Building upon the Koutecky-Levich Equation for Evaluation of Next-Generation Oxygen Reduction Reaction Catalysts

Xu, Shicheng; Kim, Yongmin; Higgins, Drew; Yusuf, Maha; Jaramillo, Thomas F.; Prinz, Fritz B.

doi:10.1016/j.electacta.2017.09.145

Cited by 82 publications

(45 citation statements)

References 64 publications

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“…with number of electrons n , Faraday constant F , electrode area A , diffusion constant D o , rotation speed ω , kinematic viscosity ν , and analyte concentration c o in the bulk solution . K‐L equation has been used recently to describe catalysis of oxygen reduction . Combining equations (1) and (2) and plotting I −1 versus ω −1/2 provides the kinetic current as an intercept:

true \begin{matrix} \frac{1}{I} = \frac{1}{I_{k}} + \frac{1}{ω^{1 / 2}} \cdot \frac{1}{0.62 n F A D_{o}^{2 / 3} ν^{- 1 / 6} c_{o}} \end{matrix}

…”

Section: Resultsmentioning

confidence: 89%

Thermoelectrochemistry of Paracetamol – Studied at Directly Heated Micro‐wire and Rotating Disk Electrodes

et al. 2018

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We compare the thermoelectrochemical behavior of paracetamol (acetaminophen) at both directly heated gold micro‐wire electrodes (1–115 °C) and rotating disk electrodes (100–8000 rpm). Koutecky‐Levich plots were recorded at various temperatures between 23 and 60 °C. The calculated Ik values (representing reaction rate at infinite mass transport) were plotted as Arrhenius‐type graphs, and the obtained energy values of 20–30 kJ/mol depended on the potential chosen for the corresponding Koutecky‐Levich plots. This led to the conclusion that these energy values are not activation energies, but rather an energy difference due to overvoltage as described in the Butler‐Volmer equation. Accordingly, Koutecky‐Levich plots recorded at various temperatures allowed to determine the Butler‐Volmer kinetics including transfer coefficients even at low concentrations. Arrhenius plots obtained at heated micro‐wire electrodes revealed two linear regions corresponding to diffusion control with 16 kJ/mol at high temperature and 20–30 kJ/mol at very low temperature. The latter activation energy values were found in a very narrow temperature range and probably belong to a transition region towards a kinetic activation energy.

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true \begin{matrix} \frac{1}{I} = \frac{1}{I_{k}} + \frac{1}{ω^{1 / 2}} \cdot \frac{1}{0.62 n F A D_{o}^{2 / 3} ν^{- 1 / 6} c_{o}} \end{matrix}

…”

Section: Resultsmentioning

confidence: 89%

Thermoelectrochemistry of Paracetamol – Studied at Directly Heated Micro‐wire and Rotating Disk Electrodes

et al. 2018

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“…This behavior has been observed with other heme‐copper oxygen reductases, including cytochrome aa 3 from Paracoccus denitrificans , cytochrome ba 3 oxidase from Thermus thermophilus and cytochrome cbb 3 oxidases from Pseudomonas stutzeri , Rhodobacter sphaeroides and Vibrio cholerae and it is typical for the electrocatalytic reduction of O 2 . The limiting current at −0.4 V increases as a function of the electrode rotation speed, and follows a Koutecky–Levich relationship (see Fig. S7 in supplementary materials).…”

Section: Resultsmentioning

confidence: 93%

Role of the tightly bound quinone for the oxygen reaction of cytochrome bo₃ oxidase from Escherichia coli

et al. 2018

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The coupling of the reaction of a tightly bound ubiquinone with the reduction of O2 in cytochrome bo3 of Escherichia coli was investigated. In the absence of the quinone, a strongly diminished rate of electrocatalytic reduction of oxygen is detected, which can be restored by adding quinones. The correlation of previous EPR data with the electrocatalytic study on mutations in the binding site at positions, Q101, D75, F93, H98, I102 and R71 reveal that the stabilization of the radical is not necessary for the oxygen reaction. The Q101 and F93 variants exhibit both well‐defined catalytic i–V curves, whereas D75H, H98F, I102W and R71H exhibit broad i–V curves with large hysteresis pointing toward a strong alteration in their catalytic activity.

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“…[13,14] In the case of ORR, owing to the low solubility,o xygen is ar eactantt hat even at very low overpotentials can be depleted at the electrode surface. The Levich-Koutecky equation is routinelyu sed to separate kinetic from diffusion effects;h owever,t he equation in its usual form is valid only in the cases where the reactionm echanism follows first order kinetics with respect to the reactant that exhibits diffusional limitation.…”

Section: Levich-koutecky Equation Appliedf or Various Kineticreactionmentioning

confidence: 99%

“…The Levich-Koutecky equation is routinelyu sed to separate kinetic from diffusion effects;h owever,t he equation in its usual form is valid only in the cases where the reactionm echanism follows first order kinetics with respect to the reactant that exhibits diffusional limitation. [13,14] In the case of ORR, owing to the low solubility,o xygen is ar eactantt hat even at very low overpotentials can be depleted at the electrode surface. However,t here is al arge possibility that the reactioni sn ot followingf irst order kinetics.…”

Section: Levich-koutecky Equation Appliedf or Various Kineticreactionmentioning

confidence: 99%

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Frequent Pitfalls in the Characterization of Electrodes Designed for Electrochemical Energy Conversion and Storage

Žeradjanin

2018

ChemSusChem

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Focus on the importance of energy conversion and storage boosted research interest in various electrocatalytic materials. Characterization of solid-liquid interfaces during faradaic and non-faradaic processes is routinely conducted in many laboratories worldwide on a daily basis. This can be deemed as a very positive tendency. However, careful insight into modern literature suggests frequent misuse of electroanalytical tools. This can have very negative implications and postpone overall development of electrocatalytic materials with the desired properties. This work points out some of the frequent pitfalls in electrochemical characterization, suggests potential solutions, and above all encourages comprehensive analysis and in-depth thinking about electrochemical phenomena.

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Building upon the Koutecky-Levich Equation for Evaluation of Next-Generation Oxygen Reduction Reaction Catalysts

Cited by 82 publications

References 64 publications

Thermoelectrochemistry of Paracetamol – Studied at Directly Heated Micro‐wire and Rotating Disk Electrodes

Thermoelectrochemistry of Paracetamol – Studied at Directly Heated Micro‐wire and Rotating Disk Electrodes

Role of the tightly bound quinone for the oxygen reaction of cytochrome bo₃ oxidase from Escherichia coli

Frequent Pitfalls in the Characterization of Electrodes Designed for Electrochemical Energy Conversion and Storage

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Building upon the Koutecky-Levich Equation for Evaluation of Next-Generation Oxygen Reduction Reaction Catalysts

Cited by 82 publications

References 64 publications

Thermoelectrochemistry of Paracetamol – Studied at Directly Heated Micro‐wire and Rotating Disk Electrodes

Thermoelectrochemistry of Paracetamol – Studied at Directly Heated Micro‐wire and Rotating Disk Electrodes

Role of the tightly bound quinone for the oxygen reaction of cytochrome bo3 oxidase from Escherichia coli

Frequent Pitfalls in the Characterization of Electrodes Designed for Electrochemical Energy Conversion and Storage

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Role of the tightly bound quinone for the oxygen reaction of cytochrome bo₃ oxidase from Escherichia coli