Rich‐Electronic Interface Promoting Hydrogen‐Bond Reversible Formation for Ultra‐Stable and Energy‐Efficient Catalytic CO ₂ Capture

CO 2 capture remains a significant industrial challenge, primarily constrained by high energy costs and poor stability. Here, we demonstrated the precise hydrogen‐bond (HB) modulation to achieve highly efficient CO 2 capture and release. With the electronic interface of Ni‐embedded porous carbon spheres (Ni@C), CO 2 has been effectively activated at the electron‐rich interfaces. Multiple evidence (in situ spectroscopy/DFT/AIMD) identifies a reversible HB‐organized CO 2 *–H 2 O– N ‐methyldiethanolamine (MDEA) trimer that shuttles protons to form HCO 3 − –MDEAH + , establishing a rate‐determining step distinct from conventional mechanisms. Tuning such an HB scaffold yields a 127% higher absorption rate, 68% shorter equilibration, 42% faster desorption, and 14% greater desorption capacity, delivering 20% lower energy consumption. Such an approach enables rapid absorption and low‐temperature desorption at 62°C, reducing energy consumption by ~60% compared with commercial amines. Over 744 h of continuous operation, the system retains 27% higher cyclical capacity, underscoring its industrial scalability. Scalable synthesis and a general metal@carbon architecture support translation. By elevating HB control to a design principle, this work outlines an energy‐minimization paradigm for practical, low‐cost CO 2 capture.