Fabrication and characterization of a novel multilayer heterojunction Si3N4-PbO2 nanocomposite electrode and its application on electrocatalysis degradation of sulfathiazole

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Vol. 490; p. 151851
• Main Authors: Yu, Naichuan, Wang, Yixuan, Cao, Hanfei, Si, Rongmei, Xu, Zhilong, Hong, Xintong, Mao, Xianhe, Shen, Kun, Wu, Junsheng
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 15.06.2024
• Subjects: Adsorption energy; Degradation mechanism; Electrocatalysis; Heterojunction; Lead dioxide; Sulfathiazole; Electrocatalysis; Sulfathiazole; Degradation mechanism; Adsorption energy; Lead dioxide; Heterojunction
• ISSN: 1385-8947
• DOI: 10.1016/j.cej.2024.151851

[Display omitted] •A novel Si3N4-PbO2 nanocomposite electrode was fabricated and characterized.•Si3N4-PbO2 electrode showed extreme long accelerated life.•Si3N4-PbO2 electrode could treat sulfathiazole and sulfonamides efficiently.•Degradation mechanism of sulfathiazole were explored by GC-MS.•Several theoretical calculations were established by VASP and Multiwfn software. To lengthen the lifetime and extend the potential commercial applications of lead dioxide electrode, herein, a novel multilayer heterojunction Ti/ SnO2-Sb2O3/ graphene oxide/ carbon nanotube/ Si3N4-PbO2 electrode (Si3N4-PbO2 electrode) was fabricated by co-electrodeposition process that doping Si3N4 nanoparticles in eletroplating solution. Various spectroscopic and microscopic techniques, including scanning electron microscopy (SEM) equipped with energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), were employed to characterize the surface of the fabricated electrode. The EDS analysis confirmed the successful attachment of 5.49 %wt Si and 2.46 %wt N elements from Si3N4 nanoparticles onto the PbO2 surface, while the XRD results indicated a shift in the preferred orientation of PbO2 grains from β(110) to β(101). The water adsorption energy and ·OH desorption energy in the electrocatalysis process were determined to be 0.71 eV and 0.241 eV through theoretical calculating. Subsequently, the Si3N4-PbO2 electrode was employed as an anode for the electrocatalytic degradation of sulfathiazole-simulated wastewater and real sulfonamides wastewater. Under optimized conditions determined via response surface methodology (RSM), the COD degradation efficiency reached 69.37 % for sulfathiazole and 62.35 % for real sulfonamides wastewater. The final COD concentration of the real sulfonamides wastewater was reduced to 77.05 mg/L, under the national urban sewage discharge standard. Finally, the degradation mechanism and pathway of sulfathiazole has been arranged based on the electron spin resonance (ESR), cyclic voltammetry (CV), while the intermediates were detected by Gas Chromatography-Mass Spectrometer (GC-MS) and the reactive sites of sulfathiazole were predicted by using Fukui function.