Enabling Resource Utilization of N ₂ O: Selective Electrocatalytic Reduction to Nitrogen and Ammonia via Competing Pathways over Ni-MoS ₂

Nitrous oxide (N2O) electrocatalytic reduction (eN2ORR) represents a promising strategy for mitigating greenhouse gas emissions, yet its potential for simultaneous resource recovery remains largely unexplored. Herein, we report a nickel-modified molybdenum disulfide catalyst (Ni-MoS2) that steers the eN2ORR through a competing reaction network, enabling the coproduction of N2 and NH3. Comprehensive characterization (XRD, Raman, HAADF-STEM, XPS, UV–vis, SECM) confirms the highly dispersed Ni species effectively modulate the electronic structure and surface properties of MoS2. This dual-pathway mechanism transforms the process into an integrated purification and resource recovery system, enabling a total Faradaic efficiency of 72.8% at −0.3 V (vs RHE) through the concurrent production of N2 (79% selectivity) and NH3 (21% selectivity). By combining in situ infrared spectroscopy and density functional theory calculations, this study successfully identified the key reaction intermediates (*N2OH, *NH, and *NH2) and elucidated how the modification of nickel guides the divergence of reaction pathways, namely, achieving the direct dissociation of nitrogen or the continuous hydrogenation process of ammonia. This work provides not only an efficient catalyst but also a novel conceptual framework for designing electrocatalytic processes that combine environmental remediation with sustainable synthesis of value-added chemicals.