Oxygen doping regulation of Co single atom catalysts for electro-Fenton degradation of tetracycline.

Electro-Fenton is an effective process for degrading hard-to-degrade organic pollutants, such as tetracycline (TC). However, the degradation efficiency of this process is limited by the activity and stability of the cathode catalyst. Herein, a temperature gradient pyrolysis strategy and oxidation treatment is proposed to modulate the coordination environment to prepare oxygen-doped cobalt monoatomic electrocatalysts (CoNOC). The CoNOC catalysts can achieve the selectivity of 93 % for HO with an electron transfer number close to 2. In the H-cell, the prepared electrocatalysts can achieve more than 100 h of HO production with good stability and the yield of 1.41 mol g h with an average Faraday efficiency (FE) of more than 88 %. The calculations indicate that the epoxy groups play a crucial role in modulating the oxygen reduction pathway. The O doping and unique N coordination of Co single-atom active sites (CoNNO) can effectively weaken the O/OOH* interaction, thereby promoting the production of HO. Finally, the electro-Fenton system could achieve a TC degradation rate of 94.9 % for 120 min with a mineralization efficiency of 87.8 % for 180 min, which provides a reliable option for antibiotic treatment. The significant involvement of OH in the electro-Fenton process was confirmed, and the plausible mineralization pathway for TC was proposed.