Efficient Electrochemical Ozone and Hydrogen Peroxide Production by Synergistic Effect of Atomically Dispersed Pt, Boron and Nitrogen Doped 2D Diamonds

Abstract

AbstractThe electrochemical co‐synthesis of H₂O₂ and O₃ holds substantial potential for environmental sustainability and energy conservation. However, synthesizing electrocatalysts with appropriate adsorption energies for intermediates in the electrochemical pairwise electrosynthesis of H₂O₂ and O₃ remains a major challenge. In this study, boron and nitrogen‐doped 2D diamonds (BND) and atomically dispersed Pt₁/BND electrocatalysts are systematically designed and synthesized to facilitate the two‐electron oxygen reduction reaction (2e⁻ ORR) and electrochemical ozone production (EOP), respectively. The BND and Pt₁/BND electrocatalysts exhibit remarkable electrochemical activity, with BND achieving 90.7% selectivity for H₂O₂ and Pt₁/BND attaining a Faradaic efficiency (FE) of 12.54% for EOP. The Pt monatomic species, with a loading of 0.13%, are predominantly distributed along the edges of the Pt₁/BND. Theoretical calculations reveal that their superior properties primarily stem from the phase transition to graphene fractions at the edges, which facilitate moderate adsorption of oxygen intermediates and modulate the electronic structure through synergistic interactions between the dopant elements. Additionally, the 2D diamonds exhibit favorable mass transfer properties. The integration of H₂O₂ and O₃ for the synergistic degradation of organic contaminants and sterilization further showcase the practical utility of BND and Pt₁/BND electrocatalysts.