In this work, we revealed a dual -pathway nonradical oxidation (NRO) system catalyzed by Ni single atom catalyst (NiN4) accommodated in the carbon nitride substrate. The monatomic Ni coordinated with four N atoms (Ni-N4) is determined as the dynamic catalytic center for peroxymonosulfate (PMS) activation, showing an exceptional specific rate constant of 3.34 min -1 g-2 L-2 (29.7 times that of CN/PMS system) in oxidizing bisphenol A and other refractory organics. In situ Raman, X-ray absorption, and electrochemical analyses as well as theoretical simulations demonstrate that the Ni-N4 sites exh...
