期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 20, 页码 10891-10900出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c02497
关键词
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资金
- Department of Atomic Energy (DAE), Government of India [12-RD-TFR-5.10-0100]
- Department of Atomic Energy, Government of India [RTI 4007]
The research demonstrates the rapid charge transfer process in host-guest supramolecular assemblies, supported by transient spectroscopy and EPR studies, showing efficient charge separation and long-lived charge in COF assemblies, paving the way for COF-based photocatalytic reaction centers.
Porous 2D covalent organic frameworks (COF) that are assembled axially through weak p-stacking interactions can provide reticular charge transport channels while playing host to kinetically stabilized reactive molecular redox states. Here we demonstrate a host-guest supramolecular charge transfer (CT) assembly using photoactive anthraquinone-based COF as an acceptor while incarcerating the electron donor N,N-dimethylaniline (DMA) inside it. Employing femtosecond broadband transient absorption spectroscopy in combination with electron paramagnetic resonance (EPR) studies, we show that the CT occurs rapidly within <110 fs after photoexcitation, subsequently leading to long-lived charge separation with 13% quantum efficiency at room temperature. The photoinduced EPR signature of the long-lived confined DMA cation radical confirms the disparate regions of charge localization while H-1-C-13 correlation experiments using solid-state NMR spectroscopy enumerate the packing of the amines inside the host-guest COF assembly. Our work demonstrates the potency of charge transport pathways in supramolecular assemblies for efficient charge separation which if optimally tuned should pave the way for COF-based photocatalytic reaction centers.
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