Engineering Nano/Microscale Chiral Self-Assembly in 3D Printed Constructs.

Helical hierarchy found in biomolecules like cellulose, chitin, and collagen underpins the remarkable mechanical strength and vibrant colors observed in living organisms. This study advances the integration of helical/chiral assembly and 3D printing technology, providing precise spatial control over chiral nano/microstructures of rod-shaped colloidal nanoparticles in intricate geometries. We designed reactive chiral inks based on cellulose nanocrystal (CNC) suspensions and acrylamide monomers, enabling the chiral assembly at nano/microscale, beyond the resolution seen in printed materials.

Size-dependent viscoelasticity in hybrid colloidal gels based on spherical soft nanoparticles and two-dimensional nanosilicates of varying size.

Hypothesis: Hetero-aggregation of oppositely charged colloidal particles with controlled architectural and interactional asymmetry allows modifying gel nanostructure and properties. We hypothesize the relative size ratio between cationic nanospheres and varied-size anionic two-dimensional nanoclays will influence the gel formation mechanisms and resulting rheological performance.

Experiments: Hybrid colloidal gels formed via hetero-aggregation of cationic gelatin nanospheres (∼400 nm diameter) and five types of nanoclays with similar 1 nm thickness but different lateral sizes ranging from ∼ 30 nm to ∼ 3000 nm.

3D Printing-Assisted Self-Assembly to Bio-Inspired Bouligand Nanostructures.

Architected materials with nano/microscale orders can provide superior mechanical properties; however, reproducing such levels of ordering in complex structures has remained challenging. Inspired by Bouligand structures in nature, here, 3D printing of complex geometries with guided long-order radially twisted chiral hierarchy, using cellulose nanocrystals (CNC)-based inks is presented. Detailed rheological measurements, in situ flow analysis, polarized optical microscopy (POM), and director field analysis are employed to evaluate the chiral assembly over the printing process.

Hybrid colloidal gels with tunable elasticity formed by charge-driven assembly between spherical soft nanoparticles and discotic nanosilicates.

Colloidal gels based on electrostatic interparticle attractions hold unexploited potential for tailoring their microstructure and properties. Here, we demonstrate that hetero-aggregation between oppositely charged particles with different geometries is a viable strategy for controlling their properties. Specifically, we studied hybrid colloidal gels prepared by the charge-driven assembly of oppositely charged spherical gelatin nanoparticles and two-dimensional (2D) nanosilicates.

Translocation Behaviors of Synthetic Polyelectrolytes through Alpha-Hemolysin (α-HL) and Porin A (MspA) Nanopores.

DNAs have been used as probes for nanopore sensing of noncharged biomacromolecules due to its negative phosphate backbone. Inspired by this, we explored the potential of diblock synthetic polyelectrolytes as more flexible and inexpensive nanopore sensing probes by investigating translocation behaviors of PEO-b-PSS and PEO-b-PVBTMA through commonly used alpha-hemolysin (α-HL) and porin A (MspA) nanopores. Translocation recordings in different configurations of pore orientation and testing voltage indicated efficient PEO-b-PSS translocations through α-HL and PEO-b-PVBTMA translocations through MspA.

Capillary Flow Characterizations of Chiral Nematic Cellulose Nanocrystal Suspensions.

Studying the flow-induced alignment of anisotropic liquid crystalline materials is of major importance in the 3D printing of advanced architectures. However, in situ characterization and quantitative measurements of local orientations during the 3D printing process are challenging. Here, we report a microfluidic strategy integrated with polarized optical microscopy (POM) to perform the in situ characterization of the alignment of cellulose nanocrystals (CNCs) under the shear-flow condition of the 3D printer's nozzle in the direct ink writing process.