Enhanced activation of peroxide to generate singlet oxygen via boron-doped Cu single-atom catalysts for efficient...

The development of advanced oxidation processes (AOPs) for environmental remediation has spurred a growing interest in catalysts that selectively generate non-radical species such as singlet oxygen (¹O₂). However, the precise engineering of catalytic sites to enhance targeted ¹O₂ production remains a formidable challenge. This study reports a B-doped graphitic carbon nitride-supported Cu single-atom catalyst (CuBCN) that significantly enhances H₂O₂ activation for efficient ¹O₂ production. Through comprehensive experimental and theoretical analysis, revealing that B doping modulates the electronic properties at the Cu active sites. This modification reduces the electron density around Cu, increasing the Cu(II) fraction essential for the formation and subsequent oxidation of ·OOH intermediates. Additionally, B influences the d-band center of Cu, optimizing the adsorption energy of ·OOH, which in turn facilitates selective ¹O₂ production. The CuBCN/H₂O₂ system exhibits exceptional Fenton-like performance, producing ¹O₂ as the principal active species, even in challenging water conditions characterized by high pH, high ionic strength, and high concentrations of humic substances. This work not only highlights the potential of tailored single-atom catalysts in pollution control but also offers significant insights for designing catalysts for efficient H₂O₂ activation.