Abstract
Three-dimensional carbon-based porous materials have proven to be quite useful for tailoring material properties in the energy conservation and environmental protection applications. In view of the three-dimensional and well-defined structure of metal–organic frameworks (MOFs), a novel carbon-based magnetic porous material (HKUST–Fe3O4) has been designed and constructed by MOF–guest interactions of high-temperature pyrolysis. The obtained HKUST–Fe3O4 exhibited the unique features of superparamagnetism, a macro/mesoporous structure, environmental protection (inexistence of toxic heavy metal ions), and physicochemical stability and has shown high adsorption capacity and rapid adsorption for carcinogenic organic pollutants (for example, rhodamine B) with an environmentally friendly character and excellent reusability. We demonstrate that the unique/superior advantages of HKUST–Fe3O4 could meet the requirements of environment cleaning, especially for removing the targeted organic pollutant from water. Moreover, the specific HKUST–Fe3O4 and organic pollutant interaction mechanism has been analyzed in detail via parameter-free calculations. This study proposes a promising strategy for constructing novel carbon-based magnetic nanomaterials for various applications, not limitated to pollutant removal.
Highlights
Water resources are more polluted by organic pollutants and many people have to face the problem of absolute water scarcity, especially the long-term residents in developing countries.[1−5] water reuse is becoming extraordinarily important and effective materials are needed to be produced and applied to sustainable wastewater treatment and for efficient water use, for populations with limited resources and/or those living in remote areas.[6,7]
As for the adsorption capacity, many works have been focused on the adjustment of central metal ions and organic ligands to improve the pore size and increase the binding sites.[18−20] no matter how magnificent the diversity of Metal− organic frameworks (MOFs) is, it is impossible to avoid the existence of toxic metals ion despite their relative stability in the frameworks of MOFs.[21,22]
As shown in Scheme 1, HKUST was first synthesized under the self-assembly of a central metal ion (Cu2+) and an organic ligand by a hydrothermal reaction
Summary
Water resources are more polluted by organic pollutants and many people have to face the problem of absolute water scarcity, especially the long-term residents in developing countries.[1−5] water reuse is becoming extraordinarily important and effective materials are needed to be produced and applied to sustainable wastewater treatment and for efficient water use, for populations with limited resources and/or those living in remote areas.[6,7] Metal− organic frameworks (MOFs) are the emerging three-dimensional (3D) and well-defined materials.[8−10] Due to their highly porous and flexible structure, MOFs have been widely used as adsorbents to remove the organic pollutants in the liquid-phase separations for environmental cleaning/water purification.[11−15] Recently, tremendous efforts have been taken to improve the adsorption capacity and separation efficiency of organic pollutants by MOFs via different approaches.[16,17] For example, as for the adsorption capacity, many works have been focused on the adjustment of central metal ions and organic ligands to improve the pore size and increase the binding sites.[18−20] no matter how magnificent the diversity of MOFs is, it is impossible to avoid the existence of toxic metals ion despite their relative stability in the frameworks of MOFs.[21,22] when the separation environment of pollutants is complex, there are threats of toxic metal leakage due to the spontaneous disintegration of MOFs.[23]. Article exploitation of magnetic metal ion-based MOFs has not involved any complex procedure, these MOFs could not debarb the disintegration and toxicity absolutely.[35] Despite having achieved enormous progress on applications of MOFs so far, it remains a great challenge to exploit MOF-based absorbents with low/no toxicity (environmentally friendly character) and magnetic property, especially with high adsorption capacity, superior chemical stability, and excellent reusability. We present a facile approach to transform a common MOF (i.e., HKUST) into a carbon-based magnetic porous material (namely, HKUST−Fe3O4) with an abundant macro/ mesoporous structure via a simple high-temperature treatment (pyrolysis followed by washing) Since this strategy is developed based on guest impregnation of the precursors of magnetic Fe3O4 (FeCl3 solution) rather than chemical functionalization or cladding of magnetic Fe3O4 nanoparticles, HKUST−Fe3O4 has shown high adsorption capacity and rapid adsorption for RhB with an environmentally friendly character and excellent reusability. The parameter-free calculations have been utilized to reveal the adsorption mechanism
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