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Ladder diagrams are useful tools for understanding redox equilibrium reactions, especially the effects of concentration changes on the electrochemical potential of the reaction. The vertical axis in the redox ladder diagrams represents the electrochemical potential, E. The area of predominance is demarcated using the Nernst equation.
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Chain-growth or addition polymerization is successive addition reactions of monomers with a polymer chain. In radical chain-growth polymerization, the reaction proceeds via a free-radical intermediate. The free radical is formed from radical initiators, which spontaneously generate free radicals by homolytic fission. Organic peroxides (such as dibenzoyl peroxide, as shown in Figure 1) or azo compounds are popular radical initiators. A low concentration ratio of radical initiator to monomer is...
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Oxidation-reduction or redox reactions involve the transfer of electrons from one molecule or atom to another. When an atom gains an electron, another atom must lose an electron, meaning oxidation and reduction must occur together. Since the redox occurs in pairs, the atom that gets oxidized is also called the reducing agent or reductant, and the atom that is reduced is also called the oxidizing agent or oxidant. A straightforward way to remember the definitions of oxidation and reduction is...
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The cationic polymerization mechanism consists of three steps: initiation, propagation, and termination. In the initiation step of the polymerization process, the π bond of a monomer gets protonated by the Lewis acid catalyst, which is formed from boron trifluoride and water. The protonation of the π bond generates a carbocation stabilized by the electron‐donating group. In the propagation step, the π bond of the second monomer acts as a nucleophile and attacks the...
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Updated: Feb 26, 2026

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El pH controla la localización de carga en polímeros de escalera redox-activos

Ana De La Fuente Durán1, Nicholas Siemons1, Adam Marks1

  • 1Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States.

Journal of the American Chemical Society
|February 25, 2026
PubMed
Resumen

El pH de un electrolito impacta significativamente el comportamiento redox de los polímeros conductores iónicos-misto-electrónicos orgánicos (OMIEC), como la poli(benzimidazobenzofenantrolina) (BBL). Este estudio revela que los estados redox acoplados a protones, no solo los estados acoplados a cationes de sal, son cruciales en condiciones neutras a básicas.

Palabras clave:
polímeros conductores orgánicoselectroquímicapolímeros de escaleraredoxpHlocalización de cargaBBL

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Área de la Ciencia:

  • Electroquímica
  • Ciencia de los materiales
  • Química de polímeros

Sus antecedentes:

  • Los polímeros conductores orgánicos iónicos-misto-electrónicos (OMIEC) son materiales clave para la electrónica avanzada.
  • Sus estructuras químicas se adaptan para controlar la localización de carga y la energética orbital.
  • La poli(benzimidazobenzofenantrolina) (BBL) es un OMIEC arquetípico de escalera.

Objetivo del estudio:

  • Investigar la influencia del pH del electrolito en el comportamiento redox del polímero BBL.
  • Elucidar el mecanismo redox de BBL bajo diversas condiciones de pH.
  • Desafiar la suposición de que los protones no participan en los procesos redox en electrolitos neutros a básicos.

Principales métodos:

  • Caracterización electroquímica
  • Espectroscopía Raman in situ
  • Simulaciones ab initio
  • Modelado electroquímico utilizando un marco de solución regular multicomponente

Principales resultados:

  • El comportamiento redox de BBL está fundamentalmente modulado por el pH del electrolito, incluso en condiciones neutras a básicas.
  • Se observó la formación competitiva de distintos estados redox acoplados a protones y acoplados a cationes de sal.
  • El redox acoplado a protones domina en pH neutro, contrariamente a las suposiciones previas de reducción bipolarónica compensada por sal.

Conclusiones:

  • Las propiedades redox de los OMIEC de escalera de tipo n como BBL son complejas y están significativamente influenciadas por el pH.
  • Un diagrama de Pourbaix modificado ilustra el equilibrio sintonizable entre los estados acoplados a protones y acoplados a cationes de sal a través del pH y el potencial.
  • La comprensión de los efectos del pH es crucial para controlar las reacciones electroquímicas acuosas que involucran OMIEC.