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Title: Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N2 and H2O

Journal Article · · Small Methods

Ammonia (NH3) electrosynthesis gains significant attention as NH3 is essentially important for fertilizer production and fuel utilization. However, electrochemical nitrogen reduction reaction (NRR) remains a great challenge because of low activity and poor selectivity. Herein, a new class of atomically dispersed Ni site electrocatalyst is reported, which exhibits the optimal NH3 yield of 115 µg cm-2 h-1 at –0.8 V versus reversible hydrogen electrode (RHE) under neutral conditions. High faradic efficiency of 21 ± 1.9% is achieved at -0.2 V versus RHE under alkaline conditions, although the ammonia yield is lower. The Ni sites are stabilized with nitrogen, which is verified by advanced X-ray absorption spectroscopy and electron microscopy. Density functional theory calculations provide insightful understanding on the possible structure of active sites, relevant reaction pathways, and confirm that the Ni-N3 sites are responsible for the experimentally observed activity and selectivity. Extensive controls strongly suggest that the atomically dispersed NiN3 site-rich catalyst provides more intrinsically active sites than those in N-doped carbon, instead of possible environmental contamination. Overall, this work further indicates that single-metal site catalysts with optimal nitrogen coordination is very promising for NRR and indeed improves the scaling relationship of transition metals.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE Advanced Research Projects Agency - Energy (ARPA-E)
Grant/Contract Number:
AC05-00OR22725; 1804534; 1804326; ACI-1053575; AC02‐06CH11357; DE‐AC02‐06CH11357
OSTI ID:
1712715
Alternate ID(s):
OSTI ID: 1597537
Journal Information:
Small Methods, Vol. 4, Issue 6; ISSN 2366-9608
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 132 works
Citation information provided by
Web of Science

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