Defect-engineered metal-organic framework with enhanced photoreduction activity toward uranium extraction from seawater

Liu, Tao; Tang, Shuai; Wei, Tao; Chen, Mengwei; Xie, Zuji; Zhang, Ruoqian; Liu, Yinjiang; Wang, Ning

doi:10.1016/j.xcrp.2022.100892

Cited by 19 publications

(12 citation statements)

References 69 publications

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“…[98][99][100][101] Through manipulating the physicochemical properties of the catalyst surface/interface, heteroatom doping and defect engineering modulate the binding energy of OER intermediates on the catalyst to achieve a highly selective OER. 26,101 On the other hand, appropriate heterojunction design can expose an anion-rich decorative interface to repel chloride ions with the help of negative electric repulsion. 101 In addition, composite strategies combining inert slow chloride layers (e.g., graphene, MnO x ) 97,102 with conventional highly active electrocatalysts also achieve excellent selectivity in chlorine-containing electrolytes.…”

Section: Strategies For Regulating Selectivitymentioning

confidence: 99%

“…26,101 On the other hand, appropriate heterojunction design can expose an anion-rich decorative interface to repel chloride ions with the help of negative electric repulsion. 101 In addition, composite strategies combining inert slow chloride layers (e.g., graphene, MnO x ) 97,102 with conventional highly active electrocatalysts also achieve excellent selectivity in chlorine-containing electrolytes.…”

Section: Strategies For Regulating Selectivitymentioning

confidence: 99%

“…23,35,46 Among the various modulation strategies, surface/interface engineering is the main instrument for catalytic selectivity modulation, mainly including heteroatom doping, defect engineering and heterojunction design. [98][99][100][101] Through manipulating the physicochemical properties of the catalyst surface/interface, heteroatom doping and defect engineering modulate the binding energy of OER intermediates on the catalyst to achieve a highly selective OER. 26,101 On the other hand, appropriate heterojunction design can expose an anion-rich decorative interface to repel chloride ions with the help of negative electric repulsion.…”

Section: Strategies For Regulating Selectivitymentioning

confidence: 99%

See 2 more Smart Citations

Designing electrocatalysts for seawater splitting: surface/interface engineering toward enhanced electrocatalytic performance

Liu

Sun

et al. 2023

Green Chem.

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Section: Strategies For Regulating Selectivitymentioning

confidence: 99%

Section: Strategies For Regulating Selectivitymentioning

confidence: 99%

Section: Strategies For Regulating Selectivitymentioning

confidence: 99%

See 1 more Smart Citation

Designing electrocatalysts for seawater splitting: surface/interface engineering toward enhanced electrocatalytic performance

Liu

Sun

et al. 2023

Green Chem.

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“…UiO-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.…”

Section: Synthesis and Structure Characterizationmentioning

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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“…Generally, constructing defects in MOF materials or compounding with other materials to construct heterojunctions can inhibit the recombination of photogenerated e − −h + and enhance the performance of photocatalytic reduction of U(VI). For example, Liu et al 62 synthesized a MOF-based photocatalytic adsorbent by defect engineering (Zr/Ti-MOF-25). The electronic structure of MOF was modulated by missing-linker defects and node metal substitution, resulting in the debasement of ΔE LMCT , which contributed to enhanced photocatalytic U(VI) extraction capacity.…”

Section: ■ Photocatalysis Techniquementioning

confidence: 99%

Highly Selective Extraction of U(VI) from Solutions by Metal Organic Framework-Based Nanomaterials through Sorption, Photochemistry, and Electrochemistry Strategies

Liu,

Li,

Tan

et al. 2023

Langmuir

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Defect-engineered metal-organic framework with enhanced photoreduction activity toward uranium extraction from seawater

Cited by 19 publications

References 69 publications

Designing electrocatalysts for seawater splitting: surface/interface engineering toward enhanced electrocatalytic performance

Designing electrocatalysts for seawater splitting: surface/interface engineering toward enhanced electrocatalytic performance

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

Highly Selective Extraction of U(VI) from Solutions by Metal Organic Framework-Based Nanomaterials through Sorption, Photochemistry, and Electrochemistry Strategies

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