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

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 and Guihua Yu ()
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Sishuang Tang: The University of Texas at Austin
Minghao Xie: The University of Texas at Austin
Saerom Yu: The University of Texas at Austin
Xun Zhan: The University of Texas at Austin
Ruilin Wei: Fudan University
Maoyu Wang: Argonne National Laboratory
Weixin Guan: The University of Texas at Austin
Bowen Zhang: The University of Texas at Austin
Yuyang Wang: The University of Texas at Austin
Hua Zhou: Argonne National Laboratory
Gengfeng Zheng: Fudan University
Yuanyue Liu: The University of Texas at Austin
Jamie H. Warner: The University of Texas at Austin
Guihua Yu: The University of Texas at Austin

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-51112-3

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