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Electrosorption of Hexavalent Chromium Ions by MnO2/Carbon Fiber Composite Electrode - Analysis and Optimization of the Process by Box-Behnken Design

MetadataDetails
Publication Date2023-03-29
JournalIraqi Journal of Chemical and Petroleum Engineering
AuthorsZainab M. Issa, Rasha H. Salman, Prashant Basavaraj Bhagawati
InstitutionsUniversity of Baghdad
AnalysisFull AI Review Included

This study successfully synthesized and optimized a high-performance Manganese Dioxide/Carbon Fiber (MnO2/CF) composite electrode for the electrosorptive removal of hexavalent chromium (Cr(VI)) ions from aqueous solutions.

  • High Efficiency: The electrode achieved a maximum Cr(VI) removal efficiency of 99.99% from a 100 ppm solution under optimized conditions.
  • High Capacity: The corresponding equilibrium adsorption capacity (qe) was determined to be 129.02 mg/g, demonstrating superior performance for heavy metal remediation.
  • Optimized Conditions: The optimal operating parameters, determined using the Box-Behnken Design (BBD), were a cell voltage of 4.6 V, a pH of 2, and a NaCl concentration of 1.5 g/L.
  • Synthesis Method: The MnO2 nanostructures were synthesized via a simple, galvanostatic anodic electrodeposition process onto activated carbon fiber (CF) at 0.3 mA/cm2.
  • Material Structure: FESEM confirmed the formation of rod-like, nanostructured gamma-MnO2 (Îł-MnO2) particles, approximately 35.11 nm in diameter, which provide short diffusion channels and high surface area for enhanced electrosorption kinetics.
  • Mechanism: The high removal rate (equilibrium reached in 3 hours) is attributed to the electrode’s faradic-capacitive behavior, combining electrostatic adsorption (CDI) with redox reactions involving MnO2.
ParameterValueUnitContext
Electrode TypeMnO2/CF Composite-Working Electrode (Anode)
Synthesis MethodAnodic Electrodeposition-Galvanostatic, 4 hours
Synthesis Current Density0.3mA/cm2Applied during deposition
Synthesis Temperature90°CSolution temperature
Initial Cr(VI) Concentration100mg/LElectrosorption test concentration
Optimal pH (X1)2-Determined by BBD optimization
Optimal Cell Voltage (X3)4.6VDetermined by BBD optimization
Optimal NaCl Conc. (X2)1.5g/LDetermined by BBD optimization
Maximum Removal Efficiency99.99%Achieved at optimal conditions
Adsorption Capacity (qe)129.02mg/gAchieved at optimal conditions
Equilibrium Time3hoursTime required for saturation
MnO2 PhaseOrthorhombic Îł-MnO2-Confirmed by XRD (JCPDS NO.14-0644)
Nanostructure MorphologySpherical brushes/Nanorods-Confirmed by FESEM
Average Nanorod Diameter35.11nmMeasured via FESEM
Model R2 (Determination Coeff.)99.42%Indicates excellent model fit to experimental data
  1. Carbon Fiber (CF) Activation: Commercial CF substrate (16.5 cm x 5 cm) was chemically activated by immersion in 5% HNO3 solution for 30 minutes at 80 °C.
  2. MnO2 Electrodeposition: Nanostructured MnO2 was deposited onto the activated CF (anode) galvanostatically for 4 hours at a constant current density of 0.3 mA/cm2.
  3. Electrolyte Composition (Synthesis): The electrolytic solution used for deposition consisted of 0.64 M H2SO4 and 0.35 M MnSO4, maintained at 90 °C and agitated by a magnetic stirrer.
  4. Electrode Characterization: The composite electrode morphology and composition were analyzed using Field Emission Scanning Electron Microscopy (FESEM) and Energy Dispersive X-ray Spectrometry (EDX). Crystal structure was confirmed via X-ray Diffraction (XRD).
  5. Electrosorption Testing (CDI): Batch experiments were performed using the MnO2/CF composite as the working electrode and a stainless steel plate as the counter electrode, separated by 1.5 cm.
  6. Analytical Measurement: Cr(VI) concentration was determined using a UV spectrophotometer at 540 nm, relying on the colorimetric reaction with diphenylcarbazide in acidic media.
  7. Optimization Strategy: Response Surface Methodology (RSM) utilizing the Box-Behnken Design (BBD) was applied to model and optimize the effects and interactions of three variables (pH, NaCl concentration, and cell voltage) on Cr(VI) removal efficiency.

The synthesized MnO2/CF composite electrode and the optimized electrosorption process are highly relevant for advanced water purification technologies, particularly those requiring high efficiency and low energy consumption.

  • Industrial Wastewater Treatment: Direct application in treating effluents from industries such as electroplating, leather tanning, and chemical manufacturing, which are primary sources of toxic Cr(VI) contamination.
  • Capacitive Deionization (CDI) Systems: The electrode serves as a high-performance component for CDI units, offering advantages over traditional carbon-only electrodes due to the enhanced pseudocapacitive behavior of the MnO2 coating.
  • Heavy Metal Remediation: Applicable for the selective removal of various heavy metal oxyanions (like Cr(VI) and potentially arsenic) from contaminated water sources, leveraging the redox activity of MnO2.
  • Electrochemical Energy Storage: The MnO2 nanostructure, known for its high theoretical pseudo capacitance (1370 F.g-1), makes this composite material suitable for development in high-rate supercapacitors and batteries.
  • Electrochemical Sensor Technology: The high surface area and controlled nanostructure of the MnO2 coating could be utilized in developing sensitive electrochemical sensors for environmental monitoring.
View Original Abstract

A nano manganese dioxide (MnO2) was electrodeposited galvanostatically onto a carbon fiber (CF) surface using the simple method of anodic electrodeposition. The composite electrode was characterized by field emission scanning electron microscopy (FESEM), and X-ray diffraction (XRD). Very few studies investigated the efficiency of this electrode for heavy metals removal, especially chromium. The electrosorption properties of the nano MnO2/CF electrode were examined by removing Cr(VI) ions from aqueous solutions. NaCl concentration, pH, and cell voltage were studied and optimized using the Box-Behnken design (BDD) to investigate their effects and interactions on the electrosorption process. The results showed that the optimal conditions for the removal of Cr(VI) ions were a cell voltage of 4.6 V, pH of 2 and NaCl concentration of 1.5 g/L. This work indicated that MnO2/CF electrode was highly effective in removing Cr(VI) ions and the BBD approach was a feasible and functional method for evaluating the experimental data.