Efficient Ammonia Production from Nitric Oxide under Real Condition Using Photo-Modulated Cu Single-Atom Catalysts

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Abstract

Efficient electrochemical reduction of nitric oxide (NORR) under practical low-concentration conditions remains challenging due to insufficient NO adsorption, sluggish proton-coupled electron transfer, and severe competition from hydrogen evolution. In this work, a photo-modulated electrocatalysis system was fabricated for driving the reduction of low concentration NO pollutant to NH 3 , based on Cu single atoms (Cu SAs) decorated MoS 2 . The light irradiation induces the Cu SAs active sites switched to a lower valence state with prolonged Cu−S bonds instantaneously, facilitating the adsorption and activation towards NO molecules even at low concentration. As anticipated, a high NH 3 yield up to 3228 µmol h − 1 mg − 1 with a Faradaic efficiency (FE) of 86.53% were achieved in a flow cell at a current density of 100 mA cm − 2 . Such NH 3 yield value and FE are much higher than that obtained by the electrocatalysis of NO reduction reaction (NORR) so far. This work demonstrates that rational modulation of the localized coordination structure of single-atom centers can unlock previously inaccessible activity for disposing low-concentration nitrogen-containing pollutants.

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