Paramagnetic States in Oxygen-Doped Boron Nitride Extend Light Harvesting and Photochemistry to the Deep Visible Region.
Chem Mater
; 35(5): 1858-1867, 2023 Mar 14.
Article
em En
| MEDLINE
| ID: mdl-36936177
ABSTRACT
A family of boron nitride (BN)-based photocatalysts for solar fuel syntheses have recently emerged. Studies have shown that oxygen doping, leading to boron oxynitride (BNO), can extend light absorption to the visible range. However, the fundamental question surrounding the origin of enhanced light harvesting and the role of specific chemical states of oxygen in BNO photochemistry remains unanswered. Here, using an integrated experimental and first-principles-based computational approach, we demonstrate that paramagnetic isolated OB3 states are paramount to inducing prominent red-shifted light absorption. Conversely, we highlight the diamagnetic nature of O-B-O states, which are shown to cause undesired larger band gaps and impaired photochemistry. This study elucidates the importance of paramagnetism in BNO semiconductors and provides fundamental insight into its photophysics. The work herein paves the way for tailoring of its optoelectronic and photochemical properties for solar fuel synthesis.
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1
Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
Chem Mater
Ano de publicação:
2023
Tipo de documento:
Article
País de afiliação:
Reino Unido