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Electrochemistry is the branch of chemistry that studies the relationship between electrical quantities and chemical reactions, particularly oxidation and reduction. Oxidation is the loss of electrons from a substance, whereas reduction refers to the gain of electrons. A substance with a strong electron affinity is called an oxidizing agent (oxidant), and a reducing agent (reductant) is a species that donates electrons. Oxidation and reduction processes are pivotal to electrochemical reactions,...
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Imagine a bucket of water. It contains many molecules, of the order of 1026 molecules. Thus, although it contains discrete elements (molecules) at the microscopic level, macroscopically, it can be considered continuous. Small volume elements of water, infinitesimal compared to the bulk of the bucket's volume, still contain many molecules. Under this framework, quantized matter is approximated as continuous for practical purposes.
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Understanding molecular and electrochemical charge transfer: theory and computations.

Renat R Nazmutdinov1, Shokirbek A Shermokhamedov1, Tamara T Zinkicheva1

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This study reviews theoretical frameworks for electron, proton, and proton-coupled electron transfer (PCET) in chemistry and biology. It bridges theory with experiments, covering molecular processes, interfaces, and single-molecule electrochemistry.

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Area of Science:

  • Physical Chemistry
  • Electrochemistry
  • Chemical Physics
  • Biophysics

Background:

  • Electron, proton, and proton-coupled electron transfer (PCET) are fundamental to chemical, electrochemical, and biological processes.
  • Understanding these charge transfer mechanisms is crucial for advancing fields from catalysis to bioenergetics.
  • Existing theoretical models require comprehensive integration with experimental observations.

Purpose of the Study:

  • To provide an overview of theoretical formalisms for molecular charge transfer processes.
  • To illustrate the application of these theories in bridging experimental data with electron, proton, and PCET phenomena.
  • To explore advanced topics including single-molecule electrochemistry and computational interface studies.

Main Methods:

  • Review of theoretical frameworks for homogeneous and interfacial charge transfer.
  • Application of theories to specific examples like S2O8(2-) reduction and dihydrogen evolution.
  • Integration of scanning probe microscopy (STM, AFM) for single-molecule electrochemistry.
  • Computational methods for analyzing electrochemical interfaces and molecular structures.

Main Results:

  • Demonstrated theoretical approaches for electron, proton, and PCET processes, including complex molecular reorganization.
  • Highlighted the utility of stochastic chemical rate theory for non-traditional charge transfer behavior.
  • Showcased single-molecule electrochemistry insights from STM/AFM studies on molecular monolayers and biomolecules.
  • Presented computational challenges and perspectives in interface science, catalysis, and spintronics.

Conclusions:

  • The presented theoretical formalisms provide a robust framework for understanding diverse charge transfer processes.
  • Bridging theory and experiment is essential for accurate modeling and prediction of molecular behavior.
  • Advanced techniques like single-molecule electrochemistry and computational modeling open new avenues for research.