Electrochemical bicarbonate reduction is a promising technology in carbon capture and conversion schemes. In this issue of Joule, Zhu et al. demonstrated an integrated strategy to facilitate bicarbonate-to-CO conversion by using a CoPc electrocatalyst that has strong CO2 adsorption and a cross-flow design to facilitate mass transfer, and achieved ∼95% Faradaic efficiency at 300 mA/cm2. Electrochemical bicarbonate reduction is a promising technology in carbon capture and conversion schemes. In this issue of Joule, Zhu et al. demonstrated an integrated strategy to facilitate bicarbonate-to-CO conversion by using a CoPc electrocatalyst that has strong CO2 adsorption and a cross-flow design to facilitate mass transfer, and achieved ∼95% Faradaic efficiency at 300 mA/cm2. Hierarchical design enables sufficient activated CO2 for efficient electrolysis of bicarbonate to COShen et al.JouleMay 8, 2024In BriefBicarbonate electrolyzers (BCEs) offer a direct coupling of carbon capture and conversion, reducing energy consumption. However, the faradaic efficiency of CO2 electrolysis in BCEs has been limited by insufficient activated CO2 on the catalyst surface in conventional BCEs. We report a hierarchical design strategy combining molecular and system-level innovations to ensure that there is sufficient activated CO2 on the catalyst in the new BCEs, achieving faradaic efficiencies exceeding 96.2% at 50–300 mA−2. Full-Text PDF