铁基金属有机凝胶衍生的三氧化二铁纳米片用于光芬顿降解罗丹明B
收稿日期: 2022-07-13
网络出版日期: 2022-11-04
基金资助
国家自然科学基金(21874109)
Iron-based Metal-organic gel-derived Ferric oxide Nanosheets for Photo-Fenton Degradation of Rhodamine B
Received date: 2022-07-13
Online published: 2022-11-04
Supported by
National Natural Science Foundation of China(21874109)
光催化剂在工业废水处理中发挥着重要作用. 本工作以室温下一步合成的片状铁基金属有机凝胶(Fe-based Metal-organic gel, Fe-MOG)为前驱体, 在不同温度下煅烧得到了片状(300-Fe2O3和400-Fe2O3)和球形(500-Fe2O3和600-Fe2O3)两种形貌的衍生三氧化二铁(Fe2O3). 通过一系列测试手段对衍生Fe2O3的晶体结构和光电性能进行了表征. 其中, 具有碳骨架结构的400-Fe2O3因其优良的电子传输性能和较高的光生电荷分离效率表现出优异的光催化活性, 可在中性条件下60 min内光降解97.5%的罗丹明B (Rh B), 并且在连续五次循环实验后其降解效率仍能达到85.3%. 本工作为开发和设计具有优异催化活性的半导体光催化剂提供了新的思路.
郭湾 , 胡聪意 , 甄淑君 , 黄承志 , 李原芳 . 铁基金属有机凝胶衍生的三氧化二铁纳米片用于光芬顿降解罗丹明B[J]. 化学学报, 2022 , 80(12) : 1583 -1591 . DOI: 10.6023/A22070304
Photocatalysts play an important role in industrial wastewater treatment. So far, the photocatalysts of photo- Fenton degradation of water pollutants include metal-organic frameworks, two-dimensional layered hydroxides, and transition metal oxides. Among them, transition metal oxides have become a research hotspot because of their easy availability of metal ions, stability and non-toxicity during degradation. In particular, ferric oxide (Fe2O3) has the advantages of wide visible light absorption range, good optical response and high thermodynamic stability, which is considered to be a promising semiconductor photocatalyst. Herein, in this work, Fe2O3 of two morphologies, flakes (namely 300-Fe2O3 and 400-Fe2O3) and spheres (namely 500-Fe2O3 and 600-Fe2O3) were obtained by calcinating sheet-like iron-based metal-organic gel (Fe-MOG) synthesized with Fe3+ and 1,10-phenanthroline-2,9-dicarboxylic acid in one step at room temperature, and were used for photo-Fenton degradation of rhodamine B (Rh B). The crystal structure and optoelectronic properties of the as-prepared Fe2O3 were characterized by powder X-ray diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy elemental mapping (EDS), the UV-Vis diffuse reflectance spectra (UV-Vis DRS) and electrochemical impedance spectroscopy (EIS). Among them, 400-Fe2O3 with carbon skeleton structure exhibited excellent electron transport performance and high photogenerated charge separation efficiency, endowing it with remarkable catalytic activity. In addition, the existence of oxygen vacancy in 400-Fe2O3 promoted the formation of Fe2+, which was the key factor to enhance the photo-Fenton activity. 400-Fe2O3 could photocatalytically degrade 97.5% Rh B within 60 min under neutral conditions, and the degradation efficiency was retained 85.3% after five consecutive cycles. Under visible light irradiation, a part of the photogenic electron (e‒) generated by 400-Fe2O3 reacted with O2 to generate superoxide anion radical (•O2‒), the other part of e‒ reduced Fe3+ to Fe2+ in situ. Subsequently, Fe2+ can catalyze the decomposition of H2O2 into hydroxyl radicals (•OH), and participated in the photodegradation of Rh B together with •O2‒. This work provides a new idea for the development and design of semiconductor photocatalysts with excellent catalytic activity.
Key words： metal-organic gel; ferric oxide; carbon skeleton; photo-Fenton; rhodamine B
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