Atomically Thin Processing of High Surface Area Nanomaterials for Electrochemical Energy Devices

As interest in renewable energy grows on both research and policy fronts, energy storage likely represents one of the most viable solutions to the problems posed by the intermittency and irregularity of renewable resources. While new classes of materials promise improved performance of energy storage systems, understanding energy storage electrode architecture and fabrication at the micro-scale allows us to fully leverage performance along different dimensions. This dissertation aims to explore the use of device architecture manipulation to improve energy storage and conversion electrodes, focusing on addressing challenges around manufacturing high-surface area electrodes. Phsyically, our approach to texturizing electrodes consists of synthesizing materials as to create high-surface area templates while physically manipulating the electrode to maximize performance. Chemically, we manipulate performance with Angstrom-level precision, utilizing atomically thin layers to induce chemical enhancement of our devices at the electrode interface. The principles of leveraging physical and chemical manipulation of electrodes is demonstrated in five unique works: (1) atomic layer deposition of titanium-nitride on carbon nanotubes for supercapacitor applications, (2) two-dimensional iron-phosphate for supercapacitor applications, (3) thiophene-based electrodeposition for photoelectrochemical water splitting, (4) titanium dioxide-coated zinc oxide nanowire arrays for photoelectrochemical water splitting, and (5) development of atomic layer deposited black titania for photoelectrochemical water splitting