Lei Zhen-Dong, Xue Yuan-Cheng, Chen Wen-Qian, Li Lin, Qiu Wen-Hui, Zhang Yong, Tang Liang
School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, P. R. China.
NUS Graduate School for Integrative Sciences & Engineering, National University of Singapore, Singapore, 117583, Singapore.
Small. 2018 Aug;14(35):e1802045. doi: 10.1002/smll.201802045. Epub 2018 Aug 7.
In this research, bulk graphitic carbon nitride (g-C N ) is exfoliated and transferred to the carbon nitride nanosheets (CNNSs), which are then coupled with MIL-88B(Fe) to form the hybrid. From the results of the powder X-ray diffraction, scanning electronic microscopy and thermogravimetric analysis, it is found that the doping of CNNSs on the surface of MIL-88(Fe) could maintain the basic structure of MIL-88B(Fe), and the smaller dimension of CNNSs might influence the crystallization process of metal-organic frameworks (MOFs) compared to bulk g-C N . Besides, the effects of the CNNSs incorporation on photocatalysis are also investigated. Through the photoluminescence spectra, electrochemical measurements, and photocatalytic experiments, the hybrid containing 6% CNNSs is certified to possess the highest catalytic activity to degrade methylene blue and reduce Cr(VI) under visible light. The improvement of the photocatalytic performance can be attributed to the matched energy level which favors the formation of the heterojunctions. Besides, it promotes the charge migration such that the contact between MOFs and CNNSs is more intimate, which can be inferred from the electronic microscopy images. Finally, a possible photocatalytic mechanism is put forward by the relative calculation and the employment of the scavengers to trap the active species.
在本研究中,将块状石墨相氮化碳(g-C₃N₄)剥离并转移至氮化碳纳米片(CNNSs),随后将其与MIL-88B(Fe)耦合以形成杂化物。通过粉末X射线衍射、扫描电子显微镜和热重分析结果发现,CNNSs在MIL-88(Fe)表面的掺杂可维持MIL-88B(Fe)的基本结构,并且与块状g-C₃N₄相比,CNNSs较小的尺寸可能会影响金属有机骨架(MOFs)的结晶过程。此外,还研究了掺入CNNSs对光催化的影响。通过光致发光光谱、电化学测量和光催化实验,证明含6% CNNSs的杂化物在可见光下对降解亚甲基蓝和还原Cr(VI)具有最高的催化活性。光催化性能的提高可归因于匹配的能级,这有利于异质结的形成。此外,它促进了电荷迁移,使得MOFs与CNNSs之间的接触更紧密,这可从电子显微镜图像推断得出。最后,通过相关计算以及使用清除剂捕获活性物种,提出了一种可能的光催化机理。