General synthesis of high-entropy single-atom nanocages for electrosynthesis of ammonia from nitrate

作者：Sishuang Tang, Minghao Xie, Saerom Yu, Xun Zhan, Ruilin Wei, Maoyu Wang, Weixin Guan, Bowen Zhang, Yuyang Wang, Hua Zhou, Gengfeng Zheng, Yuanyue Liu, Jamie H. Warner, Guihua Yu · 发表于：Nature Communications · 年份：2024 · DOI：10.1038/s41467-024-51112-3 · 被引用次数：118 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Nanomaterials for catalytic reactions、Advanced Photocatalysis Techniques

Given the growing emphasis on energy efficiency, environmental sustainability, and agricultural demand, there’s a pressing need for decentralized and scalable ammonia production. Converting nitrate ions electrochemically, which are commonly found in industrial wastewater and polluted groundwater, into ammonia offers a viable approach for both wastewater treatment and ammonia production yet limited by low producibility and scalability. Here we report a versatile and scalable solution-phase synthesis of high-entropy single-atom nanocages (HESA NCs) in which Fe and other five metals-Co, Cu, Zn, Cd, and In-are isolated via cyano-bridges and coordinated with C and N, respectively. Incorporating and isolating the five metals into the matrix of Fe resulted in Fe-C5 active sites with a minimized symmetry of lattice as well as facilitated water dissociation and thus hydrogenation process. As a result, the Fe-HESA NCs exhibited a high selectivity toward NH3 from the electrocatalytic reduction of nitrate with a Faradaic efficiency of 93.4% while maintaining a high yield rate of 81.4 mg h−1 mg−1. Converting nitrate from waste sources into ammonia provides an effective method for both wastewater treatment and ammonia production. Here the authors report a scalable solution-phase synthesis of high-entropy single-atom nanocage catalysts for efficient nitrate-to-ammonia conversion.