Direct Eight-Electron N2O Electroreduction to NH3 Enabled by an Fe Double-Atom Catalyst.

Abstract

N2O is a dominant atmosphere pollutant, causing ozone depletion and global warming. Currently, electrochemical reduction of N2O has gained increasing attention to remove N2O, but its product is worthless N2. Here, we propose a direct eight-electron (8e) pathway to electrochemically convert N2O into NH3. As a proof of concept, using density functional theory calculation, an Fe2 double-atom catalyst (DAC) anchored by N-doped porous graphene (Fe2@NG) was screened out to be the most active and selective catalyst for N2O electroreduction toward NH3 via the novel 8e pathway, which benefits from the unique bent N2O adsorption configuration. Guided by theoretical prediction, Fe2@NG DAC was fabricated experimentally, and it can achieve a high N2O-to-NH3 Faradaic efficiency of 77.8% with a large NH3 yield rate of 2.9 mg h-1 cm-2 at -0.6 V vs RHE in a neutral electrolyte. Our study offers a feasible strategy to synthesize NH3 from pollutant N2O with simultaneous N2O removal.