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Abstract
Highlights
1. 通过在COFs的模块化连接线上引入含氮基团调节其光催化性能。合成了四种β-酮烯胺结构的COFs:TpBpy-COF、TpDz-COF、TpBD-COF和TpPa-COF。
2. TpBpy-COF表现出最优异的光催化活性和选择性,能够高效催化多种硫醚化合物的氧化反应。
3. 机理研究表明,TpBpy-COF能有效吸附和激活单线态氧,促进光生载流子的分离和迁移,从而大幅提高其光催化效率。
4. 引入原子级氮位点对COFs的光电性能和催化选择性产生了重要影响。
results
Fig.1 (a) Schematic represented of the syntheses of Tp-based COFs with different pore size, termed as TpDz-COF, TpPa-COF, TpBpy-COF, and TpBD-COF. (b–e) Experimental, refined, and simulated PXRD patterns of TpBpy-COF, TpDz-COF, TpBD-COF, and TpPa-COF.
Fig.2 13C cross-polarization magic-angle-spinning (CP-MAS) solid-state NMR spectra of (a) TpBpy-COF, (b) TpDz-COF, (c) TpBD-COF, (d) TpPa-COF, (e) Wide-scan XPS spectra of COFs, (f) High-resolution N 1s XPS spectra of COFs, (g) High-resolution C 1s XPS spectra of COFs and (h) High-resolution O 1s XPS spectra of COFs.
Fig.3 (a) The SEM image of TpBpy-COF, (b-c) HR-TEM images of TpBpy-COF, (d) HAADF-STEM image of TpBpy-COF, and (e-g) The EDX mapping images for C (yellow), O (blue) and N (red).
Fig.4 (a) The UV–vis DRS, (b) the corresponding Tauc plot analysis, (c) Transient photocurrents of four COFs and (d) EIS of the four β-ketoenamine COFs.
Fig.5 HOMOs and LUMOs of the unit structures of the pores of (a) TpBpy-COF, (b) TpDz-COF, (c) TpBD-COF and (d) TpPa-COF and their fragments, NTOs pairs of lowest excited singlet state for the fragments of (e) TpBpy-COF, (f) TpDz-COF, (g) TpBD-COF and (h) TpPa-COF.
Fig.6 (a) Adsorption structure, Mulliken charge, and adsorption energy between O2 and unit structure of the pore of TpBpy-COF, (b) Spin trapping of 1O2 in the blue light-induced selective oxidation of sulfides over TpBpy-COF photocatalyst, (c) Proposed mechanism of photocatalytic thioanisole oxidation over TpBpy-COF.
Details
Linker Modulation of Covalent Organic Frameworks at Atomic Level for Enhanced and Selective Photocatalytic Oxidation of Thioether
原文链接：
https://doi.org/10.1002/adfm.202413943
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