Various cellulosic materials have replaced petroleum-derived polymers, offering natural and sustainable alternatives. Among them, cellulose nanocrystals (CNC) feature an easily modifiable surface, enabling the exploration of a wide spectrum of applications. In this work, the quaternary agent 3-chloro-2-hydroxypropyltrimethylammonium chloride (CHPTAC) was used as a cationic graft on CNCs, to form a novel water treatment flocculant. The resulting material was chemically and structurally characterized by the determination of Zeta potential; degree of substitution by elemental analysis; hydrodynamic size by dynamic light scattering (DLS) and infrared spectroscopy with Fourier Transform Infrared (FT-IR); and X-ray diffraction (XRD). The flocculation capacity of cationic cellulose nanocrystals (CNC-EPTMAC) was evaluated in a jar test filled with an 0.25 wt.% silica (SiO2) suspension. CNC-EPTMAC proved to be an effective water treatment flocculant, reducing turbidity by up to 99.7% at a concentration of only 2 ppm. This work demonstrates a natural and environmentally sustainable alternative to homologous commercial flocculants.

Aerogel objects inspired by plant cell wall components and structures were fabricated using extrusion-based 3D printing at cryogenic temperatures. The printing process combines 3D printing with the alignment of rod-shaped nanoparticles through the freeze-casting of aqueous inks. We have named this method direct cryo writing (DCW) as it encompasses in a single processing step traditional directional freeze casting and the spatial fidelity of 3D printing. DCW is demonstrated with inks that are composed of an aqueous mixture of cellulose nanocrystals (CNCs) and xyloglucan (XG), which are the major building blocks of plant cell walls. Rapid fixation of the inks is achieved through tailored rheological properties and controlled directional freezing. Morphological evaluation revealed the role of ice crystal growth in the alignment of CNCs and XG. The structure of the aerogels changed from organized and tubular to disordered and flakey pores with an increase in XG content. The internal structure of the printed objects mimics the structure of various wood species and can therefore be used to create wood-like structures via additive manufacturing technologies using only renewable wood-based materials.

Additive manufacturing technologies based on stereolithography rely on initiating spatial photopolymerization by using photoinitiators activated by UV-visible light. Many applications requiring printing in water are limited since water-soluble photoinitiators are scarce, and their price is skyrocketing. On the contrary, thermal initiators are widely used in the chemical industry for polymerization processes due to their low cost and simplicity of initiation by heat at low temperatures. However, such initiators were never used in 3D printing technologies, such as vat photopolymerization stereolithography, since localizing the heat at specific printing voxels is impossible. Here we propose using a thermal initiator for 3D printing for localized polymerization processes by near-infrared and visible light irradiation without conventional photoinitiators. This is enabled by using gold nanorods or silver nanoparticles at very low concentrations as photothermal converters in aqueous and non-aqueous mediums. Our proof of concept demonstrates the fabrication of hydrogel and polymeric objects using stereolithography-based 3D printers, vat photopolymerization, and two-photon printing.