High-Efficiency Electrocatalytic Reduction of N2O with Single-Atom Cu Supported on Nitrogen-Doped Carbon
Nitrous oxide (N2O) is a potent greenhouse gas with a high global warming potential, emphasizing the critical need to develop efficient elimination methods. Electrocatalytic N2O reduction reaction (N2ORR) stands out as a promising approach, offering room temperature conversion of N2O to N2 without the production of NOx byproducts. In this study, we present the synthesis of a copper-based single-atom catalyst featuring atomic Cu on nitrogen-doped carbon black (Cu1–NCB). Attributed to the highly dispersed single-atom Cu sites and the effective suppression of the hydrogen evolution reaction, Cu1–NCB demonstrated an optimal N2 faradaic efficiency (82.1%) and yield rate (3.53 mmol h–1 mgmetal–1) at −0.2 and −0.5 V vs RHE, respectively, outperforming previously reported N2ORR electrocatalysts. Further, a gas diffusion electrode cell was employed to improve mass transfer and achieved a 28.6% conversion rate of 30% N2O with only a 14 s residence time, demonstrating the potential for practical application. Density functional theory calculations identified Cu–N4 as the crucial active site for N2ORR, highlighting the significance of the unsaturated coordination and metal–support electronic structure. O-terminal adsorption of N2O was favored, and the dissociative adsorption (*ON2 → *O + N2) was the rate-determining step. These findings reveal the broad prospects of N2O decomposition via electrocatalysis.
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