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However, the key step of single-electron acrylonitrile reduction demands toxic heavy-metal electrodes and leads to low energy efficiency. We developed a dynamic multimodal cation-electrode interaction strategy to enable efficient synthesis with environmentally friendly carbon electrodes. Optimal benzyltrihexylammonium cations create a water-depleted interface in aqueous electrolytes by squeezing the electric double layer through multimodal noncovalent interactions between the benzyl moieties of the cations and carbon electrodes. This strategy achieves selectivity comparable to the standard lead-based system but at substantially lower overpotentials, as demonstrated from the laboratory scale to a 159\u2013square centimeter electrolyzer. 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