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Related Concept Videos

The Nernst Equation02:59

The Nernst Equation

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Nonstandard Reaction Conditions
The interconnection between standard cell potentials and various thermodynamic parameters such as the standard free energy change ΔG° and equilibrium constant K has been previously explored. For example, a redox reaction involving zinc(II) and tin(II) ions at 1 M concentration with Eºcell = +0.291 V and ΔG° = −56.2 kJ is spontaneous.
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Oxidation and Reduction of Organic Molecules01:19

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Energy production within a cell involves many coordinated chemical pathways. Most of these pathways are combinations of oxidation and reduction reactions, which occur at the same time. An oxidation reaction strips an electron from an atom in a compound, and the addition of this electron to another compound is a reduction reaction. Because oxidation and reduction usually occur together, these pairs of reactions are called redox reactions.
The removal of an electron from a molecule, results in a...
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Electron Carriers01:24

Electron Carriers

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Electron carriers can be thought of as electron shuttles. These compounds can easily accept electrons (i.e., be reduced) or lose them (i.e., be oxidized). They play an essential role in energy production because cellular respiration is contingent on the flow of electrons.
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Electron Transport Chains01:28

Electron Transport Chains

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The final stage of cellular respiration is oxidative phosphorylation that consists of two steps: the electron transport chain and chemiosmosis. The electron transport chain is a set of proteins found in the inner mitochondrial membrane in eukaryotic cells. Its primary function is to establish a proton gradient that can be used during chemiosmosis to produce ATP and generate electron carriers, such as NAD+ and FAD, that are used in glycolysis and the citric acid cycle.
The ETC is comprised of...
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Redox Equilibria: Overview01:23

Redox Equilibria: Overview

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A reduction-oxidation reaction is commonly called a redox reaction. In a redox reaction, electrons are transferred from one species to another rather than being shared between or among atoms. The reducing agent or reductant is the species that loses electrons and gets oxidized in the process. The species that gains electrons and gets reduced in the process is the oxidizing agent or oxidant. Redox reactions are represented as two separate equations called half-reactions, where one equation...
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Oxidation-Reduction Reactions03:11

Oxidation-Reduction Reactions

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Oxidation–Reduction Reactions
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Protein Film Infrared Electrochemistry Demonstrated for Study of H2 Oxidation by a [NiFe] Hydrogenase
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Proton-Relaying Adsorbates Induce Non-Nernstian Behavior in Oxygen Reduction.

Lulu Zhang1,2,3, Dongchen Zhao1, Weiqiang Tang2

  • 1Hefei National Research Center for Physical Sciences at Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China.

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|August 21, 2025
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Summary

Proton-coupled electron transfer (PCET) shows non-Nernstian behavior in oxygen reduction reactions due to sulfate anions acting as proton donors. This finding impacts electrocatalysis understanding and design.

Keywords:
adsorbed sulfate anionsanion- and cation-dependent pH effectshierarchical theoretical modellocal reaction environmentnon-Nernstian behavioroxygen reduction reactionproton-relaying role

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Area of Science:

  • Electrochemistry
  • Surface Science
  • Computational Chemistry

Background:

  • Proton-coupled electron transfer (PCET) is crucial for energy conversion.
  • Nernst equation predicts a -60 mV/pH shift for PCET equilibrium potentials.
  • Deviations from Nernstian behavior are observed in specific electrochemical reactions.

Purpose of the Study:

  • Investigate deviations from Nernstian behavior in the oxygen reduction reaction (ORR) at Pt(111).
  • Elucidate the role of anions and cations in pH-dependent electrocatalysis.
  • Understand the influence of the local reaction environment (LRE) on PCET.

Main Methods:

  • Density functional theory (DFT) calculations.
  • Multistep microkinetic modeling.
  • Local reaction environment (LRE) model incorporating mass transport and electrical double layer effects.

Main Results:

  • Observed significant deviations from Nernstian behavior in H2SO4/M2SO4 solutions, dependent on cation identity (Li, Cs).
  • Identified adsorbed sulfate anions as key mediators of proton transfer, forming bisulfate species.
  • Determined reduced proton reaction orders (0.5-0.75) in sulfate solutions compared to perchlorate (1).

Conclusions:

  • Adsorbed sulfate anions alter the proton donor mechanism in ORR, explaining non-Nernstian pH dependence.
  • Anion and cation identity significantly modulate LRE effects in electrocatalysis.
  • Combined theoretical and computational methods can unravel complex electrochemical reaction mechanisms.