Journal
ACS APPLIED NANO MATERIALS
Volume 2, Issue 12, Pages 7719-7727Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.9b01787
Keywords
HOFs; TCPP; photocatalytic activity; singlet oxygen generation; dynamic skeleton; counterstrategy
Funding
- Natural Science Foundation of China [21701023]
- Natural Science Foundation of Jiangsu Province [BK20170660]
- Zhishan Youth Scholar Program of SEU
- PAPD of Jiangsu Higher Education Institutions
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Fine tuning of the structures and properties of hydrogen-bonded organic frameworks (HOFs) has been considered to be a huge challenge. Herein, we reported the controlled synthesis of meso-tetrakis(carboxyphenyl)porphyrin (TCPP)-based HOFs via a counterstrategy of blocking the strong hydrogen-bonded building units on the TCPP backbones. Mediated by the temperatures, both the kinetically and thermodynamically favored HOF products TCPP-2(DMF), TCPP-4(DMF), and TCPP-6(DMF) can be obtained under 120, 130, and 140 degrees C, respectively. Results revealed that the numbers and binding positions of end-capped N,N-dimethylformamide (DMF) molecules not only played a key role in the thermal stability and permanent porosity of the present HOFs but also affected significantly the photocatalytic activities for the degradation of 9,10-diphenylanthracene, where a positive correlation between the numbers of DMF molecules and the photocatalytic activities has been established, which can be attributed to variation of the intermolecular van der Waals forces. In addition, upon removal of the lattice water and extra DMF molecules, respectively, HOFs TCPP-2(DMF) and TCPP-6(DMF) can be transformed into a polymorph TCPP-4(DMF)* in the solid state, suggesting a dynamic TCPP-DMF skeleton. This work will promote significantly the development of porphyrin-based HOFs and porphyrin-based photocatalysis materials.
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