Date of Award

Spring 1-1-2014

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Mechanical Engineering

First Advisor

Se-Hee Lee

Second Advisor

Chunmei Ban

Third Advisor

Steven M. George

Fourth Advisor

Yifu Ding

Fifth Advisor

Ronggui Yang

Abstract

This dissertation presents various studies that have demonstrated significant advances in the production of stable and long-lasting high-capacity silicon-based anodes for next generation lithium-ion batteries. Each study builds upon the previous, culminating in the development of a full-cell containing a nano-structured silicon anode with stable capacity retention and 1000 cycles of cell progression. Along the way, confining matrices and flexible anode architectures are explored in the effort to solve the severe volumetric expansion induced by Li-Si alloying. Several surface coatings, a more recently studied silicon electrode modification, are also developed as part of this dissertation work. Each iteration, or refinement, of the silicon electrode nano-structure or surface provides interesting insights into the electrochemomechanics of the silicon electrode, allowing for a stronger understanding of the material and its workings in a lithium-ion cell. Finally, a combinatorial approach of the designed nano-structured silicon anodes with room temperature ionic liquid (RTIL) electrolytes is explored, enabling an impressive and highly energy-dense lithium-ion full-cell. The accomplishments presented herein represent important progress towards a safer, more energy-dense lithium-ion battery.

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