Evaluation of interfacial pH change during water splitting at pulsed regime using finite element method

Wosiak, Gabriel; Silva, Mariana Cristina; Silva, Jeyse da; Carneiro‐Neto, Evaldo B.; Lopes, Mauro Chierici; Pereira, Ernesto C.

doi:10.1016/j.ijhydene.2021.02.195

Cited by 10 publications

(3 citation statements)

References 51 publications

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“…Before performing a closed cell BPE electrochemical oxidative degradation experiment, the ability of the two BDD particles to electrochemically oxidise / reduce water using the BPE set-up was explored. Electrochemical oxidation / reduction of water will result in a local decrease / increase in pH, respectively [32]. Here, electrochemical water splitting by BDD-1 (cathodic pole) and BDD-2 (anodic pole) was 11).…”

Section: Resultsmentioning

confidence: 91%

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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Section: Resultsmentioning

confidence: 91%

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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“…The time taken for the first plateau is denoted as transition time, τ. The sharp change in overpotential 14,15 could be an indication of the depletion of proton concentration and the onset of water reduction on cobalt causing a deviation of interfacial pH to alkaline value. On Co, the HER follows the V-H mechanism.…”

Section: Resultsmentioning

confidence: 99%

Butynediol’s Role beyond Brightening Additive during Electrodeposition of Cobalt

Muniyandi¹,

Lakshminarasimhan²,

Jeyabharathi³

2022

J. Electrochem. Soc.

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Butynediol (2-Butyne-1,4-diol), a well-known type-II brightening additive, changes the interfacial pH resulting in the formation of porous cobalt hydroxide film of ca. 1 µm thickness over the copper substrate in a short duration of electrodeposition (2 min.) and at a very low current density (−5 mA/cm2) from sulfate bath. In the absence of butynediol, a metallic cobalt layer was observed under identical deposition conditions. The choice of anions (sulfates, chlorides and nitrates) in the electrodeposition bath determines the kind of electrodeposited films obtained, viz., cobalt, cobalt/cobalt hydroxide, and compact cobalt hydroxide. The adsorption of butynediol enhances hydrogen evolution due to water reduction that facilitates the formation of porous microstructures of cobalt hydroxide. Competition for adsorption sites between butynediol and chloride and dissolution of cobalt hydroxide by diffusing protons result in a mixed metallic cobalt particle and porous cobalt hydroxide microstructure. The variation in the phases and microstructures of electrodeposits was evidenced through the difference in the magnetic and electrocatalytic properties of the films.

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“…2 are under the assumption of planar diffusion, which can be slower than the scenario of hemispherical growth of individual particles. For reference, the rate of local pH change at the similar overpotential is at a similar or higher order of magnitude [77], which might interact with the depositing species by forming hydroxides or changing their complexation structures [78].…”

Section: Characteristic Time For the Rate Of Local Concentration Dropmentioning

confidence: 99%

Estimated and observed nucleation densities of electrodeposited Cu and Cu-Ag particles at n-Si(001) substrate

Sun,

Zangari

2023

Preprint

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We have examined the particle density of electrodeposited Cu and Cu-Ag particles from acidic sulfate bath. Based on the potentiostatic transients, the nucleation densities of the deposits were estimated with the Scharifker-Hills model, the Scharifker-Mostany model, the Heerman-Tarallo model, the approach proposed by Sluyters-Rehbach et al., and the model based on the roughness of the planar diffusion field from the one-point correlation function. All the fitted nucleation densities significantly underestimate the particle density observed under SEM. The average grain size suggests that all the nuclei are growing with respect to time. Those behaviors suggest that the coalescence of the diffusion fields occurs much earlier than the full coalescence of the nucleation exclusion zones. Furthermore, we have also attempted to explain the observed nucleation densities with the surface defect density of heavily-doped n-Si(001) substrate and the volume of the electrolyte required for forming the critical nucleus of Cu or Ag. The assumption that the Cu(II) species are immediately consumed at the substrate has been justified, from which a characteristic time is proposed to evaluate the impact of the rate of concentration drop on the mass-transfer behavior of the system.

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Evaluation of interfacial pH change during water splitting at pulsed regime using finite element method

Cited by 10 publications

References 51 publications

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

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

Butynediol’s Role beyond Brightening Additive during Electrodeposition of Cobalt

Estimated and observed nucleation densities of electrodeposited Cu and Cu-Ag particles at n-Si(001) substrate

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