Note: When clicking on a Digital Object Identifier (DOI) number, you will be taken to an external site maintained by the publisher.
Some full text articles may not yet be available without a charge during the embargo (administrative interval).
What is a DOI Number?
Some links on this page may take you to non-federal websites. Their policies may differ from this site.
-
Engineering redox-active compounds to support stable multi-electron transfer is an emerging strategy for enhancing the energy density and reducing the cost of redox flow batteries (RFBs). However, when sequential electron transfers occur at disparate redox potentials, increases in electrolyte capacity are accompanied by decreases in voltaic efficiency, restricting the viable design space. To understand these performance tradeoffs for two-electron compounds specifically, we apply theoretical models to investigate the influence of the electron transfer mechanism and redox-active species properties on galvanostatic processes. First, we model chronopotentiometry at a planar electrode to understand how the electrochemical response and associated concentration distributions depend on thermodynamic and mass transport factors. Second, using a zero-dimensional galvanostatic charge/discharge model, we assess the effects of these key descriptors on performance (i.e., electrode polarization and voltaic efficiency) for a single half-cell. Finally, we extend the galvanostatic model to include two-electron compounds in both half-cells, demonstrating compounding voltage losses for a full cell. These results fundamentally show why multi-electron compounds with disparate redox potentials are less attractive than those with concerted electron transfer. As such, we suggest new directions for molecular and systems engineering to improve the prospects of these materials for RFBs.more » « less
An official website of the United States government
