Characterization of an Amphiphilic Janus-Type Surface in the Cellulose Nanofibril Prepared by Aqueous Counter Collision.

Cellulose nanofibrils, which attract extensive attention as a bio-based, sustainable, high-performance nanofibril, are believed to be predominantly hydrophilic. This study aimed to prove the presence of an amphiphilic "Janus-type fiber surface" in water with hydrophobic and hydrophilic faces in a cellulose nanofibril (ACC-CNF) that was prepared by the aqueous counter collision method. We clarified the surface characteristics of the ACC-CNF by confocal laser scanning microscopy with a carbohydrate-binding module and congo red probes for the hydrophobic planes on the cellulose fiber surfaces and calcofluor white as hydrophilic plane probes. The results indicated the presence of both characteristic planes on a single ACC-CNF surface, which verifies an amphiphilic Janus-type structure. Both hydrophobic probes adsorbed onto ACC-CNFs for the quantitative evaluation of the degree of ACC-CNF surface hydrophobicity by Langmuir's adsorption theory based on the optimal maximum adsorption amounts for various starting raw material types.

A uniaxially oriented nanofibrous cellulose scaffold from pellicles produced by Gluconacetobacter xylinus in dissolved oxygen culture.

An aerobic, Gram-negative bacterium, Gluconacetobacter xylinus, was successfully employed to produce a stretchable cellulose nanofiber pellicle using dissolved oxygen in a conventional cultured medium. The obtained nanofibers were highly crystalline with the metastable cellulose Iα phase being apparently the dominant phase by more than 90%. The obtained pellicle could be stretched by up to 1.5 times to provide oriented crystalline nanofibrous films. Low heating of the nanofibrous film induced the transformation of the dominant cellulose Iα crystalline phase into the Iß crystalline phase without a loss of crystallinity or the high Young's modulus. The film also exhibited unique and anisotropic viscoelastic and mechanical properties as well as superior thermal stability compared with conventional high-performance synthetic polymeric materials. In addition, when G. xylinus cells were transferred to the oriented surface after stretched, they started to synthesize cellulose ribbons that parallel the nanofiber orientation of the substrate. This function as a template was evidenced by direct video imaging of the motion of the bacteria. The application of a bacterial culture using dissolved oxygen in the medium offers the fabrication of novel anisotropic and nanofibrous scaffold of cellulose Iα.