Preparation of FePc/MXene Composite Cathode and Electro-Fenton Degradation of Sulfadimethoxine

doi:10.15541/jim20240176

Abstract

Abstract:

Development of electrode materials with high activity and stability is a key issue to achieve efficient degradation of sulfonamide pollutants by electro-Fenton (EF) system. In this work, FePc/MXene nanocomposites were prepared by using MXene material as carrier to load iron phthalocyanine (FePc) and employed as cathodic catalyst to construct EF system for the degradation of sulfadimethoxine (SDM). After loading FePc, the nanomaterials retained accordion-like lamellar structure with slightly roughened surface and narrowed interlayer spacing. Coordination number of FeN_x in FePc/MXene was about 4, in which the interaction between FePc and MXene was favorable to promote the electron transfer at the electrode surface. In the EF system, the FePc/MXene electrode achieved a 97.2% degradation rate of SDM within 50 min, showing excellent catalytic performance and stability over wide pH range. The significant improvement in degradation performance was mainly attributed to the enhanced activity of O₂ electrocatalytic reduction to H₂O₂ by the introduction of FeN₄ in the composites. Free radical (·OH and ·O₂^-) and non-radical (¹O₂) pathways were co-operative in the degradation of SDM by EF system. Frontier orbital theory and Fukui function theoretically elucidated the sites where SDM was attacked by different reactive oxygen species, primarily degrading through hydroxylation of the benzene ring, oxidation of the amino group on the benzene ring, and cleavage of C-S and S-N bonds. In addition, cycling and ion leaching experiments demonstrated the excellent stability of the prepared cathode catalysts.

Key words: electro-Fenton, FePc/MXene, sulfadimethoxine, reactive oxygen species, degradation pathway

CLC Number:

LIU Huilai, LI Zhihao, KONG Defeng, CHEN Xing. Preparation of FePc/MXene Composite Cathode and Electro-Fenton Degradation of Sulfadimethoxine[J]. Journal of Inorganic Materials, 2025, 40(1): 61-69.

Figures/Tables 14

Fig. 1 (a) SEM image, (b) TEM image, and (c) EDS elemental mappings of FePc/MXene

Fig. 2 XRD patterns of MXene, FePc, and FePc/MXene

Fig. 3 XPS spectra of FePc/Mxene (a) Survey; (b) N1s; (c) C1s; (d) O1s; (e) Ti2p; (f) Fe2p

Fig. 4 Fe K-edge XANES curves (a) and EXAFS curves in R space (b) of Fe foil, FePc and FePc/MXene

Fig. 5 CV curves (a) and Nyquist plots (b) of MXene/GCE, FePc/GCE and FePc/MXene/GCE

Fig. 6 SDM degradation rates and kinetics curves in the electro-Fenton system under different experimental conditions (a) Different cathode materials; (b) Initial SDM concentration; (c) Current density; (d) Initial pH

Fig. 7 (a) Effects of BQ, TBA and L-tryptophan radical scavengers on SDM degradation, and (b) ESR spectra of ·OH, ·O2- and 1O2 generated by catalyst in the electro-Fenton system

Fig. 8 Molecular geometry optimization of SDM (a) Optimized geometric structure; (b) HOMO and (c) LUMO distributions; (d) Molecular electrostatic potential; (e) Calculated Fukui index; (f) Degradation pathways of SDM

Fig. S1 N2 adsorption-desorption isotherms (a) and corresponding pore size distribution curves (b) of MXene and FePc/MXene Colorful figure is available on website

Fig. S2 FT-IR spectra of MXene and FePc/MXene Colorful figure is available on website

Fig. S3 EXAFS fitting curves in R space of FePc (a) and FePc/MXene (b)

Fig. S4 Cycling stability of FePc/MXene (a) and iron leaching concentration in the cycle experiment (b)

Fig. S5 SEM images (a) and XRD patterns (b) of FePc/MXene electrode before and after reaction Colorful figure is available on website

Table S1 EXAFS fitting parameters of Fe K-edge in FePc and FePc/MXene

Sample	Shell	CN	R/Å	σ²/(×10^-3, Å²)	ΔE₀/eV	R factor/%
FePc	Fe-N	4.0	1.93	7.9	3.2	1.8
FePc/MXene	Fe-N	4.1	1.96	1.1	5.1	1.5

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