Cooperative Cu with defective MXene for enhanced nitrate electroreduction to ammonia

Abstract

The electroreduction of nitrate (NO₃RR) to ammonia (NH₃) provides a promising solution to enable environmental remediation caused by NO₃⁻containing waste and also allows for energy-saving NH₃ generation. Adsorption of *NO₂ intermediate may be strengthened to decrease byproducts (e.g., NO₂⁻) and favor the eight-electron NO₃RR into NH₃. In this work, copperincorporated O-vacancy containing Ti₃C₂ MXene (Cu@Ti₃C₂O_v) is reported, which cooperatively inhibits NO₂⁻ production and facilitates hydrogenation, leading to approximately 100% Faradaic efficiencies of NH₃ and high yield rates at various potentials. Density functional theory calculations show that NO₃⁻ and the *NO₂ intermediates have a significant interaction with the Cu@Ti₃C₂O_v catalyst. Moreover, the formation of NO₂⁻ has a high energy barrier, which explains the appealing catalytic performance of the Cu@Ti₃C₂O_v toward NO₃RR with suppressed NO₂⁻ and elevated NH₃ selectivity. This work would motivate the prudent design of new catalysts for highperformance NO₃RR to NH₃ by elucidating the significance of stabilizing the *NO₂ intermediate.

Keywords

ammonia / Cu / defect / MXene / nitrate electroreduction

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