Alivand Masood S, Tehrani Neda Haj Mohammad Hossein, Askarieh Mojtaba, Ghasemy Ebrahim, Esrafili Mehdi D, Ahmadi Raziyeh, Anisi Hossein, Tavakoli Omid, Rashidi Alimorad
Department of Chemical Engineering, The University of Melbourne, Parkville, Victoria 3010, Australia; School of Chemical Engineering, College of Engineering, University of Tehran, Tehran, Iran.
School of Chemical Engineering, College of Engineering, University of Tehran, Tehran, Iran; Nanotechnology Research Center, Research Institute of Petroleum Industry, Tehran, Iran.
J Hazard Mater. 2021 Aug 15;416:125973. doi: 10.1016/j.jhazmat.2021.125973. Epub 2021 Apr 29.
The emerging environmental issues necessitate the engineering of novel and well-designed nanoadsorbents for advanced separation and purification applications. Despite recent advances, the facile synthesis of hierarchical micro-mesoporous metal-organic frameworks (MOFs) with tuned structures has remained a challenge. Herein, we report a simple defect engineering approach to manipulate the framework, induce mesoporosity, and crease large pore volumes in MIL-101(Cr) by embedding graphene quantum dots (GQDs) during its self-assembly process. For instance, MIL-101@GQD-3 (V: 0.68 and V: 1.87 cm/g) exhibited 300.0% and 53.3% more meso and total pore volume compared to those of the conventional MIL-101 (V: 0.17 and V: 1.22 cm/g), respectively, resulting in 1.7 and 2.8 times greater benzene and toluene loading at 1 bar and 25 °C. In addition, we found that MIL-101@GQD-3 retained its superiority over a wide range of VOC concentrations and operating temperature (25-55 °C) with great cyclic capacity and energy-efficient regeneration. Considering the simplicity of the adopted technique to induce mesoporosity and tune the nanoporous structure of MOFs, the presented GQD incorporation technique is expected to provide a new pathway for the facile synthesis of advanced materials for environmental applications.
新出现的环境问题使得有必要设计新颖且精心设计的纳米吸附剂用于先进的分离和纯化应用。尽管最近取得了进展，但具有可调结构的分级微介孔金属有机框架（MOF）的简便合成仍然是一个挑战。在此，我们报告了一种简单的缺陷工程方法，通过在MIL-101（Cr）的自组装过程中嵌入石墨烯量子点（GQD）来操纵框架、诱导介孔并增加大孔体积。例如，与传统的MIL-101（V：0.17和V：1.22 cm/g）相比，MIL-101@GQD-3（V：0.68和V：1.87 cm/g）的介孔体积和总孔体积分别增加了300.0%和53.3%，在1 bar和25°C下苯和甲苯的负载量分别提高了1.7倍和2.8倍。此外，我们发现MIL-101@GQD-3在很宽的VOC浓度范围和操作温度（25-55°C）内都保持其优势，具有出色的循环容量和节能再生性能。考虑到所采用的诱导介孔和调节MOF纳米孔结构技术的简便性，所提出的GQD掺入技术有望为简便合成用于环境应用的先进材料提供一条新途径。
