Electrochemical Ozone Generation Using Compacted High Pressure High Temperature Synthesized Boron Doped Diamond Microparticle Electrodes

Wood, Georgia; Rodríguez, Irina Terrero; Tully, Joshua J.; Chaudhuri, Shayantan; Macpherson, Julie V.

doi:10.1149/1945-7111/ac3ff4

Cited by 11 publications

(4 citation statements)

References 39 publications

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“…For many technological applications, the most common approach to growing diamond is via the process of chemical vapor deposition (CVD) 4 . Whilst high pressure, high temperature (HPHT) synthesis has also found use, it can be difficult to control impurity content via HPHT 5 , hence the preferred use of CVD-grown crystals in many technological applications 6 . For large-area applications, it is much cheaper to grow polycrystalline diamond (PCD) than singlecrystal diamond (SCD); PCD has numerous industrial applications, such as in thermal management 7 and electrochemistry.…”

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confidence: 99%

Coexistence of carbonyl and ether groups on oxygen-terminated (110)-oriented diamond surfaces

et al. 2022

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Diamond-based materials have unique properties that are exploited in many electrochemical, optical, thermal, and quantum applications. When grown via chemical vapor deposition (CVD), the growth rate of the (110) face is typically much faster than the other two dominant crystallographic orientations, (111) and (100). As such, achieving sufficiently large-area and high-quality (110)-oriented crystals is challenging and typically requires post-growth processing of the surface. Whilst CVD growth confers hydrogen terminations on the diamond surface, the majority of post-growth processing procedures render the surface oxygen-terminated, which in turn impacts the surface properties of the material. Here, we determine the oxygenation state of the (110) surface using a combination of density functional theory calculations and X-ray photoelectron spectroscopy experiments. We show that in the 0–1000 K temperature range, the phase diagram of the (110) surface is dominated by a highly stable phase of coexisting and adjacent carbonyl and ether groups, while the stability of peroxide groups increases at low temperatures and high pressures. We propose a mechanism for the formation of the hybrid carbonyl-ether phase and rationalize its high stability. We further corroborate our findings by comparing simulated core-level binding energies with experimental X-ray photoelectron spectroscopy data on the highest-quality (110)-oriented diamond crystal surface reported to date.

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Coexistence of carbonyl and ether groups on oxygen-terminated (110)-oriented diamond surfaces

et al. 2022

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“…For most electrochemical applications, polycrystalline diamond is used. The diamond electrode is commonly grown via chemical vapor deposition (CVD), , as opposed to high-pressure, high-temperature synthesis. Depending on CVD growth conditions, the (110) facet typically grows faster than the (111) and (100) facets. − In polycrystalline samples, which are typically cheaper to grow than single-crystal samples for large-area technological applications, the (110) facets can be revealed by mechanically polishing to a surface roughness where the surface is predominantly (110)-textured, as has been experimentally demonstrated using electron backscatter diffraction and STEM .…”

Section: Methodsmentioning

confidence: 99%

“…For most electrochemical applications, polycrystalline diamond is used. The diamond electrode is commonly grown via chemical vapor deposition (CVD), 93,94 as opposed to high-pressure, high-temperature 95 synthesis. Depending on CVD growth conditions, the (110) facet typically grows faster than the (111) and (100) facets.…”

Section: Construction Of Structuresmentioning

confidence: 99%

Stability of Single Gold Atoms on Defective and Doped Diamond Surfaces

2023

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Polycrystalline boron-doped diamond (BDD) is widely used as a working electrode material in electrochemistry, and its properties, such as its stability, make it an appealing support material for nanostructures in electrocatalytic applications. Recent experiments have shown that electrodeposition can lead to the creation of stable small nanoclusters and even single gold adatoms on the BDD surfaces. We investigate the adsorption energy and kinetic stability of single gold atoms adsorbed onto an atomistic model of BDD surfaces by using density functional theory. The surface model is constructed using hybrid quantum mechanics/ molecular mechanics embedding techniques and is based on an oxygen-terminated diamond (110) surface. We use the hybrid quantum mechanics/molecular mechanics method to assess the ability of different density functional approximations to predict the adsorption structure, energy, and barrier for diffusion on pristine and defective surfaces. We find that surface defects (vacancies and surface dopants) strongly anchor adatoms on vacancy sites. We further investigated the thermal stability of gold adatoms, which reveals high barriers associated with lateral diffusion away from the vacancy site. The result provides an explanation for the high stability of experimentally imaged single gold adatoms on BDD and a starting point to investigate the early stages of nucleation during metal surface deposition.

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“…Recently, it has been shown that aluminium diboride (AlB 2 ) can be used as both a boron source and as an agent to remove nitrogen during the HPHT growth process. This process results in the growth of BDD particles, as small as 80 μm in size and doped with enough boron > 10 20 B atoms cm − 3 [5] to demonstrate metal-like electrochemical behaviour [6,7].…”

Section: Introductionmentioning

confidence: 99%

A Closed Bipolar Electrochemical Cell for the Interrogation of BDD Single Particles: Electrochemical Advanced Oxidation

Dettlaff,

Tully,

Wood

et al. 2024

Preprint

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A closed bipolar electrochemical cell containing two conductive boron-doped diamond (BDD) particles of size 250 – 350 um, produced by high-pressure high-temperature (HPHT) synthesis, has been used to demonstrate the applicability of single BDD particles for electrochemical oxidative degradation of the dye, methylene blue (MB). The cell is fabricated using stereolithography 3D printing and the BDD particles are located at either end of a solution excluded central channel. Platinum wire electrodes placed in each of the two outer solution compartments are used to drive electrochemical reactions at the two BDD particles, which, under bipolar conditions do not require direct electrical connection to a potential source. Experiments using ultra high-performance liquid chromatography coupled with mass spectrometry (UHPLC-MS) show that the anodic pole BDD particle is able to electrochemically remove > 99% of the dye (originally present at 1 x 10-4 M) to undetectable UHPLC-MS products in 600 s. Monitoring of the time dependant change in MB peak area, from the UHPLC chromatograms, enables a pseudo first order rate constant of 0.54 min-1 to be determined for MB removal. Given the large scale at which such particles can be produced (tonnes), such data bodes well for scale up opportunities using HPHT-grown BDD particles, where the particles can be assembled into high surface area electrode formats.

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Electrochemical Ozone Generation Using Compacted High Pressure High Temperature Synthesized Boron Doped Diamond Microparticle Electrodes

Cited by 11 publications

References 39 publications

Coexistence of carbonyl and ether groups on oxygen-terminated (110)-oriented diamond surfaces

Coexistence of carbonyl and ether groups on oxygen-terminated (110)-oriented diamond surfaces

Stability of Single Gold Atoms on Defective and Doped Diamond Surfaces

A Closed Bipolar Electrochemical Cell for the Interrogation of BDD Single Particles: Electrochemical Advanced Oxidation

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