Iron-based Metal-organic gel-derived Ferric oxide Nanosheets for Photo-Fenton Degradation of Rhodamine B

doi:10.6023/A22070304

Abstract

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

Cite this article

Wan Guo, Congyi Hu, Shujun Zhen, Chengzhi Huang, Yuanfang Li. Iron-based Metal-organic gel-derived Ferric oxide Nanosheets for Photo-Fenton Degradation of Rhodamine B[J]. Acta Chimica Sinica, 2022, 80(12): 1583-1591.

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Fig. & Tab. 7

Scheme 1. Schematic representation of (A) the synthesis of Fe-MOG and derived Fe2O3 and (B) the mechanism of Fe2O3 based photo-Fenton system for Rh B degradation

Figure 1. (A) The SEM image of Fe-MOG; (B) The SEM image, (C, D) TEM images; (E) HRTEM and (F) EDS images of 400-Fe2O3

Figure 2. (A) The PXRD patterns, (B) the FT-IR spectra, (C) N2 adsorption-desorption isotherms and (D) pore size distributions of Fe-MOG and derived Fe2O3

Figure 3. The XPS survey spectrum of 400-Fe2O3, the high-resolution XPS spectra of (B) Fe 2p, (C) O 1s and (D) C 1s in 400-Fe2O3

Figure 4. (A) UV-Vis diffuse reflection spectra, (B) Tauc plots, (C) transient photocurrent response curves and (D) electrochemical impedance spectroscopy of derived Fe2O3

Figure 5. Degradation efficiency of Rh B under the dark and light in different catalytic systems; (B) degradation efficiency in different time of Rh B by derived Fe2O3 and (C) the corresponding disappearance rate constant (kabs); (D) the kinetic curves comparison and (E) the corresponding disappearance rate constant (kabs) of Rh B degradation by 400-Fe2O3 at different pH values; (F) cyclic experiments of photo-Fenton degradation of Rh B by 400-Fe2O3. Reaction conditions: Rh B, 20.0 μmol?L?1; H2O2, 1.0 mmol?L?1; 400-Fe2O3, 0.05 mg?mL?1; pH, 7.0

Figure 6. (A) The calculated band structure of 400-Fe2O3; (B) photocurrent changes upon the addition of different concentrations of H2O2 under visible light irradiation; (C) the free radical trapping experiments for degradation of Rh B by 400-Fe2O3, cinhibitors: 1.0 mmol?L?1; the ESR spectra of (D) DMPO-?OH, (E) DMPO-?O2?, and (F) TEMPO-h+ in the 400-Fe2O3 photo-Fenton systems

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