期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 9, 页码 4789-4795出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202013811
关键词
crystal structures; metal-organic frameworks; photothermal conversion; radicals; redox activity
资金
- National Basic Research Program of China [2018YFA0306004, 2017YFA0205700]
- National Natural Science Foundation of China [21875099, 21631006, 51925204]
- Australian Research Council [FT170100283]
- Fundamental Research Funds for the Central Universities [021314380179]
A series of stable radical 2D metal-organic frameworks have been assembled using (m-TTFTB)(3) (m-Tetrathiafulvalene-tetrabenzoate) trimer building blocks. The stability of the radicals is enhanced by hexanuclear rare-earth-cluster-based 1D chains. The radical characteristics are confirmed through various experiments, and the frameworks exhibit excellent photothermal properties and stability.
A series of stable radical 2D metal-organic frameworks has been assembled. (m-TTFTB)(3) (m-Tetrathiafulvalene-tetrabenzoate) trimer building blocks are beneficial for the stability of the radicals due to delocalization of the unpaired electron. Hexanuclear rare-earth-cluster-based 1D chains further enhance the stability of the frameworks. The radical state of the middle TTF in the trimer has been observed by the change of central C-C and C-S bond distances and the configuration of the TTF by single-crystal X-ray diffraction. The radical characteristics are also confirmed by electron paramagnetic resonance, UV/Vis-NIR absorption, and X-ray photoelectron spectroscopy experiments. Stability tests showed that the radicals are stable even in solutions and under acid/base environments (pH 1-12). Owing to efficient light absorption due to intramolecular charge transfer, low thermal conductivity, and outstanding stability, the radical 2D Dy-MOF shows excellent photothermal properties, an increase of 34.7 degrees C within 240 s under one-sun illumination.
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