Defect engineering-induced porosity in graphene quantum dots embedded metal-organic frameworks for enhanced benzene and toluene adsorption

Masood S Alivand; Neda Haj Mohammad Hossein Tehrani; Mojtaba Askarieh; Ebrahim Ghasemy; Mehdi D Esrafili; Raziyeh Ahmadi; Hossein Anisi; Omid Tavakoli; Alimorad Rashidi

doi:10.1016/j.jhazmat.2021.125973

Defect engineering-induced porosity in graphene quantum dots embedded metal-organic frameworks for enhanced benzene and toluene adsorption

J Hazard Mater. 2021 Aug 15:416:125973. doi: 10.1016/j.jhazmat.2021.125973. Epub 2021 Apr 29.

Authors

Masood S Alivand¹, Neda Haj Mohammad Hossein Tehrani², Mojtaba Askarieh³, Ebrahim Ghasemy⁴, Mehdi D Esrafili⁵, Raziyeh Ahmadi³, Hossein Anisi⁶, Omid Tavakoli⁷, Alimorad Rashidi⁸

Affiliations

¹ Department of Chemical Engineering, The University of Melbourne, Parkville, Victoria 3010, Australia; School of Chemical Engineering, College of Engineering, University of Tehran, Tehran, Iran.
² School of Chemical Engineering, College of Engineering, University of Tehran, Tehran, Iran; Nanotechnology Research Center, Research Institute of Petroleum Industry, Tehran, Iran.
³ Nanotechnology Research Center, Research Institute of Petroleum Industry, Tehran, Iran.
⁴ Centre Énergie Matériaux Télécommunications, Institut National De La Recherché, Varennes, Quebec, Canada.
⁵ Department of Chemistry, Faculty of Basic Sciences, University of Maragheh, Maragheh, Iran.
⁶ School of Chemical, Petroleum and Gas Engineering, Iran University of Science and Technology, Tehran, Iran.
⁷ School of Chemical Engineering, College of Engineering, University of Tehran, Tehran, Iran. Electronic address: otavakoli@ut.ac.ir.
⁸ Nanotechnology Research Center, Research Institute of Petroleum Industry, Tehran, Iran. Electronic address: rashidim@ripi.ir.

PMID: 34492882
DOI: 10.1016/j.jhazmat.2021.125973

Abstract

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_meso: 0.68 and V_tot: 1.87 cm³/g) exhibited 300.0% and 53.3% more meso and total pore volume compared to those of the conventional MIL-101 (V_meso: 0.17 and V_tot: 1.22 cm³/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.

Keywords: Benzene; Graphene quantum dot (GQD); Hierarchical micro-mesoporous MIL-101(Cr); Toluene; Volatile organic compounds (VOC).