Abstract
As one of common dynamic covalent bonds, acylhydrazone bond plays an important role in developing intelligent responsive materials. In this report, we present acylhydrazone-based dynamic polymers with multi-stimuli responsiveness, particularly metal recognition behaviours and their modulation. A series of polyacylhydrazones with different metal-binding sites were designed and prepared in a modular fashion. Titration of these receptors with a diverse set of metal ions, including Cu2+, Zn2+ and La3+, resulted in unique optical changes, and both the sensitivity and selectivity profiles can be regulated. Moreover, the metal-binding feature was facilely modulated by changing the solvent. The addition of weakly basic anions was employed to further fine-tune the responsiveness of the polymers by taking advantage of the cooperative effect with metal coordination. Finally, the sensitive detection of 6-mercaptopurine and pyrophosphate was achieved to demonstrate the application potential of these systems.
Highlights
Stimuli-responsive materials have potential applications in the research of biointerfaces, [1] optical sensing and imaging, [2,3] gas storage and transformation, [4] tissue engineering, [5] as well as drug and gene delivery [6,7]
One notable strategy for the construction of responsive materials is the use of 2 dynamic covalent bonds, such as imine [12,13] and disulfide [14,15]
The varied structures and optical signals of these polyacylhydrazones paved the way for the control of metal binding
Summary
Stimuli-responsive materials have potential applications in the research of biointerfaces, [1] optical sensing and imaging, [2,3] gas storage and transformation, [4] tissue engineering, [5] as well as drug and gene delivery [6,7]. One notable strategy for the construction of responsive materials is the use of 2 dynamic covalent bonds, such as imine [12,13] and disulfide [14,15]. Pyridine-2-carboxyaldehyde, [37] salicylaldehyde [38,39] and their corresponding derivatives are widespread building blocks in imine-based assemblies, including metal-organic cages [40,41,42] and covalent-organic frameworks [43,44,45]. Their dynamic hydrazone assemblies have received significantly less attention. Two model analytes were detected by using these polymers
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