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碳点/CeVO4纳米复合物协同可见光活化过一硫酸盐降解盐酸四环素

李世嘉 庞尔楠

李世嘉, 庞尔楠. 碳点/CeVO4纳米复合物协同可见光活化过一硫酸盐降解盐酸四环素[J]. 复合材料学报, 2024, 42(0): 1-10.
引用本文: 李世嘉, 庞尔楠. 碳点/CeVO4纳米复合物协同可见光活化过一硫酸盐降解盐酸四环素[J]. 复合材料学报, 2024, 42(0): 1-10.
LI Shijia, PANG Ernan. CDs/CeVO4 nanohybrids synergistic visible light for activation of peroxymonosulfate toward tetracycline degradation[J]. Acta Materiae Compositae Sinica.
Citation: LI Shijia, PANG Ernan. CDs/CeVO4 nanohybrids synergistic visible light for activation of peroxymonosulfate toward tetracycline degradation[J]. Acta Materiae Compositae Sinica.

碳点/CeVO4纳米复合物协同可见光活化过一硫酸盐降解盐酸四环素

基金项目: 山西工程科技职业大学校科技创新基金(202229)
详细信息
    通讯作者:

    李世嘉,博士研究生,讲师,研究方向:高级氧化法降解水中有机污染物 E-mail:lishijia@sxgkd.edu.cn

  • 中图分类号: TB333

CDs/CeVO4 nanohybrids synergistic visible light for activation of peroxymonosulfate toward tetracycline degradation

Funds: Science and Technology Innovation Fund of Shanxi Vocational University of Engineering Science and Technology (NO.202229)
  • 摘要: CeVO4因其对可见光较低的利用率和光生电子空穴对易于复合的缺点限制其在光催化领域中的应用。碳点(CDs)具有独特的π共轭结构赋予其优异的光生电子存储和转移能力。本研究采用水热和共沉淀两步法成功制备出CDs与CeVO4的纳米复合物(CDs/CeVO4),在掺入CDs后,其光生载流子的转移和分离效率得到有效提高。在可见光照射下,CDs/CeVO4能高效活化过一硫酸盐(PMS)降解盐酸四环素(TC),反应60 min后对TC的降解率达到90 %。反应速率常数是CeVO4的4.1倍(0.03815 min−1)。XPS、紫外可见漫反射光谱和时间分辨荧光光谱测试结果表明,CDs/CeVO4相比于CeVO4带隙变窄,可见光吸收能力增强,荧光寿命是CeVO4的15.1倍(7.1 ns)。EPR与XPS测试结果相互印证掺入CDs的纳米复合物中存在丰富的氧空位,进一步增强其活化PMS能力。活性物质捕获实验表明,h+、SO4·−和·OH是反应体系中的活性物质,在此基础上提出了该体系可能的降解机制。CDs/CeVO4表现出良好的稳定性,经过五次循环实验后,仍表现出良好的催化性能。CDs/CeVO4协同可见光活化PMS降解水中有机污染物为废水治理提供一种新的方法和思路。

     

  • 图  1  CeVO4和碳点(CDs)/ CeVO4复合催化剂的(a) XRD图谱,(b) FTIR图谱和(c) Raman图谱

    Figure  1.  (a) XRD patterns, (b) FTIR spectra and (c) Raman spectra of CeVO4 and carbon dots(CDs)/ CeVO4 composite catalyst

    图  2  CeVO4的(a) TEM和(b) HRTEM,CDs/CeVO4的(c) TEM和(d) HRTEM,(e) CDs/CeVO4的EDS图

    Figure  2.  (a) TEM and (b) HRTEM images of CeVO4. (c) TEM and (d) HRTEM images of CDs/CeVO4. (e) The EDS images of CDs/CeVO4

    图  3  XPS谱:CDs/CeVO4和CeVO4的(a) 全谱图,(b) O 1s,(c) Ce 3d和(d) V 2p谱图,(e) CDs/CeVO4的C 1s谱,(f) CeVO4和CDs/CeVO4的EPR谱图

    Figure  3.  XPS spectra: (a) full survey, (b) O 1s, (c) O 1s, (c) Ce 3d and (d) V 2p of CDs/CeVO4 and CeVO4. (e) C1s spectra of CDs/CeVO4. (f) EPR spectra of CeVO4 and CDs/CeVO4.

    图  4  CDs/CeVO4和CeVO4的(a) 紫外可见漫反射光谱,(b) 相应的Tauc-plot图和(c) VB-XPS图

    Figure  4.  (a) UV-visible diffuse reflectance spectra of CDs/CeVO4 and CeVO4, (b) the corresponding Tauc-plot and (c) VB-XPS

    图  5  CDs/CeVO4 and CeVO4的时间分辨荧光光谱

    Figure  5.  Time-resolved fluorescence spectra of CDs/CeVO4 and CeVO4

    图  6  (a) 不同催化体系在光照和未光照下降解TC效率,(b) 不同催化体系反应速率常数

    Figure  6.  (a) The efficiency of different catalytic systems on TC degradation with or not light irradiation. (b) Reaction rate constants for different catalytic systems

    图  7  (a) CDs/CeVO4的循环稳定性,(b) 新制备和使用过的CDs/CeVO4的XRD图

    Figure  7.  Cyclic stability of CDs/CeVO4. (b) XRD patterns of new and used CDs/CeVO4

    图  8  CDs/CeVO4和CeVO4的(a)瞬态光电流响应和(b)电化学阻抗图

    Figure  8.  (a) The photocurrent responses and (b) the electrochemical impedance spectra of CDs/CeVO4 and CeVO4

    图  9  加入不同捕获剂对TC降解率的影响

    Figure  9.  Effect of adding different trapping agents on TC degradation rate

    图  10  光照下CDs/CeVO4活化PMS机制

    Figure  10.  The activation PMS mechanism of CDs/CeVO4 under light irradiation

    表  1  不同碳点含量的复合催化剂活化PMS降解TC效率

    Table  1.   The efficiency of composite catalysts with different CDs content on TC degradation by activating PMS

    Catalyst CDs/g Ce(NO3)3/g NH4VO3/g C/C0/%
    CDs/CeVO4-2 0.027 0.271 0.059 70
    CDs/CeVO4-4 0.054 0.271 0.059 90 this work
    CDs/CeVO4-8 0.108 0.271 0.059 72
    Notes:The catalyst (CDs/CeVO4-4) with the highest degradation rate is used in this work. C0 and C represent the concentrations of TC at time 0 and t, respectively.
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  • 收稿日期:  2024-04-29
  • 修回日期:  2024-05-27
  • 录用日期:  2024-06-08
  • 网络出版日期:  2024-06-25

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