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<p>In this study, we constructed a visible-light-driven activated persulfate (PDS) system using a sulfur-doped and carbon-vacancy-modified g-C<sub>3</sub>N<sub>4</sub> photocatalyst (C/S-C<sub>3</sub>N<sub>4</sub>). The C/S-C<sub>3</sub>N<sub>4</sub> was synthesized via one-pot thermal condensation at 550°C using thioacetamide (TAA) and melamine as precursors. X-ray diffraction (XRD) analysis confirmed that the material retained the characteristic layered structure of g-C<sub>3</sub>N<sub>4</sub>, while scanning electron microscopy (SEM) and transmission electron microscopy (TEM) observations revealed a multilayered and porous morphology. The C/S-C<sub>3</sub>N<sub>4</sub>/PDS (VPC) system significantly enhanced the degradation efficiency of tetracycline hydrochloride (TCH), with a degradation reaction rate 2.79 times higher than that of the unmodified C<sub>3</sub>N<sub>4</sub>/PDS (VPg) system. The system exhibited remarkable degradation performance across a broad pH range (1.9–11.9), strong resistance to interference from multiple ions and fulvic acid, and high effectiveness even at elevated TCH concentration. Box-Behnken design (BBD) experiments indicated that PDS concentration and catalyst dosage are key factors affecting TCH degradation. Under the optimal conditions (0.05&#xa0;g/L TCH, 2.41&#xa0;mM PDS, 0.091&#xa0;g catalyst), 84.7% degradation was achieved. After five cycles, the degradation efficiency remained at 65.1%, demonstrating the catalysts’s satisfactory reusability. The synergistic effects of sulfur doping and carbon vacancies improved photocatalytic performance and PDS activation. Sulfate radicals (SO<sub>4</sub><sup><b>·</b>−</sup>), superoxide radicals (·O<sub>2</sub><sup>−</sup>), singlet oxygen (<sup>1</sup>O<sub>2</sub>), and photogenerated holes (<i>h</i><sup><i>+</i></sup>) were identified as the dominant reactive species. Intermediate analysis further elucidated the possible degradation pathways of TCH.</p> Graphical Abstract <p></p>

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Photocatalytic Activation of Persulfate on Sulfur-Doped and Carbon-Vacancy Modified Carbon Nitride: Mechanism of Tetracycline Hydrochloride Degradation

  • 期刊论文

  • 发表日期：

    2026年4月28日

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  • Chaofan Tan,
  • Ying Zhang,
  • Hubiao Zhao

摘要

In this study, we constructed a visible-light-driven activated persulfate (PDS) system using a sulfur-doped and carbon-vacancy-modified g-C3N4 photocatalyst (C/S-C3N4). The C/S-C3N4 was synthesized via one-pot thermal condensation at 550°C using thioacetamide (TAA) and melamine as precursors. X-ray diffraction (XRD) analysis confirmed that the material retained the characteristic layered structure of g-C3N4, while scanning electron microscopy (SEM) and transmission electron microscopy (TEM) observations revealed a multilayered and porous morphology. The C/S-C3N4/PDS (VPC) system significantly enhanced the degradation efficiency of tetracycline hydrochloride (TCH), with a degradation reaction rate 2.79 times higher than that of the unmodified C3N4/PDS (VPg) system. The system exhibited remarkable degradation performance across a broad pH range (1.9–11.9), strong resistance to interference from multiple ions and fulvic acid, and high effectiveness even at elevated TCH concentration. Box-Behnken design (BBD) experiments indicated that PDS concentration and catalyst dosage are key factors affecting TCH degradation. Under the optimal conditions (0.05 g/L TCH, 2.41 mM PDS, 0.091 g catalyst), 84.7% degradation was achieved. After five cycles, the degradation efficiency remained at 65.1%, demonstrating the catalysts’s satisfactory reusability. The synergistic effects of sulfur doping and carbon vacancies improved photocatalytic performance and PDS activation. Sulfate radicals (SO4·−), superoxide radicals (·O2−), singlet oxygen (1O2), and photogenerated holes (h+) were identified as the dominant reactive species. Intermediate analysis further elucidated the possible degradation pathways of TCH.

Graphical Abstract