C(sp3)-H Bond Activation by Perovskite Solar Photocatalyst Cell

© 2018 American Chemical Society. Inspired by efficient perovskite solar cells, we developed a three-component hybrid perovskite-based solar photocatalyst cell, NiO x /FAPbBr 3 /TiO 2 , for C(sp 3 )-H bond activation with high selectivity (∼90%) and high conversion rates (3800 μmol g -1 h -1 ) under ambient conditions. Time-resolved spectroscopy on our photocatalytic cell reveals efficient exciton dissociation and charge separation, where TiO 2 and NiO x serve as the electron- and hole-transporting layers, respectively. The photogenerated charge carriers injected into TiO 2 and NiO x drive the challenging C-H activation reaction via the synergetic effects of their band alignment relative to FAPbBr 3 . The reaction pathway is investigated by controlling the free-radical formation, and we find that C-H activation is mainly triggered by hole oxidation. Besides aromatic alkanes, also the C(sp 3 )-H bond in cycloalkanes can be oxidized selectively. This work demonstrates a generic strategy for engineering high-performance photocatalysts based on the perovskite solar cell concept.

Jaar van publicatie:2019

BOF-keylabel:ja

IOF-keylabel:ja

BOF-publication weight:10

CSS-citation score:3

Auteurs:International

Authors from:Higher Education

Toegankelijkheid:Open