Efficient Electrochemical Co‐Reduction of Carbon Dioxide and Nitrate to Urea with High Faradaic Efficiency on Cobalt‐Based Dual‐Sites

作者：Xiaoya Fan, Chaozhen Liu, Xun He, Zixiao Li, Luchao Yue, Wenxi Zhao, Jun Li, Yan Wang, Tingshuai Li, Yongsong Luo, Dongdong Zheng, Shengjun Sun, Qian Liu, Luming Li, Wei Chu, Feng Gong, Bo Tang, Yongchao Yao, Xuping Sun · 发表于：Advanced Materials · 年份：2024 · DOI：10.1002/adma.202401221 · 被引用次数：204 · 研究领域：CO2 Reduction Techniques and Catalysts、Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques

Abstract Renewable electricity‐powered nitrate/carbon dioxide co‐reduction reaction toward urea production paves an attractive alternative to industrial urea processes and offers a clean on‐site approach to closing the global nitrogen cycle. However, its large‐scale implantation is severely impeded by challenging C–N coupling and requires electrocatalysts with high activity/selectivity. Here, cobalt‐nanoparticles anchored on carbon nanosheet (Co NPs@C) are proposed as a catalyst electrode to boost yield and Faradaic efficiency (FE) toward urea electrosynthesis with enhanced C–N coupling. Such Co NPs@C renders superb urea‐producing activity with a high FE reaching 54.3% and a urea yield of 2217.5 µg h −1 mg cat. −1 , much superior to the Co NPs and C nanosheet counterparts, and meanwhile shows strong stability. The Co NPs@C affords rich catalytically active sites, fast reactant diffusion, and sufficient catalytic surfaces‐electrolyte contacts with favored charge and ion transfer efficiencies. The theoretical calculations reveal that the high‐rate formation of *CO and *NH 2 intermediates is crucial for facilitating urea synthesis.