Room-temperature preparation of MIL-88A as a heterogeneous photo-Fenton catalyst for degradation of rhodamine B and bisphenol a under visible light

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Highlights

  • MIL-88A, as a visible-light-driven photo-Fenton catalyst, was prepared successfully at room temperature.

  • The size of the MIL-88A can be tuned by controlling the concentrations of reactants.

  • The role of water played in the room-temperature preparation process was discussed.

  • The as-prepared MIL-88A exhibited excellent photo-Fenton catalytic performance toward RhB and BPA.

  • The main active specie, degradation mechanism and BPA degradation pathway were proposed.

Abstract

MIL-88A, a Fe-based MOF, with different sizes was prepared successfully at room-temperature, which was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR) and UV–vis diffuse reflectance spectroscopy (UV–vis DRS). Water played an important role in the room-temperature synthesis as water could facilitate the deprotonation of fumaric acid and hydrolysis of iron salt to accelerate crystal nucleation, and this room-temperature preparation is beneficial to the large-scale synthesis and is imperative to push forward the development of the MIL-88A. The as-prepared MIL-88A exhibited excellent photo-Fenton catalytic performance towards rhodamine B and bisphenol A removal under visible light irradiation (LED). The main active specie was investigated, the degradation mechanism and BPA degradation pathway were proposed. Furthermore, the as-prepared MIL-88A displayed good reusability, and there was no obvious decline of degradation performance after five cycles.

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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