Abstract
Electrochemical NO2− reduction to NH3 (NO2RR) holds significant potential for simultaneously mitigating NO2− pollutants and producing valuable NH3. Herein, we design single-atom In1 alloyed Cu (In1Cu) as an effective and long-lasting catalyst for the NO2RR. Through a combination of experimental and theoretical investigations, we discover that the enhanced NO2RR performance of In1Cu arises from its surface In1-Cu dinuclear sites to promote the NO2− activation, optimize the reaction energetics of NHO pathway and suppress the competing hydrogen evolution. As a result, In1Cu integrated into the flow cell achieves the outstanding NH3-Faradaic efficiency of 94.7 % and NH3 yield rate of 1042.1 μmol h−1 cm−2 at a high current density of 354 mA cm−2, placing it among the most effective NO2RR catalyst ever reported.
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