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In this thesis, solar-hydrogen Stand-Alone Power System (SAPS) which is planned to be built for the emergency room of a hospital is designed. The system provides continuous, off-grid electricity during the whole period of a year without any external electrical power supply. The system consists of Photovoltaic (PV) panels, Proton Exchange Membrane (PEM) based electrolyzers, PEM based fuel cells, hydrogen tanks, batteries, a control mechanism and auxiliary equipments such as DC/AC converters, water pump, pipes and hydrogen dryers. The aim of this work is to investigate the optimal system configuration and component sizing which yield to high performance and low cost for different user needs and control strategies. TRNSYS commercial software is used for the overall system design and simulations. Numerical models of the PV panels, the control mechanism and the PEM electrolyzers are developed by using theoretical and experimental data and the models are integrated into TRNSYS. Overall system models include user-defined components as well as the default software components. The electricity need of the emergency room without any shortage is supplied directly from the PV panels or by the help of the batteries and the fuel cells when the solar energy is not enough. The pressure level in the hydrogen tanks and the overall system efficiency are selected as the key design parameters. The major component parameters and various control strategies affecting the hydrogen tank pressure and the system efficiency are analyzed and the results are presented.

<p dir="ltr">A major goal of applied electrocatalysis research has been the development of electrode materials that are active, selective, stable, and cost effective in producing electricity or desired products. In recent years, developments in <i>ab initio</i> methods for the simulation of catalyst surfaces, and electrochemical reactions occurring on them, have enabled the development of a fundamental understanding of the processes occurring at the solid-liquid interface at an atomistic scale. In combination with experiments, these calculations are helpful in elucidating design principles that can then inform electrocatalyst design. In this work, we describe the application of density functional theory, <i>ab initio</i> molecular dynamics, and high throughput materials informatics approaches to understand oxygen and carbon based electrochemistries, with relevance to electricity conversion and environmental protection. We also introduce an approach, based on a Born-Haber cycle analysis, to quantify adsorbate stabilization from solvent molecules that are ubiquitous for any electrochemical reaction occurring at solid-liquid interfaces.</p><p dir="ltr">The oxygen reduction reaction (ORR) occurs at the cathode in hydrogen fuel cells and, in conjunction with the hydrogen oxidation reaction (HOR) at the anode, produces electricity and water. While platinum group metals are the current state-of-the-art catalysts for the ORR, their high cost has necessitated an extensive search for alternatives. To this end, we investigated iron-nitrogen-carbon (Fe-N-C) catalysts, which are platinum group metal-free and have been shown experimentally to have reasonable activity compared to platinum. Despite their potential as cost effective materials, however, these catalysts are not durable over long-term operation of fuel cells, impeding their commercial adoption. The mechanisms of deactivation of the iron-nitrogen-carbon catalysts under aqueous acidic electrochemical reaction conditions remain debated, and deciphering them is complicated due to the complex structure of the catalyst. We attempt to address these challenges by first examining the structural aspects of the catalyst, sampling numerous potential active site configurations, determining their in-situ structure, and linking them to intrinsic activity and intrinsic stability descriptors. Our findings reveal that an activity-stability tradeoff exists, with the most active sites being most prone to stability issues. Additionally, we explored the role of hydrogen peroxide, a side product of ORR, in degrading Fe-N-C catalysts. This analysis demonstrated that hydrogen peroxide strongly oxidizes the catalyst surface, resulting in an activity loss in the catalyst. Based on these insights, we propose design principles to enhance the activity and stability of Fe-N-C catalysts.</p><p dir="ltr">In additional work, we compared the predictions for the Fe-N-C catalysts with ORR analysis on platinum catalysts, and we further analyzed the oxygen evolution reaction (OER) on iridium oxides and the carbon dioxide reduction reaction (CO₂R) on copper catalysts in water electrolyzers. For ORR on platinum, we identified the formation of hydroxyl and water adsorbate rings on stepped surfaces, akin to hexagonal rings found on terraces but largely absent on Fe-N-C catalysts. The ORR follows an associative mechanism involving proton coupled electron transfer to these ring structures. Furthermore, we provided activity descriptors that aligned with experimental observations, showing a higher activity on stepped surfaces compared to terraces. For OER on iridium oxides, we examined transformations of IrO₂ (110) surfaces, and we pinpointed oxidation of bridge and coordinatively unsaturated top sites as key charge transfer steps that correlate with peaks in cyclic voltammograms. Finally, for CO₂R on copper, we investigated the role of water as a proton source under neutral or alkaline conditions, providing insights into the effect of coverages of surface species on the kinetics of water dissociation that, in turn, can provide protons for CO₂ reduction and the competing hydrogen evolution reaction.</p><p dir="ltr">Through this work, we have gained a deeper understanding of the properties of various catalytic materials under conditions specific to each type of electrochemistry. We elucidated the relationships between the in-situ structure, activity, and stability for the electrocatalysts, and identified key factors influencing catalyst performance. Integrating such insights from a computational perspective with experimental approaches holds great potential in making significant advancements in developing sustainable energy technologies and ultimately contributing to a greener and more energy-efficient future.</p>