Mn-Co dual sites relay activation of peroxymonosulfate for accelerated decontamination

Dual atomic catalysts are specially designed for relay activation of peroxymonosulfate (PMS). Here, a programmable metal-triazolate framework is utilized as a precursor to introduce the bimetallic sites (containing Mn and Co) for the synthesis of contiguous Mn−N and Co−N sites anchored on nitrogen-doped porous carbon polyhedral (MCNC). Excellent decontamination performance with TOF/PMS = 46.3 L2 min−1 g−2 is observed on the MCNC, which is 1.6 and 1.5 times of single Mn and single Co catalysts. Singlet oxygen quantifying, 18O isotope labeling, and theoretical simulations jointly unravel that MCNC activates PMS through a unique "relay" mode, where one site interacts with the O atom in PMS, and the other expedites producing 1O2 via PMS* activation. This work advances the origin activation of PMS and enhances the removal for the refractory pollutants by rational regulation of dual site synergistic catalyst, which deepens the on-demand design of Fenton-like reaction.