The heterogeneous electro-Fenton (hetero-e-Fenton)-coupled electrocatalytic oxygen reduction reaction (ORR) is regarded as a promising strategy for ^·OH production by simultaneously driving two-electron ORR toward H₂O₂ and stepped activating the as-generated H₂O₂ to ^·OH. However, the high-efficiency electrogeneration of ^·OH remains challengeable, as it is difficult to synchronously obtain efficient catalysis of both reaction steps above on one catalytic site. In this work, we propose a dual-atomic-site catalyst (CoFe DAC) to cooperatively catalyze ^·OH electrogeneration, where the atomically dispersed Co sites are assigned to enhance O₂ reduction to H₂O₂ intermediates and Fe sites are responsible for activation of the as-generated H₂O₂ to ^·OH. The CoFe DAC delivers a higher ^·OH production rate of 2.4 mmol L^-1 min^-1 g_cat^-1 than the single-site catalyst Co-NC (0.8 mmol L^-1 min^-1 g_cat^-1) and Fe-NC (1.0 mmol L^-1 min^-1 g_cat^-1). Significantly, the CoFe DAC hetero-e-Fenton process is demonstrated to be more energy-efficient for actual coking wastewater treatment with an energy consumption of 19.0 kWh kg^-1 COD^-1 than other electrochemical technologies that reported values of 29.7∼68.0 kW h kg^-1 COD^-1. This study shows the attractive advantages of efficiency and sustainability for ^·OH electrogeneration, which should have fresh inspiration for the development of new-generation wastewater treatment technology.

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