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氧化硅气凝胶负载铁酸钴活化过硫酸盐降解四环素性能及机理研究

谭烨1,周志宏1,吴优1,童海霞1,喻林萍1,曾巨澜1,2   

  1. 1.长沙理工大学,化学与医药工程学院 2.长沙理工大学,能源与动力工程学院

  • 收稿日期:2025-04-11 修回日期:2025-05-28 网络首发:2025-06-16 发布日期:2025-06-16
  • 通讯作者: 曾巨澜 E-mail:jlzeng@csust.edu.cn
  • 基金资助:
    国家自然科学基金(No. 22073011, No. 52074039)、湖南省自然科学基金(No. 2017JJ1026, No. 2025JJ60114)和湖南省教育厅科研项目 (No.24A0217)

Unveiling the Performance and Mechanism of CoFe?O?/Silica Aerogel in Activating Peroxymonosulfate for Tetracycline Degradation

TAN Ye1, ZHOU Zhihong1, WU You1, TONG Haixia1, YU Linping1, ZENG Julan1,2   

  1. 1. School of Chemistry and Pharmaceutical Engineering,  Changsha University of Science & Technology 2. College of Energy and Power Engineering, Changsha University of Science & Technology
  • Received:2025-04-11 Revised:2025-05-28 Online First:2025-06-16 Published:2025-06-16
  • Contact: Ju-Lan Zeng E-mail:jlzeng@csust.edu.cn
  • Supported by:
    Project supported by the National Natural Science Foundation of China (No. 22073011, No. 52074039), the Natural Science Foundation of Hunan Province, China (No. 2017JJ1026, No. 2025JJ60114), Scientific research project of Hunan Provincial Department of Education (No.24A0217)

摘要: 为解决目前过硫酸盐活化材料稳定性差,重复使用性能欠佳的问题,本工作使用二氧化硅气凝胶固定CoFe2O4纳米颗粒,成功合成了一种具有高比表面积的多孔CoFe2O4/二氧化硅气凝胶复合材料(SCF)。采用扫描电子显微镜、透射电子显微镜、X 射线衍射分析、X 射线光电子能谱、电子顺磁共振波谱仪、傅里叶变换红外光谱仪和氮气吸脱附测试等对催化剂理化性质进行了系统表征。分析表明,二氧化硅气凝胶大大缓解了CoFe2O4纳米颗粒的团聚,而CoFe2O4的成功负载在保留二氧化硅气凝胶高比表面积的同时,丰富了复合材料的孔隙结构。优化后的SCF-30在低负载(30wt%)下,PMS活化后对50 mg/L的TC溶液的去除效率达到84.79 %。通过淬灭实验,确定了SO4??,1O2和?O2?为催化反应中主要的活性物质,并推测了可能的反应机理和降解途径。此外,复合材料表现出优异的稳定性和pH耐受性。本研究为高稳定性过硫酸盐活化材料的制备与设计提供了思路。

关键词: 氧化硅气凝胶, 铁氧体, 四环素, 过硫酸盐, 高级氧化技术

Abstract: In this work, a porous CoFe2O4/silica aerogel gel composite (SCF) with high specific surface area was successfully synthesized by using silica aerogel as CoFe2O4 carrier. The catalyst was systematically characterized using scanning electron microscopy, transmission electron microscopy, X-ray diffraction analysis, X-ray photoelectron spectroscopy, electron paramagnetic resonance spectroscopy, Fourier transform infrared spectroscopy, and nitrogen adsorption desorption testing. The analysis shows that silica aerogel greatly alleviates the agglomeration of CoFe2O4 nanoparticles, and the successful loading of CoFe2O4 enriches the pore structure of the composite while retaining the high specific surface area of silica aerogel. The optimized SCF-30 achieved a removal efficiency of 84.79% for 50 mg/L TC solution after PMS activation with low loading amount. Through quenching experiments, SO4??, 1O2, and ?O2? were identified as the main active substances in the catalytic reaction, and possible reaction mechanisms and degradation pathways were speculated. In addition, composite materials exhibit excellent stability and pH tolerance. This work provides insights into the design and fabrication of highly stable persulfate-activating materials.

Key words: Silica Aerogel, Ferrite, Peroxymonosulfate, Tetracycline; Advanced oxidation processes

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