Abstract
<h2>Summary</h2> Electrochemical synthesis of high-value chemicals using renewable electricity could lead to sustainability advantages over conventional chemical manufacturing. The tight coupling between paired anodic and cathodic reactions in conventional electrochemical processes, however, constrains the products and their efficiencies. Here, we demonstrate a strategy to achieve modular electrochemical synthesis (ModES) of different chemicals by decoupling and pairing the oxidative and reductive half-reactions with a heterogeneous redox reservoir (RR). Specifically, sodium nickel hexacyanoferrate (NaNiHCF) can serve as a robust and reversible RR that enables the modular production of several strong oxidants, hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) and sodium persulfate (Na<sub>2</sub>S<sub>2</sub>O<sub>8</sub>) or active chlorine, in separate RR-coupled electrochemical processes. The system's excellent performance and operational stability is demonstrated by continuous operation over 100 cycles (∼36 h) to produce H<sub>2</sub>O<sub>2</sub> and Na<sub>2</sub>S<sub>2</sub>O<sub>8</sub> with a high voltage efficiency. The concept presented here highlights the prospects for using RRs to enable efficient, modular, and on-demand electrochemical synthesis of valuable chemicals.
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