Persistent Radical Tetrathiafulvalene-Based 2D Metal-Organic Frameworks and Their Application in Efficient Photothermal Conversion

被引：121

作者：

Su, Jian ^{[1
]}

Xu, Ning ^{[2
]}

Murase, Ryuichi ^{[3
]}

Yang, Zhi-Mei ^{[1
]}

D'Alessandro, Deanna M. ^{[3
]}

Zuo, Jing-Lin ^{[1
]}

Zhu, Jia ^{[2
]}

机构：

[1] Nanjing Univ, Sch Chem & Chem Engn, Collaborat Innovat Ctr Adv Microstruct, State Key Lab Coordinat Chem, Nanjing 210023, Peoples R China

[2] Nanjing Univ, Coll Engn & Appl Sci, Natl Lab Solid State Microstruct, Collaborat Innovat Ctr Adv Microstruct, Nanjing 210023, Peoples R China

[3] Univ Sydney, Sch Chem, Sydney, NSW 2006, Australia

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2021年 / 60卷 / 09期

基金：

澳大利亚研究理事会; 中国国家自然科学基金;

关键词：

crystal structures; metal-organic frameworks; photothermal conversion; radicals; redox activity; ELECTRICAL-CONDUCTIVITY; MOF; PLATFORM; ROBUST; SIZE;

D O I：

10.1002/anie.202013811

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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.

引用

页码：4789 / 4795

页数：7

共 61 条

[31] Slow magnetic relaxation in radical cation tetrathiafulvalene-based lanthanide(III) dinuclear complexes [J].