Powerful Orbital Hybridization of Copper-Silver Bimetallic Nanosheets for Electrocatalytic Nitrogen Reduction to Ammonia.

Electrochemical nitrogen reduction (eNRR) is a promising strategy to replace the energy- and capital-intensive Haber-Bosch process. Unfortunately, the low selectivity of the eNRR process impedes the industrial application of this approach. In this work, a highly efficient and stable NRR electrocatalyst is obtained via coreduction of Cu and Ag precursors using the holly leaves as reducing agents. The as-obtained Cu 3 Ag bimetallic nanosheets exhibit excellent NRR performance with an NH 3 production rate of 31.3 μg h -1 mg -1 cat. and a Faradaic efficiency of 31.3% at -0.2 V vs RHE. According to density functional theory (DFT) calculation, the outstanding performance of Cu 3 Ag bimetallic nanosheets could be caused by the fact that Ag optimizes the 3d orbital occupation of Cu and synergistically enhances the charge transfer during the NRR process, resulting in a suitable adsorption strength of the intermediates.