Jiang Zhifeng, Wei Wei, Mao Danjun, Chen Cheng, Shi Yunfei, Lv Xiaomeng, Xie Jimin
School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang, 212013, P.R. China.
Nanoscale. 2015 Jan 14;7(2):784-97. doi: 10.1039/c4nr05963h.
Silver-loaded nitrogen-doped yolk-shell mesoporous TiO2 hollow microspheres (Ag-N-TiO2-YSM) were prepared by employing acetic acid as the hollowing controller and triethanolamine as the N source for the first time. Ag nanoparticles (NPs) were uniformly deposited by a simple in situ photo-reduction method, which can prevent the aggregation of Ag NPs. The efficiency of the as-prepared samples was investigated by monitoring the degradation of rhodamine B and ciprofloxacin under visible light irradiation. The experimental results indicate that N-doped yolk-shell mesoporous TiO2 hollow microspheres show higher photocatalytic activity than P25 TiO2 under visible light irradiation because of N doping and the unique yolk-shell structure. In addition, Ag-N-TiO2-YSM shows enhanced activity compared with N-TiO2-YSM due to the SPR absorption of silver NPs and the fast generation, separation and transportation of the photogenerated carriers. Moreover, the Ag contents can affect the photocatalytic activity of the Ag-N-TiO2-YSM composite. A suitable amount of Ag deposition gives the highest photocatalytic activity. A higher loading does not improve the photocatalytic activity of N-TiO2-YSM further. The active species generated in the photocatalytic system were also investigated. Based on our experimental results, a possible photocatalytic mechanism was proposed. The strategy presented here gives a promising route towards the development of delicate metal@hollow semiconductor composites for many applications in photocatalysis.
首次以乙酸作为中空控制剂、三乙醇胺作为氮源制备了负载银的氮掺杂蛋黄壳介孔TiO₂空心微球(Ag-N-TiO₂-YSM)。通过简单的原位光还原法将银纳米颗粒(NPs)均匀沉积,该方法可防止银纳米颗粒聚集。通过监测罗丹明B和环丙沙星在可见光照射下的降解来研究所制备样品的效率。实验结果表明,由于氮掺杂和独特的蛋黄壳结构,氮掺杂蛋黄壳介孔TiO₂空心微球在可见光照射下比P25 TiO₂表现出更高的光催化活性。此外,由于银纳米颗粒的表面等离子体共振吸收以及光生载流子的快速产生、分离和传输,Ag-N-TiO₂-YSM与N-TiO₂-YSM相比活性增强。而且,银含量会影响Ag-N-TiO₂-YSM复合材料的光催化活性。适量的银沉积具有最高的光催化活性。更高的负载量并不能进一步提高N-TiO₂-YSM的光催化活性。还研究了光催化体系中产生的活性物种。基于我们的实验结果,提出了一种可能的光催化机理。这里提出的策略为开发用于光催化许多应用的精细金属@中空半导体复合材料提供了一条有前景的途径。