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Dual-Channel Charge Transfer in Olefin-Linked Covalent Organic Frameworks for Efficient Photocatalytic Hydrogen Evolution from Seawater
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DOI：10.1002/adfm.202530802.png)
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Abstract
En 中文
Covalent organic frameworks (COFs) represent promising candidates for solar-driven hydrogen (H2) production via water splitting, yet the performance remains constrained by intrinsically inefficient charge transfer dynamics. Herein, a rationally engineered 2D olefin-linked COFs is presented, featuring dual-channel charge transfer (i.e., in-plane and interlayer) pathways for efficient photocatalytic H2 evolution from seawater. Through systematic modulation of pi-electron density distribution in electron donor-acceptor units, the optimized fully pi-conjugated TTh-Ph-COF exhibits exceptional charge separation and transfer kinetics. Comprehensive density functional theory (DFT) calculations indicate that the in-plane charge transfer is accelerated by sp2 C & boxH;C linked bridges with a large dipole moment (8.71 Debye), while vertically aligned pi-pi stacking interactions facilitate interlayer charge migration. This synergistic dual-channel electronic transport architecture enables TTh-Ph-COF to achieve a remarkable H2-evolution rate of 28.38 mmol h-1 g-1 in seawater and 55.36 mmol h-1 g-1 in deionized water, along with 20.31% apparent quantum efficiency at 420 nm irradiation. This research presents a novel design strategy aimed at enhancing light conversion efficiency within the molecular engineering framework through multi-channel charge transfer systems.
Keywords:
covalent organic frameworks
hydrogen
interlayer charge transfer
photocatalysis
seawater
Journal
IF:
19
Papers:
3.4W
Citations:
32.1W
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