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La luz hace que una superficie se rompa: fotodesorción de hidrógeno molecular de RuO2

Michael A Henderson¹, Rentao Mu¹, Arjun Dahal¹

¹Physical Sciences Division, Physical & Computational Sciences Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.

Journal of the American Chemical Society

|July 9, 2016

Resumen

La luz visible puede romper el enlace rutenio-hidrógeno en los complejos de Kubas en superficies de dióxido de rutenio. Esta fotodesorción de hidrógeno sugiere que el dióxido de rutenio es fotoactivo, lo que afecta a las aplicaciones de fotocatálisis.

Área de la Ciencia:

Ciencias de la superficie
La fotoquímica
Ciencias de los materiales

Sus antecedentes:

Los complejos de Kubas describen la coordinación H2 a los centros metálicos a través de la polarización de enlaces σ.
El dióxido de rutenio (RuO2) es un cocatalizador térmico común en la fotocatálisis.
La interacción Ru-H2 en RuO2{\displaystyle RuO2{\text{1}}} forma un "vínculo bananero" a través de los sitios Ru{\text{\text{4}}+).

Objetivo del estudio:

Investigar la fotoactividad de la superficie de RuO2 en relación con la quimiosorbción de H2.
Para determinar si la luz visible puede desestabilizar y romper el enlace Ru-H2 con el plátano.
Para aclarar el mecanismo detrás de la disociación H2 inducida por la luz.

Principales métodos:

Estudios experimentales de fotodesorción mediante espectrometría de masas y microscopía de túnel de barrido.
Cálculos de la teoría funcional de la densidad dependiente del tiempo (TD-DFT).
Análisis de la estructura electrónica y las excitaciones ópticas en RuO2.

Principales resultados:

Se demostró que la luz visible desestabiliza y rompe el enlace Ru-H2 con el plátano.
Se observó fotodesorción de H2 y D2 y se confirmó mediante técnicas experimentales.
TD-DFT reveló que una transición entre bandas en RuO2 debilita la acidez de Lewis, rompiendo el complejo de Kubas.

Conclusiones:

El complejo de Ru-H2 Kubas en RuO2 es fotoactivo y puede ser escindido por la luz visible.
El dióxido de rutenio, un cocatalizador térmico común, también es fotoactivo.
Este hallazgo tiene implicaciones para la comprensión y el diseño de sistemas fotocatalíticos.

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