Defence of doctoral thesis: Justin Xuan Yang – Eco-friendly Holocellulose Materials for Mechanical Performance and Optical Transmittance

Abstract

Cellulosic materials can be sustainable replacements for fossil-based plastics; yet for some applications improvements are needed for mechanical properties, optical transmittance and eco-friendly characteristics. In this thesis, holocellulose materials are investigated for this purpose, and processing-structure-property relationships are discussed. Molded fibers, without added polymer binder, is of particular interest for semi-structural applications, where facile recycling is possible with highly preserved fiber properties.

Mild delignification is carried out to obtain ramie fibers, spruce holocellulose fibers and holocellulose nanofibrils. The chemical composition, molar mass, crystallinity, fiber length/width, and single fiber strength are measured. Fibers and fibrils show well-preserved native structure. Using water-based hot-pressing, fibers and fibrils are processed into different fiber network materials, including paper structures of 50% porosity, high density molded fibers, and high density nanopaper films. Biocomposites are obtained through methyl methacrylate impregnation and polymerization with molded fibers as reinforcing networks. Fiber orientation is quantified using 2D X-ray diffraction, mechanical properties are determined by tensile testing, and optical properties are measured by transmittance/haze tests in an integrating sphere. Holocellulose materials show much superior mechanical properties and optical transmittance to comparable materials based on industrially available kraft fiber grades. Strong effects from micro-, nano- and molecular scale structures are observed and discussed.

The colloidal stability, redispersibility, and surface modification of holocellulose nanofibrils, as well as recycling and 3D-shaping performance of paper-like structures are investigated. Eco-friendly characteristics include high fiber yield, reduced need for chemical modification and excellent recycling performance with reduced embodied energy in the final material. The enhanced performance of holocellulose materials, compared with materials from kraft fibers, are related to the effects of well-preserved cellulose and hemicellulose structures, as well as structural homogeneity at both molecular, nanofibril and fiber length scales.