Yanjie Zhai, Shanhe Gong, Weisong Li, Qing Xia, Tingting Li, Jianyu Guan, Shao‐Yuan Leu, Zhenyu Wu, Shu Ping Lau, Xiao Zhang
Electrochemical carbon capture offers a sustainable pathway for carbon management, yet current systems are hindered by low concentration of atmospheric carbon dioxide (CO2), 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 CO2 ( >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 CO2 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 cm2). 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 kgair day-1 m-2), thus contributing to the goal of achieving net-zero emissions. Electrochemical carbon capture provides a sustainable method for effective carbon management. Here, the authors develop a modular porous solid electrolyte reactor system, achieving continuous carbon capture from air and flue gases through a recirculation mode with high efficiency and stability.