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铁铜双金属掺杂介孔 γ-Al2O3 用于类 Fenton 氧化 4-氯苯酚的协同效应:结构、组成、电化学行为和催化性能。

Synergistic effects in iron-copper bimetal doped mesoporous γ-AlO for Fenton-like oxidation of 4-chlorophenol: Structure, composition, electrochemical behaviors and catalytic performance.

机构信息

Ministry of Education Key Laboratory of Pollution Control and Ecological Remediation for Industrial Agglomeration Area, School of Environment and Energy, State Key Laboratory of Pulp and Paper Engineering, South China University of Technology Guangzhou, 510006, China.

Ministry of Education Key Laboratory of Pollution Control and Ecological Remediation for Industrial Agglomeration Area, School of Environment and Energy, State Key Laboratory of Pulp and Paper Engineering, South China University of Technology Guangzhou, 510006, China.

出版信息

Chemosphere. 2018 Jul;203:442-449. doi: 10.1016/j.chemosphere.2018.04.001. Epub 2018 Apr 3.

Abstract

Iron-copper bimetal supported on mesoporous γ-AlO with different Fe/Cu ratios was prepared via a modified evaporation-induced self-assembly method and employed to degrade 4-chlorophenol (4-CP) in a Fenton-like process. The X-ray photoelectron spectroscopy, X-ray diffraction spectrum and UV-vis diffuse reflectance spectroscopy results confirmed the co-doping of Fe/Fe and Cu/Cu into the lattice of γ-AlO through the bonds of AlOFe and AlOCu. With the iron and copper co-doped in γ-AlO, three-fold oxygen vacancies (V) could be achieved compared with that of non-metal catalysts, which was favorable for the reduction of iron and copper species. The 1Fe3Cu-γ-AlO with a Fe/Cu mass ratio of 1:3 exhibited the highest activity on Fenton-like degradation of 4-CP due to the synergistic effects of Fe and Cu by facilitating the electron transfer in the recycles of Cu/Cu and Fe/Fe based on the results of X-ray photoelectron spectroscopy, cyclic voltammetry and electro paramagnetic resonance analysis. The utilization efficiency of HO was as high as 86.0% when 4-CP almost disappeared (i.e., 99.7 percent of 0.78 mM 4-CP) at 240 min and pH 7.0, additionally, their dechlorination and TOC removal efficiencies were 92.0% and 81.6%, respectively. The catalyst also displayed a good performance after 5th cycles. Furthermore, a possible mechanism for activation of OH on the catalyst surface was also proposed.

摘要

通过一种改进的蒸发诱导自组装方法制备了不同 Fe/Cu 比的负载在介孔 γ-AlO 上的铁铜双金属,并将其用于类芬顿过程中降解 4-氯苯酚(4-CP)。X 射线光电子能谱、X 射线衍射谱和紫外可见漫反射光谱结果证实,Fe/Fe 和 Cu/Cu 通过 AlOFe 和 AlOCu 键共掺杂到 γ-AlO 的晶格中。与非金属催化剂相比,铁和铜共掺杂到 γ-AlO 中可以实现三倍的氧空位(V),这有利于铁和铜物种的还原。在类芬顿降解 4-CP 中,Fe/Cu 质量比为 1:3 的 1Fe3Cu-γ-AlO 表现出最高的活性,这是由于 Fe 和 Cu 的协同作用,促进了 Cu/Cu 和基于 X 射线光电子能谱、循环伏安法和电子顺磁共振分析的 Fe/Fe 循环中的电子转移。当 4-CP 几乎消失(即 0.78mM 4-CP 的 99.7%)时,HO 的利用率高达 86.0%,在 pH 7.0 下 240min 时,其脱氯和 TOC 去除效率分别为 92.0%和 81.6%。催化剂在第 5 次循环后也表现出良好的性能。此外,还提出了一种在催化剂表面激活 OH 的可能机制。

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