无模板合成磁性核壳Fe3O4@MoS2@介孔TiO2光催化剂及其在废水处理中的应用

袁静舒; 张瑶; 张笑妍; 赵亮; 沈汉林; 张深根

doi:10.1007/s12613-022-2473-9

Volume 30 Issue 1

Jan. 2023

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文章导航 > 矿物冶金与材料学报（英文） > 2023 > 30(1): 177-191

Jingshu Yuan, Yao Zhang, Xiaoyan Zhang, Liang Zhao, Hanlin Shen, and Shengen Zhang, Template-free synthesis of core–shell Fe₃O₄@MoS₂@mesoporous TiO₂ magnetic photocatalyst for wastewater treatment, Int. J. Miner. Metall. Mater., 30(2023), No. 1, pp. 177-191. https://doi.org/10.1007/s12613-022-2473-9

Cite this article as:

Jingshu Yuan, Yao Zhang, Xiaoyan Zhang, Liang Zhao, Hanlin Shen, and Shengen Zhang, Template-free synthesis of core–shell Fe3O4@MoS2@mesoporous TiO2 magnetic photocatalyst for wastewater treatment, Int. J. Miner. Metall. Mater., 30(2023), No. 1, pp. 177-191. https://doi.org/10.1007/s12613-022-2473-9

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研究论文

无模板合成磁性核壳Fe₃O₄@MoS₂@介孔TiO₂光催化剂及其在废水处理中的应用

1)
北京科技大学新材料技术研究院，北京 100083，中国
2)
西安翻译学院，西安 710105，中国
3)
密歇根州立大学土木与环境工程系，东兰辛 MI 48824，美国

* 共同第一作者

通讯作者:
张深根 E-mail: zhangshengen@mater.ustb.edu.cn

文章亮点

(1) 提出了一种简单、绿色、无模板的方法用于制备磁性核壳FMmT光催化剂。

(2) 首次引入MoS₂活性中间层以避免Fe₃O₄@TiO₂发生光致解离。

(3) TiO₂壳层的介孔网络结构可有效提高FMmT的光催化活性。

中文摘要

二氧化钛(TiO₂)光催化剂在环境修复领域被重点关注和广泛研究。然而，仅响应紫外光(<5%的太阳光)、光生电荷分离效率低和回收困难等缺点严重阻碍了其实际应用。本文通过结合简单、绿色、无模板的溶剂热法和超声水解法制备出可磁分离的Fe₃O₄@MoS₂@介孔TiO₂ (FMmT)光催化剂。研究发现，FMmT具有更大的比表面积(55.09 m²·g⁻¹)，更强的可见光响应能力(~521 nm)以及更高的光生电荷分离效率。此外，光照300 min后，FMmT对亚甲基蓝(MB)、罗丹明B(RhB)和四环素(TC)的光催化降解效率分别为99.4%、98.5%和89.3%，相应的降解速率常数分别是纯TiO₂的4.5、4.3和3.1倍。由于具有高饱和磁化强度(43.1 A·m²·kg⁻¹)，FMmT可在外加磁场作用下实现有效回收。光催化活性的提高与活性中间层(MoS₂)对光生电子的有效传输以及异质结(MoS₂@TiO₂)对电子–空穴的高效分离密切相关。同时，介孔TiO₂壳层优异的光捕集能力和丰富的反应位点可使FMmT的光催化效率得到进一步提高。本工作首次提出将MoS₂作为活性中间层，并将其与介孔TiO₂壳层相结合，为磁性光催化剂的设计和性能优化提供了新方法和实验依据。

关键词:

Research Article

Template-free synthesis of core–shell Fe₃O₄@MoS₂@mesoporous TiO₂ magnetic photocatalyst for wastewater treatment

+ Author Affiliations

Abstract

Abstract

TiO₂ is the dominant and most widely researched photocatalyst for environmental remediation, however, the drawbacks, such as only responding to UV light (<5% of sunlight), low charge separation efficiency, and difficulties in recycling, have severely hindered its practical application. Herein, we synthesized magnetically separable Fe₃O₄@MoS₂@mesoporous TiO₂ (FMmT) photocatalysts via a simple, green, and template-free solvothermal method combined with ultrasonic hydrolysis. It is found that FMmT possesses a high specific surface area (55.09 m²·g⁻¹), enhanced visible-light responsiveness (~521 nm), and remarkable photogenerated charge separation efficiency. In addition, the photocatalytic degradation efficiencies of FMmT for methylene blue (MB), rhodamine B (RhB), and tetracycline (TC) are 99.4%, 98.5%, and 89.3% within 300 min, respectively. The corresponding degradation rates are 4.5, 4.3, and 3.1 times higher than those of pure TiO₂ separately. Owing to the high saturation magnetization (43.1 A·m²·kg⁻¹), FMmT can achieve effective recycling with an applied magnetic field. The improved photocatalytic activity is closely related to the effective transport of photogenerated electrons by the active interlayer MoS₂ and the electron–hole separation caused by the MoS₂@TiO₂ heterojunction. Meanwhile, the excellent light-harvesting ability and abundant reactive sites of the mesoporous TiO₂ shell further boost the photocatalytic efficiency of FMmT. This work provides a new approach and some experimental basis for the design and performance improvement of magnetic photocatalysts by innovatively incorporating MoS₂ as the active interlayer and integrating it with a mesoporous shell.
- core–shell;
- MoS₂;
- mesoporous TiO₂;
- photocatalytic degradation;
- heterojunction;
- magnetic recycling

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