Abstract
Developing adsorbents that combine high capacity with structural robustness remains a critical challenge for dye wastewater treatment. In this study, we propose a "pollutant-induced gelation" strategy to address this limitation, using Fe(III)-activated palygorskite nanorod aggregates as a model system for the highly efficient sequestration of Congo red (CR). Unlike conventional modification methods that rely solely on surface functionalization, this approach leverages the adsorbed dye itself as a synergistic assembly promoter. The addition of CR significantly consolidates the Fe(III)-mediated aggregation of palygorskite nanorods, leading to the formation of an integrated three-dimensional porous network with distinct gel-like rheological behavior. This dye-induced gel network not only provides abundant confined spaces for pollutant entrapment but also enhances the structural integrity of the adsorbent, facilitating separation and potential reuse. Compared to pristine palygorskite, the Fe(III)-activated material exhibited a 95.4-277% increase in adsorption capacity across a pH range of 4-10. The adsorption process followed pseudo-second-order kinetics and the Temkin isotherm model, and was thermodynamically spontaneous and exothermic. Mechanistic studies revealed a synergistic interplay: Fe(III) served as primary cross-linking nodes to construct the network framework, while CR molecules acted as inducers to reinforce the gel architecture, enabling strong physical immobilization of dye aggregates. This work provides a new paradigm for designing intelligent, gel-based adsorbents from natural nanoclays, transforming a pollutant into a structural promoter.