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Electrochemical oxidation and electroanalysis of paracetamol on a boron-doped diamond anode material in aqueous electrolytes

MetadataDetails
Publication Date2021-02-16
JournalJournal of Electrochemical Science and Engineering
AuthorsKouakou Etienne Kouadio, Kambiré Ollo, Konan Sylvestre Koffi, Lassiné Ouattara
InstitutionsUniversité Félix Houphouët-Boigny
Citations10
AnalysisFull AI Review Included

Technical Documentation & Analysis: High-Performance BDD Electrodes for Electrochemical Oxidation

Section titled “Technical Documentation & Analysis: High-Performance BDD Electrodes for Electrochemical Oxidation”

This analysis confirms the exceptional utility of Boron-Doped Diamond (BDD) electrodes, manufactured via Chemical Vapor Deposition (CVD), for advanced electrochemical applications, specifically the detection and degradation of pharmaceutical pollutants like paracetamol.

  • Material Validation: The study validates the BDD electrode’s “metallic character” and its suitability as a robust, high-performance anode for both electroanalytical sensing and Advanced Oxidation Processes (AOPs).
  • Sensing Performance: Achieved ultra-low detection limits (LOD = 0.167 µM) for paracetamol quantification using Differential Pulse Voltammetry (DPV), demonstrating superior sensitivity compared to many modified carbon electrodes.
  • Degradation Efficiency: Demonstrated rapid and near-complete paracetamol degradation, reaching 99 % conversion in just 1 hour for 1 mM solutions under optimized conditions (70 mA cm⁻²).
  • Process Optimization: Confirmed that high current density (up to 100 mA cm⁻²) and elevated temperature (up to 75 °C, yielding 97 % degradation) significantly accelerate the mineralization kinetics, placing the process under mass transport control.
  • Electrolyte Selection: Britton-Robinson buffer solution was identified as the optimal supporting electrolyte, providing the widest linear working range (2.0-130.66 µM) and lowest detection limits.
  • 6CCVD Advantage: The results directly support the demand for high-quality, low-resistivity MPCVD BDD wafers, a core offering of 6CCVD, for scaling up environmental remediation and sensor technologies.

The following hard data points were extracted from the research paper detailing the BDD electrode characteristics and performance metrics.

ParameterValueUnitContext
Electrode MaterialBoron-Doped Diamond (BDD)N/APrepared via HF-CVD
Film Thickness~1µmGrown on p-Si wafer substrate
Substrate Resistivity1 - 3mΩ cmLow resistivity p-Si wafer
Growth Rate0.24µm h⁻¹CVD deposition rate
Working Electrode Area1cm²Voltammetric measurements
Applied Current Density (Max)100mA cm⁻²Preparative electrolysis
Optimal Degradation pH3N/AOxidation is most favorable in acidic solution
Limit of Detection (LOD)0.167µMDPV in Britton-Robinson buffer
Limit of Quantification (LOQ)0.559µMDPV in Britton-Robinson buffer
Degradation Rate (1 mM, 1h)99%At 70 mA cm⁻² and pH 0.6
Degradation Rate (75 °C, 2h)97%At 70 mA cm⁻²
Paracetamol Oxidation Peak~0.9V vs. SHECyclic Voltammetry
Electrolysis Cell Volume32cm³Preparative electrolysis setup

The BDD electrodes were fabricated and tested using the following key methodologies:

  1. BDD Synthesis: Boron-doped diamond films were prepared using Hot-Filament Chemical Vapor Deposition (HF-CVD).
  2. Precursor Gases: The process gas mixture consisted of 1 % CH4 in H2, with trimethylboron used as the boron doping source to achieve the desired low resistivity.
  3. Substrate Selection: Low resistivity (1-3 mΩ cm) p-Si wafers (10 cm diameter, 0.5 mm thickness) were used as the growth substrate.
  4. Electrochemical Setup: A standard three-electrode single compartment glass cell was employed, featuring the BDD working electrode, a Saturated Calomel Electrode (SCE) reference, and a Platinum wire counter electrode.
  5. Analytical Technique: Differential Pulse Voltammetry (DPV) was the primary technique for paracetamol quantification, preceded by electrochemical pretreatment (seven cycles of Cyclic Voltammetry in 0.5 M H2SO4).
  6. Preparative Electrolysis Setup: A batch mode setup was utilized for degradation studies, featuring a BDD anode (16 cm²) and a Zirconium plate cathode (16 cm²), with the solution recirculated at a flow rate of 2.7 mL s⁻¹.
  7. Electrolyte Optimization: Britton-Robinson buffer solution (0.04 M) was selected as the optimal supporting electrolyte for monitoring paracetamol concentration during degradation.

The successful implementation of BDD electrodes for high-efficiency paracetamol degradation and sensing highlights a critical need for high-quality, scalable diamond materials. 6CCVD’s advanced MPCVD capabilities are perfectly positioned to meet and exceed the requirements demonstrated in this research.

To replicate or extend this research, 6CCVD recommends the following materials:

  • Heavy Boron Doped PCD Wafers: Required for high-performance electrochemical oxidation (AOPs). Our MPCVD process ensures superior doping uniformity and low resistivity (mΩ cm range), critical for minimizing ohmic losses and maximizing current efficiency at high current densities (up to 100 mA cm⁻²).
  • BDD on Silicon Substrates: We offer BDD films grown on silicon substrates (up to 10mm thick) that match the experimental setup, facilitating easy integration into existing flow cells and electrochemical reactors.

The research utilized specific electrode dimensions (16 cm²) and required robust performance under high current loads. 6CCVD offers comprehensive customization services essential for scaling this technology:

Research Requirement6CCVD Solution & Value Proposition
Electrode Dimensions (16 cm²)Custom Dimensions up to 125mm: We provide large-area PCD/BDD plates up to 125mm in diameter. This capability is crucial for scaling laboratory-scale degradation experiments (16 cm²) into pilot or industrial flow-through reactors for wastewater treatment.
Thin Film Requirement (~1 µm)Precision Thickness Control (0.1 µm - 500 µm): 6CCVD guarantees precise control over BDD film thickness, allowing engineers to optimize the active layer depth for specific applications, whether for ultra-sensitive DPV sensing or robust, thick-film AOP anodes.
Electrode Integration & ContactingCustom Metalization Services: For reliable electrical contact and device packaging, 6CCVD offers in-house deposition of standard metals (Au, Pt, Pd, Ti, W, Cu). This is vital for creating robust, low-resistance ohmic contacts necessary for high current density operation (100 mA cm⁻²).
Surface Quality for SensingAdvanced Polishing (Ra < 5nm): While the degradation study used as-grown BDD, for high-sensitivity DPV sensor development, 6CCVD can provide highly polished PCD surfaces (Ra < 5nm for inch-size wafers), minimizing surface defects and maximizing signal integrity.

The successful optimization of paracetamol degradation relied heavily on controlling parameters like pH, current density, and temperature. 6CCVD’s in-house PhD team specializes in the material science of diamond electrochemistry.

  • We offer expert consultation on material selection, doping levels, and surface termination (e.g., hydrogen or oxygen termination) to optimize BDD performance for similar pharmaceutical wastewater remediation and trace organic sensing projects.
  • Our technical sales engineers can assist in translating laboratory-scale current density requirements (e.g., 70-100 mA cm⁻²) into scalable, cost-effective BDD electrode designs.

For custom specifications or material consultation, visit 6ccvd.com or contact our engineering team directly.

View Original Abstract

Electrochemical oxidation of paracetamol on boron-doped diamond (BDD) anode has been studied by cyclic voltammetry and preparative electrolysis. Quantification of paracetamol during electrolysis has been mainly realized by differential pulse voltammetry technique in the Britton-Robinson buffer solutions used as the supporting electrolyte. Various parameters such as current intensity, nature of the supporting electrolyte, temperature, and initial concentration of paracetamol have been investigated. The electrochemical characterization by the outer sphere Fe(III)/Fe(II) redox couple has also been performed, showing the metallic character of BDD electrode. The obtained linear dependency of the oxidation peak current intensity and paracetamol concentration indicates that BDD electrode can be used as an electrochemical sensor for the detection and quantification of paracetamol. The investi­gation of paracetamol degradation during preparative electrolysis showed that: (i) the degradation rate of paracetamol increases with increase of current intensity applied; (ii) for the initial concentrations of 10, 6 and 1 mM of paracetamol, its oxidation rate reaches 60, 78 and 99 % respectively, after 1 h of electrolysis in 0.3 M H2SO4 (pH 0.6) at applied current density of 70 mA cm-2; (iii) at temperatures of electrolyte solution of 28, 55 and 75 °C, paracetamol oxidation rate reached 85, 92 and 97 % respectively, after 2 h at applied current density of 70 mA cm2. From the investigation of the effect of pH value of electrolyte solution, it appears that oxidation of paracetamol is more favorable in acidic solution at pH 3 than solutions of higher pH values.