Synthesis and characterization of boron-doped graphitic carbon for energy storage applications

Abstract

Carbonaceous materials offer great utility as a medium for electrochemical energy storage of ions or for the storage of chemical fuels. The low molecular weight of the second-row element carbon affords access to materials that express remarkably high gravimetric energy densities, and the robust nature of carbon-carbon bonds allow for good cyclability and longevity of carbon-based materials for use in energy storage applications. With the growing popularity and recent advancement of electric vehicles, current battery technologies are pushed to their limits in terms of capacities as well as in minimizing charging times. This has motivated great efforts to discover new lightweight materials that outperform what has traditionally been used in these applications. Alternative energy carriers, such as hydrogen, are also critical for the development of our energy landscape yet are plagued with their own technical challenges; mainly low volumetric energy densities and safety concerns associated with high pressure gas storage systems. Chapter 2 reviews hydrogen storage in today's society as well as provides a review of past synthetic methods to generate high boron content graphite (BC 3'); being a promising metastable material for the storage of alkali metal ions as well as for solid state hydrogen storage at near ambient conditions. Chapter 3 focuses on the discovery of a new lithium storage mechanism within a novel carbon-based material possessing a high hydrogen content that is tolerant of extremely fast charging, yet still expresses high reversible capacities. Chapter 4 presents a systematic investigation for the detection of chemical environments within BC 3' through an examination of unique spectroscopic properties that originate from the materials phonon structure. Chapter 5 explores the generation of boron and carbon binary phases by the co-pyrolysis of molecular precursors and establishes a density functional theory based approach to align the cracking temperatures of molecular feedstocks; affording access to bulk metastable materials that contain a homogeneous distribution of chemical environments. This work is concluded with an assessment of the materials investigated herein from the perspective of energy storage, as well as provides directions for future work.