Transient-State Self-Bipolarized Organic Frameworks of Single Aromatic Units for Natural Sunlight-Driven Photosynthesis of H2O2.
Adv Sci (Weinh)
; 11(24): e2308322, 2024 Jun.
Article
en En
| MEDLINE
| ID: mdl-38493490
ABSTRACT
Constructing π-conjugated polymer structures through covalent bonds dominates the design of organic framework photocatalysts, which significantly depends on the selection of multiple donor-acceptor building blocks to narrow the optical gap and increase the lifetimes of charge carriers. In this work, self-bipolarized organic frameworks of single aromatic units are demonstrated as novel broad-spectrum-responsive photocatalysts for H2O2 production. The preparation of such photocatalysts is only to fix the aromatic units (such as 1,3,5-triphenylbenzene) with alkane linkers in 3D space. Self-bipolarized aromatic units can drive the H2O2 production from H2O and O2 under natural sunlight, wide pH ranges (3.0-10.0) and natural water sources. Moreover, it can be extended to catalyze the oxidative coupling of amines. Experimental and theoretical investigation demonstrate that such a strategy obeys the mechanism of through-space π-conjugation, where the closely face-to-face overlapped aromatic rings permit the electron and energy transfer through the large-area delocalization of the electron cloud under visible light irradiation. This work introduces a novel design concept for the development of organic photocatalysts, which will break the restriction of conventional through-band π-conjugation structure and will open a new way in the synthesis of organic photocatalysts.
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Colección:
01-internacional
Base de datos:
MEDLINE
Idioma:
En
Revista:
Adv Sci (Weinh)
Año:
2024
Tipo del documento:
Article
País de afiliación:
China
Pais de publicación:
Alemania