Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
State Key Laboratory of Chemical Engineering, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
Angew Chem Int Ed Engl. 2021 Jul 26;60(31):17155-17163. doi: 10.1002/anie.202105736. Epub 2021 Jul 1.
Although Fenton or Fenton-like reactions have been widely used in the environment, biology, life science, and other fields, the sharp decrease in their activity under macroneutral conditions is still a large problem. This study reports a MoS cocatalytic heterogeneous Fenton (CoFe O /MoS ) system capable of sustainably degrading organic pollutants, such as phenol, in a macroneutral buffer solution. An acidic microenvironment in the slipping plane of CoFe O is successfully constructed by chemically bonding with MoS . This microenvironment is not affected by the surrounding pH, which ensures the stable circulation of Fe /Fe on the surface of CoFe O /MoS under neutral or even alkaline conditions. Additionally, CoFe O /MoS always exposes "fresh" active sites for the decomposition of H O and the generation of O , effectively inhibiting the production of iron sludge and enhancing the remediation of organic pollutants, even in actual wastewater. This work not only experimentally verifies the existence of an acidic microenvironment on the surface of heterogeneous catalysts for the first time, but also eliminates the pH limitation of the Fenton reaction for pollutant remediation, thereby expanding the applicability of Fenton technology.
尽管芬顿或类芬顿反应已广泛应用于环境、生物学、生命科学等领域,但在大中性条件下其活性急剧下降仍然是一个大问题。本研究报道了一种 MoS 共催化非均相芬顿(CoFeO/MoS )体系,能够在大中性缓冲溶液中持续降解有机污染物,如苯酚。通过与 MoS 化学结合,成功地在 CoFeO 的滑移面上构建了一个酸性微环境。该微环境不受周围 pH 值的影响,这确保了 Fe/Fe 在 CoFeO/MoS 表面的稳定循环,即使在中性甚至碱性条件下也是如此。此外,CoFeO/MoS 始终暴露“新鲜”的活性位点,用于 H2O2 的分解和·O2-的生成,有效抑制铁污泥的生成并增强有机污染物的修复,即使在实际废水中也是如此。这项工作不仅首次从实验上验证了非均相催化剂表面存在酸性微环境,而且消除了 Fenton 反应修复污染物的 pH 限制,从而扩展了 Fenton 技术的适用性。