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Rich-Electronic Interface Promoting Hydrogen-Bond Reversible Formation for Ultra-Stable and Energy-Efficient Catalytic CO2 Capture
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DOI：10.1002/cey2.70304.png)
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Abstract
En 中文
CO2 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 CO2 capture and release. With the electronic interface of Ni-embedded porous carbon spheres (Ni@C), CO2 has been effectively activated at the electron-rich interfaces. Multiple evidence (in situ spectroscopy/DFT/AIMD) identifies a reversible HB-organized CO2*–H2O–N-methyldiethanolamine (MDEA) trimer that shuttles protons to form HCO3−–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 CO2 capture.
Keywords:
carbon capture
electron-rich micro-region
heterogeneous catalysis
hydrogen-bond mediation
Ni-embedded porous carbon spheres
proton shuttling
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