Developing supramolecular gels that effectively integrate multi-stimuli responsiveness with high-performance heavy metal adsorption remains a significant challenge, primarily due to the limited functionality and weak synergistic effects of conventional gelators. To address this issue, we have designed and synthesized two novel ferrocene-cored poly(aryl ether) dendritic organometallic gelators, designated as FC-D1 and FC-D2, which are functionalized with amide and acylhydrazide linkages. The chemical structures of both gelators were thoroughly characterized using standard spectroscopic techniques. Our experimental results demonstrate that both FC-D1 and FC-D2 exhibit outstanding gelation ability across a broad spectrum of pure organic solvents and binary solvent mixtures, forming highly stable organogels at remarkably low critical gelation concentrations (CGC). Mechanistic investigations employing Fourier-transform infrared (FT-IR) spectroscopy and variable-concentration proton nuclear magnetic resonance (¹H NMR) spectroscopy reveal that the self-assembly process is synergistically driven by two key non-covalent interactions: intermolecular hydrogen bonding originating from the acylhydrazone and amide moieties, and π-π stacking interactions among the aromatic rings of the dendritic branches. This cooperative assembly leads to the formation of robust three-dimensional network structures. The resulting metallogels exhibit excellent and reversible multi-stimuli-responsive properties, enabling reliable gel-to-sol transitions upon exposure to various external stimuli, including temperature changes, redox reactions (using ceric ammonium nitrate (CAN) and glutathione (GSH) as an oxidizing/reducing pair), chemical triggers (specifically fluoride ions), and mechanical thixotropic stimuli. Beyond their stimuli-responsive behavior, we also evaluated the potential of the FC-D1 dendron as an effective and recyclable adsorbent for the removal of toxic heavy metal ions from aqueous environments. The results show that FC-D1 achieves impressive removal efficiencies of 72%, 51%, and 73% for Hg2+, Pb2+, and Cd2+, respectively. Furthermore, the gel system maintains stable adsorption performance over four consecutive adsorption-desorption cycles, demonstrating good reusability. Overall, this work not only provides a new and effective molecular design strategy for constructing multifunctional dendritic organometallic gels but also significantly expands their potential applications in the fields of intelligent sensing and heavy metal wastewater remediation.
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