On As(III) Adsorption Characteristics of Innovative Magnetite Graphene Oxide Chitosan Microsphere

Materials (Basel). 2022 Oct 14;15(20):7156. doi: 10.3390/ma15207156.

Abstract

A magnetite graphene oxide chitosan (MGOCS) composite microsphere was specifically prepared to efficiently adsorb As(III) from aqueous solutions. The characterization analysis of BET, XRD, VSM, TG, FTIR, XPS, and SEM-EDS was used to identify the characteristics and adsorption mechanism. Batch experiments were carried out to determine the effects of the operational parameters and to evaluate the adsorption kinetic and equilibrium isotherm. The results show that the MGOCS composite microsphere with a particle size of about 1.5 mm can be prepared by a straightforward method of dropping FeCl2, graphene oxide (GO), and chitosan (CS) mixtures into NaOH solutions and then drying the mixed solutions at 45 °C. The produced MGOCS had a strong thermal stability with a mass loss of <30% below 620 °C. The specific surface area and saturation magnetization of the produced MGOCS was 66.85 m2/g and 24.35 emu/g, respectively. The As(III) adsorption capacity (Qe) and removal efficiency (Re) was only 0.25 mg/g and 5.81% for GOCS, respectively. After 0.08 mol of Fe3O4 modification, more than 53% of As(III) was efficiently removed by the formed MGOCS from aqueous solutions over a wide pH range of 5−10, and this was almost unaffected by temperature. The coexisting ion of PO43− decreased Qe from 3.81 mg/g to 1.32 mg/g, but Mn2+ increased Qe from 3.50 mg/g to 4.19 mg/g. The As(III) adsorption fitted the best to the pseudo-second-order kinetic model, and the maximum Qe was 20.72 mg/g as fitted by the Sips model. After four times regeneration, the Re value of As(III) slightly decreased from 76.2% to 73.8%, and no secondary pollution of Fe happened. Chemisorption is the major mechanism for As(III) adsorption, and As(III) was adsorbed on the surface and interior of the MGOCS, while the adsorbed As(III) was partially oxidized to As(V) accompanied by the reduction of Fe(III) to Fe(II). The produced As(V) was further adsorbed through ligand exchange (by forming Fe−O−As complexes) and electrostatic attraction, enhancing the As(III) removal. As an easily prepared and environmental-friendly composite, MGOCS not only greatly adsorbs As(III) but also effectively removes Cr(VI) and As(V) (Re > 60%) and other metals, showing a great advantage in the treatment of heavy metal-contaminated water.

Keywords: As(III) removal; chitosan; graphene oxide; magnetite.

Grants and funding

This research was funded by the National Natural Science Foundation of China (No. 41877194, No. 42167026), the Natural Science Foundation of Guangxi (2022GXNSFBA035600), Guangxi Education Department (Qiangu Program), Guangxi Key Laboratory of Theory and Technology for Environmental Pollution Control, and Guilin University of Technology Program (GLUTQD 2016047).