Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 6, Pages 7162-7178Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b19516
Keywords
Zr-based sorbent; lead(II); selective removal; adsorption energy; binding mechanisms
Funding
- National Natural Science Foundation of China-SINOPEC Joint Fund [U1663220]
- National Natural Science Foundation of China [21938001, 21961160741, 21425627]
- Guangdong Provincial Key RD Programme [2019B110206002]
- Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program [2017BT01C102]
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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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