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Cables de dirutenio-poli-diil-dirutenio: acoplamiento electrónico en el régimen de larga distancia

Zhi Cao¹, Bin Xi, Diane S Jodoin

¹Department of Chemistry, Purdue University , West Lafayette, Indiana 47907, United States.

Journal of the American Chemical Society

|August 14, 2014

Resumen

Este estudio sintetizó nuevos compuestos de dirutenio-polidiil. Se investigó el acoplamiento electrónico a través del puente poliindiol, revelando la dependencia de la longitud del puente y mediada por orbitales específicos.

Área de la Ciencia:

Coordinación Química de la Coordinación
Ciencia de los materiales Ciencia de los materiales.
La electroquímica es electroquímica.

Sus antecedentes:

Los complejos de dirutenio con ligandos puentes son cruciales para comprender la transferencia de electrones.
Los puentes poliindiilo ofrecen vías de comunicación electrónica sintonizables en sistemas moleculares.

Objetivo del estudio:

Para sintetizar y caracterizar una serie de compuestos de dirutenio-polidiilo-diilo.
Para investigar el acoplamiento electrónico a través de diferentes longitudes de puentes poliindiilo.
Para aclarar la naturaleza de las órbitas que median en la comunicación electrónica de larga distancia.

Principales métodos:

Síntesis de compuestos simétricos y no simétricos de dirutenio-polidiilo a través del acoplamiento Glaser.
Caracterización estructural utilizando difracción de rayos X. Caracterización estructural utilizando difracción de rayos X. Caracterización estructural utilizando difracción de rayos X. Caracterización estructural utilizando difracción de rayos X. Caracterización estructural utilizando difracción de rayos X. Caracterización estructural utilizando difracción de rayos X.
Análisis electroquímico utilizando voltametría cíclica (CV) y voltametría de pulso diferencial (DPV).
Estudios espectroelectroquímicos y cálculos de la Teoría Funcional de Densidad (DFT) sin restricciones de espín.

Principales resultados:

Síntesis exitosa de compuestos poliindiilo Ru2(Xap) 4-capped con diferentes longitudes de puente.
La difracción de rayos X confirmó la topología sigmoidal del puente poliindiilo y la estructura del núcleo Ru2.
Los monoaniones reducidos ([Ru2-C2m-Ru2](-1)) muestran valencia mixta de clase II de Robin-Day.
El acoplamiento electrónico muestra atenuación con la longitud del puente (γ = 0.120.15 Å(-1)).
Los cálculos de DFT identificaron órbitas mediadoras para el acoplamiento electrónico de larga distancia.

Conclusiones:

Los compuestos sintetizados de diruthenium-polyyn-diyl sirven como excelentes plataformas para estudiar la comunicación electrónica.
La longitud del puente poliindiilo influye significativamente en la resistencia del acoplamiento electrónico.
Las ideas de DFT proporcionan una comprensión fundamental de los mecanismos de transferencia de electrones en estos sistemas.

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