“…The heterogeneous enolization reaction in carbonyl redox chemistry between CO and C–O – is an essential physiological process in organisms that widely exist in nature. , It sheds light on the broad utilization of organic carbonyl-based aqueous organic electrode materials, where the electrochemical performance could be regulated by tailoring the structure and functional groups of the carbonyls. − Specifically, due to the high theoretical capacity and fast reaction kinetics, the carbonyl-based organics with small molecular weights are the widely studied cathodes for high-performance aqueous energy storage, especially when coupled with the Zn metal anode. − However, the low energy density and the poor cycling stability make the overall electrochemical performance of these carbonyl-based organic electrodes still not comparable with the inorganic counterparts. , To solve this problem, various strategies have been adopted to modify the carbonyl-based electrodes, such as hybridization with carbon materials, molecular polymerization, functional group manipulation, , and constructing the conjugate structure. , Although the electrochemical performance of the organic electrodes has been accordingly improved to a certain extent, the corresponding synthesis complexity, high costs, and more nonactive components might make their practical application more difficult. − Recently, the electrochemical behaviors of the organic electrodes were revealed to be differentiated when storing different charge carriers in electrolytes. , It shed light on electrolyte engineering by adjusting the components in the electrolyte, which could accommodate more simplicity and efficiency in performance improvement compared with the complex electrode modifications . Thus, it can potentially improve the performance of organic electrode materials by tailoring ion species being stored by the carbonyl electrodes, while clarifying the charge storage manners of organic materials is a prerequisite.…”