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Thesis advisor: Udayan Mohanty / Thesis advisor: Dunwei Wang / With the fast development of society, the demand for batteries has been increasing dramatically over the years. To satisfy the ever-increasing demand for high energy density, different chemistries were explored. From the first-generation lead–acid batteries to the state-of-the-art LIBs (lithium ion batteries), the energy density has been improved from 40 to over 200 Wh kg⁻¹. However, the development of LIBs has approached the upper limit. Electrode materials based on insertion chemistry generally deliver a low capacity of no more than 400 mAh/g. To break the bottleneck of current battery technologies, new chemistries are needed. Moving from the intercalation chemistry to conversion chemistry is a trend. The conversion electrode materials feature much higher capacity than the conventional intercalation-type materials, especially for the O₂ cathode and Li metal anode. The combination of these two can bring about a ten-folds of energy density increase to the current LIBs. Moreover, to satisfy the safety requirements, either using non-flammable electrolytes to reduce the safety risk of Li metal anode or switch to dendrite-free Mg anode is a good strategy toward high energy density batteries. First, to enable the conversion-type O₂ cathode, a wood-derived, free-standing porous carbon electrode was demonstrated and successfully be applied as a cathode in Li-O₂ batteries. The spontaneously formed hierarchical porous structure exhibits good performance in facilitating the mass transport and hosting the discharge products of Li₂O₂. Heteroatom (N) doping further improves the catalytic activity of the carbon cathode with lower overpotential and higher capacity. Next, to solve the irreversible Li plating/stripping and safety issues related with Li metal anode, we introduced O₂ as additives to enable Li metal anode operation in non-flammable triethyl phosphate (TEP) electrolyte. The electrochemically induced chemical reaction between O₂- derived species and TEP solvent molecules facilitated the beneficial SEI components formation and effectively suppressed the TEP decomposition. The promise of safe TEP electrolyte was also demonstrated in Li-O₂ battery and Li-LFP battery. If we think beyond Li chemistries, Mg anode with dendrite-free property can be a promising candidate to further reduce the safety concerns while remaining the high energy density advantage. Toward the end of this thesis, we developed a thin film metal–organic framework (MOF) for selective Mg²⁺ transport to solve the incompatibility issues between the anode and the cathode chemistry for Mg batteries. / Thesis (PhD) — Boston College, 2020. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Chemistry.

Indiana University-Purdue University Indianapolis (IUPUI) / Recycling valuable cathode material from end-of-life (EOL) Li-ion batteries (LIBs) is essential to preserve raw material depletion and environmental sustainability. Direct recycling reclaims the cathode material without jeopardizing its original functional structures and maximizing return values from spent LIBs compared to other regeneration processes. This work employed two chemically delithiated lithium cobalt oxide (LCO) cathodes at different states of health (SOH), which are analogous to the spent cathodes but free of any impurities, to investigate the effectiveness of cathode regeneration. The material and electrochemical properties of both delithiated SOHs were systematically examined and compared to pristine LCO cathode. Further, those model materials were regenerated by a hydrothermal-based approach. The direct cathode regeneration of both low and high SOH cathode samples restored their reversible capacity and cycle performance comparable to pristine LCO cathode. However, the inferior performance observed in higher current density (2C) rate was not comparable to pristine LCO. In addition, the higher resistance of regenerated cathodes is attributed to lower high-rate performance, which was pointed out as the key challenge of the cathode recycling process. This study provides valuable knowledge about the effectiveness of cathode regeneration by investigating how the disordered, lithium-deficient cathode at different SOH from spent EOL batteries are rejuvenated without changing any material and electrochemical functional properties.

<p>Recycling valuable cathode material from end-of-life (EOL) Li-ion batteries (LIBs) is essential to preserve raw material depletion and environmental sustainability. Direct recycling reclaims the cathode material without jeopardizing its original functional structures and maximizing return values from spent LIBs compared to other regeneration processes. This work employed two chemically delithiated lithium cobalt oxide (LCO) cathodes at different states of health (SOH), which are analogous to the spent cathodes but free of any impurities, to investigate the effectiveness of cathode regeneration. The material and electrochemical properties of both delithiated SOHs were systematically examined and compared to pristine LCO cathode. Further, those model materials were regenerated by a hydrothermal-based approach. The direct cathode regeneration of both low and high SOH cathode samples restored their reversible capacity and cycle performance comparable to pristine LCO cathode. However, the inferior performance observed in higher current density (2C) rate was not comparable to pristine LCO. In addition, the higher resistance of regenerated cathodes is attributed to lower high-rate performance, which was pointed out as the key challenge of the cathode recycling process. This study provides valuable knowledge about the effectiveness of cathode regeneration by investigating how the disordered, lithium-deficient cathode at different SOH from spent EOL batteries are rejuvenated without changing any material and electrochemical functional properties.</p>

This thesis conducts research into different rechargeable battery technologies and their applicability to the high altitude balloon flights conducted at Esrange space center. The research focuses on the possible use of lithium ion batteries’, sodium ion batteries, nickel metal hydrate, and Metal hydridelithiumion batteries. Resulting in lithium ion batteries in 18650 cells being recommended. The thesis continues with a modular power distribution system architecture design. The system architecture is established with solarcharging capabilities, up to 1500W peak output power, over 600W continuous output power, multiple output voltages, more than six output channels, remote output power switching, and monitoring of power consumption. A prototype is built from this architecture on which limited testing is performed.The testing shines light on future improvements and displays proof of concept for some parts.

[pt] No Brasil, existem muitos projetos em sistemas fotovoltaicos, e a projeção para os próximos anos é de crescimento devido incentivos governamentais e os elevados preços das tarifas de energia. Associado a isso, o mercado de armazenamento de energia com baterias de íons de lítio tem se mostrado promissor devido a uma considerável queda nos preços dessas baterias nos últimos anos. Isso pode representar uma oportunidade para o mercado de sistemas fotovoltaicos quando os incentivos acabarem. Este trabalho propõe um modelo PLIM (Programação Linear Inteira Mista) estocástico para dimensionar um sistema fotovoltaico integrado com armazenamento de energia em baterias para grandes consumidores de energia, usando cenários de geração e consumo, podendo considerar diferentes modalidades tarifárias. As variáveis de decisão são o número de painéis, inversores, baterias, a operação diária do sistema de armazenamento e a demanda contratada do consumidor. A função objetivo busca minimizar o custo de investimento no sistema fotovoltaico, baterias e fatura de energia. A abordagem proposta será analisada sob diferentes premissas, uma com incentivos governamentais sobre a anergia injetada na rede e outra na qual a injeção de energia na rede não é permitida, a fim de avaliar a importância das baterias para manter a atratividade econômica do sistema fotovoltaico. Os resultados indicaram que o efeito sinérgico do sistema fotovoltaico com baterias potencializa a arbitragem, que está relacionada com a diferença entre as tarifas de energia de ponta e fora ponta. Isso ocorre principalmente com operação zero exportação porque somente assim o consumidor é livre para escolher a capacidade do seu sistema fotovoltaico, que hoje é limitado no Brasil quando o sistema é conectado na rede de distribuição. / [en] In Brazil, there are many projects in photovoltaic systems, and the projection for the coming years is positive due to the government incentives and the expensive energy tariffs. Associated with this, the Lithium-ion battery storage systems market has been promising due to a significant drop in battery prices in the last few years. This may represent an opportunity for the photovoltaic system market when the incentives run-out. This work proposes a stochastic mixed integer linear programming (MILP) model to design a photovoltaic system integrated with battery energy storage for big electricity consumers, using generation and consumption scenarios, being able to consider different Time-of-Use tariffs. The decision variables are the number of panels, inverters and batteries, its daily operation and the power demand contracted. The objective function aims to minimize the cost of investment, in the photovoltaic system, batteries and electricity bill. The proposed approach will be analyzed under different assumptions, one with the government incentive about injected surplus and another in which the injection into the network is not possible, in order to assess the importance of a storage system to keep the economic attraction of the photovoltaic system. Results indicated that the synergic effect of the photovoltaic system and battery potentialize the arbitrage, which is related to the difference between peak and off-peak energy tariff. This occurs, mainly with Zero Export operation because only this way the consumer is free to choose the capacity of the photovoltaic system, which is limited in Brazil when the system is allowed to inject energy into the network.