Pore–solid architectures in which the redox-active solid and void are co-continuous amplify the addressable electrified interface per geometric area, simplifying analytical characterization. Hundreds of square centimeters per square centimeter of footprint makes that an inevitability, but it also innately distributes reaction fronts in space imparting more uniform current distribution. We use such architected electrodes because their structural characteristics ensure (i) interconnected pathways that maintain long-range electronic conductivity within the electrode volume; (ii) ionic and molecular flux approaching open-medium diffusion through the pore network; and (iii) confined internal void volume that controls precipitation/dissolution dynamics and product redistribution. Such architected electrodes physically impose a means to control undesirable morphological changes that too often accompany local electrochemistry during charge/discharge cycling of batteries. As examples of this architectural approach to control local electrochemistry, formulating zinc in a sponge form factor creates an alkaline anode that cannot form zinc dendrites while painting layered MnOx as a nanometric coating throughout a carbon nanofoam improves the rate performance of zinc-ion cathodes.

Architected control of local effects in electrochemistry

ACS Spring 2022

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