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Tuning Molecular Chromophores of Isoreticular Covalent Organic Frameworks for Visible Light-Induced Hydrogen Generation

机译：Tuning Molecular Chromophores of Isoreticular Covalent Organic Frameworks for Visible Light-Induced Hydrogen Generation

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摘要

The functions of covalent organic frameworks (COFs) can be tailored by covalently reticulating advanced molecular modules into well-defined porous ordered materials. Herein, four COFs, USTB-7-USTB-10, are prepared from the solvothermal reaction of photoactive tetraaldehydes, 5,5″-(benzo[c]-[1,2,5] thiadiazole-4,7-diyl)diisophthalaldehyde and 5,5″-(naphtho[2,3-c][1,2,5]thiadiazole- 4,9-diyl)diisophthalaldehyde, with p-phenylenediamine and benzidine, respectively. Comprehensive studies of powder X-ray diffraction, theoretical simulation, and pore size distribution disclose their isoreticular 2D dual porous structures. In contrast to benzo[c][1,2,5]thiadiazole-based chromophore, employment of naphtho[2,3-c][1,2,5]thiadiazole-based tetraaldehyde enables enlarged conjugation systems for USTB-9 and USTB-10, rather than USTB-7 and USTB-8. This, in combination with the longer benzidine unit, endows USTB-10 with a porous structure with bigger pore size than that of USTB-9, resulting in the highest photocatalytic hydrogen production rate of 21.8 mmol g~(?1) h~(?1) with the help of a Pt cocatalyst. Experimental and theoretical studies reveal the outstanding photocatalytic activity for USTB-10 among the four COFs associated with the narrowed bandgap and increased chargecarrier separation efficiency.

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