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Catalizadores de indio para la copolimerización de apertura de anillos de epoxido de baja presión CO2: ¿Evidencia de

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  • 1Department of Chemistry , University of Oxford , 13 Mansfield Road , Oxford OX1 3TA , United Kingdom.

Journal of the American Chemical Society
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Resumen
Este resumen es generado por máquina.

Los nuevos catalizadores de indio permiten una eficiente copolimización de dióxido de carbono y epóxidos a través de una vía mononuclear distinta. Estos complejos de fosfasaleno logran una alta selectividad y permiten la caracterización de los productos intermedios clave.

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Área de la Ciencia:

  • Química de los polímeros
  • Química organometálica
  • Catálisis

Sus antecedentes:

  • La copolimización alterna de dióxido de carbono (CO2) y epóxidos es crucial para la utilización de CO2 en la síntesis de polímeros.
  • Las vías catalíticas existentes son típicamente bimetálicas o bicomponentes, lo que limita la comprensión mecánica.
  • Es necesario desarrollar nuevos catalizadores para explorar mecanismos de reacción alternativos.

Objetivo del estudio:

  • Introducir los primeros catalizadores de indio para la copolimerización de CO2/epoxido.
  • Para elucidar una vía catalítica mononuclear distinta.
  • Caracterizar los intermediarios catalíticos clave y comprender su comportamiento de coordinación.

Principales métodos:

  • Síntesis y caracterización de los complejos de indio ligados al fosfazaleno.
  • Investigación de la actividad catalítica bajo baja presión de CO2 (1 bar).
  • Aislamiento y análisis espectroscópico de los intermediarios catalíticos (complejos de alcóxido y carbonato).
  • Estudios cinéticos y seguimiento espectroscópico in situ.

Principales resultados:

  • Los complejos de fosfazaleno de indio presentan una alta actividad y selectividad (>99% de enlace de carbonato, >70% de isoselectividad) para la copolimización de CO2/epoxido.
  • Los catalizadores funcionan eficazmente sin cocatalizadores a una presión de 1 bar de CO2.
  • Se aislaron y caracterizaron los compuestos intermedios mononucleares de alcóxido de indio (pentacoordinado) y carbonato (hexacoordinado).
  • Los datos cinéticos y los estudios in situ confirman una vía mononuclear con dependencia de primer orden de la concentración del catalizador y dependencia de orden cero de la presión de CO2.

Conclusiones:

  • Los catalizadores de indio, en particular los complejos de fosfasalenos, funcionan a través de una nueva vía mononuclear en la copolimización de CO2 / epoxido.
  • La capacidad de aislar y caracterizar los intermedios proporciona raras perspectivas sobre el ciclo catalítico.
  • Este trabajo abre caminos para diseñar otros catalizadores homogéneos, potencialmente utilizando metales más grandes, para operar a través de mecanismos mononucleares.