Insights into multi-pathway peroxymonosulfate activation by copper-doped Ca/Mn perovskite oxides for diethyl phthalate degradation

作者：Liu, Chenhui; Chen, Meiqing; Ye, Quanyun; Wu, Pingxiao^*; Liu, Jieyu; Wu, Jiayan; Shang, Zhongbo; Niu, Wenchao; Zhu, Nengwu

来源：Journal of Environmental Chemical Engineering, 2023, 11(3): 109845.

DOI：10.1016/j.jece.2023.109845

• Heterostructure perovskites
• CaMnO3
• PMS activation
• Dual redox cycles
• Density functional theory

Peroxymonosulfate (PMS) activation based on metallic catalysts with versatile mineral structures and superior catalytic properties has attracted much attention. In this study, we built a CaMnO3(CMO) with copper dopped to promote PMS activation by Mn(III)/Mn(IV) and Cu(I)/Cu(II) redox cycles with the synergistic effect of bimetal for efficient degradation of diethyl phthalate (DEP). Under optimal conditions, 95.7% of DEP (10 mg L-1) degradation was realized in 60 min, and the mineralization reached 75%, while only 26.9% of DEP was removed with little TOC removal by CaMnO3. Unexpectedly, not only & BULL;OH, O2 & BULL;? and SO4 & BULL;?, but also nonradical pathway singlet oxygen (1O2) was found to be involved in the CMO-Cu/PMS system. The redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) effectively promoted PMS activation to reactive oxygen species (ROS), which were responsible for DEP degradation. Furthermore, density functional theory (DFT) calculations and liquid chromatograph-mass spectrometer (LC-MS) were combined to explore the degradation pathway. This work provides a new insight for developing heterogeneous perovskites for PMS activation to construct more efficient method for water treatment.

• 单位
  环境保护部华南环境科学研究所