UiO-66-(SH)<sub>2</sub>as stable, selective and regenerable adsorbent for the removal of mercury from water under environmentally-relevant conditions

Leus, Karen; Perez, Jeffrey Paulo H.; Folens, Karel; Meledina, Maria; Tendeloo, Gustaaf Van; Laing, Gijs Du; Voort, Pascal Van Der

doi:10.1039/c7fd00012j

Cited by 78 publications

(33 citation statements)

References 64 publications

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“…Equilibrium adsorption data were fitted to Langmuir and Freundlich isotherm models and the calculated fitting parameters for both models are shown in Table S7. Based on the fitting, the adsorption of As species on GR SO4 is best described using the Langmuir model, indicating a homogenous monolayer binding of As surface complexes at the solid/water interface (Leus et al, 2017). Using the Langmuir adsorption model, we determined the maximum As adsorption capacities for both As species onto GR SO4 (Table 1).…”

Section: Adsorption Isotherms and Mechanismmentioning

confidence: 99%

“…There is an imminent challenge regarding the development, testing and validating the usefulness of adequate mineral phases that have high metal-specific uptake capacities, strong binding affinities and excellent stabilities. Adsorption-based technologies are promising groundwater clean-up strategies because of their facile implementation, relative costeffectiveness and high removal efficiency (Leus et al, 2017). However, to optimize the efficiency of subsurface remediation strategies, the interactions between inorganic As species and the surfaces of redoxactive minerals such as GR must be quantified in detail.…”

Section: Introductionmentioning

confidence: 99%

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The interfacial reactivity of arsenic species with green rust sulfate (GRSO4)

Perez

Freeman

Schuessler

et al. 2019

Science of The Total Environment

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GR SO4 is among the best performing Febearing minerals for As removal.• Both pH and the presence of competing aqueous ions affect As removal efficiency. • Long term experiments showed that GR SO4 with As adsorbed onto its surface is stable for up to 90 days. • High-resolution electron microscopy revealed that As is preferentially adsorbed at the GR particle edges.Editor: José Virgílio Cruz Arsenic (As) contamination in groundwater is a significant health and environmental concern worldwide because of its wide distribution and toxicity. The fate and mobility of As is greatly influenced by its interaction with redox-active mineral phases, among which green rust (GR), an Fe II -Fe III layered double hydroxide mineral, plays a crucial role. However, the controlling parameters of As uptake by GR are not yet fully understood. To fill this gap, we determined the interfacial reactions between GR sulfate (GR SO4 ) and aqueous inorganic As(III) and As(V) through batch adsorption experiments, under environmentally-relevant groundwater conditions. Our data showed that, under anoxic conditions, GR SO4 is a stable and effective mineral adsorbent for the removal of As(III) and As(V). At an initial concentration of 10 mg L −1 , As(III) removal was higher at alkaline pH conditions (~95% removal at pH 9) while As(V) was more efficiently removed at near-neutral conditions (N99% at pH 7). The calculated maximum As adsorption capacities on GR SO4 were 160 mg g −1 (pH 8-9) for As(III) and 105 mg g −1 (pH 7) for As(V). The presence of other common groundwater ions such as Mg 2+ and PO 4 3− reduces the efficiency of As removal, especially at high ionic strengths. Long-term batch adsorption experiments (up to 90 days) revealed that As-interacted GR SO4 remained stable, with no mineral transformation or release of adsorbed As species. Overall, our work shows that GR SO4 is one of the most effective As adsorbents among iron (oxyhydr)oxide phases.

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Section: Adsorption Isotherms and Mechanismmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

The interfacial reactivity of arsenic species with green rust sulfate (GRSO4)

Perez

Freeman

Schuessler

et al. 2019

Science of The Total Environment

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“…For example, NC appeared at a binding energy value of 399.1 eV, but after Hg removal, the value shifted to 399.4 eV due to the formation of the (Hg–NC) complex. Similarly, the C–S bond has a binding energy value of 162.2 eV, but after the removal of Hg(II), this peak moved to 161.6 eV due to the formation of the (Hg–S–C) bond. , …”

Section: Results and Discussionmentioning

confidence: 99%

“…have attracted great attention due to their exceptional water stability and high adsorption capacities. − UiO-66-NH 2 exhibits no significant changes in the X-ray diffraction (XRD) pattern and the crystalline structure after exposure to liquid water and other solvents due to inorganic unit strength, where each Zr 6 O 4 (OH) 4 unit is 12-coordinated to terephthalic acid ligands. − Therefore, in this study, UiO-66-NH 2 was selected as an adsorbent for the removal of heavy metals from wastewater because of its high stability in water and over a wide pH range (1–14). − Additionally, NH 2 groups in UiO-666-NH 2 have free lone pairs of electrons and can act as a Lewis base and form coordinate bonds with metal ions (Lewis acids) . Recently, there have been efforts to chemically functionalize UiO-66-NH 2 with strong chelating ligands to increase the adsorbent selectivity and capacity toward heavy metals. ,, For examples, UIO-66-thiol, UIO-66-(SH) 2 , UIO-66-2,5-dimercapto-1,3,4-thiadiazol, UIO-66-Cys, UIO-66-NHC(S)NHME, and UIO-66-Syst were utilized to purify polluted water from mercury and the results showed the maximum removal efficiencies of 171.5, 263.4, 670.5, 350.1, 769.0, and 110.5 mg/g, respectively. Moreover, Zr-MOFs have been utilized to purify water from phosphate ions due to the high affinity of Zr to interact with phosphate ions.…”

Section: Introductionmentioning

confidence: 99%

Thiol- and Amine-Incorporated UIO-66-NH₂ as an Efficient Adsorbent for the Removal of Mercury(II) and Phosphate Ions from Aqueous Solutions

Awad

Bakry

Ibrahim

et al. 2021

Ind. Eng. Chem. Res.

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In this study, the novel adsorbent UIO-66-IT was synthesized to extract mercury and phosphate ions from contaminated water. The synthetic strategy involved the preparation of the metal−organic framework (UIO-66-NH 2 ) followed by post-synthetic modification using the chelating ligand 2-imino-4-thiobiuret to form the UIO-66-IT adsorbent. The structure and the morphology of the adsorbent were investigated by a variety of analytical techniques including Fourier transform infrared, X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, and Brunauer−Emmett−Teller surface area measurements. The adsorption of mercury and phosphate was optimized by studying the effect of pH, initial concentration, contact time, dose, temperature, and competitive ions. The results revealed exceptionally high adsorption capacities toward mercury and phosphate ions of 580 and 178 mg/g, respectively, at pH = 5.5 and an initial concentration of 1500 and 1000 mg/L. The adsorption isotherms are in excellent agreement with the Langmuir isotherm model, indicating the formation of a monolayer on the surface of UIO-66-IT. The kinetics of adsorption fit well with the pseudo-second-order kinetics model, which suggests the chemical adsorption of mercury ions via the nitrogen and sulfur functional groups of the adsorbent and the physical adsorption of phosphate anions by protonated functional groups on the surface of the UIO-66-IT adsorbent. Selectivity studies showed removal efficiencies of 98.9% Hg(II) from a solution containing a mixture of metal ions at 25 mg/L. Regeneration studies showed that the adsorbent can be recycled several times by using nitric acid for mercury removal and sodium chloride for phosphate removal. Removal efficiencies were higher than 99% for both regenerations. Due to the simple synthetic strategy via cost-effective starting materials, unique chemical structure, rapid adsorption kinetics, and high surface area, which lead to excellent removal efficiency, stability, and excellent regeneration, UIO-66-IT is introduced as a unique adsorbent for the selective removal of mercury and phosphate ions to remediate polluted water.

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“…The values for the pristine MOFs are consistent with literature reports. 42 The collected isotherms were found to be type IV (IUPAC classification) isotherms presenting hysteresis loops. This behavior is typical of MOF beads made by spray-drying and can be attributed to the presence of some mesoporosity derived from the nanocrystal assembly that forms the beads.…”

Section: Synthesis and Characterizationmentioning

confidence: 97%

MOF-Beads Containing Inorganic Nanoparticles for the Simultaneous Removal of Multiple Heavy Metals from Water

Boix

Troyano

Garzón‐Tovar

et al. 2020

ACS Appl. Mater. Interfaces

110

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Pollution of water with heavy metals is a global environmental problem whose impact is especially severe in developing countries. Among water-purification methods, adsorption of heavy metals has proven to be simple, versatile and cost-effective. However, there is still a need to develop adsorbents with a capacity to remove multiple metal pollutants from the same water sample. Herein we report the complementary adsorption capacities of metal-organic frameworks (MOFs; here, UiO-66 and UiO-66(SH)2) and inorganic nanoparticles (iNPs; here, cerium-oxide NPs) into composite materials. These adsorbents, which are spherical microbeads generated in one step by continuous-flow spray-drying, efficiently and simultaneously remove multiple heavy metals from water, including As(III and V), Cd(II), Cr(III and VI), Cu(II), Pb(II) and Hg(II). We further show that these microbeads can be used as packing material in a prototype of a continuous-flow water treatment system, in which they retain their metal-removal capacities upon regeneration with a gentle acidic treatment. As proof-of-concept, we evaluated these adsorbents for purification of laboratory water samples prepared to independently recapitulate each of two strongly-polluted rivers: the Bone (Indonesia) and Buringanga (Bangladesh) rivers. In both cases, our microbeads reduced the levels of all the metal contaminants to below the corresponding permissible limits established by the World Health Organization (WHO). Moreover, we demonstrated the capacity of these microbeads to lower levels of Cr(VI) in a water sample collected from the Sarno River (Italy). Finally, to create adsorbents that could be magnetically recovered following their use in water purification, we extended our spraydrying technique to simultaneously incorporate two types of iNPs (CeO2 and Fe3O4) into UiO-66(SH)2, obtaining CeO2/Fe3O4@UiO-66-(SH)2 microbeads that adsorb heavy metals and are magnetically responsive.water by a magnet. Given their ready formation and tunability, we are confident that such iNP@MOF-Beads will prove utile in future water-purification applications.

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UiO-66-(SH)₂as stable, selective and regenerable adsorbent for the removal of mercury from water under environmentally-relevant conditions

Cited by 78 publications

References 64 publications

The interfacial reactivity of arsenic species with green rust sulfate (GRSO4)

The interfacial reactivity of arsenic species with green rust sulfate (GRSO4)

Thiol- and Amine-Incorporated UIO-66-NH₂ as an Efficient Adsorbent for the Removal of Mercury(II) and Phosphate Ions from Aqueous Solutions

MOF-Beads Containing Inorganic Nanoparticles for the Simultaneous Removal of Multiple Heavy Metals from Water

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UiO-66-(SH)2as stable, selective and regenerable adsorbent for the removal of mercury from water under environmentally-relevant conditions

Cited by 78 publications

References 64 publications

The interfacial reactivity of arsenic species with green rust sulfate (GRSO4)

The interfacial reactivity of arsenic species with green rust sulfate (GRSO4)

Thiol- and Amine-Incorporated UIO-66-NH2 as an Efficient Adsorbent for the Removal of Mercury(II) and Phosphate Ions from Aqueous Solutions

MOF-Beads Containing Inorganic Nanoparticles for the Simultaneous Removal of Multiple Heavy Metals from Water

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Product

Resources

About

UiO-66-(SH)₂as stable, selective and regenerable adsorbent for the removal of mercury from water under environmentally-relevant conditions

Thiol- and Amine-Incorporated UIO-66-NH₂ as an Efficient Adsorbent for the Removal of Mercury(II) and Phosphate Ions from Aqueous Solutions