Departamento de Química, Facultad de Ciencias Exactas y Naturales (FCEyN), Universidad Nacional de Mar del Plata (UNMdP) , 7600 Mar del Plata, Argentina.
Instituto de Física de Mar del Plata (IFIMAR), FCEyN, UNMdP - CONICET , 7600 Mar del Plata, Argentina.
ACS Appl Mater Interfaces. 2017 Jul 12;9(27):22941-22949. doi: 10.1021/acsami.7b04745. Epub 2017 Jun 27.
Photocatalytically active composites comprising potassium poly(heptazine imide) (PHIK) and a Ti-based metal-organic framework (MOF, MIL-125-NH) are prepared in situ by simply dispersing both materials in water. The driving forces of composite formation are the electrostatic interactions between the solids and the diffusion of potassium ions from PHIK to MIL-125-NH. This mechanism implies that other composites of poly(heptazine imide) salts and different MOFs bearing positive surface charge can potentially be obtained in a similar fashion. The suggested strategy thus opens a new avenue for the facile synthesis of such materials. The composites are shown to have a superior photocatalytic activity in Rhodamine B degradation under blue light irradiation. The reaction rate is doubled compared to that of pure MOF compound and is 7 times higher than the activity of the pristine PHIK. The results of the electron paramagnetic resonance (EPR) investigations and the analysis of the electronic structures of the solids suggest the electron transfer from MIL-125-NH to PHIK in the composite. The possible pathways for the dye degradation and the rationalization of the increased activity of the composites are elaborated.
由钾聚(六嗪亚胺)(PHIK)和基于钛的金属-有机骨架(MOF,MIL-125-NH)组成的光催化活性复合材料通过简单地将两种材料分散在水中原位制备。复合材料形成的驱动力是固体之间的静电相互作用以及钾离子从 PHIK 扩散到 MIL-125-NH。该机制意味着其他带有正表面电荷的聚(六嗪亚胺)盐和不同 MOF 的复合材料可以以类似的方式潜在获得。因此,所提出的策略为这些材料的简便合成开辟了新途径。在蓝光照射下,罗丹明 B 降解中显示出复合材料具有优异的光催化活性。与纯 MOF 化合物相比,反应速率提高了一倍,比原始 PHIK 的活性高 7 倍。电子顺磁共振(EPR)研究的结果和对固体电子结构的分析表明,在复合材料中存在从 MIL-125-NH 到 PHIK 的电子转移。阐述了染料降解的可能途径和复合材料活性提高的合理化。