Abstract
Electrochemical carbon capture offers a sustainable pathway for carbon management, yet current systems are hindered by low concentration of atmospheric carbon dioxide (CO(2)), resulting in inefficiencies and limited stability. Here, we develop an electrochemical system employing a modular porous solid electrolyte (PSE) reactor for continuous, scalable carbon capture from diverse sources, including ambient air and flue gas, while regenerating high-purity CO(2) ( >99%) without additional chemical input through a recirculation mode. By leveraging oxygen evolution and reduction reactions (OER/ORR) and employing sodium (bi)carbonate as a reversible cyclic mediator, the system achieves continuous CO(2) capture from flue gas, delivering high Faradaic efficiencies for Na⁺ transport (~85%), and high carbon capture rates (3060 ml h(-)(1) at 10 A, 100 cm(2)). Notably, direct air capture is demonstrated using ambient air, showing a long-term stability of over 2000 hours while maintaining high carbon removal efficiency (>93%) at 30 mA cm(-2) and a large air treatment capacity (approximately 8820 kg(air) day(-1) m(-2)), thus contributing to the goal of achieving net-zero emissions.