Pore Engineering for Directional CO 2 Enrichment in Urea Electrosynthesis

作者：Chun Li, Haoyang Xu, Nan Zou, Ruoting Liu, Yimin Zeng, Ying Zheng · 发表于：ACS Applied Materials & Interfaces · 年份：2025 · DOI：10.1021/acsami.5c09970 · 被引用次数：3 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、CO2 Reduction Techniques and Catalysts、Covalent Organic Framework Applications

Electrochemical synthesis of urea from CO 2 and nitrate offers a sustainable pathway to address both carbon emissions and nitrogen pollution. However, achieving high C–N coupling selectivity remains challenging due to competing hydrogen evolution reactions and insufficient CO 2 utilization. Herein, we implement a nanopore-structure engineering strategy to precisely tailor pore length and surface chemistry in metal-free porous carbon frameworks. Oxygen-functionalized surfaces augment CO 2 binding affinity via dipole–quadrupole interactions, while elongated pores induce directional CO 2 enrichment by establishing a H 2 O-deficient nanoenvironment that prolongs the residence time of CO 2 through capillary gating. This dual modulation of gas–liquid–solid interactions enhances urea selectivity and suppresses hydrogen evolution, yielding a 28% increase in Faradaic efficiency and 12% improvement in urea yield. Our findings propose a novel nanopore-level design concept that shall support the rational development of porous carbon supports across gas–liquid–solid electrocatalytic systems.