Size-exclusion non-aqueous redox flow batteries (NRFBs) are emerging technologies for energy storage that promise higher energy densities than their aqueous counterparts. In NRFBs, redoxmers (i.e. mono-, oligo-, or polymeric redox-active species) in electrolyte solutions are used as charge storing media. Reaction of concentrated redoxmer solutions at electrode interfaces is necessary to operate these devices. However, the interactions between these electrodes and the redoxmers can lead to phenomena such as film formation and decomposition of the redoxmer solutions. Thus designing systems capable of removing the risk of redoxmer accumulation and reverting the damage is highly desirable. For these purpose, we have recently investigated the use of homobenzylic ethers (HBEs) as potential structural motifs in which redox-triggered reactions create conditions for breaking up and removing damaged material at the electrode surface. In this presentation, we will focus on the in situ investigation of the redox-trigger process. Using advanced generation-collection devices, as well as the scanning electrochemical microscope (SECM), we have detected reaction intermediates from the mesolytic cleavage of HBEs in solution. Characterization of the redox nature of the detected fragments together with computational approaches of the possible intermediates allowed us to better understand the bond breaking process. This information is key for the design of HBE redoxmers with redox-active groups attached to them. We will discuss the relevant design criteria for achieving this goal. The prospects of using the SECM and related methods in different modalities to understand the formation of short-lived intermediates, redoxmer blocking films, and the changes in electrode redox kinetics accompanying the cleavage process will be discussed.<br/>

<i>In situ</i> investigation of reactive intermediates during the programmable degradation of redoxmers for advanced redox flow battery interfaces

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.

In situ investigation of reactive intermediates during the programmable degradation of redoxmers for advanced redox flow battery interfaces