Porous electrodes are utilized across electrochemical technologies including flow reactors and redox flow batteries. Controlling mass transport, conduction, and surface reaction in the electrodes is central to attaining peak device performance. Traditional methods often rely on manipulating the macroscopic electrode dimensions, device-level architecture, and flow distribution (e.g. via flow fields). However, beyond using traditional materials like felts or papers, engineering the internal electrode structure itself has recently emerged as a new design degree-of-freedom. These architected, porous electrodes are enabled by advanced and additive manufacturing techniques and are a promising route to provide greater control over the local transport and reactive environment, further improving device performance. New design tools will be necessary to fully exploit this expanded design space. Here we present a collection of computational design methodologies to automatically generate architected electrode design across scales. Resolved optimization techniques are used to determine optimal electrode architectures at the pore scale. Using homogenization, these techniques are then extended to scale-up the designs beyond typical benchtop dimensions. Using vanadium as a model chemistry, we demonstrate that the computationally designed electrodes yield improved performance across cost-functions and focus particularly on energy efficiency. Further, we analyze the resultant designs to highlight the structural features leading to improved performance.

This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

LLNL-ABS-830166