Ni Single‐Atoms Supported on N‐Doped Carbon Prepared by Cation Exchange: Ultrafast Catalyst For The Reduction of Nitroarene Compounds Under Ambient Conditions

Abstract We present a highly efficient single‐atom catalyst (SACs) tailored for nitroarene reduction using NaBH4 under ambient conditions. Employing an unique approach, we harnessed NaCl under high temperature to create host materials enriched with negatively charged nitrogenous and oxygenated functional groups, capable of anchoring and stabilizing Ni ions within the aromatic structure. The nickel single sites were prepared by a straightforward cation exchange method. STEM‐HAADF imaging confirmed the presence of nickel single‐atoms, while XPS, FTIR, and Raman spectra validated nickel coordination within the catalyst. Remarkably, the CN−Ni catalyst exhibited exceptional catalytic performance under ambient conditions, achieving a high catalytic activity with NaBH4 (TOF 2246 452 h−1 and 107 47 mmol g−1 min−1). It also demonstrated remarkable conversion exceeding 90 % and outstanding selectivity. Equally impressive was its ability to maintain full catalytic activity over multiple reaction cycles, highlighting its robustness. This work is a significant leap in SACs design, offering a versatile and highly effective preparation method for SACs based on N‐doped carbon with far‐reaching implications in industrial reduction reactions.