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Organic redox-active polymers (RAPs) have emerged as promising energy storage materials since their alternate material feedstocks would reduce dependence on strategic minerals such as lithium, cobalt, and nickel. In typical polymer composite electrodes, a large fraction of the mass loading (30-50%) is occupied by high molecular weight polymer binder such as polyvinylidine fluoride (PVDF) and conductive carbon additive, representing a large proportion of inactive mass on the electrode. This work aims to increase the active mass loading efficiency and demonstrates an additive free, solution processable, and crosslinkable polymer containing phenothiazines as the redox active moiety for charge storage. Tradeoffs in electrochemical properties such as (dis)charge rate capability, accessible capacity, and coulombic efficiency are demonstrated as a function of crosslinking density. These results suggest that the thermophysical properties that result from changing crosslinking densities have profound effects on their electrochemical performance and help to guide the design of new polymer-based active materials.
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