Document Type

Dissertation

Degree

Doctor of Philosophy (PhD)

Major/Program

Materials Science and Engineering

First Advisor's Name

Bilal El-Zahab

First Advisor's Committee Title

Committee chair

Second Advisor's Name

Chunlei Wang

Second Advisor's Committee Title

Committee member

Third Advisor's Name

Norman Munroe

Third Advisor's Committee Title

Committee member

Fourth Advisor's Name

Yu Zhong

Fourth Advisor's Committee Title

Committee member

Fifth Advisor's Name

Irene Calizo

Fifth Advisor's Committee Title

Committee member

Keywords

lithium oxygen batteries, cathode, catalysis, electrochemical characterization, EIS

Date of Defense

5-23-2018

Abstract

High energy density batteries have garnered much attention in recent years due to their demand in electric vehicles. Lithium-oxygen (Li-O2) batteries are becoming some of the most promising energy storage and conversion technologies due to their ultra-high energy density. They are still in the infancy stage of development and there are many challenges needing to be overcome before their practical commercial application. Some of these challenges include low round-trip efficiency, lower than theoretical capacity, and poor rechargeability. Most of these issued stem from the poor catalytic performance of the cathode that leads to a high overpotential of the battery. In this doctoral work, Li-O2 cathodes containing nanoparticles of palladium were used to alleviate this problem. Cathodes composed of palladium-coated and palladium-filled carbon nanotubes (CNTs) were prepared and investigated for their battery performance. The full discharge of batteries showed 6-fold increase in the first discharge of the Pdfilled over the pristine CNTs and 35% increase over their Pd-coated counterparts. The Pd-filled CNTs also exhibited improved cyclability with 58 full cycles of 500 mAh·g-1 at current density of 250 mA·g-1 versus 35 and 43 cycles for pristine and Pd-coated CNTs, respectively. The effect of encapsulating the Pd catalysts inside the CNTs proved to increase the stability of the electrolyte during both discharging and charging. Voltammetry, Raman spectroscopy, XRD, UV/Vis spectroscopy, and visual inspection of the discharge products using scanning electron microscopy confirmed the increased stability of the electrolyte due catalyst shielding. The electrochemical oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) on carbon nanotubes (CNT) cathodes with palladium (Pd) catalyst, Pd-coated CNT and Pd-filled CNT, have been evaluated in an ether-based electrolyte solution to develop a lithium oxygen (Li−O2) battery with a high specific energy. The electrochemical properties of CNT cathodes were studied using electrochemical impedance spectroscopy (EIS). The infrared spectroscopy and SEM are employed to analyze the reaction products adsorbed on the electrode surface of the Li-O2 battery developed using Pd-coated and Pd-filled CNTs as cathode and an ether based electrolyte. vii Studies in this dissertation conclude that the use of nanocatalysts composed of palladium improved the overall performance of the Li-O2 batteries, while shielding these catalysts from direct contact with the electrolyte prolonged the life of the battery by stabilizing the electrolyte.

Identifier

FIDC006823

Available for download on Tuesday, May 12, 2020

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