One-step green synthesis of melamine-modified cellulose nanofiber composite aerogels for efficient removal of Pb(II) and Cu(II): Experiments and DFT calculations.

A composite aerogel (CGMA) with high porosity (98.32 %) and multiple active sites was prepared for the adsorption of Pb(II) and Cu(II) by sol-gel combined with freeze-drying process using melamine and (3-Glycidyloxypropyl)trimethoxysilane as cellulose nanofiber modifying materials. Characterized by SEM-EDS, XPS, FTIR, BET, MIP and TG, CGMA has a hierarchical pore structure and abundant adsorption sites. At pH = 6, the adsorption reached equilibrium within 120 min, following the Pseudo second-order kinetic model and the Langmuir model, with maximum capacities of 268.1 mg/g for Pb(II) and 152.6 mg/g for Cu(II). The process was primarily governed by homogeneous chemisorption. The coexisting ion, organic matter, and water quality experiments confirmed the excellent anti-interference properties of CGMA. Competitive adsorption experiments showed that CGMA has excellent selective adsorption performance for Pb(II). After 5 cycles, Pb(II) and Cu(II) adsorption performance decreased to 79.21 % and 83.40 %, respectively. FTIR, XPS, DFT and RDG analysis showed that amino groups and oxygen-containing groups were the main sites of adsorption. CGMA forms coordination bonds and complexes with Pb(II) and Cu(II) via amine and oxygen groups and adsorbs via electron transfer, hydrogen bonding, and van der Waals forces, with Pb(II) being more selective. CGMA has good prospects for application in heavy metal ion treatment.