Solid-state lithium-ion batteries promise to deliver the next generation of energy storage with necessary improvements in safety, energy density, and durability. However, their broad commercial success requires the development of scalable manufacturing processes to address fabrication challenges associated with composite electrodes, electrode/solid electrolyte interfaces, and thin solid electrolyte layers. In parallel with the need for innovation in solid-state battery fabrication, there is a rapid progress in the field of 3D printing of functional materials. Hence, there is now the opportunity to consider how additive manufacturing informs fabrication processes for solid-state lithium-ion batteries. Herein, the fabrication requirements of solid-state lithium-ion batteries are described and recent examples of digitally fabricated solid-state lithium-ion batteries, components, and materials are highlighted. A critical review of initial efforts toward 3D printing of solid-state lithium-ion batteries provides the prospective to identify future challenges and prospects.

The effect of the deposition substrate on the performance of inkjet-printed membrane electrode assemblies (MEAs) is investigated. MEAs are fabricated from inkjet-printed catalyst-coated membranes (CCMs), gas diffusion electrodes (GDEs), and a bilateral sandwich of a CCM and a GDE. All MEAs are tested in proton exchange membrane fuel cells (PEMFCs). When a hot-pressing step is included in the MEA construction, the power density achieved with the GDE-based MEA is 1.067 W cm À2 , exceeding that achieved with the CCM-based MEA (0.579 W cm À2 ), and the bilateral sandwich MEA (0.792 W cm À2 ). The origin of the superior performance of the inkjet-printed GDE-based MEAs is investigated through electrochemical impedance spectroscopy and analysis of the microstructure of the printed membranes and electrodes. Atomic force microscopy and energy dispersive X-ray spectroscopy suggest that the greater surface and interfacial areas of the GDE-printed catalyst layer may drive the unexpectedly high performance of the GDE-based MEA as compared with its CCM and bilateral sandwich counterparts. These results provide new insights into the connections between the substrate, inkjet-printed catalyst layer microstructure, and catalyst utilization.

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Agradeço de forma especial ao meu orientador Prof. Dr. Germano Tremiliosi-Filho pela orientação, paciência e confiança durante a realização deste trabalho.Agradeço aos professores do Grupo de Eletroquímica do Instituto de Química de São Carlos (IQSC) pela acolhida e pelas oportunidades de discussões acerca de temas relacionados a este trabalho. Agradeço aos colegas doGrupo de Eletroquímica pelas discussões científicas, pelas trocas de experiências acerca de diversos temas da química e pelos momentos de companheirismo e descontração que também são fundamentais para o desenvolvimento humano. Agradeço de forma muito especial aos meus pais Antônia Gomes Bezerra e Raimundo Bezerra, e aos meus irmãos Adriano, Andréia, Agostinho, Antônio Francisco e Maria Adriele por todo amor, carinho e incentivo. Agradeço à minha esposa Larissa Sousa Pereira Bezerra pelo amor, companheirismo e incentivo ao longo dessa caminhada. Agradeço aos funcionários técnicos e administrativos do IQSC em especial aos técnicos do Grupo de Eletroquímica, Mauro Fernandes, Jonas e Valdecir por todo auxílio prestado durante a realização deste trabalho. O presente trabalho foi realizado com apoio da Coordenação de Aperfeiçoamento de Pessoal de Nível Superior -Brasil (CAPES) -Código de Financiamento 001. Por fim, agradeço a todos que me ajudaram ao longo da realização deste trabalho e que não foram aqui mencionados. "Estude para ajudar seu povo" (Lema do Colégio Santa Teresa -Presidente Médici/MA) RESUMO BEZERRA, C. A. G. Estudo da eletrooxidação de etanol e glicerol assistida por fótons utilizando substrato de nanotubos de TiO 2 modificado. 2022. 116 f. Tese (Doutorado

In order to optimize the mass transport, catalyst utilization, and ohmic resistance of membrane electrolyte assemblies (MEAs) in Polymer Electrolyte Membrane Fuel Cells (PEMFCs), a series of low Pt-loading double-layered cathodes was fabricated through inkjet printing. The printed cathodes were designed such that the total Pt/C catalyst loading was 0.1 mg cm −2 with X% of the catalyst printed on the carbon substrate and (100−X)% on the Nafion membrane (X = 100, 75, 50, 25, 0). Semi-empirical fits of fuel cell polarization curves show that voltage losses vary inversely with the percentage of material printed on the carbon substrate. Accordingly, the best fuel cell performance (2.0 A cm −2 ) was observed for the cell with 100% of the Pt/C deposited on the carbon substrate. Thus, for inkjet printed low Pt-loading cathodes, the double-layered structure show a performance intermediate between MEAs fabricated in the gas diffusion electrode (GDE) method, and MEAs fabricated with catalyst deposition solely on the Nafion membrane. This performance trend is unexpected when compared to double-layered cathodes created through conventional methods of catalyst deposition.