Single-Atom MnN 5 Catalytic Sites Enable Efficient Peroxymonosulfate Activation by Forming Highly Reactive Mn(IV)–Oxo Species

Four-nitrogen-coordinated transitional metal (MN4) configurations in single-atom catalysts (SACs) are broadly recognized as the most efficient active sites in peroxymonosulfate (PMS)-based advanced oxidation processes. However, SACs with a coordination number higher than four are rarely explored, which represents a fundamental missed opportunity for coordination chemistry to boost PMS activation and degradation of recalcitrant organic pollutants. We experimentally and theoretically demonstrate here that five-nitrogen-coordinated Mn (MnN5) sites more effectively activate PMS than MnN4 sites, by facilitating the cleavage of the O–O bond into high-valent Mn(IV)–oxo species with nearly 100% selectivity. The high…

• NN
  National Natural Science Foundation of China

  Awards: 52070128, 21876108, 21936003, 22111530110, 22106104
• DO
  Division of Engineering Education and Centers

  Award: EEC-1449500