Architecting Hierarchically Porous Electrocatalyst for Direct Liquid Carbon Utilization

Carbon dioxide (CO₂) capture and utilization (CCU), driven by renewable electricity, are pivotal technologies to achieve the mitigation of CO₂ emissions and further valorization, respectively. Integrating CO₂ capture with upgrading represents an emerging cutting-edge approach, given that each individual process step incurs significant energetic and economic costs. Herein, hierarchically porous N-doped carbon-supported Ni catalyst (Ni-HP) is architected for KOH-based reactive CO₂ capture. Benefiting from the hierarchical porous structures with enriched exposure of active sites as well as accelerated mass transfer, this catalyst achieves a high Faradaic efficiency (FE) for CO exceeding 90%. Moreover, this catalyst facilitates industrial syngas production over 60 h of cyclic operation at -100 mA cm^-2 in alkaline solutions saturated with simulated flue gas containing 20 vol% CO₂. This work not only provides in-depth insight into the origin of the catalytic activity of porous carbon-based catalysts but also offers electrochemical guidance for the rational integration of reactive CO₂ capture within the broader carbon management community.