Zhang Yunxiao, Yan Pengfei, Zhou Yannan, Xu Qun
College of Materials Science & Engineering, Zhengzhou University, Zhengzhou 450052, P. R. China.
Institute of Advanced Technology, Zhengzhou University, Zhengzhou 450052, P. R. China.
Phys Chem Chem Phys. 2022 Nov 18;24(44):27515-27523. doi: 10.1039/d2cp04543e.
Impregnating noble metals in metal-organic frameworks (MOFs) for obtaining effective catalysts for the photocatalytic process is of great significance but remains very challenging. Herein, for the first time, atomically dispersed Pt atoms were successfully impregated inside the MOF UiO-66 with the assistance of supercritical carbon dioxide (SC CO). Our study demonstrated that the SC CO-directed strategy makes Pt undergo a stable encapsulation inside UiO-66, realizing a stage for the rapid transfer of photogenerated electrons between the components of the composite, hence dramatically increasing the catalytic effect. Further, theoretical calculations demonstrated the experimental characterization of the unique structure. Moreover, the as-prepared hybrid structure of Pt@UiO-66 composites presented an extremely high photocatalytic efficiency for hydrogen evolution under visible-light irradiation. An unusual H production rate of 3871.4 μmol h g could be achieved by Pt@UiO-66 under visible-light irradiation. This was nearly 50 times higher than the H-evolution rate achieved by pure UiO-66 under the full spectrum.
将贵金属浸渍在金属有机框架（MOF）中以获得用于光催化过程的有效催化剂具有重要意义，但仍然极具挑战性。在此，首次在超临界二氧化碳（SC CO₂）的辅助下，将原子分散的铂原子成功浸渍到MOF UiO-66内部。我们的研究表明，SC CO₂导向策略使铂在UiO-66内部实现稳定封装，实现了光生电子在复合材料各组分之间快速转移的阶段，从而显著提高了催化效果。此外，理论计算证实了这种独特结构的实验表征。而且，所制备的Pt@UiO-66复合材料的杂化结构在可见光照射下对析氢表现出极高的光催化效率。在可见光照射下，Pt@UiO-66可实现3871.4 μmol h⁻¹ g⁻¹的异常产氢速率。这几乎是纯UiO-66在全光谱下析氢速率的50倍。
