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

Tang, Sishuang; Xie, Minghao; Yu, Saerom; Zhan, Xun; Wei, Ruilin; Wang, Maoyu; Guan, Weixin; Zhang, Bowen; Wang, Yuyang; Zhou, Hua; Zheng, Gengfeng; Liu, Yuanyue; Warner, Jamie H.; Yu, Guihua

doi:10.1038/s41467-024-51112-3

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

Journal Article · Tue Aug 13 00:00:00 EDT 2024 · Nature Communications

DOI:https://doi.org/10.1038/s41467-024-51112-3· OSTI ID:2472338

Tang, Sishuang ^[1]; Xie, Minghao ^[2]; Yu, Saerom ^[2]; Zhan, Xun ^[2]; Wei, Ruilin ^[3]; ^[4]; ^[2]; Zhang, Bowen ^[2]; Wang, Yuyang ^[2]; ^[4]; ^[3]; ^[2]; ^[2]; ^[2]

Univ. of Texas, Austin, TX (United States); Univ. of Texas, Austin, TX (United States)
Univ. of Texas, Austin, TX (United States)
Fudan Univ., Shanghai (China)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

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 m h^-1 mg^-1.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0012704; SC0019019

OSTI ID:: 2472338

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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