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Triggering photocatalytic performance of La 2 Co x Mn 2-x O 6 via heat activation
Ist Teil von
Proceedings of the National Academy of Sciences - PNAS, 2023-10, Vol.120 (44), p.e2310004120
Ort / Verlag
United States
Erscheinungsjahr
2023
Quelle
EZB Electronic Journals Library
Beschreibungen/Notizen
The La-based perovskite (LaBO
) exhibits excellent optical properties. However, its valence band (VB) potential is not sufficiently positive to reach the oxidation potential required for the cleavage of chemical bonds (such as benzylic C-H), limiting its application in photocatalysis. Herein, we report the unconventional effects of heat activation on the reduction of the dissociation energy of benzylic C-H and aqueous H-O, thereby triggering the photocatalytic activity of La
Co
Mn
O
perovskites. Additionally, we demonstrate that photocatalysis is the main contributor to substrate conversion in the selective oxidation of toluene and reduction of CO
. Particularly, La
Co
Mn
O
shows excellent performance with a product yield of 550.00 mmol g
and a toluene conversion of 22,866.67 μmol g
h
. To the best of our knowledge, this is the highest reported product yield for the selective oxidation of benzylic C-H bond of toluene. Our findings provide insight into the specific role of heat activation in photocatalysis, which is crucial for breaking and overcoming the VB barrier to realize challenging reactions.