Metal single-site catalyst design for electrocatalytic production of hydrogen peroxide at industrial-relevant...

Direct hydrogen peroxide (H₂O₂) electrosynthesis via the two-electron oxygen reduction reaction is a sustainable alternative to the traditional energy-intensive anthraquinone technology. However, high-performance and scalable electrocatalysts with industrial-relevant production rates remain to be challenging, partially due to insufficient atomic level understanding in catalyst design. Here we utilize theoretical approaches to identify transition-metal single-site catalysts for two-electron oxygen reduction using the *OOH binding energy as a descriptor. The theoretical predictions are then used as guidance to synthesize the desired cobalt single-site catalyst with a O-modified Co-(pyrrolic N)₄ configuration that can achieve industrial-relevant current densities up to 300 mA cm^-2 with 96-100% Faradaic efficiencies for H₂O₂ production at a record rate of 11,527 mmol h^-1 g_cat^-1. Here, we show the feasibility and versatility of metal single-site catalyst design using various commercial carbon and cobalt phthalocyanine as starting materials and the high applicability for H₂O₂ electrosynthesis in acidic, neutral and alkaline electrolytes.