Electromethanation of CO has received intensive attention due to its high calorific value and convenient storage along with transportation to accommodate industrial demands. However, it is limited by sluggish multi-step proton-coupled electron transfer kinetics and undesired H coupling under high current density, posing great challenges to its commercialization. Herein, carbon nitride (CN) with superior hydrogen adsorption ability is used as an active-hydrogen adsorption and supply material. Through a facile liquid-assisted exfoliation and electrostatic self-assembly strategy to strengthen its interfacial contacts with CuO catalysts, yielding a strengthened CH production 52 times higher than that of pristine CuO. Flow-cell test ultimately achieved FE and remarkably CH partial current density of 61% and 561 mA cm, respectively. With in situ ATR-FTIR spectra and DFT calculations, it is established that strengthened interfaces enabled abundant H tethered by ─C─N═C─ sites in CN nanosheets and oriented to the CO hydrogenation to CHO and CHx on Cu species. This work reveals the profound influence of fine-expanded interfaces with dimensional materials on the product distribution and yield through the active-hydrogen management, which is of reference value for other small-molecule electro-polarization dominated by the proton-coupled electron transfer (PCET) process (e.g., N, O, etc.).
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