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一种新型可见光驱动的氧掺杂 CN/BiOCl/高铁酸盐(VI)体系用于双酚 A 的降解:自由基和非自由基途径。

A novel visible light-driven oxygen doped CN/BiOCl/ferrate(VI) system for Bisphenol A degradation: Radical and nonradical pathways.

机构信息

School of Chemistry and Chemical Engineering, Hainan University, Haikou, 570228, China.

School of Chemistry and Chemical Engineering, Hainan University, Haikou, 570228, China; Key Laboratory of Solid Waste Resource Utilization and Environmental Protection of Haikou City, Haikou, 570228, China.

出版信息

Chemosphere. 2024 Sep;364:143227. doi: 10.1016/j.chemosphere.2024.143227. Epub 2024 Aug 30.

Abstract

In this study, visible light-activated photocatalyst oxygen-doped CN@BiOCl (OCN@BOC) and Fe(VI) coupling system was proposed for the efficient degradation of bisphenol A (BPA). The comprehensive characterization of the OCN@BOC photocatalyst revealed its excellent photogenerated carrier separation rate in heterogeneous structures. The OCN@BOC/Fe(VI)/Vis system exhibited a remarkable BPA removal efficiency of over 84% within 5 min. Comparatively, only 37% and 59% of BPA were degraded by single OCN@BOC and Fe(VI) in 5 min, respectively. Reactive species scavenging experiments, phenyl sulfoxide transformation experiments, and electron paramagnetic resonance experiments confirmed the involvement of superoxide radicals (⋅O), singlet oxygen (O), as well as iron(V)/iron(IV) (Fe(V)/Fe(IV)) species in the degradation process of BPA. Furthermore, density functional theoretical calculations and identification of intermediates provided insights into the potential degradation mechanism of BPA during these reactions. Additionally, simulation evaluations using an ecological structure activity relationship model demonstrated that the toxicity of BPA to the ecological environment was mitigated during its degradation process. This study presented a novel strategy for removing BPA utilizing visible light photocatalysts, highlighting promising applications for practical water environment remediation with the OCN@BOC/Fe(VI)/Vis system.

摘要

在这项研究中,提出了可见光激活光催化剂氧掺杂 CN@BiOCl(OCN@BOC)和 Fe(VI) 耦合系统,用于有效降解双酚 A (BPA)。对 OCN@BOC 光催化剂的综合表征揭示了其在异质结构中优异的光生载流子分离速率。在 5 分钟内,OCN@BOC/Fe(VI)/Vis 系统表现出超过 84%的高效 BPA 去除效率。相比之下,在 5 分钟内,单独的 OCN@BOC 和 Fe(VI) 分别仅降解了 37%和 59%的 BPA。活性物质捕获实验、苯基亚砜转化实验和电子顺磁共振实验证实了超氧自由基 (⋅O)、单线态氧 (O) 以及铁(V)/铁(IV) (Fe(V)/Fe(IV)) 物种在 BPA 降解过程中的参与。此外,密度泛函理论计算和中间体的鉴定提供了对这些反应中 BPA 潜在降解机制的深入了解。此外,使用生态结构活性关系模型进行的模拟评估表明,BPA 对生态环境的毒性在其降解过程中得到减轻。本研究提出了一种利用可见光光催化剂去除 BPA 的新策略,为 OCN@BOC/Fe(VI)/Vis 系统在实际水环境修复中的应用提供了有前景的应用。

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