Unveiling the influence of hydrophobicity on inhibiting hydrogen dissociation for enhanced photocatalytic hydrogen evolution of covalent organic frameworks

Journal of Colloid and Interface Science(2024)

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Abstract
Covalent organic frameworks (COFs) have gained considerable interest as candidate photocatalysts for hydrogen evolution. In this work, we synthesized β-keto-enamine-based COFs (TpPa-X, TpDB, and TpDTP) to explore the relations between structures and photocatalytic hydrogen evolution. COFs were divided into two groups: (1) TpPa-X with different substituents attached to the TpPa backbone and (2) COFs featuring diamine linkers of varied lengths (TpDB and TpDTP). Experiments and density functional theory (DFT) calculations show that moderate hydrophobicity is favorable for the photocatalytic hydrogen evolution process, and acceptable contact angles are anticipated to range from 65° to 80°. Naturally, there are comprehensive factors that affect photocatalytic reactions, and the regulation of different backbones and substituents can considerably affect the performance of COFs for photocatalytic hydrogen evolution in terms of electronic structure, specific surface area, surface wettability, carrier separation efficiency, and hydrogen dissociation energy. Results show that TpPa-Cl2 (TpPa-X, X  = Cl2) demonstrates the highest photocatalytic activity, approximately 14.51 mmol g-1h−1, with an apparent quantum efficiency of 4.62 % at 420 nm. This work provides guidance for designing efficient COF-based photocatalysts.
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Key words
Covalent-organic frameworks,Hydrophobicity,Contact angle,Photocatalytic hydrogen evolution
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