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Electrochemical Determination of Chemical Oxygen Demand Based on Boron-Doped Diamond Electrode

MetadataDetails
Publication Date2023-03-20
JournalJournal of Electrochemical Science and Technology
AuthorsDian S. Latifah, Subin Jeon, Ilwhan Oh
InstitutionsKumoh National Institute of Technology
Citations3
AnalysisFull AI Review Included

This research details the development and validation of a rapid, environment-friendly electrochemical sensor for Chemical Oxygen Demand (E-COD) utilizing a Boron-Doped Diamond (BDD) electrode.

  • Core Value Proposition: The BDD-based E-COD sensor provides a fast (steady-state reached in ~10 seconds) and non-toxic alternative to the conventional dichromate method, which is slow (2-4 hours) and uses hazardous reagents (chromium, mercury).
  • Mechanism: The BDD anode fully oxidizes organic pollutants, primarily via hydroxyl radicals (‱OH) generated at high anodic potential, resulting in a mass-transfer-limited steady-state current proportional to the COD concentration.
  • Material Specification: The sensor employs a BDD thin film (3 ”m thick, 5000 ppm B doping) grown on a silicon substrate via Hot Filament CVD.
  • Optimized Performance: Optimal analytical conditions were determined at an applied potential of 2.5 V (vs. SHE) and a neutral solution pH (range 3 to 10).
  • Performance Metrics: The sensor exhibits a linear range of 0 to 80 mg/L and a low detection limit of 1.1 mg/L (S/N=5).
  • Validation: The E-COD results show excellent correlation (R2=0.96) and high compatibility with the conventional dichromate COD method, with an average difference of only ~7%.
ParameterValueUnitContext
Anode MaterialBoron-Doped Diamond (BDD)-Thin film grown on monocrystalline Si.
Boron Doping Level5000ppmUsed in HFCVD growth process.
Film Thickness3”mBDD layer thickness.
Resistivity100mΩ·cmBDD film property.
Working Electrode Area2.54cm2Exposed area (18 mm diameter).
Optimized Applied Potential2.5Vvs. SHE (Selected for sensitive response and stability).
Optimized Solution pH3 to 10-Neutral range (avoids excessive O2 evolution).
Linear Range (E-COD)0 to 80mg/LChemical Oxygen Demand (O2 equivalent).
Detection Limit (LOD)1.1mg/LCalculated at S/N=5.
Steady-State Response Time~10secondsTime to reach stable current after sample injection.
Correlation Coefficient (R2)0.96-E-COD vs. Conventional Dichromate Method.
Calibration Equation (KHP standard)E-COD = 123 × Inetmg/LInet in mA.
  1. BDD Electrode Preparation: BDD thin film was grown on a thick monocrystalline Si substrate using the Hot Filament Chemical Vapor Deposition (HFCVD) method, achieving a 5000 ppm boron doping level.
  2. Cleaning and Activation: The electrode was degreased by sonication in acetone, isopropyl alcohol, and deionized water (10 minutes each), followed by surface treatment in 1.0 M HNO3 for one hour to remove impurities.
  3. Electrochemical Setup: Measurements were performed in a three-electrode cell configuration: BDD (working electrode), Pt coil (counter electrode), and Saturated Calomel Electrode (SCE) (reference electrode).
  4. Pre-conditioning: The BDD electrode was pre-conditioned by conducting 20 potential cycles in a blank 0.1 M KNO3 supporting electrolyte.
  5. Amperometric Detection: The E-COD value was determined using amperometric detection under well-stirred conditions. A constant potential (optimized at 2.5 V vs. SHE) was applied until the background current stabilized.
  6. Response Measurement: Aliquots of organic compounds were injected, and the resulting increase in steady-state anodic current (Inet) was measured as the sensor response, which is directly proportional to the COD concentration.
  7. Validation: E-COD results for model organic compounds (KHP, glucose, phenol, etc.) were compared against results obtained using the standard colorimetric dichromate digestion method (heating at 150 °C for 2 hours).

The development of a rapid, robust, and non-toxic COD sensor based on BDD electrodes is highly relevant for several industries:

  • Wastewater Treatment and Environmental Monitoring:
    • Real-time, continuous monitoring of industrial and municipal effluent quality, replacing slow, centralized laboratory testing.
    • Field-deployable, portable COD meters for rapid environmental surveys of rivers and lakes.
  • Process Control in Manufacturing:
    • Integration into chemical, pharmaceutical, and food processing plants to provide immediate feedback on organic load and water recycling efficiency.
  • Advanced Electrochemical Oxidation Processes (EAOP):
    • The BDD material, known for its wide potential window and high stability, is critical for high-efficiency electrochemical incineration and water remediation systems.
  • Sensor Technology:
    • Commercialization of compact, safer COD devices that eliminate the need for toxic reagents (e.g., chromium and mercury salts).
View Original Abstract

A rapid and environment-friendly electrochemical sensor to determine the chemical oxygen demand (COD) has been developed. The boron-doped diamond (BDD) thin-film electrode is employed as the anode, which fully oxidizes organic pollutants and provides a current response in proportion to the COD values of the sample solution. The BDD-based amperometric COD sensor is optimized in terms of the applied potential and the solution pH. At the optimized conditions, the COD sensor exhibits a linear range of 0 to 80 mg/L and the detection limit of 1.1 mg/L. Using a set of model organic compounds, the electrochemical COD sensor is compared with the conventional dichromate COD method. The result shows an excellent correlation between the two methods.