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Voltammetric quantification of a nonsteroidal anti-inflammatory agent diflunisal based on the enhancement effect of cationic surfactant on boron-doped diamond electrode

MetadataDetails
Publication Date2021-05-11
JournalMacedonian Journal of Chemistry and Chemical Engineering
AuthorsErtuğrul Keskin, Shabnam Allahverdiyeva, Amer S. Alali, Yavuz Yardım
InstitutionsVan YĂŒzĂŒncĂŒ Yıl Üniversitesi, Adıyaman University
Citations5
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Technical Documentation & Analysis: BDD for High-Sensitivity Voltammetry

Section titled “Technical Documentation & Analysis: BDD for High-Sensitivity Voltammetry”

This research successfully demonstrates a simple, fast, and highly sensitive voltammetric method for quantifying the nonsteroidal anti-inflammatory drug (NSAID) Diflunisal (DIF) using an unmodified Boron-Doped Diamond (BDD) electrode.

  • Core Achievement: Developed a robust Square-Wave Adsorptive Stripping Voltammetry (SW-AdSV) protocol for DIF quantification in pharmaceutical formulations.
  • Material Advantage: The BDD electrode provided the necessary wide working potential window and low background current for the irreversible, diffusion-controlled oxidation of DIF.
  • Sensitivity Enhancement: The presence of the cationic surfactant, cetyltrimethylammonium bromide (CTAB), combined with a 30 s accumulation step, increased the DIF oxidation signal sensitivity by a factor of 6.8.
  • High Performance: The optimized method achieved a low Limit of Detection (LOD) of 5.2·10-8 mol l-1 (0.013 ”g ml-1) and excellent linearity (r = 0.999).
  • Practical Application: The protocol proved highly selective and accurate, demonstrating successful quantification of DIF in commercial tablet samples with high recovery rates (99.3% to 108.4%).
  • Surface Management: An optimized anodic/cathodic pretreatment procedure was essential to maintain the BDD surface’s oxygen- and hydrogen-terminated properties, ensuring stable and reproducible voltammetric responses.

The following hard data points were extracted from the optimized electroanalytical protocol utilizing the BDD electrode:

ParameterValueUnitContext
Electrode MaterialBoron-Doped Diamond (BDD)N/AUnmodified working electrode
Boron Doping Level1000ppmSpecified concentration
Electrode Diameter3mmPhysical dimension of the working electrode
Technique UsedSW-AdSV (Square-Wave Adsorptive Stripping Voltammetry)N/AOptimized pulse technique
Supporting Electrolyte0.1 mol l-1 Phosphate Buffer Solution (PBS)N/AOptimized for highest peak morphology
Optimum pH2.5N/ASelected buffer acidity
Cationic SurfactantCTAB (Cetyltrimethylammonium bromide)N/AUsed for sensitivity enhancement
Optimum CTAB Concentration5·10-5mol l-1Concentration yielding 6.8x sensitivity increase
Accumulation Time30sApplied at open-circuit potential
Oxidation Peak Potential (Ep)+1.07Vvs. Ag/AgCl reference electrode
Linear Range (Molar)2.0·10-7 - 8.0·10-6mol l-1Analytical working range
Limit of Detection (LOD)5.2·10-8mol l-1High sensitivity achieved
SWV Frequency (f)75HzOptimized instrumental parameter
SWV Pulse Amplitude (ΔEsw)40mVOptimized instrumental parameter
SWV Step Potential (ΔEs)10mVOptimized instrumental parameter

The successful quantification of DIF relied on precise control over the BDD electrode surface and optimized SWV parameters:

  1. Electrode Pretreatment (Surface Termination): The BDD electrode was subjected to a sequential anodic/cathodic pretreatment at the start of each experiment day to achieve stable oxygen- and hydrogen-terminated properties.
    • Anodic Step: +1.8 V applied for 180 s in 0.5 mol l-1 H2SO4.
    • Cathodic Step: -1.8 V applied for 180 s in 0.5 mol l-1 H2SO4.
  2. Physical Cleaning: The electrode was gently polished with a polishing pad and rinsed with deionized water before each voltammetric experiment to ensure stable responses.
  3. Electrolyte Optimization: Phosphate Buffer Solution (PBS) at pH 2.5 was selected as the optimum supporting electrolyte, providing the highest and most uniform peak morphology compared to Britton-Robinson (BR) buffer and HNO3 solutions.
  4. SWV Parameter Optimization: Instrumental parameters were tuned for maximum sensitivity and peak shape: frequency (75 Hz), pulse amplitude (40 mV), and step potential (10 mV).
  5. Adsorptive Stripping Protocol (SW-AdSV):
    • The three electrodes were immersed in the supporting electrolyte containing DIF and the optimum CTAB concentration (5·10-5 mol l-1).
    • Accumulation: 30 s at open-circuit potential while stirring (500 rpm).
    • Equilibration: 5 s pause after stirring stopped.
    • Measurement: Anodic scanning from 0 V to +1.5 V using the optimized SWV technique.

6CCVD is the premier supplier of MPCVD diamond materials necessary to replicate and advance this high-sensitivity electroanalytical research. Our expertise in custom BDD fabrication ensures optimal performance for demanding applications like pharmaceutical sensing.

To replicate or extend the high-sensitivity DIF detection achieved in this paper, researchers require highly controlled Boron-Doped Diamond (BDD) material:

  • Heavy Boron Doped PCD/SCD (BDD): The core material required. 6CCVD offers BDD with precise control over boron concentration, easily meeting or exceeding the 1000 ppm doping level used in this study. We provide BDD optimized for electrochemical applications, ensuring the wide working window and low background current critical for SW-AdSV.
  • Electroanalytical Grade PCD: For applications requiring larger surface areas or arrays, our Polycrystalline Diamond (PCD) substrates can be heavily doped with boron, offering robust, scalable platforms up to 125 mm in diameter.

The success of this research hinges on precise electrode geometry and surface quality. 6CCVD provides tailored solutions that eliminate the need for external processing:

Research Requirement6CCVD Custom CapabilityValue Proposition
Specific DimensionsCustom laser cutting and shaping.We can supply BDD wafers cut precisely to 3 mm diameter electrodes, or larger plates (up to 125 mm) for fabricating multi-electrode arrays.
Doping UniformityTight control over gas phase B/C ratio during MPCVD growth.Ensures highly uniform 1000 ppm (or custom) boron incorporation, guaranteeing reproducible electrochemical performance across batches.
Surface FinishUltra-smooth polishing services.We offer polishing down to Ra < 5 nm for inch-size PCD/BDD, which is essential for minimizing fouling and maximizing the stability and reproducibility of the voltammetric response, as noted in the paper.
Integrated ContactsCustom metalization services (Au, Pt, Ti, W, Cu).We can deposit custom metal contacts directly onto the BDD substrate, streamlining integration into electrochemical cell setups and ensuring low-resistance connections for high-frequency SWV measurements.

The optimization of BDD surface termination (anodic/cathodic pretreatment) is crucial for achieving the reported sensitivity. 6CCVD’s in-house PhD team specializes in diamond surface chemistry and electrochemistry.

  • Application Expertise: Our team can assist engineers and scientists in selecting the optimal BDD material (doping level, thickness, and surface termination) for similar pharmaceutical electroanalytical sensing projects, including the detection of other NSAIDs or complex organic molecules.
  • Process Consultation: We provide consultation on best practices for BDD electrode preparation and pretreatment procedures to maximize sensitivity and lifetime in corrosive environments (e.g., 0.5 mol l-1 H2SO4).

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

View Original Abstract

The present work describes a simple, fast, and inexpensive voltammetric method for diflunisal measurement using a non-modified boron-doped diamond (BDD) electrode. The oxidation of the agent was irreversible and presented a diffusion‐controlled process. The sensitivity of the square wave voltammetric measurements were significantly improved when the cationic surfactant, cetyltrimethylammonium bromide (CTAB), was present in the supporting electrolyte solution. Using square-wave mode, a linear response was obtained for diflunisal quantification in 0.1 mol L-1 phosphate buffer solution (pH 2.5) solution containing 5×10-5 mol L-1 CTAB at +1.07 V (vs. Ag/AgCl) (after 30 s accumulation under open-circuit conditions). Linearity was found for 0.05 to 2.0 ÎŒg mL-1 (2.0×10-7-8.0×10-6 mol L-1) with a detection limit 0.013 ÎŒg mL-1 (5.2×10-8 mol L-1). The developed approach could be used for the quantification of diflunisal in pharmaceutical formulations.