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Sequential electrodeposition of Cu–Pt bimetallic nanocatalysts on boron-doped diamond electrodes for the simple and rapid detection of methanol

MetadataDetails
Publication Date2021-07-13
JournalScientific Reports
AuthorsSurinya Traipop, Abdulhadee Yakoh, Sakda Jampasa, Sudkate Chaiyo, Yuttanant Boonyongmaneerat
InstitutionsChulalongkorn University
Citations10
AnalysisFull AI Review Included
  • Novel Sensor Architecture: A highly effective electrochemical sensor for methanol (MetOH) detection was developed using sequential electrodeposition of Cu-Pt bimetallic nanocatalysts onto a Boron-Doped Diamond (BDD) electrode (Cu/Pt/BDD).
  • Synergistic Catalysis: The Pt base layer provides high electrocatalytic activity, while the subsequent Cu layer enhances conductivity and, critically, suppresses the adsorption of carbonaceous intermediates (CO poisoning), leading to superior long-term stability.
  • Optimized Morphology: Sequential deposition (Pt first, then Cu) resulted in a favorable flower-like Pt structure covered by Cu particles, maximizing the active surface area and promoting MetOH oxidation.
  • Enhanced Sensitivity via SIA: Coupling the sensor with a Sequential Injection Analysis (SIA) system improved the detection limit by approximately 100 times compared to traditional Cyclic Voltammetry (CV).
  • High Performance Metrics: The sensor achieved a low Limit of Detection (LOD) of 83 µM (S/N = 3) and demonstrated a remarkably wide linear range spanning 0.1 mM up to 1000 mM.
  • Robustness and Applicability: The sensor exhibited excellent stability (92% signal retention after 2 weeks) and high selectivity, successfully applied for MetOH detection in complex fruit and vegetable beverage samples.
ParameterValueUnitContext
Limit of Detection (LOD)83µMS/N = 3, Low concentration range
Linear Range (Low)0.1 to 10mMHigh sensitivity region
Linear Range (High)10 to 1000mMWide dynamic range
Sensitivity (Low Range)0.829µA/mM0.1-10 mM MetOH
Sensitivity (High Range)0.229µA/mM10-1000 mM MetOH
Pt Deposition Potential-0.4Vvs Ag/AgCl
Cu Deposition Potential-0.5Vvs Ag/AgCl
Pt Deposition Time600sOptimized multiple-step deposition
Cu Deposition Time900sOptimized one-step deposition
Supporting Electrolyte0.1MNaOH (Optimized for alkaline oxidation)
Reproducibility (RSD)3.2%Five independently fabricated electrodes
Storage Stability2weeks92% signal retained at room temperature
BDD Doping Level10,000ppmBoron
BDD Geometric Area0.07cm2Working electrode area
  1. BDD Electrode Pre-treatment: The BDD substrate was pre-treated via potentiostatic anodic polarization in 0.1 M H2SO4 at 2.0 V for 5 minutes to eliminate adsorbed hydrogen and undesirable sp2 graphitic carbon phases, reducing background current.
  2. Pt Base Layer Deposition: Platinum was deposited first using a multiple-step electrodeposition technique (optimized for better dispersion and morphology) from 1 mM K2[PtCl4] in 0.1 M H2SO4. The process involved applying a deposition potential of -0.4 V and a relaxation potential of 0.0 V for 600 s.
  3. Cu Top Layer Deposition: Copper was subsequently deposited onto the Pt/BDD electrode using a one-step electrodeposition technique from 1 mM Cu(CH3COO)2 in 0.1 M CH3COONa. The optimized deposition potential was -0.5 V for 900 s.
  4. Morphological and Chemical Characterization:
    • Scanning Electron Microscopy (SEM) confirmed the resulting Cu/Pt/BDD structure featured flower-like Pt microclusters covered by Cu particles, providing high surface area.
    • X-ray Photoelectron Spectroscopy (XPS) confirmed the presence of metallic Pt0 and/or Pt-Cu alloy, indicating electronic coupling between the metals.
  5. Electrochemical Characterization: Electrochemical Impedance Spectroscopy (EIS) confirmed the Cu/Pt/BDD electrode had the lowest charge transfer resistance (Rct = 14.8 kΩ) and highest conductivity among all tested configurations.
  6. Automated Analysis: The Cu/Pt/BDD sensor was integrated into a Sequential Injection Analysis (SIA) system, and methanol detection was performed using chronoamperometry at an applied potential of 0.5 V vs Ag/AgCl in 0.1 M NaOH.
  • Food and Beverage Quality Control: Rapid, high-throughput screening for trace methanol contamination in fruit juices, vegetable beverages, coffee, and fermented products, ensuring consumer safety.
  • Chemical and Fuel Cell Industries: Monitoring and control of methanol oxidation reactions (MOR) kinetics, particularly in direct methanol fuel cells (DMFCs), where catalyst poisoning is a major challenge.
  • Environmental Safety: Detection of methanol in industrial effluent and wastewater streams, leveraging the sensor’s low detection limit and robustness.
  • Non-Enzymatic Sensing: Development of stable, long-life sensors for alcohol detection, bypassing the thermal and chemical instability issues associated with traditional enzyme-based electrodes.
  • Automated Laboratory Testing: Utilizing the SIA integration for high-efficiency, automated analysis in regulatory or industrial laboratories requiring precise control and high sample throughput.