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<p>A g-C<sub>3</sub>N<sub>4</sub>@ Fe/Ti bimetallic metal–organic framework (MOF) derivative Fenton-like catalyst (Fe/Ti-CN<sub>600</sub>) was synthesized via high-temperature calcination of a mixture of melamine and Fe/Ti bimetallic MOF under a nitrogen atmosphere. The incorporation of g-C<sub>3</sub>N<sub>4</sub> provides electron-rich nitrogen sites, which facilitate electron transfer and thereby enhance redox reactions. The synergistical interplay between surface Fe<sup>3+</sup>/Fe<sup>2+</sup> and Ti<sup>4+</sup>/Ti<sup>3+</sup> redox couples promoted the reduction reaction of Fe<sup>3+</sup> and collectively accelerates the activation of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) for the degradation of tetracycline hydrochloride (TCH). Fe/Ti-CN<sub>600</sub> revealed significantly enhanced catalytic activity compared to Fe/Ti<sub>600</sub> and maintained high performance over five consecutive cycles. Notably, the iron leaching concentration (≤ 0.30 mg<sup>.</sup>L<sup>−1</sup>) during cyclic operation of the Fe/Ti-CN<sub>600</sub>/H<sub>2</sub>O<sub>2</sub> system was substantially below the permissible level of surface water. The primary active species responsible for TCH degradation were identified as <InlineEquation ID="IEq1111"> <EquationSource Format="TEX">\({\text{HO}}^{ \cdot }\)</EquationSource> <EquationSource Format="MATHML"><math> <msup> <mrow> <mtext>HO</mtext> </mrow> <mo>·</mo> </msup> </math></EquationSource> </InlineEquation>, <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\({\text{O}}_{2}^{ \cdot - }\)</EquationSource> <EquationSource Format="MATHML"><math> <msubsup> <mtext>O</mtext> <mrow> <mn>2</mn> </mrow> <mrow> <mo>·</mo> <mo>-</mo> </mrow> </msubsup> </math></EquationSource> </InlineEquation>, and <sup>1</sup>O<sub>2</sub>. In addition, toxicity assessment using ECOSAR 2.2 software indicated a significant reduction in the toxicity of the degraded solution. Based on active species analysis and LC–MS results, a plausible degradation pathway was proposed. The Fe/Ti-CN<sub>600</sub> demonstrated outstanding catalytic performance and shows great promise as an effective catalyst for TCH removal.</p>

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Dual redox cycles of Fe(III)/Fe(II) and Ti(IV)/Ti(III) on g-C3N4 jointly promoted hydrogen peroxide activation for tetracycline hydrochloride degradation: performance, mechanism and toxicity analysis

  • 期刊论文

  • 发表日期：

    2026年2月19日

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  • Longhui Nie,
  • Yiting Zheng,
  • Yiqiong Yang,
  • Xingru Chen,
  • Xueling Li,
  • Ruihao Li

摘要

A g-C3N4@ Fe/Ti bimetallic metal–organic framework (MOF) derivative Fenton-like catalyst (Fe/Ti-CN600) was synthesized via high-temperature calcination of a mixture of melamine and Fe/Ti bimetallic MOF under a nitrogen atmosphere. The incorporation of g-C3N4 provides electron-rich nitrogen sites, which facilitate electron transfer and thereby enhance redox reactions. The synergistical interplay between surface Fe3+/Fe2+ and Ti4+/Ti3+ redox couples promoted the reduction reaction of Fe3+ and collectively accelerates the activation of hydrogen peroxide (H2O2) for the degradation of tetracycline hydrochloride (TCH). Fe/Ti-CN600 revealed significantly enhanced catalytic activity compared to Fe/Ti600 and maintained high performance over five consecutive cycles. Notably, the iron leaching concentration (≤ 0.30 mg.L−1) during cyclic operation of the Fe/Ti-CN600/H2O2 system was substantially below the permissible level of surface water. The primary active species responsible for TCH degradation were identified as \({\text{HO}}^{ \cdot }\) HO · , \({\text{O}}_{2}^{ \cdot - }\) O 2 · - , and 1O2. In addition, toxicity assessment using ECOSAR 2.2 software indicated a significant reduction in the toxicity of the degraded solution. Based on active species analysis and LC–MS results, a plausible degradation pathway was proposed. The Fe/Ti-CN600 demonstrated outstanding catalytic performance and shows great promise as an effective catalyst for TCH removal.