Journal of colloid and interface science · 2021
Complex supramolecular fiber formed by coordination-induced self-assembly of benzene-1,3,5-tricarboxamide (BTA).
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Wu Bohang, Liu Lin, Zhou Lu, Magana Jose Rodrigo, Hendrix Marco M R M, Wang Jiahua, Li Chendan, Ding Peng, Wang Yiming, Guo Xuhong, Voets Ilja K, Cohen Stuart Martien A, Wang Junyou
Аннотация
HYPOTHESIS: In the quest for large but well-controlled supramolecular structures, the discotic benzene-1,3,5-tricarboxamide (BTA) has received quite some attention, because it can form hydrogen-bonded stacks that can be regarded as supramolecular polymers of which the single BTA molecule is the monomer. In this report, we consider a more complex BTA-based supramolecular polymer, namely one that is built up from supramolecular 'monomers'.
EXPERIMENTS: We design a tris-ligand L3 consisting of a BTA core carrying three dipicolinic acid (DPA) groups. L3 itself is too small to form polymers, but in the presence of appropriate metal ions, each L3 can form three coordination bonds and so form (L3)n clusters that are large enough to stack successfully: at an appropriate metal dose, long and stable filaments with a cross-sectional diameter of 12 nm appear. We monitor the growth process by UV-vis spectroscopy and light scattering, and use small angle X-ray scattering (SAXS), TEM as well as molecular simulation to confirm the filamentous structure of the fibers and determine their dimensions.
FINDINGS: The formation and structure of the fiber are very similar for various transition metal ions, which enables introducing different functionalities, e.g., magnetic relaxivity, by proper choice of the metal ions. Hence, we obtain a doubly supramolecular polymer, connected axially by hydrogen bonds, and radially by coordination bonds. Not only does this realize a higher level of complexity, but it also allows to easily introduce and vary metal-derived functionalities.
EXPERIMENTS: We design a tris-ligand L3 consisting of a BTA core carrying three dipicolinic acid (DPA) groups. L3 itself is too small to form polymers, but in the presence of appropriate metal ions, each L3 can form three coordination bonds and so form (L3)n clusters that are large enough to stack successfully: at an appropriate metal dose, long and stable filaments with a cross-sectional diameter of 12 nm appear. We monitor the growth process by UV-vis spectroscopy and light scattering, and use small angle X-ray scattering (SAXS), TEM as well as molecular simulation to confirm the filamentous structure of the fibers and determine their dimensions.
FINDINGS: The formation and structure of the fiber are very similar for various transition metal ions, which enables introducing different functionalities, e.g., magnetic relaxivity, by proper choice of the metal ions. Hence, we obtain a doubly supramolecular polymer, connected axially by hydrogen bonds, and radially by coordination bonds. Not only does this realize a higher level of complexity, but it also allows to easily introduce and vary metal-derived functionalities.