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3D花状MoS2/O-g-C3N4 Z型异质结增强光催化剂降解BPA

张家晶 郑永杰 荆涛 赵云鹏 杨万丽

张家晶, 郑永杰, 荆涛, 等. 3D花状MoS2/O-g-C3N4 Z型异质结增强光催化剂降解BPA[J]. 复合材料学报, 2021, 39(0): 1-14
引用本文: 张家晶, 郑永杰, 荆涛, 等. 3D花状MoS2/O-g-C3N4 Z型异质结增强光催化剂降解BPA[J]. 复合材料学报, 2021, 39(0): 1-14
Jiajing ZHANG, Yongjie ZHENG, Tao JING, Yunpeng ZHAO, Wanli YANG. 3D flower-shaped MoS2/O-g-C3N4 Z-type heterojunction enhances the photocatalyst degradation of BPA[J]. Acta Materiae Compositae Sinica.
Citation: Jiajing ZHANG, Yongjie ZHENG, Tao JING, Yunpeng ZHAO, Wanli YANG. 3D flower-shaped MoS2/O-g-C3N4 Z-type heterojunction enhances the photocatalyst degradation of BPA[J]. Acta Materiae Compositae Sinica.

3D花状MoS2/O-g-C3N4 Z型异质结增强光催化剂降解BPA

基金项目: 黑龙江省教育厅基本业务项目(135309109);黑龙江省教育厅基本业务项目(135209226);国家自然科学基金面上项目(52172092)
详细信息
    通讯作者:

    郑永杰,博士研究生,教授,硕士生导师,研究方向为材料制备与环境治理 E-mail: zyj1964@163.com

  • 中图分类号: O643.36; O644.1

3D flower-shaped MoS2/O-g-C3N4 Z-type heterojunction enhances the photocatalyst degradation of BPA

  • 摘要: 光催化降解是一种很有应用前景的污染物处理方法。采用溶剂热法制备了3D/2D二硫化钼负载氧掺杂石墨相氮化碳(MoS2/O-g-C3N4)复合材料,通过XRD、XPS、SEM、TEM、FTIR和PL等表征了MoS2与O-g-C3N4之间Z型异质结的成功构建。在模拟太阳光下,当MoS2的负载量为0.2wt%时,MoS2/O-g-C3N4的光催化活性最高,双酚A(BPA)的降解率为92.6%,是纯g-C3N4的7倍。此外,MoS2和O-g-C3N4之间界面的紧密接触和相互的协同效应,显著增强了光催化反应活性位点和可见光吸收能力,有效提高了光生载流子的分离。根据液相质谱联用仪(LC-MS)和自由基捕获实验,提出了0.2%MoS2/O-g-C3N4异质结复合材料降解BPA可能的光催化降解机制。本研究为制备高效异质结光催化剂提供了新的方法。

     

  • 图  1  (a) g-C3N4、O-g-C3N4、MoS2X% MoS2/O-g-C3N4的XRD图(插图为g-C3N4和O-g-C3N4的放大图);(b) g-C3N4、(c) O-g-C3N4和(d) 0.2% MoS2/O-g-C3N4的TEM图

    Figure  1.  (a) XRD patterns of g-C3N4, O-g-C3N4, MoS2 and X% MoS2/O-g-C3N4 (The illustration is an enlarged view of g-C3N4 and O-g-C3N4); TEM images of g-C3N4 (b) O-g-C3N4 (c) and 0.2% MoS2/O-g-C3N4(d)

    图  2  (a)0.2% MoS2/O-g-C3N4的XPS全谱;(b)为g-C3N4、O-g-C3N4、MoS2和0.2% MoS2/O-g-C3N4的C1s谱;(c)为O-g-C3N4和0.2% MoS2/O-g-C3N4的N1s谱;(d)为g-C3N4、O-g-C3N4和0.2% MoS2/O-g-C3N4的O1s谱、(e)为MoS2和0.2% MoS2/O-g-C3N4的Mo3d谱;(f)为MoS2和0.2% MoS2/O-g-C3N4的S2p谱

    Figure  2.  (a) XPS survey of 0.2% MoS2/O-g-C3N4; (b) C1s spectrum of g-C3N4, O-g-C3N4, MoS2 and 0.2% MoS2/O-g-C3N4; (c) N1s spectrum of O-g-C3N4 and 0.2% MoS2/O-g-C3N4; (d) O1s spectrum of g-C3N4, O-g-C3N4 and 0.2% MoS2/O-g-C3N4; (e) Mo3d spectrum of MoS2 and 0.2% MoS2/O-g-C3N4; (f) S2p spectrum of MoS2 and 0.2% MoS2/O-g-C3N4

    图  3  (a) g-C3N4、(b) O-g-C3N4、(c) MoS2、(d) 0.2% MoS2/O-g-C3N4的SEM图;(e) 0.2% MoS2/O-g-C3N4的元素分布图

    Figure  3.  SEM images of (a) g-C3N4; (b) O-g-C3N4; (c) MoS2; (d) 0.2% MoS2/O-g-C3N4; (e) Element mapping images of 0.2% MoS2/O-g-C3N4

    图  4  (a) g-C3N4、O-g-C3N4和0.2% MoS2/O-g-C3N4的氮气吸附脱附图;(b) g-C3N4、O-g-C3N4、MoS2和0.2% MoS2/O-g-C3N4的FTIR图

    Figure  4.  (a) N2 adsorption–desorption isotherms of g-C3N4, O-g-C3N4 and 0.2% MoS2/O-g-C3N4; (b) FT-IR spectra of g-C3N4, O-g-C3N4, MoS2 and 0.2% MoS2/O-g-C3N4

    图  5  (a) g-C3N4、O-g-C3N4和X% MoS2/O-g-C3N4的UV–vis DRS光谱图;(b) O-g-C3N4、MoS2和0.2% MoS2/O-g-C3N4的(αhv)1/2hv曲线;(c) g-C3N4、O-g-C3N4和0.2% MoS2/O-g-C3N4的PL光谱图;(d) g-C3N4、O-g-C3N4和0.2% MoS2/O-g-C3N4的电化学阻抗图

    Figure  5.  (a) UV–vis DRS spectra of g-C3N4, O-g-C3N4 and 0.2% MoS2/O-g-C3N4; (b) the plots of (αhv)1/2versus band-gap energy (hv) of O-g-C3N4, MoS2 and 0.2% MoS2/O-g-C3N4; (c) PL spectra of g-C3N4, O-g-C3N4 and 0.2% MoS2/O-g-C3N4; (d) Nyquist plots of EIS of g-C3N4, O-g-C3N4 and 0.2% MoS2/O-g-C3N4

    图  6  (a) g-C3N4、O-g-C3N4、MoS2X% MoS2/O-g-C3N4的光催化降解图;(b) g-C3N4、O-g-C3N4、MoS2X% MoS2/O-g-C3N4的降解动力学曲线;(c) 0.2% MoS2/O-g-C3N4催化剂循环实验;(d) 0.2% MoS2/O-g-C3N4循环前后的XRD图;(e) 0.2% MoS2/O-g-C3N4循环前后的FTIR图

    Figure  6.  Photocatalytic degradation diagrams of g-C3N4, O-g-C3N4, MoS2 and X% MoS2/O-g-C3N4; (b) degradation kinetic curve of g-C3N4, O-g-C3N4, MoS2 and X% MoS2/O-g-C3N4; (c) 0.2% MoS2/O-g-C3N4 catalyst cycle test; (d) XRD patterns before and after cycles of 0.2% MoS2/O-g-C3N4; (e) FTIR patterns before and after cycles of 0.2% MoS2/O-g-C3N4

    C—BPA concentration after t time; C0—BPA concentration at the initial time

    图  7  0.2% MoS2/O-g-C3N4复合材料BPA可能的降解途径

    Figure  7.  Possible degradation pathway of BPA under 0.2% MoS2/O-g-C3N4 system

    图  8  不同自由基捕获剂对BPA光降解速率的影响

    Figure  8.  Effect on photo-degradation rate of BPA with different radical scavengers

    BQ—benzoquinone;EDTA-2Na—Ethylenediaminetetraacetic acid disodium salt;IPA—isopropanol;KBrO3—Potassium bromate

    图  9  0.2% MoS2/O-g-C3N4对BPA降解机制图的推断

    Figure  9.  Proposed mechanism of the photocatalytic photodegradation of BPA on 0.2% MoS2/O-g-C3N4

    表  1  g-C3N4、O-g-C3N4和0.2% MoS2/O-g-C3N4的质构特性

    Table  1.   Textural properties of g-C3N4, O-g-C3N4 and 0.2% MoS2/O-g-C3N4

    SamplesSBET/(m2·g−1)Pore size/nm
    g-C3N414.940.092
    O-g-C3N448.280.313
    0.2% MoS2/O-g-C3N439.890.228
    Notes:SBET—specific surface area
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  • 收稿日期:  2021-10-08
  • 录用日期:  2021-11-19
  • 修回日期:  2021-11-10
  • 网络出版日期:  2021-12-31

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