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Analysis of Quadrol Additives in Pyrophosphate Copper-Plating Bath by Use of Boron-Doped Diamond Electrode

MetadataDetails
Publication Date2023-07-01
JournalJournal of The Surface Finishing Society of Japan
AuthorsTaiga SAEKI, T. Onuki, Sachio YOSHIHARA, Yoshifusa ISHIKAWA, Kenichiro MOTOI
InstitutionsUtsunomiya University
AnalysisFull AI Review Included

Technical Documentation & Analysis: Boron-Doped Diamond for Electrochemical Sensing

Section titled “Technical Documentation & Analysis: Boron-Doped Diamond for Electrochemical Sensing”

This research validates the superior performance of Microwave Plasma Chemical Vapor Deposition (MPCVD) grown Boron-Doped Diamond (BDD) electrodes for complex electrochemical analysis, specifically targeting the quantification of organic additives in industrial plating baths.

  • Superior Electrode Performance: BDD electrodes demonstrated a clear advantage over traditional Glassy Carbon (GC) electrodes for the oxidation of Quadrol (an organic additive), confirming BDD’s unique electrochemical stability and wide potential window.
  • Oxidation Mechanism Confirmed: The oxidation of Quadrol occurred at 1.65 V vs. SCE on the BDD surface, attributed to the generation of highly reactive hydroxyl (OH) radicals, a mechanism favored by the sp3-rich structure of high-quality MPCVD diamond.
  • High Sensitivity and Quantification: Linear Sweep Voltammetry (LSV) established a highly linear relationship (r2 = 0.9991) between current density and Quadrol concentration in the range of 0 to 0.075 mol dm-3.
  • Industrial Relevance: This methodology enables precise, high-sensitivity quantification of organic components in complex electrolytes, offering a robust solution for quality control and maintenance in copper pyrophosphate plating processes.
  • Interference Mitigation: BDD successfully allowed for the analysis of Quadrol even in the presence of other common additives (like L-histidine), provided the target analyte oxidizes at a less noble potential.

The following hard data points were extracted from the BDD deposition conditions and electrochemical results:

ParameterValueUnitContext
BDD Growth MethodMPCVDN/AStandard 6CCVD capability
Substrate MaterialSi (111)N/AUsed for heteroepitaxial growth
BDD Film Thickness20”mTarget thickness for electrode
Boron/Carbon Ratio10,000ppmRequired for metallic conductivity
Deposition Temperature700°CMPCVD process parameter
Microwave Output1500WMPCVD process parameter
Deposition Pressure70TorrMPCVD process parameter
Quadrol Oxidation Potential1.65V vs. SCEObserved on BDD electrode
Linear Quantification Range0 to 0.075mol dm-3Concentration range for LSV (r2 = 0.9991)
Electrode Area (GC/BDD)0.28cm2Working electrode size

The experiment relied on precise MPCVD growth and advanced electrochemical techniques to characterize the BDD material and its performance in the plating bath environment.

  1. BDD Film Growth: Boron-Doped Diamond (BDD) films were grown on mirror-polished Si (111) wafers (0.5 mm thick) using the MPCVD method following standard diamond nucleation/seeding procedures.
  2. Deposition Parameters: Growth was conducted at 700 °C and 70 Torr, utilizing 1500 W microwave power. The critical Boron/Carbon doping ratio was maintained at 10,000 ppm to ensure metallic conductivity.
  3. Electrode Fabrication: The 20 ”m thick BDD film and a comparative Glassy Carbon (GC) electrode (0.28 cm2 area) were masked and sealed using epoxy resin to define the active electrode surface.
  4. Electrolyte Preparation: The base electrolyte was a copper pyrophosphate plating bath (0.944 mol dm-3 K4P2O7, 0.213 mol dm-3 Cu2P2O7 3H2O). Quadrol and other additives (L-histidine, N,N,N’,N’-ethylenediamine tetrakis- (methylenephosphonic acid)) were added for comparative studies.
  5. Electrochemical Measurement: Cyclic Voltammetry (CV) and Linear Sweep Voltammetry (LSV) were performed at room temperature using a three-electrode system (BDD/GC working, Pt mesh counter, Saturated Calomel Electrode (SCE) reference).
  6. Quantification: LSV measurements were used to establish the relationship between the anodic current density (at 2.20 V vs. SCE) and the Quadrol concentration, confirming diffusion-limited kinetics.

6CCVD is uniquely positioned to supply the high-specification BDD materials required to replicate, scale, and advance this research into industrial applications for plating bath control and electrochemical sensing.

To achieve the high conductivity and chemical stability demonstrated in this paper, 6CCVD recommends the following material specifications:

  • Heavy Boron-Doped Diamond (BDD): We provide BDD with doping concentrations precisely tailored to achieve metallic conductivity, easily meeting the 10,000 ppm B/C ratio used in this study. Our BDD material ensures the optimal sp3 surface quality necessary for efficient OH radical generation and high-sensitivity organic oxidation.
  • Substrate Options: While the paper utilized Si (111), 6CCVD offers BDD grown on various substrates or as Free-Standing BDD Plates up to 125 mm in diameter. Free-standing BDD offers superior thermal management and mechanical robustness for long-term industrial sensor deployment.

The successful transition of this laboratory technique to an industrial sensor requires precise material engineering, a core competency of 6CCVD.

Requirement from Research6CCVD Customization CapabilityValue Proposition
Custom ThicknessSCD/PCD/BDD thickness from 0.1 ”m up to 500 ”m.We can match the 20 ”m thickness or provide thicker, more robust films for extended sensor life.
Large Area ElectrodesPCD/BDD plates available up to 125 mm in diameter.Enables the fabrication of large-scale, multi-sensor arrays for comprehensive bath monitoring.
Custom MetalizationIn-house deposition of Au, Pt, Pd, Ti, W, and Cu.Essential for creating reliable, corrosion-resistant electrical contacts and interconnects on the BDD sensor surface.
Surface FinishPolishing capabilities to achieve Ra < 5 nm on inch-size PCD/BDD.Optimized surface finish ensures consistent electrochemical performance and minimizes background current noise.

6CCVD provides comprehensive support to ensure successful implementation of diamond technology in advanced electrochemical applications:

  • Expert Consultation: 6CCVD’s in-house PhD team specializes in optimizing BDD material properties (doping profile, sp3/sp2 ratio, and surface termination) specifically for complex organic oxidation and plating bath control projects.
  • Material Selection: We assist engineers in selecting the ideal BDD grade (e.g., optimizing doping levels for maximum OH radical yield vs. minimizing resistance) to extend the linear quantification range beyond the 0.075 mol dm-3 limit observed in the paper.
  • Global Supply Chain: We offer reliable global shipping (DDU default, DDP available) to ensure rapid delivery of custom BDD wafers and plates worldwide.

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

View Original Abstract

The purpose of this study is the use of boron-doped diamond BDD electrodes for the electrochemical analysis of N,N,N’,N’-Tetrakis 2-hydroxypropyl ethylenediamine Quadrol as an additive in copper pyrophosphate plating baths. Actually, BDD is a quite new electrode material. Non-doped diamond shows electrical insulating properties, but its conductivity changes according to the doping concentration of boron from semiconductive, metallic conductive, to superconductivity. Moreover, BDD has unique electrochemical properties such as a wide potential window, low background current, and chemical stability. Metallic conductive BDD electrodes have been used for the electrochemical analysis of Quadrol additives. Earlier, we reported that Quadrol additives included in copper pyrophosphate plating baths had the effect of improving the appearance of thus-plated film, even under high current density. Cyclic voltammogram CV measurements for Quadrol in a copper pyrophosphate plating bath using BDD or Glassy carbon GC electrodes suggest that the BDD electrode showed anodic current, which was thought to be attributed to the oxidation of Quadrol at ca. 1.65 Vvs. SCE. Comparison with GC electrodes has clarified differences in the oxidation mechanism of Quadrol on each electrode. Furthermore, LSV measurements for BDD electrodes suggest the possibility of quantification of Quadrol in the bath.