2024
DOI: 10.1021/acs.chemmater.3c03226
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Tuning Electron Transfer in Pyrene-Based Two Dimensional Covalent Organic Frameworks: Unveiling the Impact of Semi-isomerism on Physicochemical Properties

Bingwei Bao,
Ran Li,
Yingying Hao
et al.

Abstract: Constitutional isomerism of covalent organic frameworks (COFs) has recently garnered attention for its potential applications in advanced photoelectrochemical fields. However, there have been no reports of materials in which half of the linkages between building blocks of the COFs are isomerized (so-called semi-isomerism) as a means of modulating the physicochemical properties of COFs. In this work, semi-isomeric pyrene-based COFs with the same topology were synthesized with imine linkages, namely, Py-Py and S… Show more

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Cited by 6 publications
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“…Benefiting from the tunability of COFs, we delicately designed 10 pairs of COF-based ratchets with mutually reversed orientations of polar CHN bonds between D–A units. We anticipated that the polarized CHN bonds could serve as ratchet teeth, which preferentially direct the electron transfer from the N-end units to the C-end units and impede the reversed electron migration during electron–hole combination (Figure a), in analogy to the recently reported “ICT Tesla Valve.” , Similar to the space charge in semiconductor heterojunctions, the CHN bond in COFs with reversed orientation could cause inverted band bending (Figures b and S2), where the C-end band bends upward, and the N-end band bends downward. Consequently, the direction of CHN bonds not only affects the conduction band minimum (CBM) and valence band maximum (VBM) but also dictates the electron–hole combination and the resulting ECL performance (Figure c).…”
Section: Resultsmentioning
confidence: 99%
“…Benefiting from the tunability of COFs, we delicately designed 10 pairs of COF-based ratchets with mutually reversed orientations of polar CHN bonds between D–A units. We anticipated that the polarized CHN bonds could serve as ratchet teeth, which preferentially direct the electron transfer from the N-end units to the C-end units and impede the reversed electron migration during electron–hole combination (Figure a), in analogy to the recently reported “ICT Tesla Valve.” , Similar to the space charge in semiconductor heterojunctions, the CHN bond in COFs with reversed orientation could cause inverted band bending (Figures b and S2), where the C-end band bends upward, and the N-end band bends downward. Consequently, the direction of CHN bonds not only affects the conduction band minimum (CBM) and valence band maximum (VBM) but also dictates the electron–hole combination and the resulting ECL performance (Figure c).…”
Section: Resultsmentioning
confidence: 99%