Guidelines for the Rational Design and Engineering of 3D Manufactured Solid Oxide Fuel Cell Composite Electrodes

Abstract

The growth of 3D printing has opened the scope for designing microstructures for solid oxide fuel cells (SOFCs) with improved power density and lifetime. This technique can introduce structural modifications at a scale larger than particle size but smaller than cell size, such as by inserting electrolyte pillars of ∼5-100 μm. This study sets the minimum requirements for the rational design of 3D printed electrodes based on an electrochemical model and analytical solutions for functional layers with negligible electronic resistance and no mixed conduction. Results show that this structural modification enhances the power density when the ratio k eff between effective conductivity and bulk conductivity of the ionic phase is smaller than 0.5. The maximum performance improvement is predicted as a function of k eff . A design study on a wide range of pillar shapes indicates that improvements are achieved by any structural modification which provides ionic conduction up to a characteristic thickness ∼10-40 μm without removing active volume at the electrolyte interface. The best performance is reached for thin (<∼2 μm) and long (>∼80 μm) pillars when the composite electrode is optimised for maximum three-phase boundary density, pointing toward the design of scaffolds with well-defined geometry and fractal structures. Many studies in the literature have recognised the importance of the electrode microstructure in affecting the power density and the lifetime of solid oxide fuel cells (SOFCs).1-7 Significant enhancements in power density have been achieved through the statistical control of the microstructural properties by tuning porosity, 8,9 volume fractions, 2,8,10 particle size 11-13 and even tortuosity of the phases.14 However, nowadays the design of the electrode microstructure can be optimised with unprecedented precision through the advent of 3D printing and additive manufacturing techniques. 15-17Additive manufacturing allows for the development of electrodes with 3D architectures, thus going beyond what conventional fabrication techniques, such as tape casting and screen printing, can produce. The exploitation of 3D additive manufacturing has been successfully applied by the battery community [18][19][20] and the implementation of this approach to SOFCs is currently under investigation.15,21 One of the most promising applications consists of the insertion of ionconducting pillars connected to the electrolyte 15,[22][23][24][25] as reported in Figure 1. Such a modification can be regarded as the mesoscale structural control of electrode microstructure, where the term mesoscale here refers to a dimension larger than the typical constituent particle size (<1 μm) but smaller than the characteristic length of the cell, that is, falling in the order of 5-100 μm.26 Ideally, 3D printing offers the opportunity to controllably manufacture pillars of any shape, with the desired geometric and spacing requirements, in order to provide a preferential pathway for ionic conduction. 22,25 It is important to note that this mesos...

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