Zhang Zhenfang, Li Yitong, Zhong Yiwen, Li Peng, Zhu Lingfeng, Zheng Zhi, Jia Baohua, David Matthew, Fu Yang, Yu Hai, Ma Tianyi
Centre for Atomaterials and Nanomanufacturing (CAN), School of Science, RMIT University, Melbourne, VIC 3000, Australia.
School of Textile Science and Engineering, Xi'an Polytechnic University, Xi'an 710048, China.
Sci Adv. 2025 Jun 20;11(25):eadw6592. doi: 10.1126/sciadv.adw6592.
Electrochemical carbon dioxide (CO) capture and utilization, powered by renewable energy, are essential to achieving net-zero emissions and CO valorization. While remarkable progress has been made in catalysts, solution design, and system engineering, recent breakthroughs reveal that nitrogen-containing molecules-specifically sp-hybridized structures (e.g., pyridine) and sp-hybridized moieties (e.g., ethanolamine) -hold untapped potential to revolutionize both CO capture and conversion. These structures have been demonstrated as the Holy Grail in facilitating CO activation, stabilizing key intermediates, and streamlining reaction pathways-capabilities rarely achievable with conventional strategies. However, limited mechanistic understanding of their physicochemical properties and interactions with CO hampers broader application. This review highlights recent advances in leveraging sp/sp-hybridized nitrogen structures, unpacks their molecular roles in electrochemical CO management, and offers a unifying framework for their dual-functionality across capture and conversion. By illuminating these nitrogen-based motifs, we uncover practical design principles and open avenues for integrating expanded N-containing compounds into energy technologies-paving the way for next-generation carbon management strategies.
由可再生能源驱动的电化学二氧化碳（CO）捕集与利用对于实现净零排放和CO资源化至关重要。尽管在催化剂、溶液设计和系统工程方面已取得显著进展，但最近的突破表明，含氮分子——特别是sp杂化结构（如吡啶）和sp杂化部分（如乙醇胺）——在彻底改变CO捕集与转化方面具有尚未开发的潜力。这些结构已被证明是促进CO活化、稳定关键中间体和简化反应途径的圣杯——这是传统策略很少能实现的能力。然而，对其物理化学性质以及与CO相互作用的机理理解有限，阻碍了其更广泛的应用。本综述重点介绍了利用sp/sp杂化氮结构的最新进展，剖析了它们在电化学CO管理中的分子作用，并为其在捕集和转化中的双重功能提供了一个统一框架。通过阐明这些基于氮的基序，我们揭示了实际的设计原则，并为将扩展的含氮化合物整合到能源技术中开辟了途径——为下一代碳管理策略铺平了道路。
