polymer electrodes in aqueous electrolytes. The functionality of the devices is verified by powering a red light-emitting diode with the device in different mechanically challenging states.
The effect of surface functionalization of nanofibrillated cellulose (NFC) on monocyte/macrophage (MM) behavior is investigated to understand how the physicochemical properties of nanocelluloses influence the interactions of such materials with biological systems. Films of anionic (a-), cationic (c-), and unmodified (u-) NFC were synthesized and characterized in terms of surface charge. THP-1 monocytes were cultured on the surface of the films for 24 h in the presence and absence of lipopolysaccharide, and the cell response was evaluated in terms of cell adhesion, morphology, and secretion of TNF-α, IL-10, and IL-1ra. The results show that MMs cultured on carboxymethylated-NFC films (a-NFC) are activated toward a proinflammatory phenotype, whereas u-NFC promotes a mild activation of the studied cells. The presence of hydroxypropyltrimethylammonium groups on c-NFC, however, does not promote the activation of MMs, indicating that c-NFC closely behaves as an inert material in terms of MM activation. None of the materials is able to directly activate the MMs toward an anti-inflammatory response. These results may provide a foundation for the design of future NFC-based materials with the ability to control MM activation and may expand the use of NFC in biomedical applications.
This work presents an insight into the relationship between cell response and physicochemical properties of Cladophora cellulose (CC) by investigating the effect of CC functional group density on the response of model cell lines. CC was carboxylated by electrochemical TEMPO-mediated oxidation. By varying the amount of charge passed through the electrolysis setup, CC materials with different degrees of oxidation were obtained. The effect of carboxyl group density on the material's physicochemical properties was investigated together with the response of human dermal fibroblasts (hDF) and human osteoblastic cells (Saos-2) to the carboxylated CC films. The introduction of carboxyl groups resulted in CC films with decreased specific surface area and smaller total pore volume compared with the unmodified CC (u-CC). While u-CC films presented a porous network of randomly oriented fibers, a compact and aligned fiber pattern was depicted for the carboxylated-CC films. The decrease in surface area and total pore volume, and the orientation and aggregation of the fibers tended to augment parallel to the increase in the carboxyl group density. hDF and Saos-2 cells presented poor cell adhesion and spreading on u-CC, which gradually increased for the carboxylated CC as the degree of oxidation increased. It was found that a threshold value in carboxyl group density needs be reached to obtain a carboxylated-CC film with cytocompatibility comparable to commercial tissue culture material. Hence, this study demonstrates that a normally bioinert nanomaterial can be rendered bioactive by carefully tuning the density of charged groups on the material surface, a finding that not only may contribute to the fundamental understanding of biointerface phenomena, but also to the development of bioinert/bioactive materials.
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