Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage

Electrified reactive capture upgrades CO₂ from post-air-capture alkali carbonate liquid to value-added products while regenerating the capture medium. Previous processes exhibited limited energy efficiency (<18%) due to high full-cell voltage (>3.7 V) and modest CO selectivity (<45%). To address this, we developed a Co molecular catalyst featuring an electron-deficient Co center, lowering the required reduction voltage. We then grafted the catalyst onto a conductive support, enhancing charge transfer. An electrified pH-downshifter improved CO₂ availability, increasing CO selectivity. The system achieved 70% CO selectivity at 2.7 V and 100 mA cm⁻², corresponding to an energy intensity of 35 GJ/ton CO. The energy cost is comparable to that of direct air capture (DAC) followed by reverse water-gas shift (RWGS), but it offers ambient temperature operation.