<p>The low transfer and utilization efficiency of photogenerated charges is the main obstacle restricting the degradation efficiency of photocatalytic materials. Herein, a novel composite photocatalyst carbon quantum dots(CQDs)/g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 was synthesized. Dual channels for electron transfer were constructed, one is the S-scheme heterojunction between g-C<sub>3</sub>N<sub>4</sub> and NH<sub>2</sub>-MIL-125 and the other is the transfer from g-C<sub>3</sub>N<sub>4</sub> to CQDs, which maximize the spatial separation of electrons and holes and preserve their redox capacity. The CQDs/g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 exhibited higher photocatalytic degradation activity for chlortetracycline hydrochloride (CTC) than individual components. The degradation efficiency can reach 94.95% under catalyst dosage of 100&#xa0;mg/L, CTC concentration of 5&#xa0;mg/L, and reaction time of 120&#xa0;min. The effects of initial pH, catalyst dosage, and typical ions in water on photocatalytic degradation efficiency were investigated. CQDs/g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 demonstrated good stability. •O<sub>2</sub><sup>−</sup>, •OH, and h<sup>+</sup> were the main active free radicals participating in CTC degradation, and a reasonable mechanism of electron transfer and utilization was proposed. The degradation intermediates and pathways of CTC were identified by DFT calculations and HPLC/MS measurements. The developmental toxicity of most of the intermediates is lower than that of CTC. This study provided a novel strategy for constructing composite photocatalyst for highly efficient removal of antibiotics in water.</p> Graphical Abstract <p></p>

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Constructing Dual Channels for Electron Transfer by Synthesis of CQDs/g-C3N4/NH2-MIL-125 for Efficient Photocatalytic Removal of Chlortetracycline Hydrochloride

  • Delong Meng,
  • Mengmeng Zhang,
  • Dingxun Ma,
  • Shanshan Li,
  • Guodong Zhang,
  • Guangshan Zhang,
  • Yanjun Xin,
  • Huijuan Li,
  • Qinghua Chen

摘要

The low transfer and utilization efficiency of photogenerated charges is the main obstacle restricting the degradation efficiency of photocatalytic materials. Herein, a novel composite photocatalyst carbon quantum dots(CQDs)/g-C3N4/NH2-MIL-125 was synthesized. Dual channels for electron transfer were constructed, one is the S-scheme heterojunction between g-C3N4 and NH2-MIL-125 and the other is the transfer from g-C3N4 to CQDs, which maximize the spatial separation of electrons and holes and preserve their redox capacity. The CQDs/g-C3N4/NH2-MIL-125 exhibited higher photocatalytic degradation activity for chlortetracycline hydrochloride (CTC) than individual components. The degradation efficiency can reach 94.95% under catalyst dosage of 100 mg/L, CTC concentration of 5 mg/L, and reaction time of 120 min. The effects of initial pH, catalyst dosage, and typical ions in water on photocatalytic degradation efficiency were investigated. CQDs/g-C3N4/NH2-MIL-125 demonstrated good stability. •O2, •OH, and h+ were the main active free radicals participating in CTC degradation, and a reasonable mechanism of electron transfer and utilization was proposed. The degradation intermediates and pathways of CTC were identified by DFT calculations and HPLC/MS measurements. The developmental toxicity of most of the intermediates is lower than that of CTC. This study provided a novel strategy for constructing composite photocatalyst for highly efficient removal of antibiotics in water.

Graphical Abstract