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ELECTROCATALYSTS FOR ALKALINE WATER ELECTROCATALYSIS
Title
ELECTROCATALYSTS FOR ALKALINE WATER ELECTROCATALYSIS
Creator
Jain, Anchal
Date
2016, 2016-07
Description
Hydrogen is an attractive energy carrier and is part of an idealistic future wherein it serves as a clean energy source. In the presence of...
Show moreHydrogen is an attractive energy carrier and is part of an idealistic future wherein it serves as a clean energy source. In the presence of oxygen, it can be converted to water in fuel cells with the release of heat and electrical work. Electrolysis of water is an important route to hydrogen generation. Alkaline water electrolysis is preferred over electrolysis in acidic medium due to the possibility of lowering stack costs and enhancing the library of stable electrocatalyst materials available for the electrochemical reactions. The high anode overpotential arising from the sluggish oxygen evolution reaction (OER) has led to significant interest in developing stable and active OER electrocatalysts. IrO2 (state of the art catalyst), RuO2 and PGM-based pyrochlores are suitable catalyst materials that exist today, but there is benefit in finding cost-effective alternatives. In this study, the pyrochlore oxides containing non- Platinum Group Metals (non-PGM) metals were synthesized by solid state reaction and were tested for their OER activity but none of the materials tested, exhibited OER activity and a comparison was attempted between the pyrochlores containing PGM metals as against those containing non-PGM metals. Additionally, perovskite oxides of the form La[Ni(1-x-y)CoxFey]O3 (where 0≤x≤1 and 0≤y≤1) were synthesized by the co-precipitation method. Many of these perovskites exhibited electron conductivities greater than 0.1S/cm, eliminating the need to add carbon for OER studies and implying the likelihood of making conducting electrodes with these materials without the additives like carbon. The perovskites LaNi0.6Co0.4O3 or LaNi0.6Fe0.4O3 with x/y =0.4 had conductivities of the order of 10S/cm. The electrocatalytic activity for the OER was studied using a rotating disk electrode (RDE) in 0.1M KOH and catalyst loading of ~100μg/cm2. The perovskite LaNi0.5Co0.5O3 (x=0.5, y=0) had the onset potential of ~1.50V against RHE, and all these perovskites had onset potentials ~0.1-0.15V higher than the benchmark IrO2 that has an onset potential of ~1.43V. Few of the perovskites were also evaluated for their oxygen reduction activity (ORR) implying that these materials can be used as bi-functional catalysts.
M.S. in Chemical Engineering, July 2016
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Design and Synthesis of New Sulfur Cathodes Containing Polysulfide Adsorbing Materials
Title
Design and Synthesis of New Sulfur Cathodes Containing Polysulfide Adsorbing Materials
Creator
Suzanowicz, Artur M
Date
2023
Description
Lithium-sulfur battery (LSB) technology has tremendous prospects to substitute lithium-ion battery (LIB) technology due to its high...
Show moreLithium-sulfur battery (LSB) technology has tremendous prospects to substitute lithium-ion battery (LIB) technology due to its high theoretical specific capacity and energy density. However, escaping polysulfide intermediates (produced during the redox reaction process) from the cathode structure is the primary reason for rapid capacity fading. Suppressing the polysulfide shuttle (PSS) is a viable solution for this technology to move closer to commercialization and supersede the established LIB technology. In this dissertation, I have analyzed the challenges faced by LSBs and selected methods and materials to address these problems. I have concluded that in order to further pioneer LSBs, it is necessary to address these essential features of the sulfur cathode: superior electrical conductivity to ensure faster redox reaction kinetics and high discharge capacity, high pore volume of the cathode host to maximize sulfur loading/utilization, and polar polysulfide-resistive materials to anchor and suppress the migration of lithium polysulfides.Furthermore, a versatile, low-cost, and practical scalable synthesis method is essential for translating bench-level development to large-scale production. This dissertation covers designing and synthesizing new scalable cathode structures for lithium-sulfur batteries that are inexpensive and highly functional. The rationally chosen cathode components accommodate sulfur, suppress the migration of polysulfide intermediates via chemical interactions, enhance redox kinetics, and provide electrical conductivity to sulfur, rendering excellent electrochemical performance in terms of high initial specific capacity and good long-term cycling performance. TiO2, Ni12P5, and g-C3N4 as polysulfide adsorbing materials (PAMs) have been fully studied in this thesis along with three distinct types of host structures for lithium-sulfur batteries: Polymer, Carbon Cloth, and Reduced Graphene Oxide. I have created adaptable bulk synthesis techniques that are inexpensive, easily scalable, and suitable for bench-level research as well as large-scale manufacturing. The exceptional performance and scalability of these materials make my cathodes attractive options for the commercialization of lithium-sulfur batteries.
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