Direct Eight-Electron N<sub>2</sub>O Electroreduction to NH<sub>3</sub> Enabled by an Fe Double-Atom Catalyst.

Wu, Donghai; Chen, Kai; Lv, Peng; Ma, Ziyu; Chu, Ke; Ma, Dongwei · Nano Lett · 2024

basic_science · Level V

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Abstract

N<sub>2</sub>O is a dominant atmosphere pollutant, causing ozone depletion and global warming. Currently, electrochemical reduction of N<sub>2</sub>O has gained increasing attention to remove N<sub>2</sub>O, but its product is worthless N<sub>2</sub>. Here, we propose a direct eight-electron (8<i>e</i>) pathway to electrochemically convert N<sub>2</sub>O into NH<sub>3</sub>. As a proof of concept, using density functional theory calculation, an Fe<sub>2</sub> double-atom catalyst (DAC) anchored by N-doped porous graphene (Fe<sub>2</sub>@NG) was screened out to be the most active and selective catalyst for N<sub>2</sub>O electroreduction toward NH<sub>3</sub> via the novel 8<i>e</i> pathway, which benefits from the unique bent N<sub>2</sub>O adsorption configuration. Guided by theoretical prediction, Fe<sub>2</sub>@NG DAC was fabricated experimentally, and it can achieve a high N<sub>2</sub>O-to-NH<sub>3</sub> Faradaic efficiency of 77.8% with a large NH<sub>3</sub> yield rate of 2.9 mg h<sup>-1</sup> cm<sup>-2</sup> at -0.6 V vs RHE in a neutral electrolyte. Our study offers a feasible strategy to synthesize NH<sub>3</sub> from pollutant N<sub>2</sub>O with simultaneous N<sub>2</sub>O removal.