A Free-Standing Boron-Doped Diamond Grid Electrode for Fundamental SpectroelectrochemistryClick to copy article linkArticle link copied!
- Hannah K. PatenaudeHannah K. PatenaudeRadiochemistry Program, Department of Chemistry and Biochemistry, University of Nevada, Las Vegas, Las Vegas, Nevada 89154, United StatesInorganic, Isotope, and Actinide Chemistry, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United StatesMore by Hannah K. Patenaude
- Nastasija DamjanovicNastasija DamjanovicRadiochemistry Program, Department of Chemistry and Biochemistry, University of Nevada, Las Vegas, Las Vegas, Nevada 89154, United StatesMore by Nastasija Damjanovic
- Jason RakosJason RakosRadiochemistry Program, Department of Chemistry and Biochemistry, University of Nevada, Las Vegas, Las Vegas, Nevada 89154, United StatesDepartment of Chemistry and Biochemistry, Miami University, Oxford, Ohio 45056, United StatesNuclear and Chemical Engineering, Pacific Northwest National Laboratory, Richland, Washington 99352, United StatesMore by Jason Rakos
- Dustyn C. WeberDustyn C. WeberRadiochemistry Program, Department of Chemistry and Biochemistry, University of Nevada, Las Vegas, Las Vegas, Nevada 89154, United StatesDepartment of Chemistry and Biochemistry, Miami University, Oxford, Ohio 45056, United StatesMore by Dustyn C. Weber
- Aaron I. JacobsAaron I. JacobsDepartment of Chemistry, Michigan State University, East Lansing, Michigan 48823, United StatesMore by Aaron I. Jacobs
- Samuel A. BryanSamuel A. BryanNuclear and Chemical Engineering, Pacific Northwest National Laboratory, Richland, Washington 99352, United StatesMore by Samuel A. Bryan
- Amanda M. LinesAmanda M. LinesNuclear and Chemical Engineering, Pacific Northwest National Laboratory, Richland, Washington 99352, United StatesMore by Amanda M. Lines
- William R. HeinemanWilliam R. HeinemanDepartment of Chemistry, University of Cincinnati, Cincinnati, Ohio 45221, United StatesMore by William R. Heineman
- Shirmir D. BranchShirmir D. BranchNuclear and Chemical Engineering, Pacific Northwest National Laboratory, Richland, Washington 99352, United StatesMore by Shirmir D. Branch
- Cory A. Rusinek*Cory A. Rusinek*Email: [email protected]. Tel.: 01-513-529-2457.Radiochemistry Program, Department of Chemistry and Biochemistry, University of Nevada, Las Vegas, Las Vegas, Nevada 89154, United StatesDepartment of Chemistry and Biochemistry, Miami University, Oxford, Ohio 45056, United StatesMore by Cory A. Rusinek
Abstract
Spectroelectrochemistry (SEC) is a powerful technique that enables a variety of redox properties to be studied, including formal potential (Eo), thermodynamic values (ΔG, ΔH, ΔS), diffusion coefficient (D), electron transfer stoichiometry (n), and others. SEC requires an electrode which light can pass through while maintaining sufficient electrical conductivity. This has been traditionally composed of metal or metal oxide films atop transparent substrates like glass, quartz, or metallic mesh. Robust electrode materials like boron-doped diamond (BDD) could help expand the environments in which SEC can be performed, but most designs are limited to thin films (∼100–200 nm) on transparent substrates less resilient than free-standing BDD. This work presents a free-standing BDD grid electrode (G-BDD) for fundamental SEC measurements, using the well-characterized Fe(CN)63–/4– redox couple as proof-of-concept. With a combination of cyclic voltammetry (CV), thin-layer SEC, and chronoabsorptometry, several of the redox properties mentioned above were calculated and compared. For Eo′, n, and D, similar results were obtained when comparing the CV [Eo′ = +0.279 (±0.002) V vs Ag/AgCl; n = 0.97; D = 4.1 × 10–6 cm2·s–1] and SEC [Eo′ = +0.278 (±0.001) V vs Ag/AgCl; n = 0.91; D = 5.2 × 10–6 cm2·s–1] techniques. Both values align with what has been previously reported. To calculate D from the SEC data, modification of the classical equation used in chronoabsorptometry was required to accommodate the G-BDD electrode geometry. Overall, this work expands on the applicability of SEC techniques and BDD as a versatile electrode material.
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