Electrochemistry needs electrochemists: “goodbye to rotating discs”

Compton, Richard G.; Sokolov, Stanislav V.

doi:10.1007/s10008-023-05443-8

Cited by 5 publications

(4 citation statements)

References 45 publications

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“…With the modification of the different molecules at the GCE interface, the impedance of the GCE increased gradually (TPE-2SO 3 Na > TPE-4SO 3 Na > C 4 H 8 -2SO 3 Na > Bare GCE). The increasing impedance indicated that the electrode interface coverage increased gradually, which further indicated that π-conjugated molecules were increasingly modified on the electrode. , It was confirmed that the gradual increase of the GCE interface of the π-conjugated structure could promote the π–π interaction with Ru(bpy) 3 2+ , resulting in signal amplification, which was consistent with the ECL signal enhancement trend shown in Figure A. To further study the effect of the π–π interaction on the Ru(bpy) 3 2+ -TPA ECL system, CV curves were measured on the bare GCE and the sulfonic acid-functionalized molecule-modified electrode (Figure S19).…”

Section: Resultssupporting

confidence: 67%

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Sulfonic Acid-Functionalized Tetraphenylethylene-Amplified Electrochemiluminescence by Regulating π–π Interaction

Fu,

Pan,

Liu

et al. 2024

Anal. Chem.

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The electrochemiluminescence (ECL) effectiveness of the tris-(bipyridine) ruthenium(II) (Ru(bpy) 3 2+ ) system is hampered by aggregation-caused quenching (ACQ) in optoelectronic systems as a result of π−π accumulation of the aromatic ring structure. In this work, a negatively charged tetraphenylvinyl molecule (TPE-2SO 3 Na, TPE-4SO 3 Na) was synthesized to modify the electrode interface, and the π−π accumulation between Ru(bpy) 3 2+ molecules was transformed into the π−π interaction between Ru(bpy) 3 2+ and TPE molecules. Interestingly, the ECL signal intensity of the Ru(bpy) 3 2+ -tripropylamine (TPA) system in the presence of TPE-2SO 3 Na was increased by about 15 times due to the π−π action and electrostatic action. In comparison with traditional physical packaging with porous zeolites, metal− organic frameworks (MOFs), and covalent organic frameworks (COFs), the fabricated electrode interface modification strategy was simple and efficient to avoid π−π accumulation in aqueous solutions. Our success will inspire other researchers to investigate the supramolecular interaction (π−π interaction, electrostatic interaction, hydrophilic interaction, and host−guest interaction) at the electrode interface to amplify the ECL intensities of Ru(bpy) 3 2+ .

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Section: Resultssupporting

confidence: 67%

“…The increasing impedance indicated that the electrode interface coverage increased gradually, which further indicated that π-conjugated molecules were increasingly modified on the electrode. 36,37 It was confirmed that the gradual increase of the GCE interface of the π-conjugated structure could promote the π−π interaction with Ru(bpy) 3…”

Section: +mentioning

confidence: 92%

Sulfonic Acid-Functionalized Tetraphenylethylene-Amplified Electrochemiluminescence by Regulating π–π Interaction

Fu,

Pan,

Liu

et al. 2024

Anal. Chem.

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“…The desire to extract more information from the RDE and RRDE measurements than possible leads to the misuse of these techniques . The models are based on flat and smooth electrodes, meaning the macroscopically rough (nonflat and nonuniform) catalyst layers can cause additional complications.…”

Section: Comparison Of Methods: Critical Differencesmentioning

confidence: 99%

Design and Impact: Navigating the Electrochemical Characterization Methods for Supported Catalysts

Kasuk,

Nerut,

Grozovski

et al. 2024

ACS Catal.

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This review will investigate the impact of electrochemical characterization method design choices on intrinsic catalyst activity measurements by predominantly using the oxygen reduction reaction (ORR) on supported catalysts as a model reaction. The wider use of hydrogen for transportation or electrical grid stabilization requires improvements in proton exchange membrane fuel cell (PEMFC) performance. One of the areas for improvement is the (ORR) catalyst efficiency and durability. Research and development of the traditional platinum-based catalysts have commonly been performed using rotating disk electrodes (RDE), rotating ring disk electrodes (RRDE), and membrane electrode assemblies (MEAs). However, the mass transport conditions of RDE and RRDE limit their usefulness in characterizing supported catalysts at high current densities, and MEA characterizations can be complex, lengthy, and costly. Ultramicroelectrode with a catalyst-filled cavity addresses some of these problems, but with limited success. Due to the properties discussed in this review, the recent floating electrode (FE) and the gas diffusion electrode (GDE) methods offer additional capabilities in the electrochemical characterization process. With the FE technique, the intrinsic activity of catalysts for ORR can be investigated, leading to a better understanding of the ORR mechanism through more reliable experimental data from applicationrelevant high-mass transport conditions. The GDEs are helpful bridging tools between RDE and MEA experiments, simplifying the fuel cell and electrolyzer manufacturing and operating optimization process.

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“…The rotating disk electrode is the most popular hydrodynamic electrode and is widely used by electro-analysts as well as fundamental electrochemists, not least since the device provides a well-defined convective flow of solution (analyte) to the electrode surface, allowing steady-state measurements. 12 A schematic flow profile is shown in Figure 1 a,b and the resulting diffusion-controlled currents have long been known, arising from the theoretical work of Levich 13 and rigorously validated experimentally by the Frumkin School of Electrochemistry. 14 In particular, Levich established the following equation for the transport-controlled steady-state current and diffusion layer thickness at the rotating electrode where the symbols are defined in Table 1 .…”

Section: Introductionmentioning

confidence: 99%

Rotating Disk Electrodes beyond the Levich Approximation: Physics-Informed Neural Networks Reveal and Quantify Edge Effects

Chen,

Kätelhön,

Compton

2023

Anal. Chem.

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Physics-informed neural networks are used to characterize the mass transport to the rotating disk electrode (RDE), the most widely employed hydrodynamic electrode in electroanalysis. The PINN approach was first quantitatively verified via 1D simulations under the Levich approximation for cyclic voltammetry and chronoamperometry, allowing comparison of the results with finite difference simulations and analytical equations. However, the Levich approximation is only accurate for high Schmidt numbers (Sc > 1000). The PINN approach allowed consideration of smaller Sc, achieving an analytical level of accuracy (error <0.1%) comparable with independent numerical evaluation and confirming that the errors in the Levich equation can be as high as 3% when Sc = 1000 for rapidly diffusing species in aqueous solution. Entirely novel, the PINNs permit the solution of the 2D diffusion equation under cylindrical geometry incorporating radial diffusion and reveal the rotating disk electrode edge effect as a consequence of the nonuniform accessibility of the disc with greater currents flowing near the extremities. The contribution to the total current is quantified as a function of the rotation speed, disk radius, and analyte diffusion coefficient. The success in extending the theory for the rotating disk electrode beyond the Levich equation shows that PINNs can be an easier and more powerful substitute for conventional methods, both analytical and simulation based.

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Electrochemistry needs electrochemists: “goodbye to rotating discs”

Cited by 5 publications

References 45 publications

Sulfonic Acid-Functionalized Tetraphenylethylene-Amplified Electrochemiluminescence by Regulating π–π Interaction

Sulfonic Acid-Functionalized Tetraphenylethylene-Amplified Electrochemiluminescence by Regulating π–π Interaction

Design and Impact: Navigating the Electrochemical Characterization Methods for Supported Catalysts

Rotating Disk Electrodes beyond the Levich Approximation: Physics-Informed Neural Networks Reveal and Quantify Edge Effects

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