Porous electrodes are critical components in redox flow batteries where they are responsible for multiple critical functions in the cell, such as providing surfaces for electrochemical reactions, an open structure for fluid flow and mass transport, and the conductive scaffold for electronic and thermal conduction. However, our current portfolio of materials is limited to carbon-fiber-based electrodes which are assembled using various mechanical methods (e.g., paper making, weaving, hydro-entangling) resulting in distinct structures such as papers, cloths, and felts (1). These fabrication methods involve multiple complex subprocessing steps impacting the final product cost and limiting the achievable range of electrode properties, which ultimately restricts device performance (2). Thus, there is a need to develop new material sets with precise control over microstructure and surface composition while employing synthetic methods that are compatible with large-scale manufacturing.In this lecture, I will discuss our efforts to design tailored electrodes for redox flow batteries, which hold promise for long-duration stationary energy storage (3). First, I will introduce a pore network modeling framework that captures electrochemical performance in complex microstructures with low computational requirements (4), and then show the coupling of this framework with a genetic algorithm to enable bottom-up electrode design (5). In our most recent effort, we are building topology optimization models of porous electrodes using multi-scale modeling of redox flow batteries, coupling computational macro- and meso-scale models of transport processes constructed using finite element and finite volume methods. We then couple these approaches with upscaling strategies that enable manufacturability of the structures. Second, I will describe a new approach to synthesizing porous electrodes based on non-solvent induced phase separation (NIPS) (6). NIPS is a simple and versatile fabrication method that can be used to synthesize morphologically-diverse electrode microstructures (e.g., isoporous, pore-size gradients, and multimodal porosity) by tuning simple parameters in the polymer solution, such as polymer concentration, solvent type, and temperature. Using a suite of microscopic, spectroscopic, and electrochemical diagnostic tools, I will present synthesis-property-performance relationships of the NIPS electrodes (7). Third and finally, I will highlight our efforts to functionalize porous electrode interfaces with organic molecules to impart targeted functional properties including hydrophilicity, kinetic activity (8), and selectivity (e.g. H2 evolution suppression). References A. Forner-Cuenca, F. R. Brushett, Curr. Opin. Electrochem. 18, 113–122 (2019).C. Minke, U. Kunz, T. Turek, J. Power Sources. 342, 116–124 (2017).M. L. Perry, K. E. Rodby, F. R. Brushett, ACS Energy Lett. 7, 659–667 (2022).M. van der Heijden, R. van Gorp, M. A. Sadeghi, J. Gostick, A. Forner-Cuenca, J. Electrochem. Soc. 169, 040505 (2022).R. van Gorp, M. van der Heijden, M. A. Sadeghi, J. Gostick, A. Forner-Cuenca, Chem. Eng. J. 455, 139947 (2023).C. T. Wan et al., Adv. Mater. 33, 2006716 (2021).R. R. Jacquemond et al., Cell Reports Phys. Sci. 3, 100943 (2022).E. B. Boz, P. Boillat, A. Forner-Cuenca, ACS Appl. Mater. Interfaces. 14, 41883–41895 (2022).