期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 16, 页码 19054-19061出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c03280
关键词
conductivity switching; covalent organic frameworks; interlayer sliding; reversible phase transformation; solvent responsive; tetrathiafulvalene
资金
- Office of Science, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC02-05CH11231]
- National Natural Science Foundation of P. R. China [21603076, 21571070, 21802128]
- Natural Science Foundation of Guangdong Province [2018A030313193]
- Consejeria de Economia y Conocimiento, Junta de Andalucia [FQM-337]
- Ministerio de Economia y Competitividad (Spain) [CTQ201784561-P]
- South China Normal University
- China Scholarship Council (CSC)
Ordered interlayer stacking is intrinsic in two-dimensional covalent organic frameworks (2D COFs) and has strong implications on COF's optoelectronic properties. Reversible interlayer sliding, corresponding to shearing of 2D layers along their basal plane, is an appealing dynamic control of both structures and properties, yet it remains unexplored in the 2D COF field. Herein, we demonstrate that the reversible interlayer sliding can be realized in an imine-linked tetrathiafulvalene (TTF)-based COF TTF-DMTA. The solvent treatment induces crystalline phase changes between the proposed staircase-like sql net structure and a slightly slipped eclipsed sql net structure. The solvation-induced crystallinity changes correlate well with reversible spectroscopic and electrical conductivity changes as demonstrated in oriented COF thin films. In contrast, no reversible switching is observed in a related TTF-TA COF, which differs from TTF-DMTA in terms of the absence of methoxy groups on the phenylene linkers. This work represents the first 2D COF example of which eclipsed and staircase-like aggregated states are interchangeably accessed via interlayer sliding, an uncharted structural feature that may enable applications such as chemiresistive sensors.
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