Aminated Wood Aerogel via Tannic Acid/Polyethylenimine Co-Deposition for Enhanced Congo Red Removal

Wood aerogel has emerged as a highly promising substrate for advanced adsorbents due to its green nature, low cost, high porosity, and unique three-dimensional (3D) interconnected network structure. Harnessing forest resources for developing high-performance aerogel materials is crucial for tackling organic dye pollution. This study presents a novel aminated wood-based aerogel engineered through the co-deposition of tannic acid (TA) and polyethylenimine (PEI) on a cellulose skeleton. The fabrication involved a top–down delignification process to create a porous wood aerogel framework, followed by the in situ loading of TA and the grafting of amino-rich PEI, resulting in the final TAPI-DW composite. Benefiting from the abundant active sites deposited on the aerogel’s hierarchically porous surface and the grafted –NH2 groups, TAPI-DW demonstrated an exceptional adsorption capacity for the anionic azo dye Congo red (CR). The adsorption equilibrium was achieved within approximately 6 h, with a lower pH environment promoting removal efficiency. Coexisting ion experiments indicated that the introduction of Ca2+ ions dramatically enhanced the CR adsorption capacity from 168.71 mg·g−1 to 301.14 mg·g−1. This superior capture performance is attributed to the synergistic interplay of the aerogel’s aligned microchannels (derived from the native wood structure) for rapid mass transfer and the intensive chemical interactions, including electrostatic attraction, hydrogen bonding, and π-π stacking between CR molecules and the functional groups (–NH2 and –OH) on the 3D skeleton. The Freundlich model fitting suggests a complex multilayer adsorption process on this heterogeneous wood aerogel surface. This work establishes a green and sustainable pathway for fabricating high-value biomass aerogel materials that show promise as candidates for the efficient remediation of dye-contaminated water. Further studies on reusability and long-term stability are needed to fully validate their potential for practical application.