School of Environmental Science and Engineering, Key Laboratory of Thin Film and Microfabrication Technology (Ministry of Education), Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China.
Faculty of Civil and Environmental Engineering, Technion-Israel Institute of Technology, Technion City, Haifa, 32000, Israel.
Chemosphere. 2021 May;270:128639. doi: 10.1016/j.chemosphere.2020.128639. Epub 2020 Oct 16.
Fenton-like reactions at near neutral pHs are limited by the slow reduction of ferric species. Enhancing generation of from solid peroxides is a promising strategy to accelerate the rate-limiting step. Herein, the HO release and Fenton-like reactions of four solid peroxides, MgO, CaO, ZnO and urea hydrogen peroxide (UHP), were investigated. Results indicated that UHP can release HO instantly and show a similar behavior as HO in the Fenton-like reactions. MgO released HO quickly in phosphate buffered solutions, which was comparable to CaO but faster than ZnO. Metal peroxides induced higher initial phenol degradation rates than UHP and HO when the same theoretic HO dosages and Fe(III)-EDTA were used. MgO displayed a superior performance for phenol degradation at pH 5, resulting in more than 93% phenol reduction at 1.5 h. According to kinetic analyses, the generation rate of in the MgO system was 18 and 3.4 times higher than those in ZnO and CaO systems, respectively. The addition of MgO significantly promoted HO based Fenton-like reactions by increasing production of , and the mixture of MgO and HO had an improved utilization efficiency of active oxygen than the MgO system. The findings suggested the critical roles of metal peroxides in favoring Fenton-like reactions and inspired strategies to simultaneously accelerate Fenton-like reactions and improve utilization efficiency of active oxygen.
在近中性 pH 条件下,芬顿反应受到铁物种还原缓慢的限制。增强过氧化物生成 是加速限速步骤的一种很有前途的策略。本文研究了四种固体过氧化物(MgO、CaO、ZnO 和尿素过氧化氢(UHP))的 HO 释放和芬顿反应。结果表明,UHP 可以立即释放 HO,并且在芬顿反应中表现出与 HO 相似的行为。MgO 在磷酸盐缓冲溶液中快速释放 HO,其释放速度与 CaO 相当,但比 ZnO 快。当使用相同的理论 HO 剂量和 Fe(III)-EDTA 时,金属过氧化物诱导的初始苯酚降解速率高于 UHP 和 HO。在 pH 5 下,MgO 对苯酚降解表现出优异的性能,在 1.5 h 内可将苯酚去除率超过 93%。根据动力学分析,在 MgO 体系中 的生成速率分别比 ZnO 和 CaO 体系高 18 倍和 3.4 倍。MgO 的添加通过增加 的生成,显著促进了基于 HO 的芬顿反应,并且 MgO 和 HO 的混合物比 MgO 体系具有更高的活性氧利用率。这些发现表明金属过氧化物在促进芬顿反应方面起着关键作用,并为同时加速芬顿反应和提高活性氧利用率的策略提供了启示。