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Efficient Selective Removal of Pb(II) by Using 6-Aminothiouracil-Modified Zr-Based Organic Frameworks: From
Chao Xiong1, Shixing Wang2, Peng Hu1
1Fine Chemical Industry Research Institute, School of Chemistry , Sun Yat-Sen University , Guangzhou 510275 , P. R. China.
Abstract:
We report an efficient, reusable, and selective 6-aminothiouracil (ATA)-modified Zr(IV)-based adsorbent (defined as UiO-66-ATA(Zr)) for lead ion removal in water. The adsorption equilibrium time and the maximum sorption capacity of UiO-66-ATA(Zr) for Pb(II) are, respectively, 120 min and 386.98 mg/g at pH 4 and 298 K. The Pb(II) removal rate reaches 96% at 60 min and exceeds 99% at the equilibrium state in the pH range of 2.0-5.8. Hill and pseudo-second-order models can well describe the sorption process. Pb(II) adsorbing onto UiO-66-ATA(Zr) is an irreversible, favorable chemisorption process with multimolecule participation and film diffusion control. The calculations of density functional theory, the experimental results, and the characterization analyses suggest that the binding mechanisms are the chelation and ion-exchange/electrostatic interactions between hydroxyl/amino/sulfhydryl groups of UiO-66-ATA(Zr) and Pb(II). Besides, UiO-66-ATA(Zr) has a better affinity to Pb(II) than the coexisting ions in water and an excellent repeatability at eight cycles of adsorption. Moreover, the thermodynamic study shows that UiO-66-ATA(Zr) adsorbing Pb(II) is an endothermic reaction. Thus, UiO-66-ATA(Zr) is a prospective sorbent for Pb(II) removal under the initiative of environmental protection and water purification, and this work may also provide an idea for industrial catalysis.
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