Graphitic carbon nitride (CN) has emerged as a promising metal-free photocatalyst for environmental remediation and clean energy production. In this study, CN materials were synthesized from urea combined with melamine, dicyandiamide, and ammonium thiocyanate via a simple pyrolysis method. Structural, morphological, and optical properties were analyzed using X-ray diffraction, Fourier-transform infrared spectroscopy, scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy, nitrogen adsorption-desorption isotherms, X-ray photoelectron spectroscopy, UV–Vis diffuse reflectance spectroscopy, and electron spin resonance spectroscopy (ESR). Among the prepared samples, 10UM-CN exhibited outstanding photocatalytic activity toward tetracycline (TC) degradation and photocatalytic hydrogen peroxide (H2O2) production. Specifically, 10UM-CN achieved a TC removal efficiency of approximately 94% TC removal (10 ppm, 100 mL), with a kinetic rate constant k = 0.0375 min−1 in 75 min and produced over 74.27 mM g−1 h−1 of H2O2 after 30 min of light irradiation. Mechanistic investigations combined with ESR analysis revealed that photogenerated electrons and superoxide radicals were the dominant reactive oxygen species. Electrochemical analyses, including electrochemical impedance spectroscopy, photocurrent response, and linear sweep voltammetry, confirmed enhanced charge transport, reduced recombination, and the H2O2 production pathway following a two-step single-electron reduction mechanism. In addition, the reusability and stability of 10UM-CN were evaluated through four consecutive cycles of photocatalytic TC degradation, demonstrating consistent performance and structural stability. Moreover, the toxicity of the antibiotic solution after photodegradation was investigated using deoxyribonucleic acid (DNA) cleavage analysis and toxicity prediction tools. This study provides a facile and effective strategy for improving the photocatalytic efficiency of CN by combining compatible precursors, offering a practical approach for the development of metal-free photocatalysts for environmental remediation and sustainable energy production.
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