National Engineering Laboratory for Reducing Emissions from Coal Combustion, Engineering Research Center of Environmental Thermal Technology of Ministry of Education, Shandong Key Laboratory of Energy Carbon Reduction and Resource Utilization, School of Energy and Power Engineering, Shandong University, Jinan, Shandong 250061, PR China.
National Engineering Laboratory for Reducing Emissions from Coal Combustion, Engineering Research Center of Environmental Thermal Technology of Ministry of Education, Shandong Key Laboratory of Energy Carbon Reduction and Resource Utilization, School of Energy and Power Engineering, Shandong University, Jinan, Shandong 250061, PR China.
Sci Total Environ. 2021 Nov 1;793:148622. doi: 10.1016/j.scitotenv.2021.148622. Epub 2021 Jun 22.
In light of the promising merits of large surface area, uniform pore size, and tunable functional groups, metal-organic frameworks (MOFs) have great potential to be utilized for adsorbing volatile organic compounds (VOCs). In this study, three Fe-based MOFs, MIL-100(Fe), MIL-101(Fe), and MIL-53(Fe), were synthesized systematically and used to adsorb a typical VOC, toluene. Static adsorption, dynamic breakthrough curves, and adsorption kinetics were conducted to assess the adsorption performance. Additionally, the surface functional groups, pore structure, and morphology were systematically characterized by means of XRD, SEM, XPS, FTIR and N adsorption-desorption analyses to reveal the cause of the difference in adsorption of these Fe-based MOFs. The results revealed that the maximum equilibrium adsorption capacity of 663 mg/g was achieved by MIL-100(Fe) with the highest specific surface area and pore volume. The dynamic adsorption of toluene on MIL-100(Fe) was in accordance with the pseudo-first order kinetic model and the Langmuir isothermal model. The formed π-π stacking interaction between organic ligands and the benzene ring in the MIL-100(Fe) cluster is the primary adsorption mechanism based on XPS analysis. Moreover, MIL-100(Fe) was easily regenerated via microwave irradiation with a negligible adsorption capacity decrease after three cycles. This work highlights the feasibility of hierarchical porous Fe-based MOFs as toluene adsorbents and promotes the application of MOFs in the field of pollution control.
鉴于大比表面积、均匀孔径和可调官能团的优异特性,金属有机骨架(MOFs)在吸附挥发性有机化合物(VOCs)方面具有很大的应用潜力。在这项研究中,系统地合成了三种基于 Fe 的 MOFs,即 MIL-100(Fe)、MIL-101(Fe) 和 MIL-53(Fe),并将其用于吸附一种典型的 VOC,即甲苯。通过静态吸附、动态穿透曲线和吸附动力学评估了吸附性能。此外,通过 XRD、SEM、XPS、FTIR 和 N2 吸附-解吸分析对表面官能团、孔结构和形貌进行了系统的表征,以揭示这些基于 Fe 的 MOFs 吸附差异的原因。结果表明,MIL-100(Fe)的最大平衡吸附容量为 663mg/g,具有最高的比表面积和孔体积。甲苯在 MIL-100(Fe)上的动态吸附符合伪一级动力学模型和 Langmuir 等温模型。基于 XPS 分析,有机配体与 MIL-100(Fe) 团簇中苯环之间形成的π-π堆积相互作用是主要的吸附机制。此外,MIL-100(Fe) 可以通过微波辐射轻松再生,经过三个循环后,吸附容量几乎没有下降。这项工作突出了分级多孔 Fe 基 MOFs 作为甲苯吸附剂的可行性,并促进了 MOFs 在污染控制领域的应用。