Year of Publication

2017

Degree Name

Doctor of Philosophy (PhD)

Document Type

Doctoral Dissertation

College

Engineering

Department

Chemical and Materials Engineering

First Advisor

Dr. Yang-Tse Cheng

Second Advisor

Dr. Susan Odom

Abstract

Silicon-based electrodes are the most promising negative electrodes for the next generation high capacity lithium ion batteries (LIB) as silicon provides a theoretical capacity of 3579 mAh g-1, more than 10 times higher than that of the state-of-the-art graphite negative electrodes. However, silicon-based electrodes suffer from poor cycle life due to large volume expansion and contraction during lithiation/delithiation. In order to improve the electrochemical performance a number of strategies have been employed, such as dispersion of silicon in active/inactive matrixes, devising of novel nanostructures, and various coatings for protection. Amongst these strategies, silicon-carbon coating based composites are one of the most promising because carbon coating is comparatively flexible, easy to obtain, and scalable with various industrial processes.

Low cost and renewable lignin, which constitutes up to 30% dry mass of the organic carbon on earth, is widely available from paper and pulp mills which produce lignin in excess of 50 million tons annually worldwide. It is a natural bio-polymer with high carbon content and highly interconnected aromatic network existing as a structural adhesive found in plants. Generally burnt for energy on site, lignin is gradually finding its way into high value-added products such as precursor for carbon fibers, active material in negative electrodes, and raw material for supercapacitors.

This dissertation focuses on high performance silicon-based negative electrodes utilizing lignin as the carbon precursor for conductive additive, binder, and carbon coating. To my knowledge this is one of the first works attempting to utilize and summarize the performance of lignin in silicon-based negative electrodes. The first part of the dissertation shows that silicon-lignin composites treated at 800 ºC displayed good capacity and cycling performance. The second part goes to generalize the effect of temperature on silicon-lignin composites and shows that a low temperature treatment granted an electrode with superior performance and cycling properties owing to the preservation of polymeric properties of lignin. The final part of the dissertation discusses the current research trends in SiOx based negative electrodes and extends lignin to that field.

This dissertation will, hopefully, provide knowledge and insight for fellow researchers wishing to utilize lignin or other renewable resources in devising advanced battery electrodes.

Digital Object Identifier (DOI)

https://doi.org/10.13023/ETD.2017.219

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