Key Laboratory for Advanced Materials and Institute of Fine Chemicals, School of Chemistry and Molecular Engineering , East China University of Science and Technology , 130 Meilong Road , Shanghai 200237 , P.R. China.
Environ Sci Technol. 2019 Aug 20;53(16):9725-9733. doi: 10.1021/acs.est.9b01676. Epub 2019 Aug 2.
As an important reactive oxygen species (ROS) with selective oxidation, singlet oxygen (O) has wide application prospects in biology and the environment. However, the mechanism of O formation, especially the conversion of superoxide radicals (·O) to O, 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 to O on the premise of minimizing ·OH. The Mo exposed on the surface of molybdenum powder can significantly improve the Fe/Fe cycling efficiency and weaken the production of ·OH, leading to the generation of ·O. Meanwhile, the exposed Mo can realize the transformation of ·O to O. The molybdenum cocatalytic effect makes the conventional Fenton reaction have high oxidation activity for the remediation of organic pollutants and prompts the inactivation of , as well as the adsorption and reduction of heavy metal ions (Cu, Ni, and Cr). Compared with iron powder, molybdenum powder is more likely to promote the conversion from Fe to Fe during the Fenton reaction, resulting in a higher Fe/Fe ratio and better activity regarding the remediation of organics. Our findings clarify the transformation mechanism from ·O to O during the Fenton-like reaction and provide a promising REDOX Fenton-like system for water treatment.
作为一种具有选择性氧化能力的重要活性氧物种（ROS），单线态氧（1O2）在生物学和环境领域具有广泛的应用前景。然而，1O2 的形成机制，特别是超氧自由基（·O2-）向 1O2 的转化机制，一直存在很大争议。这一过程通常会受到羟基自由基（·OH）的干扰。在这里，我们开发了一种钼共催化芬顿体系，它可以在最小化·OH 的前提下实现·O2-向 1O2 的转化。钼粉末表面暴露的钼可以显著提高 Fe/Fe 循环效率，并削弱·OH 的产生，从而导致·O2-的生成。同时，暴露的钼可以实现 1O2 的转化。钼的共催化作用使传统芬顿反应对有机污染物的修复具有高氧化活性，并促使 灭活，以及重金属离子（Cu、Ni 和 Cr）的吸附和还原。与铁粉相比，在芬顿反应过程中，钼粉更有可能促进 Fe 向 Fe 的转化，从而导致更高的 Fe/Fe 比和更好的有机修复活性。我们的研究结果阐明了类芬顿反应中 1O2 转化的机制，并为水处理提供了一种有前途的 REDOX 类芬顿体系。
