In this pioneering study, electrostatic spraying (ES) technology with high voltages is proposed to reduce the size of hydrogel microbeads further, aiming to enhance the adsorption rate of cationic methylene blue (MB) dye. The increased voltages, ranging from 0.0 to 13.0 kV, further decreased the size of electrostatically sprayed hydrogel microbeads crosslinked by hydrogen bonds between sodium alginate (SA) and carboxymethyl chitosan (CMCS) in hydrochloric acid. The size of SA/CMCS hydrogel microbeads was successfully reduced from 2000 ± 121 μm (SC-2000) to 400 ± 15 μm (SC-400). Notably, SC-400 exhibits the highest maximum adsorption capacity (qm) and rate constant (k2) at 840.3 mg/g and 0.0598 g/mg/min, respectively, at pH 9.0 and a temperature of 25 °C in the absence of ionic compounds, which is three times higher than that of SC-2000, due to their high specific surface area and pore volume. Through a series of adsorption studies and characterization analyses, SA/CMCS hydrogel microbeads displayed heterogeneous adsorption behaviors towards MB dye through electrostatic interactions between the deprotonated carboxylic groups and cationic MB molecules, where MB adsorption efficiency could be significantly influenced by pH and ionic strength. These findings suggest that ES technology is effective in synthesizing smaller SA/CMCS hydrogel microbeads with enhanced MB removal rates and stable adsorption capacities and their applications could be further explored for removing other organic dyes and toxic metals in subsequent research studies.
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