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构建三维还原氧化石墨烯包裹 nZVI 掺杂 AlO 的三元类 Fenton 催化剂:优化、表征和催化机制。

Construction of three-dimensional reduced graphene oxide wrapped nZVI doped with AlO as the ternary Fenton-like catalyst: Optimization, characterization and catalytic mechanism.

机构信息

Department of Nuclear Engineering and Technology, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan 430074, PR China.

Department of Nuclear Engineering and Technology, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan 430074, PR China.

出版信息

Sci Total Environ. 2021 Aug 1;780:146576. doi: 10.1016/j.scitotenv.2021.146576. Epub 2021 Mar 19.

Abstract

The rational design and synthesis of novel nanocomposites as effective heterogeneous catalysts is meaningful for the advances in Fenton-like technology. Herein, multiple variants of three-dimensional reduced graphene oxide wrapped nZVI doped with AlO (3D-RGO@nZVI/AlO) were prepared by three different self-assembly methods. The composites were characterized by field emission scanning electron microscopy, nitrogen adsorption/desorption isotherms, Raman spectrum analysis, X-ray diffraction, and X-ray photoelectron spectroscopy. A series of experiments on chloramphenicol degradation at different pH values were employed to evaluate the catalytic properties of the prepared catalysts. With the systematical investigation of their morphologies, chemical components and catalytic performance, the optimal 3D-RGO@nZVI/AlO catalyst was synthesized, which was favorable for inducing the Fenton-like reaction by activation of dissolved oxygen (DO) within a wide pH range. The anchored nZVI particles were the main active sites for catalytic oxidation, and doped Al played a major role in buffering the pH of CAP solution. Electron spin resonance spectroscopy revealed the existence of the superoxide radicals (·O) and singlet oxygen (O), which provides a new insight into the reaction mechanism of reactive oxygen species in the Fenton-like system. This work is an essential effort to explore the promoting effect of synthesis methods on the catalytic behavior of catalysts, and to further study the Fenton-like reaction triggered by DO activation.

摘要

新型纳米复合材料作为高效非均相催化剂的合理设计与合成对于类 Fenton 技术的发展具有重要意义。在此,通过三种不同的自组装方法制备了多种变体的三维还原氧化石墨烯包裹的 nZVI 掺杂 AlO(3D-RGO@nZVI/AlO)。通过场发射扫描电子显微镜、氮气吸附/脱附等温线、拉曼光谱分析、X 射线衍射和 X 射线光电子能谱对复合材料进行了表征。在不同 pH 值下进行了一系列氯霉素降解实验,以评估所制备催化剂的催化性能。通过对其形貌、化学成分和催化性能的系统研究,合成了最佳的 3D-RGO@nZVI/AlO 催化剂,该催化剂有利于通过激活溶解氧(DO)在较宽的 pH 范围内诱导类 Fenton 反应。锚定的 nZVI 颗粒是催化氧化的主要活性位点,掺杂的 Al 主要起缓冲 CAP 溶液 pH 值的作用。电子顺磁共振光谱揭示了超氧自由基(·O)和单线态氧(O)的存在,为类 Fenton 体系中活性氧物种的反应机制提供了新的见解。这项工作对于探索合成方法对催化剂催化行为的促进作用具有重要意义,并进一步研究了 DO 激活引发的类 Fenton 反应。

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