Room-temperature preparation of MIL-88A as a heterogeneous photo-Fenton catalyst for degradation of rhodamine B and bisphenol a under visible light
Graphical abstract
Introduction
Organic dyes and pharmaceuticals and personal care products (PPCPs) are typical organic pollutants in water pollution, which pose risks to the ecological environment and human health [1,2]. It is reported that organic pollutants, including dyes and PPCPs, widely existed in surface water, ground water, and even drinking water due to their widespread use. Currently, various methods have been applied to the treatment of organic pollutants in water, such as adsorption [3,4], biodegradation [5], photocatalysis [[6], [7], [8]], advanced oxidation processes (AOPs) [[9], [10], [11], [12]] and so on. Among these methods, AOPs is considered to be a promising technology for organic contaminants removal.
Metal-organic frameworks (MOFs), an emerging porous crystalline material constructed from metal and organic linker, with the merits of large surface area and tunable pore size, received widespread attention in many fields, such as sensor, [[13], [14], [15]] gas storage [16,17], gas separation,17,18] adsorption, [[19], [20], [21]] electrochemistry [22], catalysis [23], and photocatalysis [24,25]. Fe-based MOF, as a heterogeneous photo-Fenton materials, has been widely investigated [26]. Liang and coworkers prepared Pd@MIL-100(Fe) to accomplish outstanding photocatalytic activity for PPCPs (theophylline, ibuprofen and bisphenol) degradation with the help of H2O2 [27]. Li and coworkers prepared Fe3O4@MIL-100(Fe) that exhibited excellent removal efficient of diclofenac sodium via adsorption removal and the consequent photocatalytic degradation in the presence of H2O2 [28]. Recently, Fe-based MOFs, such as MIL-100 [29,30], MIL-101 [31,32], MIL-53 [33,34], MIL-88A [35], and MIL-88B [36,37] as visible-light-driven photocatalysts and photo-Fenton catalysts had attracted great attention. Among these Fe-based MOFs, MIL-88A, built from Fe3+ and fumaric acid, was a good candidate for the scale applications because of the low price.
Currently, there are a large number of MOFs being synthesized via solvothermal method [38,39]. However, much concerns should be put on the facile preparation method of MOFs, which can not only reduce energy consumption but also facilitate the development and application of the MOFs [40,41]. In this work, a room-temperature preparation method of MIL-88A was firstly reported, in which the sizes of MIL-88A can be easily controlled by changing the amounts of the reactants. The obtained MIL-88A presented excellent photo-Fenton degradation efficiency towards rhodamine B (RhB) and bisphenol A (BPA) under visible light irradiation. Furthermore, the MIL-88A can be recycled without obvious decrease of the degradation efficiency.
Section snippets
Reagents
Fumaric acid, bisphenol A (BPA) and isopropanol (IPA) was bought from J&K Scientific Ltd. FeCl3·6H2O, ethylenediaminetetraacetic acid (EDTA) and terephthalic acid were bought from Sinopharm. Rhodamine B (RhB) was bought from Beichen Founder Reagent Factory. All the reagents were used directly without further treatment.
Preparation of MIL-88A
10 mmol fumaric acid and 10 mmol FeCl3·6H2O were dissolved in 75 mL ethanol and 75 mL ultrapure water, respectively. The two solutions were mixed, and stirred for 24 h at room
Results and discussions
As reported, Fe3+ can react with fumaric acid to form MIL-88A at high temperature [42]. In our case, MIL-88A can be harvested via the reaction between aqueous solution of FeCl3 and alcohol solution of fumaric acid at room temperature, which was affirmed by the XRD patterns, FTIR spectra and SEM images as illustrated in Fig. 1. It can be seen from Fig. 1a that the XRD characteristic diffraction peaks of the MIL-88A-1 and MIL-88A-2 matched well with those of the simulated one [43,44]. It was
Conclusion
In conclusion, MIL-88A with different sizes was prepared successfully at room temperature. This method is green and facilitates the large-scale synthesis, which is imperative to push forward development of MIL-88A. During the preparation process, water played an important role as water could facilitate the deprotonation of fumaric acid and hydrolysis of iron salt to accelerate crystal nucleation. Both MIL-88A-1 and MIL-88A-2 exhibited excellent photo-Fenton catalytic degradation efficiency
CRediT authorship contribution statement
Huifen Fu: Data curation, Investigation, Visualization, Writing - original draft. Xiao-Xu Song: Data curation, Methodology, Software. Lin Wu: Visualization, Software. Chen Zhao: Validation, Software. Peng Wang: Resources. Chong-Chen Wang: Conceptualization, Funding acquisition, Supervision, Project administration, Writing - review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
This work was supported by the National Natural Science Foundation of China (21806008, 21876008, 51878023, 51578034), Beijing Natural Science Foundation (8202016), Beijing Talent Project (2019A22), Great Wall Scholars Training Program Project of Beijing Municipality Universities (CIT&TCD20180323), Project of Construction of Innovation Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality (IDHT20170508).
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