SYNTHETIC DEVELOPMENT AND ELECTRODE PROCESSING OF LOW-DIMENSIONAL NANOMATERIALS FOR ADVANCED ELECTROCHEMICAL SYSTEMS
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Future advancements in terms of energy storage systems (lithium-ion batteries [LIBs] and beyond) rely on the development of novel materials, innovative electrode/device architectures, and scalable processing techniques or a combination thereof. In this thesis, each of these three facets will be explored to elucidate material-structure-property relationships of novel low-dimensional nanomaterials (LDNMs; i.e. 2D to 0D) and their assembled electrode/device architectures from a fundamental perspective or through performance demonstrations in conventional (LIBs) as well as advanced battery chemistries (e.g. lithium-oxygen batteries [LOBs]).
The first part of the thesis employs an advanced in-situ/operando technique with a newly developed planar microbattery platform to study alkali-metal-ion battery operation at the nanoscale with a model intercalation (2D) material: molybdenum disulfide. By coupling an atomic force microscope (AFM) with an open liquid electrochemical cell, real-time topographical observations, including structural evolution and concomitant solid electrolyte interphase (SEI) formation, can be readily achieved for numerous electrode-electrolyte systems. The second portion focuses on the development and importance of nanoporous carbon-based materials (2D holey graphene [hG], hG/nanohybrids, and holey graphene oxide) to fabricate unique electrode architectures via alternative electrode processing techniques (dry/cold pressing, extrusion-based 3D printing) for LIBs and beyond. Material properties, such as nanoporosity and surface chemistry, enable the processability of these LDNMs into structurally-conscious, additive-free electrode designs and lead to improved overall electrochemical performance, especially for high-energy dense applications such as LOBs. The final portion of this thesis reports a novel high temperature synthesis technique, referred to as carbothermal shock (CTS), capable of combining up to 8 immiscible elements into a single solid solution (0D) nanoparticle on carbon supports. Through exploratory studies, the synthetic capabilities and potential applications of CTS are identified by developing and evaluating novel multimetallic solid solution nanoparticles for both catalytic and energy-related applications, including LOBs.