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<p>Tetracycline (TC) has the characteristics of widespread use and environmental persistence, and has become a widely residual high ecological risk pollutant. In this study, we developed a natural suspended sediment (SS)-based adsorption-catalysis bifunctional system, achieving peroxymonosulfate activation and used for efficient removal of TC. Under optimized reaction conditions (pH = 7.0, [peroxymonosulfate] = 0.4&#xa0;mM, SS = 2.5&#xa0;g/L, [TC]<sub>0</sub> = 50&#xa0;mg/L), the TC removal efficiency reaches 83.9%. Adsorption analysis shows that TC adsorption by SS follows a pseudo-second-order kinetic model (<i>R</i><sup>2</sup> &gt; 0.99), with a maximum theoretical adsorption capacity of 237.51&#xa0;mg/g. The adsorption process combines monolayer and multilayer mechanisms. X-ray photoelectron spectroscopy (XPS) analysis and electron paramagnetic resonance (EPR) detection confirm that Fe active sites in SS facilitate electron transfer pathways for peroxymonosulfate activation, with singlet oxygen (<sup>1</sup>O<sub>2</sub>) identified as the dominant reactive species responsible for TC degradation. Liquid chromatography-mass spectrometry (LC–MS) analysis elucidates three major TC degradation pathways: hydroxylation, demethylation, and demethyleneation, ultimately yielding low-toxicity or non-toxic small organic molecules and inorganic products. The SS/peroxymonosulfate system achieves a TC removal efficiency exceeding 80% across a pH range of 4–11 and demonstrates strong adaptability to TC concentrations ranging from 10 to 110&#xa0;mg/L. Inorganic anions and natural organic matter (humic acid, HA) affect TC removal to varying degrees. This system effectively reduces the expression levels of antibiotic resistance genes (ARGs) in sediments by 12–17%, suggesting its suitability for the in situ remediation of antibiotic-contaminated water. Furthermore, it offers potential for the development of SS-based advanced oxidation processes (AOPs) for environmental applications.</p>

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Tetracycline degradation in water via adsorption and peroxymonosulfate activation by natural sediments: removal mechanisms, toxicity assessment, and environmental implications

  • 期刊论文

  • 发表日期：

    2025年10月12日

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  • Zehui Wu,
  • Yanxia You,
  • Lei Song,
  • Xuejun Zhang,
  • Si Hu,
  • Yizhuo Niu,
  • Kexin Chen

摘要

Tetracycline (TC) has the characteristics of widespread use and environmental persistence, and has become a widely residual high ecological risk pollutant. In this study, we developed a natural suspended sediment (SS)-based adsorption-catalysis bifunctional system, achieving peroxymonosulfate activation and used for efficient removal of TC. Under optimized reaction conditions (pH = 7.0, [peroxymonosulfate] = 0.4 mM, SS = 2.5 g/L, [TC]0 = 50 mg/L), the TC removal efficiency reaches 83.9%. Adsorption analysis shows that TC adsorption by SS follows a pseudo-second-order kinetic model (R2 > 0.99), with a maximum theoretical adsorption capacity of 237.51 mg/g. The adsorption process combines monolayer and multilayer mechanisms. X-ray photoelectron spectroscopy (XPS) analysis and electron paramagnetic resonance (EPR) detection confirm that Fe active sites in SS facilitate electron transfer pathways for peroxymonosulfate activation, with singlet oxygen (1O2) identified as the dominant reactive species responsible for TC degradation. Liquid chromatography-mass spectrometry (LC–MS) analysis elucidates three major TC degradation pathways: hydroxylation, demethylation, and demethyleneation, ultimately yielding low-toxicity or non-toxic small organic molecules and inorganic products. The SS/peroxymonosulfate system achieves a TC removal efficiency exceeding 80% across a pH range of 4–11 and demonstrates strong adaptability to TC concentrations ranging from 10 to 110 mg/L. Inorganic anions and natural organic matter (humic acid, HA) affect TC removal to varying degrees. This system effectively reduces the expression levels of antibiotic resistance genes (ARGs) in sediments by 12–17%, suggesting its suitability for the in situ remediation of antibiotic-contaminated water. Furthermore, it offers potential for the development of SS-based advanced oxidation processes (AOPs) for environmental applications.