Biobased amphoteric aerogel with core-shell structure for the hierarchically efficient adsorption of anionic and...

Efficient and simultaneous removal of anionic and cationic dyes from wastewater using low-cost and environmentally-friendly adsorbent is highly required. Herein, the carboxylated cellulose (carboxyl content: 2.97 mmol/g) derived from pomelo peel was extracted by a one-step H₂O₂/H₂SO₄-mediated oxidation method. Subsequently, a novel pomelo-peel cellulose/chitosan/sodium alginate (PCS) amphoteric aerogel with a specific core-shell structure was synthesized by multiple physical cross-linking strategies. The shell layer and core layer of the optimized P₃CS_0.75 aerogel can selectively adsorb cationic dyes and anionic dyes, in which, the theoretical maximum adsorption capacities were 888.27 mg/g and 1816.87 mg/g towards methylene blue (MB) and Congo red (CR), respectively. Especially, the aerogel's core/shell layer exhibited hierarchical adsorption behavior without overlapping sites even in the binary dye systems. The adsorption performance of obtained amphoteric aerogel remained effective in a wide pH range and under different practical water systems. Moreover, the removal efficiencies for MB and CR were slightly reduced from 90.76 % and 99.66 % to 88.08 % and 91.39 %, respectively, after 5 adsorption-desorption cycles, and the aerogel's structural integrity was also maintained due to its good compressive strength (487.16 KPa). In addition, the adsorption mechanism of PCS aerogel was investigated using adsorption kinetics, isotherm, thermodynamics, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. It was proved that the adsorption process was endothermic spontaneous-monolayer adsorption driven by electrostatic attraction and hydrogen bonding. Therefore, the prepared biobased aerogel was expected to be a prospective material for removing mixed dyes from wastewater.