Elucidating uranium interactions with synthetic Na-P1 zeolite/Ca2+-substituted alginate composite granules through batch and spectroscopic studies: Emphasizing the significance of ion exchange and complexation.

Uranium, a key member of the actinides series, is radioactive and may cause severe environmental hazards once discharged into the water due to high toxicity. Removal of uranium via adsorption by applying tailored, functional adsorbents is at the forefront of tackling such pollution. Here, we report the optimized functionalization of the powder coal fly-ash (CFA) derived Na-P1 synthetic zeolite to the form of granules by employing the biodegradable polymer-calcium alginate (CA) and their application to remove aqueous U. The optimized synthesis showed that granules are formed at the CA concentration equals to 0.5 % wt., and that application of 1% wt. solution renders the most effective U scavengers. The maximum U adsorption capacity (qmax) increases significantly after CA modification from 44.48 mgU/g for native, powder Na-P1 zeolite to 62.53 mg U/g and 76.70 mg U/g for 0.5 % wt. and 1 % wt. CA respectively. The U adsorption follows the Radlich-Peterson isotherm model, being the highest at acidic pH (pHeq∼4). The U adsorption kinetics reveals swift U uptake, reaching equilibrium after 2h for 1 % ZACB and 3 h for 0.5 % wt. ZACB following the pseudo-second-order (PSO) kinetic model. SEM-EDXS investigation elucidates that adsorbed U occurs onto materials as an inhomogenous, well-dispersed, and micrometer-scale aggregate. Further, XPS and µ-XRF spectroscopies complementarily confirmed the hexavalent oxidation state of adsorbed U and its altered distribution on ZACBs with varying CA concentrations. U distribution was probed "in-situ" onto materials while correlations between the major elements (Al, Si, Ca, U) contributing to U scavenging were calculated and compared. Finally, a real-life coal mine wastewater (CMW) polluted by 238U and 228,226Ra was successfully purified, satisfying WHO guidelines after treatment using ZACBs. These findings offer new insights on successful yet optimized Na-P1 zeolite modification using biodegradable polymer (Ca2+-exchanged alginate) aimed at efficient U removal, displaying a near-zero environmental impact.