Der präexponentielle Faktor in der Elektrochemie

He, Zheng‐Da; Chen, Yan‐Xia; Santos, Elizabeth; Schmickler, Wolfgang

doi:10.1002/ange.201800130

Cited by 4 publications

(2 citation statements)

References 53 publications

(101 reference statements)

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“…This has, unfortunately, remained unattainable due to theoretical and methodological difficulties and omissions. [25] Surprisingly, a general GCE rate theory has not yet been established; mending this deficiency is the central goal of the present work.…”

Section: Introductionmentioning

confidence: 95%

“…In particular, both vibronic and electronic non-adiabatic effects are frequently encountered in outer-sphere and long-range ET, PT, and PCET reactions. [25,33] Even for electrocatalytic reactions, non-adiabaticity may be present and the importance and contribution of non-adiabaticity may depend on the electrode potential. [34,35] As a concrete example, it has been shown that only the inclusion of vibronic non-adiabaticity in electrochemical hydrogen evolution reaction can explain experimentally observed Tafel slopes and kinetic isotope effects.…”

Section: Introductionmentioning

confidence: 99%

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Grand canonical rate theory for electrochemical and electrocatalytic systems I: General formulation and proton-coupled electron transfer reactions

Melander

2020

Preprint

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Section: Introductionmentioning

confidence: 95%

Section: Introductionmentioning

confidence: 99%

Grand canonical rate theory for electrochemical and electrocatalytic systems I: General formulation and proton-coupled electron transfer reactions

Melander

2020

Preprint

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Electrocatalysis Beyond 2020: How to Tune the Preexponential Frequency Factor

et al. 2021

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After a century of research on electrocatalytic reactions, a universal theory of electrocatalysis is still not established due to limited understanding of complex energy conversion processes at electrified electrode‐electrolyte interfaces. Most of the research efforts directed toward the acceleration of important electrocatalytic reactions (e. g. hydrogen evolution reaction) were in the direction of minimizing activation energy by tuning the adsorption energies of key intermediates. This kind of approach is well‐established and, importantly, in some cases it was valuable by predicting the design of electrocatalysts with advanced properties. However, in some very important research endeavors, advancement in performance of newly designed electrocatalysts could not be attributed to altered/minimized activation energy. Important to note is that modern electrocatalysis almost completely disregards influence of the preexponential factor on reaction rate. In this work, we open some important questions relevant for future of electrocatalysis and electrochemical energy conversion, with special focus on preexponential factor as major contributor to electrocatalytic reaction rate.

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Structure–Reactivity Effects of Biomass‐based Hydroxyacids for Sustainable Electrochemical Hydrogen Production

et al. 2021

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Biomass electro‐oxidation is a promising approach for the sustainable generation of H2 by electrolysis with simultaneous synthesis of value‐added chemicals. In this work, the electro‐oxidation of two structurally different organic hydroxyacids, lactic acid and gluconic acid, was studied comparatively to understand how the chemical structure of the hydroxyacid affects the electrochemical reactivity under various conditions. It was concluded that hydroxyacids such as gluconic acid, with a considerable density of C−OH groups, are highly reactive and promising for the sustainable generation of H2 by electrolysis at low potentials and high conversion rates (less than −0.15 V vs. Hg/HgO at 400 mA cm−2) but with low selectivity to specific final products. In contrast, the lower reactivity of lactic acid did not enable H2 generation at very high conversion rates (<100 mA cm−2), but the reaction was significantly more selective (64 % to pyruvic acid). This work shows the potential of biomass‐based organic hydroxyacids for sustainable generation of H2 and highlights the importance of the chemical structure on the reactivity and selectivity of the electro‐oxidation reactions.

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Der präexponentielle Faktor in der Elektrochemie

Cited by 4 publications

References 53 publications

Grand canonical rate theory for electrochemical and electrocatalytic systems I: General formulation and proton-coupled electron transfer reactions

Grand canonical rate theory for electrochemical and electrocatalytic systems I: General formulation and proton-coupled electron transfer reactions

Electrocatalysis Beyond 2020: How to Tune the Preexponential Frequency Factor

Structure–Reactivity Effects of Biomass‐based Hydroxyacids for Sustainable Electrochemical Hydrogen Production

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