Highly efficient uranium uptake by the eco-designed cocamidopropyl betaine-decorated Na-P1 coal fly-ash zeolite

• Published in: Journal of hazardous materials Vol. 477; p. 135230
• Main Authors: Sobczyk, M., Rossberg, A., Santhana Krishna Kumar, A., Marzec, M., Cwanek, A., Łokas, E., Nguyen Dinh, C., Bajda, T.
• Format: Journal Article
• Language: English
• Published: Netherlands Elsevier B.V 15.09.2024
• Subjects: Biosurfactants; Functional adsorbents; Organo-minerals; Uranium; XAS; CTAB-Br; BJH; XANES; CPS; FT-IR; ICP-MS/MS; XAS; PNP; BSE; PFO; Na-P1 @ 0.44CAPB composite; SLS; EA; ECEC; PXRD; WHO; CEC; SDS; TOC; PSO; ECECHDTMA-Br; AAS; IEP; MMT; SEM; CFA; ESRF; WD-XRF; CCBPs; UHVAC; EXAFS; FT; CAPB; Functional adsorbents; Uranium; COD; XPS; XAFS; SSA; ROBL; CE; TDS; IUPAC; Na-P1; pHPZC; Biosurfactants; Na-P1 @ 0.88CAPB composite; TC; TIC; BET; Na-P1 @ 1.59CAPB composite; Barn b; WtM; Organo-minerals; PDCA; EDXS; PET
• ISSN: 0304-3894; 1873-3336; 1873-3336
• DOI: 10.1016/j.jhazmat.2024.135230

In some locations around the globe, the U concentrations may exceed WHO standards by 2-folds therefore, effective yet environmentally wise solutions to purify radioactive waters are of significant importance. Here, the optimized and fully controlled coal-fly-ash based Na-P1 zeolite functionalization by employing novel, biodegradable biosurfactant molecule - cocamidopropyl betaine (CAPB) is showcased. The zeolite’s surface decoration renders three composites with varying amounts of introduced CAPB molecule (Na-P1 @ CAPB), with 0.44, 0.88, and 1.59-times External Cation Exchange Capacity (ECEC). Wet-chemistry experiments revealed extremely high U adsorption capacity (qmax = 137.1 mg U/g) unveiling preferential interactions of uranyl dimers with CAPB molecules coupled with ion-exchange between Na+ ions. Multimodal spectroscopic analyses, including Fourier-Transformed Infra-Red (FT-IR), X-ray Photoelectron (XPS), and X-ray Absorption Fine Structure (XAFS), showed the hexavalent oxidation state of U, and no secondary release of the CAPB molecule from the composite. The EXAFS signals fingerprint changes in the interatomic distances of adsorbed U, showing the impact of the O and N, heteroatoms present in the CAPB molecule on U binding mechanism. The presented research outcomes showcase the easy, scalable, optimized, and environmentally friendly synthesis of biofunctional zeolite effectively purifying the real-life U-bearing wastewaters from the vicinity of the Pribram deposit (Czech Republic). [Display omitted] ●An eco-designed cocamidopropyl betaine (CAPB)-decorated Na-P1 zeolite was engineered.●Zeolite’s surface decoration precisely controlled by adjusting pH, and CAPB content.●The amount of CAPB comprehensively verified by combining FT-IR, XPS, and EA.●Qmax equals 137.11 mgU/gNa-P1@0.44CAPB, at pHeq ∼ 6, and S/Lratio = 2.5 g/L.●U dimeric hydroxy-complexes [(UO2)2(OH)22+] unveiled by U-L3 edge XAFS spectroscopy.