Comparative Study of Functionalized Cellulose Nanocrystal–Silica Aerogels for Methylene Blue Adsorption

Abstract

The removal of cationic dyes from industrial wastewater presents a significant environmental challenge. This research examines the effectiveness of functionalized cellulose-based silica aerogels as sustainable adsorbents for methylene blue (MB) dye. This research provides a systematic comparative study on the effectiveness of four distinct functionalization strategies, carboxylate (CCNC), double carboxylate (DCCNC), carboxymethyl (CMC), and thiol-modification, applied to cellulose-based silica aerogels as sustainable adsorbents for methylene blue (MB) dye. Cellulose nanocrystals (CNCs) were extracted from sugarcane bagasse waste and subsequently functionalized into carboxylate (CCNC), double carboxylate (DCCNC), carboxymethyl (CMC), and thiol-modified variants. The materials were later integrated into a silica matrix, resulting in the formation of porous aerogel nanocomposites. The materials underwent thorough characterization through FTIR, XRD, SEM, TGA, and BET analyses, validating successful functionalization and the development of mesoporous structures. Batch adsorption tests demonstrated that the CMC-silica aerogel exhibited superior performance, attaining a maximum adsorption capacity of 197 mg/g and complete removal efficiency under ideal circumstances (pH 10, 25 °C, 60 min). The adsorption process is accurately characterized by the Langmuir isotherm and pseudo-second-order kinetic models, signifying monolayer adsorption and chemisorption as the rate-limiting step. The thermodynamic parameters indicate that the adsorption process is exothermic and spontaneous. The CMC-silica aerogel exhibited significant reusability, maintaining over 90% efficiency after six consecutive cycles. The findings illustrate the efficacy of functionalized cellulose-silica aerogels, especially the CMC form, as effective, environmentally sustainable, and reusable adsorbents for the treatment of dye-polluted water.