Singlet Oxygen Triggered by Superoxide Radicals in a Molybdenum Cocatalytic Fenton Reaction with Enhanced REDOX Activity in the Environment

作者：Qiuying Yi, Jiahui Ji, Bin Shen, Chencheng Dong, Jun Liu, Jinlong Zhang, Mingyang Xing · 发表于：Environmental Science & Technology · 年份：2019 · DOI：10.1021/acs.est.9b01676 · 被引用次数：849 · 研究领域：Advanced oxidation water treatment、Catalytic Processes in Materials Science、Advanced Photocatalysis Techniques

As an important reactive oxygen species (ROS) with selective oxidation, singlet oxygen ( 1 O 2 ) has wide application prospects in biology and the environment. However, the mechanism of 1 O 2 formation, especially the conversion of superoxide radicals (·O 2 – ) to 1 O 2, has been a great controversy. This process is often disturbed by hydroxyl radicals (·OH). Here, we develop a molybdenum cocatalytic Fenton system, which can realize the transformation from ·O 2 – to 1 O 2 on the premise of minimizing ·OH. The Mo 0 exposed on the surface of molybdenum powder can significantly improve the Fe 3+ /Fe 2+ cycling efficiency and weaken the production of ·OH, leading to the generation of ·O 2 – . Meanwhile, the exposed Mo 6+ can realize the transformation of ·O 2 – to 1 O 2 . The molybdenum cocatalytic effect makes the conventional Fenton reaction have high oxidation activity for the remediation of organic pollutants and prompts the inactivation of Staphylococcus aureus, as well as the adsorption and reduction of heavy metal ions (Cu 2+, Ni 2+, and Cr 6+ ). Compared with iron powder, molybdenum powder is more likely to promote the conversion from Fe 3+ to Fe 2+ during the Fenton reaction, resulting in a higher Fe 2+ /Fe 3+ ratio and better activity regarding the remediation of organics. Our findings clarify the transformation mechanism from ·O 2 – to 1 O 2 during the Fenton-like reaction and provide a promising REDOX Fenton-like system for water treatment.