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Title

NANOMATERIALS FOR ADVANCED BATTERY CATHODES

Creator

Moazzen, Elahe

Date

2020

Description

Cathode materials are key components that directly determine the power density of a battery. One of the most effective ways of developing high...
Show moreCathode materials are key components that directly determine the power density of a battery. One of the most effective ways of developing high power density cathodes is bringing them into the nano-scale world, which results in many expected and unexpected properties. Some of the desired characteristics include faster charge/discharge kinetics, improved capacity retention and structural stability due to the higher surface to volume ratio and shorter ion diffusion paths. In this dissertation a number of uniquely designed nano-sized cathode materials and nanocomposites are developed and investigated for alkaline aqueous and lithium ion battery applications. Nickel hydroxide (Ni(OH)2), which is one of the most important cathode materials in alkaline batteries, suffers from low conductivity, which usually leads to inefficient discharge and incomplete utilization of the material. A series of Ni(OH)2/Co(OH)2 core/shell nanoplatelets were synthesized and systematically investigated as cathode materials. Structure-property correlations revealed that electrochemical behavior and reversibility of Co(OH)2 redox conversion depended non-linearly on the average shell thickness, with the best performance (99.6% of theoretical capacity of the composite material) achieved at shell thickness of 1.9 ± 0.3 nm. Two fundamental phenomena were suggested to be responsible for the superior performance: templated shell deposition and galvanic coupling of core and shell materials.Manganese (IV) oxide (MnO2), which is another practical cathode that has a great potential to be utilized for a variety of energy storage systems, still has some major challenges including reversible cycling in rechargeable batteries. One of the most crucial challenges is the fact that polymorphs of MnO2 have different electrochemical activities as aqueous and Li-ion battery cathodes. However, most synthetic samples contain a mixture of polymorphs, which makes the structure-property correlations more complicated. This dissertation reports on systematic studies correlating synthesis, thermal and mechanical processing, and composite formation with polymorph composition, electrochemical performance and ion intercalation mechanisms. Among all the results, several main conclusions were reached: 1) Through control of the synthesis parameters and post-processing, desired phase compositions and nanoparticle morphologies, which optimize MnO2 performance in aqueous alkaline electrolyte, can be achieved. Nanoparticles with higher fraction of the akhtenskite polymorph showed higher reversible capacities in LiOH electrolyte (~210 mAh g-1), with stable performance for over 50 cycles. The effects of sub-nanoparticle organization of MnO2 polymorphs by thermal treatment without any morphology change on cycling performance, phase activation, and charge/discharge mechanisms in LiOH electrolyte as well as the detailed mechanism of the polymorph conversion during annealing were studied and for the first time, demonstrating that the electrochemical activity of MnO2 material strongly depends not only on the lattice structure of individual polymorphs but also on the sub-nanoparticle polymorph architecture and interphases.2) Several processing strategies, including thermal and mechanical processing, and composite fabrication were utilized to develop functional MnO2 cathodes for Li-ion batteries. Improvements in capacity and cycling performance were correlated to the presence of the pyrolusite phase of MnO2 and the crystallite size. Composite fabrication by graphene oxide wrapping also provided significant performance improvements through polymorph composition control and improved conductivity.
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Title

Developing Advanced Materials for Carbon Dioxide Electroreduction to Value-Added Chemicals and Fuels

Creator

Esmaeilirad, Mohammadreza

Date

2023

Description

Developing highly efficient electrocatalysts for the carbon dioxide reductionreaction (CO2RR) to value-added fuels and chemicals offers a...
Show moreDeveloping highly efficient electrocatalysts for the carbon dioxide reductionreaction (CO2RR) to value-added fuels and chemicals offers a feasible pathway for renewable energy storage and could help mitigate the ever-increasing carbon dioxide (CO2) emissions from human activities. Different catalysts are known to catalyze CO2RR in aqueous solutions. Most known catalysts are only capable of transferring 2 electrons with needed protons to CO2 producing either carbon monoxide (CO) or formic acid (HCOOH). Copper (Cu) is the only electrocatalytic material that converts CO2 into different types of hydrocarbon products. Additionally, owing to Cu’s natural abundance and low cost, it has been intensively studied for CO2RR for decades. However, the required high input energy (overpotential), low product selectivity towards valuable fuel products, and the lack of long-term stability remain major challenges for Cu-based catalysts. This work aims to develop new materials that produce hydrocarbons at lower overpotentials with higher rates and greater selectivity than current copper catalysts. By implementing a process referred to as the electrocatalyst discovery cycle iterations between predications, catalyst testing, and active site characterization allow for the rational design and discovery of new and improved electrocatalysts for CO2RR. This methodology led to the discovery of different heteroatomic catalysts as low overpotential catalysts for electroreduction of CO2 high energy density hydrocarbon products.
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