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阳光驱动下水中邻苯二甲酸二乙酯通过磁性修饰生物炭催化剂的降解:内电子转移机制。

Sunlight-driven degradation of diethyl phthalate via magnetically modified biochar catalysts in water: Internal electron transfer mechanism.

机构信息

College of Resources and Environment, Hunan Agricultural University, Changsha, 410128, PR China; College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, PR China.

College of Resources and Environment, Hunan Agricultural University, Changsha, 410128, PR China.

出版信息

Chemosphere. 2021 Apr;269:129366. doi: 10.1016/j.chemosphere.2020.129366. Epub 2020 Dec 22.

DOI:10.1016/j.chemosphere.2020.129366
PMID:33385662
Abstract

This study presents a one-step synthetic approach for magnetic biochar (MBC) photo-degradation of diethyl phthalate (DEP). The results showed that MBC exhibited better catalytic property for DEP degradation than BC, and its catalytic performance was influenced by the amount of Fe doping. Electron paramagnetic resonance (EPR), quenching experiments, and chemical probe studies confirmed the presence of persistent free radicals (PFRs), hydroxyl radicals (·OH), and superoxide anion radical (·O) in both of BC and MBC. Solar light promoted the formation of PFRs in BC system, which transferred electrons to oxygen to form ·O, thus yielding ·OH. On the other hand, electron transfer occurred between PFRs and Fe for MBC, Fe played an important role in activation of O and ·O production. Subsequently, photo-Fenton reaction was primarily responsible for ·OH formation. This work compared the different generation pathways for ROS between BC and MBC and provides new insight into the possible mediatory roles of BC in O activation under solar light by transition metals.

摘要

本研究提出了一种一步法合成磁性生物炭(MBC)光降解邻苯二甲酸二乙酯(DEP)的方法。结果表明,MBC 对 DEP 降解表现出比 BC 更好的催化性能,其催化性能受到 Fe 掺杂量的影响。电子顺磁共振(EPR)、猝灭实验和化学探针研究证实,BC 和 MBC 中均存在持久性自由基(PFRs)、羟基自由基(·OH)和超氧阴离子自由基(·O)。太阳光照促进了 BC 体系中 PFRs 的形成,PFRs 将电子转移给氧气形成·O,从而产生·OH。另一方面,MBC 中 PFRs 和 Fe 之间发生电子转移,Fe 在激活 O 和·O 生成中发挥重要作用。随后,光芬顿反应主要负责·OH 的生成。本工作比较了 BC 和 MBC 中 ROS 的不同生成途径,为太阳能下过渡金属介导 BC 激活 O 提供了新的见解。

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