Improving Generation Performance of <sup>1</sup>O<sub>2</sub> by Atomic Doping for Efficient Catalytic Advanced Oxidation Processes
Defeng Qi, Jiaqi Wang, Jian Zhang, Ke Su, Jie Xu, Weiqiang Lv, Yong Wang, Zhen Zhang, Yin Xiao
Abstract
Abstract Singlet oxygen ( 1 O 2 ) has attracted great attention owing to its superior comprehensive oxidizing performance and extensive application in dealing with ever‐growing environmental pollution. However, the efficient catalytic generation of 1 O 2 is very challenging due to the low catalytic activity of most catalysts and the generation of oxygen‐containing radicals in the catalytic reaction. Herein, C‐doped Co nanoparticles (CoNPs) supported on porous carbon (C─Co/C) as highly reactive and selective 1 O 2 ‐producing catalysts are demonstrated for efficient catalytic oxidation of recalcitrant organics via activation of peroxymonosulfate (PMS). The doped C 2p orbitals can accept Co 3d electrons, thereby weakening the Co─O bonding between Co and PMS or other oxygen‐containing intermediates such as *SO 4 , *OH, *OOH, and *O. The adsorption and cleavage energy of PMS on Co nanoparticle is reduced from 8.09 to 4.64 eV by C doping. The energy barrier of the *OOH to 1 O 2 step is also lowered significantly, thereby kinetically improving the activity for the generation of 1 O 2 . The C─Co/C catalysts promotes the efficient and 100% selective generation of 1 O 2 with high modified kinetic model ( K ) values of 457.0 and 94.5 µmol s −1 g −1 for rhodamine (RhB) and 2,4‐dichlorophenol (2,4‐DCP), respectively.