Abstract
Herein, the systematic and novel formation pathway of singlet oxygen (1O2) on single iron atom during advanced oxidation process was investigated and revealed. Graphitic carbon matrix supported single iron atom and iron nanoclusters configurations as model catalysts were synthesized via calcinating Prussian blue, which showed admirable catalytic efficiency towards bisphenol A (BPA) oxidation even under high salinity conditions. 1O2 directly generated on Fe-pyridinic N moiety bonded with terminal O of PMS (HSO5-) was proposed as predominant reactive species. Experimental results and theoretical analysis further detailly demonstrated the evolutionary pathway of 1O2 formation, which occurred through the interaction of two O atoms from adsorbed PMS, accompanying two HSO4- molecules generation with the lowest energy barrier. This study proposed novel insights into direct 1O2-modulated mechanism via Fe-N4 configuration, providing essential atomic-scale understanding of FeNx/PMS based Fenton-like system, as well as a new strategy for the practical environmental remediation with high salinity.
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