Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination

Shifting electrochemical oxygen reduction towards 2e(–) pathway to hydrogen peroxide (H(2)O(2)), instead of the traditional 4e(–) to water, becomes increasingly important as a green method for H(2)O(2) generation. Here, through a flexible control of oxygen reduction pathways on different transition metal single atom coordination in carbon nanotube, we discovered Fe-C-O as an efficient H(2)O(2) catalyst, with an unprecedented onset of 0.822 V versus reversible hydrogen electrode in 0.1 M KOH to deliver 0.1 mA cm(−2) H(2)O(2) current, and a high H(2)O(2) selectivity of above 95% in both alkaline and neutral pH. A wide range tuning of 2e(–)/4e(–) ORR pathways was achieved via different metal centers or neighboring metalloid coordination. Density functional theory calculations indicate that the Fe-C-O motifs, in a sharp contrast to the well-known Fe-C-N for 4e(–), are responsible for the H(2)O(2) pathway. This iron single atom catalyst demonstrated an effective water disinfection as a representative application.