Probing the Structure, Organization, and Oligomerization of Biomolecular Ligands on Silica Surfaces with an Emphasis in Origin of Life

Nanotechnology is an integral part of advancements in material science and biomedical devices. The surface of nanomaterials govern how they behave in various media and what properties they possess. Decades of research have gone into fine tuning nanomaterial production for various applications, but the fundamental understanding of the chemistry that occurs at the interface is surprisingly underdeveloped. Achieving atomic-level resolution is possible with few analytical techniques. Systems that are amorphous and/or dynamic are even more challenging to characterize. Solid-state nuclear magnetic resonance is a vital tool capable of bridging this gap. The work presented in this dissertation has three objectives: (1) understand how different biomolecular ligands organize on the surface of silica nanoparticles (2) characterize structural differences among silica nanomaterials, and (3) apply these techniques to understand chemical evolution and the origin of life on Earth. Silica, or SiO2, was selected as the focus of this investigation because it is ubiquitous in biomedical applications due to high surface area, tunable features, and biocompatibility. Silica and silica-based clays are also the most abundant mineral on our planet, composing the majority of Earth’s crust. Many advancements in origin of life research suggest silica could have played an important role in directing prebiotic reactions. It is capable of directing self-assembly of amino acids and lipids, concentrating dilute solutions of organic molecules, and lowering the activation energy for polymerization. Understanding the relationship between biochemical ligands and silica substrates can offer unique insights into our past and advancements in the future