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Electrically Conductive Diamond Membrane for Electrochemical Separation Processes

MetadataDetails
Publication Date2016-07-11
JournalACS Applied Materials & Interfaces
AuthorsFang Gao, Christoph E. Nebel
InstitutionsFraunhofer Institute for Applied Solid State Physics
Citations24
AnalysisFull AI Review Included

6CCVD Technical Analysis & Product Solution: Boron-Doped Diamond Membranes for Electrochemical Separation

Section titled “6CCVD Technical Analysis & Product Solution: Boron-Doped Diamond Membranes for Electrochemical Separation”

This paper presents a robust methodology for fabricating highly stable, electrically conductive Boron-Doped Diamond (BDD) membranes via Microwave Plasma Chemical Vapor Deposition (MWCVD) template growth on quartz fibers. These BDD membranes are successfully demonstrated as electrochemically switchable filters for selective separation processes, crucial for applications in water treatment and chemical analysis.

  • Ultra-High Conductivity: Achieved boron doping levels exceeding $10^{21}$ cm-3 (four times the threshold for metallic conductivity), ensuring fast electron transfer kinetics essential for high-efficiency electrodes.
  • Enhanced Surface Area: Templated growth results in a massive surface enlargement, estimated at $\sim$250 times that of a planar electrode, boosting the efficiency of flow-through electrolysis.
  • Wide Electrochemical Window: The membrane exhibits an exceptionally wide potential window (3.1 V total, from -1.6 V to +1.5 V vs. Ag/AgCl), minimizing water splitting interference and maximizing chemical reaction space.
  • Selective Removal Demonstrated: Selective trapping and removal of heavy metal ions (Cu2+, Ni2+) via reduction, and organic species (Rhodamine B) via oxidation/decomposition, confirming electro-selectivity.
  • Extreme Stability and Self-Cleaning: Diamond’s stability allows for in situ oxidative regeneration (2.0 V bias or high current density) to remove fouling, with minimal loss of active area (only 7.47% loss in 5 min), a critical advantage over sp2 carbon materials in corrosive environments.
  • Industrial Scalability: The successful demonstration paves the way for industrial scale-up, potentially reaching 6-inch diameters for applications in desalination, waste water treatment, and chlor-alkali processes.

Data extracted from MWCVD recipe and electrochemical characterization:

ParameterValueUnitContext
MaterialBoron-Doped Diamond (BDD)N/AHighly Conductive Porous Electrode
Minimum Doping Required (Metallic)5 x 1020cm-3Threshold confirmed for porous electrode functionality
Achieved Doping (Upper Surface)4 x 1021cm-3High-quality boron incorporation level
Achieved Doping (Bottom Layer)1 x 1021cm-3Doping profile variance due to temperature gradient
Diamond Coating Depth$\sim$80”mCoating thickness reached within the quartz fiber network
Electrochemical Potential Window3.1VRange: -1.6 V to +1.5 V vs. Ag/AgCl (1 M KCl)
Effective Surface Enlargement$\sim$250TimesRelative to planar BDD electrode (via capacitive current)
Regeneration Potential (Oxidative)2.0VApplied bias for in situ self-cleaning (5 min duration)
Active Area Loss (Post-Regeneration)7.47%Loss measured after 5 minutes at 2.0 V (stabilization observed)
Flow Rate (Filtration)$\sim$0.2mL/minMeasured flow rate through the membrane

The fabrication of the conductive diamond membrane relies on precise MWCVD parameters and specific post-growth chemical treatments:

  1. Template Selection: 2-inch quartz fiber filters (Macherey-Nagel) were utilized as the porous growth scaffold.
  2. Seeding Preparation: Filters were immersed in an H-terminated nanodiamond seeding solution. Electrostatic self-assembly created a uniform nanodiamond layer on the SiO2 surface.
  3. MWCVD Parameters (High-Quality Growth): Conditions were set near normal diamond growth temperatures (800 ± 40 °C) to ensure high-quality diamond crystallinity and maximize boron incorporation, unlike low-temperature approaches.
  4. Gas Composition & Doping: A 1% Methane concentration in H2 mixture was used. A high [B]/[C] gas ratio of 1% was required to achieve the necessary doping level for metallic conductivity.
  5. sp2 Content Removal: Post-growth cleaning involved boiling the filters in a highly corrosive mixture of H2SO4 and HNO3 at 250 °C to eliminate non-diamond (sp2) carbon impurities, crucial for maximizing diamond quality.
  6. Freestanding Membrane Fabrication: Hydrofluoric acid (HF) etching was used to dissolve the underlying SiO2 quartz filter, producing a durable, free-standing porous BDD diamond paper structure.

This research highlights the demand for large-area, high-stability Boron-Doped Diamond (BDD) films, a core product focus for 6CCVD. Our MPCVD technology is perfectly suited to meet and extend the requirements demonstrated in this application.

The successful replication and scaling of this work requires high-quality, heavily doped material:

  • Heavy Boron-Doped PCD (BDD): Required to achieve the metallic conductivity (> 1021 cm-3) and robust mechanical properties necessary for a porous flow-through electrode. 6CCVD provides BDD material optimized for minimal sp2 content, maximizing the electrochemical stability and potential window demonstrated in the paper.
  • Freestanding BDD Films: The method requires removing the template to yield a freestanding membrane. 6CCVD routinely delivers high-purity Polycrystalline Diamond (PCD) wafers and films designed for release, facilitating the complex acid etching process (HF) used in this template removal step.

The constraints and proposed scale-up targets of this research directly align with 6CCVD’s advanced manufacturing capabilities:

Research Requirement6CCVD CapabilitySales Value Proposition
Scale-Up (Industrial Goal)Wafers/Plates up to 125mm (PCD)Facilitates immediate scale-up to near 6-inch industrial standards for high-throughput waste water and chlor-alkali systems.
Thickness ControlSCD/PCD thickness from 0.1”m to 500”mAllows engineers to precisely tune membrane coating depth (the paper used $\sim$80 ”m) for optimal mechanical stability and electrochemical active area.
Metalization IntegrationCustom deposition of Au, Pt, Pd, Ti, W, CuCrucial for high-efficiency current collection and integration into custom reactor setups (e.g., replacement of the Stainless Steel 316 current collector).
Surface FinishPCD polishing to Ra < 5nmWhile porous is required, 6CCVD can ensure the crystalline grains forming the membrane surface meet ultra-low roughness requirements for improved stability and characterization.
LogisticsGlobal shipping (DDU default, DDP available)Secure, reliable supply chain ensures material delivery globally to support R&D and industrial partners working on extreme condition applications.

6CCVD’s in-house PhD team can assist with material selection for similar Electrochemical Separation and Environmental Monitoring projects.

  • Doping Uniformity: We provide consultation to achieve homogeneous BDD doping profiles across large wafers, optimizing electron transfer properties vital for large-scale flow-through reactors.
  • Stability for Extreme Conditions: Our engineers specialize in materials designed for harsh environments, ensuring the BDD selection is compatible with the corrosive (acidic/alkaline) media and high anodic current densities required for chlor-alkali processes and in situ regeneration.
  • Custom Geometric Design: We offer laser cutting and shaping services to produce BDD films with the precise diameters (e.g., the 1 cm diameter working electrode used in the study) and mounting requirements needed for complex electrochemical cell architectures.

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

View Original Abstract

Electrochemically switchable selective membranes play an important role in selective filtration processes such as water desalination, industrial waste treatment, and hemodialysis. Currently, membranes for these purposes need to be optimized in terms of electrical conductivity and stability against fouling and corrosion. In this paper, we report the fabrication of boron-doped diamond membrane by template diamond growth on quartz fiber filters. The morphology and quality of the diamond coating are characterized via SEM and Raman spectroscopy. The membrane is heavily boron doped (>10(21) cm(-3)) with >3 V potential window in aqueous electrolyte. By applying a membrane potential against the electrolyte, the redox active species can be removed via flow-through electrolysis. Compared to planar diamond electrodes, the ∌250 times surface enlargement provided by such a membrane ensures an effective removal of target chemicals from the input electrolyte. The high stability of diamond enables the membrane to not only work at high membrane bias but also to be self-cleaning via in situ electrochemical oxidation. Therefore, we believe that the diamond membrane presented in this paper will provide a solution to future selective filtration applications especially in extreme conditions.