Benchmark uranium extraction from seawater using an ionic macroporous metal–organic framework

Mollick, Samraj; Saurabh, Satyam; More, Yogeshwar D.; Fajal, Sahel; Shirolkar, Mandar M.; Mandal, Writakshi; Ghosh, Sujit K.

doi:10.1039/d2ee01199a

Cited by 64 publications

(44 citation statements)

References 49 publications

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“…Before turning on the Xenon lamp, the COFs were immersed in the uranium-spiked seawater overnight to achieve adsorption equilibrium. The uranium is mainly in the speciation of [UO 2 (CO 3 ) 3 ] 4- in seawater, and the adsorbent needs to compete with carbonate groups for binding uranyl ions 55 , 57 , 60 , 61 , 63 , 64 . In comparison with the binding affinity of CO 3 2- to UO 2 2+ , hydrazine-carbonyl groups through COFs 1 to 3 and the hydrazine sites in COF-4 showed stronger binding affinities towards UO 2 2+ than towards CO 3 2- , therefore the [U(VI)O 2 (H 2 O) 2 ] 2+ adsorbed spontaneously on all the COFs 64 .…”

Section: Resultsmentioning

confidence: 99%

Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance

et al. 2023

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Covalent organic frameworks (COFs) represent an emerging class of organic photocatalysts. However, their complicated structures lead to indeterminacy about photocatalytic active sites and reaction mechanisms. Herein, we use reticular chemistry to construct a family of isoreticular crystalline hydrazide-based COF photocatalysts, with the optoelectronic properties and local pore characteristics of the COFs modulated using different linkers. The excited state electronic distribution and transport pathways in the COFs are probed using a host of experimental methods and theoretical calculations at a molecular level. One of our developed COFs (denoted as COF-4) exhibits a remarkable excited state electron utilization efficiency and charge transfer properties, achieving a record-high photocatalytic uranium extraction performance of ~6.84 mg/g/day in natural seawater among all techniques reported so far. This study brings a new understanding about the operation of COF-based photocatalysts, guiding the design of improved COF photocatalysts for many applications.

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Section: Resultsmentioning

confidence: 99%

Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance

et al. 2023

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“…With a view toward harvesting marine uranium resources, it is essential to develop materials that can resist biofouling and selectively capture uranium under high ionic strength conditions. Adsorbent materials such as porous carbon-based adsorbents, − layered organic–inorganic materials, organic polymers, − biomaterials, − and metal–organic frameworks (MOFs) − have all been investigated for uranium extraction from seawater. However, these adsorbents possess drawbacks, including one or more of the following: slow adsorption kinetics, low adsorption capacities, poor stability, inferior recyclability, or rapid marine biological passivation.…”

Section: Introductionmentioning

confidence: 99%

Modulating Uranium Extraction Performance of Multivariate Covalent Organic Frameworks through Donor–Acceptor Linkers and Amidoxime Nanotraps

Hao

Xie

Liu

et al. 2023

JACS Au

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Covalent organic frameworks (COFs) can be designed to allow uranium extraction from seawater by incorporating photocatalytic linkers. However, often sacrificial reagents are required for separating photogenerated charges which limits their practical applications. Herein, we present a COF-based adsorption-photocatalysis strategy for selective removal of uranyl from seawater in the absence of sacrificial reagents. A series of ternary and quaternary COFs were synthesized containing the electron-rich linker 2,4,6-triformylphloroglucinol as the electron donor, the electron-deficient linker 4,4′-(thiazolo[5,4- d ]thiazole-2,5-diyl)dibenzaldehyde as the acceptor, and amidoxime nanotraps for selective uranyl capture (with the quaternary COFs incorporating [2,2′-bipyridine-5,5′-diamine-Ru(Bp) 2 ]Cl 2 as a secondary photosensitizer). The ordered porous structure of the quaternary COFs ensured efficient mass transfer during the adsorption-photocatalysis capture of uranium from seawater samples, with photocatalytically generated electrons resulting in the reduction of adsorbed U(VI) to U(IV) in the form of UO 2 . A quaternary COF, denoted as COF 2-Ru-AO, possessed a high uranium uptake capacity of 2.45 mg/g/day in natural seawater and good anti-biofouling abilities, surpassing most adsorbents thus far. This work shows that multivariate COF adsorption-photocatalysts can be rationally engineered to work efficiently and stably without sacrificial electron donors, thus opening the pathway for the economic and efficient extraction of uranium from the earth’s oceans.

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“…9,10 Materials being developed for effective U(VI) extraction from natural water include organic natural ber materials, inorganic porous materials, metal-organic frameworks (MOF), covalent organic frameworks (COF), and porous aromatic frameworks. [11][12][13][14][15][16] However, most of these sorbents are in powder form and therefore not suitable for practical applications. 17 Compared to inorganic powders, macroscopic materials such as ber-based materials and foam materials have the advantages of cheapness, ease of delivery, abundance of functional groups, high selectivity, and more practical application prospects.…”

Section: Introductionmentioning

confidence: 99%

Biomimetic porous cellular foam with space thermal domains for efficient uranium extraction from seawater

Zhu

Zhang

et al. 2023

J. Mater. Chem. A

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Benchmark uranium extraction from seawater using an ionic macroporous metal–organic framework

Abstract: Large-scale uranium extraction from seawater (UES) is widely considered as reconciliation to increasing global energy demand and climate change crises. However, an ideal uranium sorbent combining features of high capacity,...

Cited by 64 publications

References 49 publications

Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance

Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance

Modulating Uranium Extraction Performance of Multivariate Covalent Organic Frameworks through Donor–Acceptor Linkers and Amidoxime Nanotraps

Biomimetic porous cellular foam with space thermal domains for efficient uranium extraction from seawater

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