Fundamental research plays a pivotal role in the development of sustainable solutions that benefitboth our environment and everyday lives. Cellulose, as an abundant and renewable resource, holds immense potential for sustainable applications. However, navigating the complexities of molecular and supramolecular structure of cellulose poses significant challenges in harnessing its full potential. By delving into fundamental research, we aim to uncover the underlying mechanisms governing cellulose interactions, paving the way for innovative advancements in sustainable material development.This thesis uncovers the intricate relationship between fundamental research and appliedmethodologies by showing how molecular contact and structure at the interface of cellulose-richmaterials will control the development of the macroscopic mechanical properties of networks fromcellulose-rich fibres. The study encompasses various facets, ranging from the development of model materials for studying interfacial interactions to the preparation of fibrous networks with tailored properties.In the initial part of the work, the research delves into the development of model materials to investigate interactions at smooth interfaces of regenerated cellulose. The study reveals the crucial role of the making and breaking of cellulose interface, or sometimes interphase, in the development of adhesive joints. Experimental findings demonstrate how chemical additives influence the interactions between cellulose surfaces, thereby modulating the structural and adhesive properties at the interface. Furthermore, by utilizing model materials, insights are gained into fibre-fibre interactions and the influence of surface treatments on network formation and mechanical performance. Lastly, the research focused on investigating the preparation of fibrous networks atdifferent densities and amount of adsorbed additives, providing a comprehensive understanding ofhow network density and composition affect mechanical properties of the networks.This work not only exemplifies a synergistic approach, where fundamental insights into molecularcontacts and interface structures are translated into practical applications for enhancing macroscopicproperties but also highlights the importance of integrating fundamental and applied methodologies in molecular engineering, offering novel strategies for advancing sustainable paper production practices and contributing to the attainment of sustainable development goals.
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