Mixed-linker strategy toward enhanced photoreduction-assisted uranium recovery from wastewater and seawater

Chen, Mengwei; Liu, Tao; Tang, Shuai; Wei, Tao; Gu, Anping; Zhang, Ruoqian; Liu, Yinjiang; Wang, Hui; Xie, Zuji; Yuan, Yihui; Li, Zhandong; Wang, Ning

doi:10.1016/j.cej.2022.137264

Cited by 37 publications

(22 citation statements)

References 75 publications

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“…The R 2 of the Langmuir model was 0.99 for both adsorbents and higher than that of the Freundlich model, which indicates that the uranium adsorption behaviors of GTA and AO-GTA were dominated by a strong monolayer chemical process. 40 The R 2 of the Redlich-Peterson model was 0.99, further proving the above-mentioned conclusion. 41 The maximum adsorption capacity of GTA and AO-GTA calculated using the Langmuir model was 614.6 and 875.2 mg g −1 at 298 K, respectively, which is close to the experimental values and higher than other reported adsorbents (Fig.…”

Section: The Isotherms and Thermodynamicssupporting

confidence: 58%

One-pot synthesis of a graphene oxide-supported Ti_xAl_1−xO_y-based material modified with amidoxime for highly efficient uranium(vi) adsorption

Ding,

Wan,

Zheng

et al. 2024

J. Mater. Chem. A

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Section: The Isotherms and Thermodynamicssupporting

confidence: 58%

One-pot synthesis of a graphene oxide-supported Ti_xAl_1−xO_y-based material modified with amidoxime for highly efficient uranium(vi) adsorption

Ding,

Wan,

Zheng

et al. 2024

J. Mater. Chem. A

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“…calculation (Figure 3a,b). By combining Tauc and Mott-schottky (Figure S11, Supporting Information) data, [15] the band-edge positions are listed in Table S4, Supporting Information. As shown in Figure 5a, the derived band structures clearly demonstrate that CBM positions of all three samples are located above the reduction potential of U(VI)/U(IV), indicating the thermodynamically favorable photocatalytic reduction conversion of soluble U(VI) to insoluble U(IV).…”

Section: Uranium Adsorption In U-spiked Simulated Seawater Under Ligh...mentioning

confidence: 99%

Ligand‐Assistant Iced Photocatalytic Reduction to Synthesize Atomically Dispersed Cu Implanted Metal‐Organic Frameworks for Photo‐Enhanced Uranium Extraction from Seawater

Liu

Wei

et al. 2023

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and natural seawater. [5] Recently, porous framework materials (e.g., metal-organic framework (MOF), [6] covalent organic framework (COF), [7] hydrogen-bonded organic framework (HOF) [8] ) have been developed for uranium uptake by combination of ligand complexation and photocatalytic reduction. Most photocatalysts still suffer from inefficient ligand-tometal charge transfer (LMCT), [9] which severely restrict the photocatalytic activity. Recently, single-atom (SA) catalysts have attracted considerable research interest in heterogeneous catalysis over the recent years. [10] Some studies have reported a continuous decrease in catalytic activity with increasing particle size. [11] Hence, it is of great significance to rationally design and control the synthesis of monodispersed metal at the atomic level. Inspired by the iced-photochemical synthesis, [12] we developed ligand-assistant frozen photoreduction approach to anchor atomically dispersed Cu on aminofunctionalized Zr-MOF (Cu SA@UiO-66-NH 2 ). High angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure (XAFS) spectroscopy measurements confirm the atomically dispersed Cu in the form of N-Cu-N. By contrast, there are Cu nanoclusters decorated on UiO-66-NH 2 support (Cu Clu@UiO-66-NH 2 ) by the routine photochemical solution-phase reaction. Compared to the agglomerated active sites, isolated dispersed Cu sites contribute to higher photocatalytic activity, which endow Cu SA@UiO-66-NH 2 adsorbent with enhanced photoreduction-assistant uranium extraction performance from natural seawater together with superior antibacterial ability. Results and Discussion Synthesis and Structure CharacterizationUiO-66-NH 2 crystals were synthesized by the traditional solvothermal method [13] and then employed as the catalyst support. The Cu SA@UiO-66-NH 2 sample was prepared through ligandassistant iced photocatalytic reduction route, as illustrated in Uranium extraction from natural seawater is one of the most promising routes to address the shortage of uranium resources. By combination of ligand complexation and photocatalytic reduction, porous framework-based photocatalysts have been widely applied to uranium enrichment. However, their practical applicability is limited by poor photocatalytic activity and low adsorption capacity. Herein, atomically dispersed Cu implanted UiO-66-NH 2 (Cu SA@UiO-66-NH 2 ) photocatalysts are prepared via ligand-assistant iced photocatalytic reduction route. N-Cu-N moiety acts as an effective electron acceptor to potentially facilitate charge transfer kinetics. By contrast, there exist Cu sub-nanometer clusters by the typical liquid phase photoreduction, resulting in a relatively low photocatalytic activity. Cu SA@UiO-66-NH 2 adsorbents exhibit superior antibacterial ability and improved photoreduction conversion of the adsorbed U(VI) to insoluble U(IV), leading to a high uranium sorption capacity of 9.16 mg-U/g-Ads from natural seawater. This study provides new insight for enhancing uranium...

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“…However, a distinct amorphous signal appeared in the XRD pattern of M-UiO-66(Ce) at about 20 min of light irradiation time, displaying the collapse of the UiO-66 framework structure (Figure S14). This suggested that UiO-66(Ce) showed tolerance toward conversion from the ligand BDC to BDC-OH, 39 and thus the light irradiation time cannot be indefinitely prolonged. Different from the light irradiation time, a reduced concentration of UiO-66(Ce) contributed to the enhanced fluorescence intensity of M-UiO-66(Ce) (Figure 6b).…”

Section: Rapid Rt Synthesis Of M-uio-66(ce) and The Possible Mechanis...mentioning

confidence: 99%

Concentration- and Self-Catalysis-Dominated Rapid Synthesis of Multifunctional UiO-66(Ce) for Dual-Mode Sensing of Tetracycline

Shi,

Pu,

et al. 2023

Inorg. Chem.

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Simple and rapid synthesis of multifunctional metal–organic frameworks (MOFs) at room temperature (RT) with their multifunction controllable is still appealing for further expansion of the practical applications of MOFs. Herein, in this work, rapid RT synthesis of a multifunctional UiO-66(Ce) [M-UiO-66(Ce)] with both oxidase-like activity and fluorescence emission properties was facilely achieved within 15 min through a straightforward reactant concentration modulation and self-catalytic postmodification strategy. Appropriate concentrations of cerium ammonium nitrate or 1,4-benzenedicarboxylic acid (BDC) were beneficial for the synthesis of UiO-66(Ce) with better crystallization. During the postmodification process, through regulation of the self-photocatalysis of UiO-66(Ce), a high conversion rate from BDC to BDC-OH of up to 14% can be obtained, resulting in a significantly enhanced fluorescence signal of M-UiO-66(Ce) within 2 min. Moreover, M-UiO-66(Ce) enabled the accurate and reliable detection of tetracycline (TC) in real samples. Besides, the colorimetric and fluorescence modes complemented each other, expanding the linear range of TC detection and exhibiting its great potential for practical applications. This work provides new insights for the convenient and rapid synthesis of multifunctional materials based on MOFs, which is favorable for promoting the large-scale preparation of MOFs and their practical application in on-site environmental pollutant sensing.

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Mixed-linker strategy toward enhanced photoreduction-assisted uranium recovery from wastewater and seawater

Cited by 37 publications

References 75 publications

One-pot synthesis of a graphene oxide-supported Ti_xAl_1−xO_y-based material modified with amidoxime for highly efficient uranium(vi) adsorption

One-pot synthesis of a graphene oxide-supported Ti_xAl_1−xO_y-based material modified with amidoxime for highly efficient uranium(vi) adsorption

Ligand‐Assistant Iced Photocatalytic Reduction to Synthesize Atomically Dispersed Cu Implanted Metal‐Organic Frameworks for Photo‐Enhanced Uranium Extraction from Seawater

Concentration- and Self-Catalysis-Dominated Rapid Synthesis of Multifunctional UiO-66(Ce) for Dual-Mode Sensing of Tetracycline

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Mixed-linker strategy toward enhanced photoreduction-assisted uranium recovery from wastewater and seawater

Cited by 37 publications

References 75 publications

One-pot synthesis of a graphene oxide-supported TixAl1−xOy-based material modified with amidoxime for highly efficient uranium(vi) adsorption

One-pot synthesis of a graphene oxide-supported TixAl1−xOy-based material modified with amidoxime for highly efficient uranium(vi) adsorption

Ligand‐Assistant Iced Photocatalytic Reduction to Synthesize Atomically Dispersed Cu Implanted Metal‐Organic Frameworks for Photo‐Enhanced Uranium Extraction from Seawater

Concentration- and Self-Catalysis-Dominated Rapid Synthesis of Multifunctional UiO-66(Ce) for Dual-Mode Sensing of Tetracycline

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One-pot synthesis of a graphene oxide-supported Ti_xAl_1−xO_y-based material modified with amidoxime for highly efficient uranium(vi) adsorption

One-pot synthesis of a graphene oxide-supported Ti_xAl_1−xO_y-based material modified with amidoxime for highly efficient uranium(vi) adsorption