On-demand uranium extraction from seawater (UES) can mitigate growing sustainable energy needs, while high salinity and low concentration hinder its recovery. A novel anionic metal-organic framework (iMOF-1A) is demonstrated adorned with rare Lewis basic pyrazinic sites as uranyl-specific nanotrap serving as robust ion exchange material for selective uranium extraction, rendering its intrinsic ionic characteristics to minimize leaching. Ionic adsorbents sequestrate 99.8% of the uranium in 120 mins (from 20,000 ppb to 24 ppb) and adsorb large amounts of 1336.8 mg g-1 and 625.6 mg g-1 from uranium-spiked deionized water and artificial seawater, respectively, with high distribution coefficient, KdU & GE; 0.97 x 106 mL g-1. The material offers a very high enrichment index of & AP;5754 and it achieves the UES standard of 6.0 mg g-1 in 16 days, and harvests 9.42 mg g-1 in 30 days from natural seawater. Isothermal titration calorimetry (ITC) studies quantify thermodynamic parameters, previously uncharted in uranium sorption experiments. Infrared nearfield nanospectroscopy (nano-FTIR) and tip-force microscopy (TFM) enable chemical and mechanical elucidation of host-guest interaction at atomic level in sub-micron crystals revealing extant capture events throughout the crystal rather than surface solely. Comprehensive experimentally guided computational studies reveal ultrahigh-selectivity for uranium from seawater, marking mechanistic insight.A novel anionic metal-organic framework adorned with a Lewis basic pyrazinic nitrogen (Pyz-N) site acting as a uranyl-specific nanotrap that functions as an effective adsorbent is reported herein. The resulting ionic adsorbent is deployed in uranium sequestration with state-of-the-art mechanistic understanding, delivering epitome performance by selectively capturing remarkable amounts of uranium from seawater and a range of water bodies.image
Nanotrap Grafted Anionic MOF for Superior Uranium Extraction from Seawater / More, Yogeshwar D.; Mollick, Samraj; Saurabh, Satyam; Fajal, Sahel; Tricarico, Michele; Dutta, Subhajit; Shirolkar, Mandar M.; Mandal, Writakshi; Tan, Jin‐chong; Ghosh, Sujit K.. - In: SMALL. - ISSN 1613-6810. - STAMPA. - 20:3(2024). [10.1002/smll.202302014]
Nanotrap Grafted Anionic MOF for Superior Uranium Extraction from Seawater
Tricarico, Michele;
2024-01-01
Abstract
On-demand uranium extraction from seawater (UES) can mitigate growing sustainable energy needs, while high salinity and low concentration hinder its recovery. A novel anionic metal-organic framework (iMOF-1A) is demonstrated adorned with rare Lewis basic pyrazinic sites as uranyl-specific nanotrap serving as robust ion exchange material for selective uranium extraction, rendering its intrinsic ionic characteristics to minimize leaching. Ionic adsorbents sequestrate 99.8% of the uranium in 120 mins (from 20,000 ppb to 24 ppb) and adsorb large amounts of 1336.8 mg g-1 and 625.6 mg g-1 from uranium-spiked deionized water and artificial seawater, respectively, with high distribution coefficient, KdU & GE; 0.97 x 106 mL g-1. The material offers a very high enrichment index of & AP;5754 and it achieves the UES standard of 6.0 mg g-1 in 16 days, and harvests 9.42 mg g-1 in 30 days from natural seawater. Isothermal titration calorimetry (ITC) studies quantify thermodynamic parameters, previously uncharted in uranium sorption experiments. Infrared nearfield nanospectroscopy (nano-FTIR) and tip-force microscopy (TFM) enable chemical and mechanical elucidation of host-guest interaction at atomic level in sub-micron crystals revealing extant capture events throughout the crystal rather than surface solely. Comprehensive experimentally guided computational studies reveal ultrahigh-selectivity for uranium from seawater, marking mechanistic insight.A novel anionic metal-organic framework adorned with a Lewis basic pyrazinic nitrogen (Pyz-N) site acting as a uranyl-specific nanotrap that functions as an effective adsorbent is reported herein. The resulting ionic adsorbent is deployed in uranium sequestration with state-of-the-art mechanistic understanding, delivering epitome performance by selectively capturing remarkable amounts of uranium from seawater and a range of water bodies.imageI documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.