INNOVATIVE SCANNING PROBE METHODS FOR ENERGY STORAGE SCIENCE: ELUCIDATING THE PHYSICS OF BATTERY MATERIALS AT THE NANO-TO-MICROSCALE

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Date

2017

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Abstract

In recent decades, approaches to generate electrical energy through renewable

means has greatly benefited from technological advancements. However, the need

for robust schemes to store that energy in safe and cost-effective manners persists.

Thus, there is a shared global call to advance electrical energy storage science and

technology. Breakthroughs in the field stand to impact humans, ecosystems,

environments, economies, and even international security. Currently, many

innovative routes rooted in basic science are being taken to develop novel concepts,

chemistries, electrolytes, and geometries for electrical energy storage. Many of

these approaches make use of nano-to-mesoscale structures and technologies which

increases the demand for new methods of characterization and scientific discovery

at those scales. Still, progress to address this demand is stymied by practical

scientific and technological challenges associated with the buried interfaces in

battery systems.

In this dissertation, I present how my PhD work has precisely targeted this need

within the energy storage community, and made lasting impact. I detail why, and

how, I have pioneered scanning-probe based technologies and techniques that make

use of “battery probes” consisting of electrochemically active materials. A suite of

techniques is developed and leveraged for basic electrical energy storage science:

scanning nanopipette and probe microscopy, pascalammetry with microbattery

probes, inverted scanning tunneling spectroscopy, and nanoscale solid-state

electrochemistry with nanobattery probes. The use of these techniques motivated

finite-element numerical simulations of electrostatic potentials, and electric fields,

at play during field-driven lithiation of multi-walled carbon nanotubes. Also

motivated were analytical models for surface diffusion and diffusion through a

stressed electrolyte simultaneously experiencing latent-species activation.

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