Metal-free g-C3N5 photocatalysts with defect sites as efficient peroxymonosulfate activators for antibiotic removal in aqueous media

Abstract

Nitrogen-rich graphitic carbon nitride (g-C3N5) has emerged as a promising and fascinating photocatalyst for tackling problems related to antibiotic pollution. Herein, porous O-doped g-C3N5 with N vacancy (g-C3N5-x-O) was fabricated via a facile two-step pyrolysis technique using 3-amino-1,2,4-triazole and oxalic acid as precursors. The sample modified with 2.0 mol.% oxalic acid (CN-2.0) exhibits a porous structure with a specific surface area of 249.78 m2. g−1, 2.77 times greater than that of pristine g-C3N5 (CN-0). In addition, the existence of O-doping and N vacancies in g-C3N5 framework not only promotes charge transfer properties but also suppresses photogenerated electron-hole recombination according to the results of transient photocurrent responses, photoluminescence and electrochemical impedance spectra. The CN-2.0 sample displays the highest photocatalytic activity, which eliminates 77.3% sulfamethoxazole (SMX, 20 mg. L−1) after 60 min irradiation under UV 365 nm light source. The addition of peroxymonosulfate (PMS, HSO5-) significantly accelerates SMX photodegradation rate as well as reduces the influence of pH solution during treatment process. The reactive oxygen species including •O2−, 1O2, SO4•−, •OH, h+ contribute to SMX removal. The efficient degradation of numerous antibiotic classes highlights the possible applicability of g-C3N5-x-O. Interestingly, the catalyst retains its high activity and stability even after four consecutive reuse cycles. The intermediates of SMX degradation were determined and plausible SMX degradation pathways were proposed. Toxicity assessments demonstrated that the overall toxicity of the solution decreased after treatment. This work provides a feasible strategy to design and modulate g-C3N5 photocatalyst activated by PMS for antibiotic removal in wastewater.