Journal
SMALL METHODS
Volume 4, Issue 6, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smtd.201900821
Keywords
electrocatalysis; electrocatalytic NH3 synthesis; first-principle calculations; metal organic frameworks; single-atom catalysts
Funding
- University at Buffalo, SUNY
- U.S. Department of Energy's Advanced Research Projects Agency-Energy (ARPA-E) office's REFUL program
- U.S. National Science Foundation (NSF CBET) [1804534, 1804326]
- Oregon State University
- PNNL-OSU Distinguished Graduate Research Program Fellowship
- DOE [DE-AC02-06CH11357]
- National Science Foundation [ACI-1053575]
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1804534] Funding Source: National Science Foundation
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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 mu g 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-N-3 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. 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.
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