Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, College of Environment, Zhejiang University of Technology, Hangzhou 310014, China.
Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, College of Environment, Zhejiang University of Technology, Hangzhou 310014, China; Shaoxing Research Institute, Zhejiang University of Technology, Shaoxing 312085, China.
Sci Total Environ. 2024 Apr 10;920:170982. doi: 10.1016/j.scitotenv.2024.170982. Epub 2024 Feb 15.
The application of iron-doped biochar in peroxymonosulfate (PMS) activation systems has gained increasing attention due to their effectiveness and environmental friendliness in addressing environmental issues. However, the behavioral mechanism of iron doping and the detailed O generation mechanism in PMS activation systems remain ambiguous. Here, we investigated the effects of three anions (Cl, NOand SO) on the process of iron doping into bone char, leading to the synthesis of three iron-doped bone char (Fe-ClBC, Fe-NBC and Fe -SBC). These iron-doped bone char were used to catalyze PMS to degrade acetaminophen (APAP) and exhibited the following activity order: Fe-ClBC > Fe-NBC > Fe-SBC. Characterization results indicated that iron doping primarily occurred through the substitution of calcium in hydroxyapatite within BC. In the course of the impregnation, the binding of SO and Ca hindered the exchange of iron ions, resulting in lower catalytic activity of Fe-SBC. The primary reactive oxygen species in the Fe-ClBC/PMS and Fe-NBC/PMS systems were both O. O is produced through O conversion and PMS self-dissociation, which involves the generation of metastable iron intermediates and electron transfer within iron species. The presence of oxygen vacancies and more carbon defects in the Fe-ClBC catalyst facilitates O generation, thereby enhancing APAP degradation within the Fe-ClBC/PMS system. This study is dedicated to in-depth exploration of the mechanisms underlying iron doping and defect materials in promoting O generation.
铁掺杂生物炭在过一硫酸盐(PMS)活化体系中的应用因其在解决环境问题方面的有效性和环境友好性而受到越来越多的关注。然而,铁掺杂的行为机制和 PMS 活化体系中详细的 O 生成机制仍不清楚。在这里,我们研究了三种阴离子(Cl、NO 和 SO )对铁掺杂到骨炭中的过程的影响,导致合成了三种铁掺杂骨炭(Fe-ClBC、Fe-NBC 和 Fe-SBC)。这些铁掺杂骨炭被用于催化 PMS 降解扑热息痛(APAP),表现出以下活性顺序:Fe-ClBC > Fe-NBC > Fe-SBC。表征结果表明,铁掺杂主要通过取代骨炭中羟磷灰石中的钙来实现。在浸渍过程中,SO 和 Ca 的结合阻碍了铁离子的交换,导致 Fe-SBC 的催化活性较低。在 Fe-ClBC/PMS 和 Fe-NBC/PMS 体系中,主要的活性氧物质都是 O。O 通过 O 转化和 PMS 自分解产生,涉及到亚稳铁中间体的生成和铁物种内的电子转移。Fe-ClBC 催化剂中氧空位和更多的碳缺陷促进了 O 的生成,从而增强了 Fe-ClBC/PMS 体系中 APAP 的降解。本研究致力于深入探讨铁掺杂和缺陷材料在促进 O 生成中的机制。