Abstract

In this study, a graphene oxide metal–organic framework (MIL-53(Fe)/GO) composite adsorbent was successfully synthesized using a simple method at room temperature. The specific surface area of the synthesized MIL-53(Fe)/GO nanoparticles was 268.43 m2 g−1, with an average pore size of 2.52 nm. The Box–Behnken response surface method was applied to optimize the adsorption time, dosage, pH, temperature, and initial concentration of Sb(iii) in the MIL-53(Fe)/GO adsorption treatment employed for synthetic wastewater containing Sb(iii). We determined the optimal adsorption conditions and explored the isotherm model, adsorption kinetic model, and adsorption mechanism during the adsorption process. For an optimal adsorption of Sb(iii) by MIL-53(Fe)/GO, the adsorption time, dosage, pH, temperature, and initial Sb(iii) concentration should be set to 4.86 h, 85.79 mg L−1, 10.00, 39.29 °C, and 10.09 mg L−1, respectively. Under these optimal conditions, the removal rate of Sb(iii) will be as high as 97.97%. The adsorption of Sb(iii) by MIL-53(Fe)/GO conformed to the Freundlich isotherm adsorption model, and its maximum adsorption capacity was 69.014 mg g−1. The adsorption kinetics process, which is a nonhomogeneous reaction, could be fitted using a quasi-first-order kinetic model. A Fourier transform infrared spectroscopy analysis showed that MIL-53(Fe)/GO hydroxyl and amine groups play a vital role in the adsorption process. MIL-53(Fe)/GO did not exhibit any changes in its adsorption efficiency in the presence of its anion and showed high specificity to Sb(iii). XPS characterization showed that Sb successfully adsorbed onto the adsorbent and that no oxidation–reduction reaction occurred during the adsorption process. The adsorption efficiency remained high even after four cycles of use. MIL-53(Fe)/GO is highly recyclable with significant application potential for treating wastewater containing Sb(iii).

Highlights

  • Antimony and its compounds are widely used as ame retardants, polymerization catalysts, and pigments; it is highly toxic

  • A total of 46 runs were undertaken for optimizing the three individual parameters in the BBD; the experimental conditions based on the factorial design are shown in Electronic supplementary information (ESI) 1.† The results show that the Sb(III) removal rate varied in the range of 65.82– 97.03%

  • The response surface optimization experiments showed that the dosage, pH, temperature, and initial concentration of Sb(III) signi cantly affect the adsorption of Sb(III) by MIL-53(Fe)/GO

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Summary

Introduction

Antimony and its compounds are widely used as ame retardants, polymerization catalysts, and pigments; it is highly toxic. The toxicity of Sb(III) is approximately 10 times that of Sb(V),[1,2] and long-term exposure to antimony can cause pneumoconiosis, emphysema, and myocardial degeneration.[3] Severe damage to human DNA4 can cause damage to the lungs, heart, and liver, increasing the risk of cancer.[5,6] the European Union, the U.S Environmental Protection Agency, and other organizations have listed antimony as a pollutant.[7] China has one of the largest antimony mines in the world. Antimony is being mined in large quantities, and its usage is increasing year by year. From the initial 20 000 tons, China surpassed the United States, Japan, and other countries in 2004, becoming the world's largest consumer of antimony

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