Amide Linkages in Pyrene-Based Covalent Organic Frameworks toward Efficient Photocatalytic Reduction of Uranyl

Kang, Jinyang; Hang, Jiahui; Chen, Bo; Chen, Lang; Zhao, Pengxiang; Xu, Yongbin; Luo, Yu; Xia, Chuanqin

doi:10.1021/acsami.2c16702

Cited by 15 publications

(7 citation statements)

References 59 publications

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“…The amide COFs have large bandgaps and more negative CBs, which is beneficial for U(VI) photoreduction. The electron paramagnetic resonance analysis showed that single electrons were the main active species for U(VI) reduction, which was further evidenced by the intramolecular charge transfer calculation 51 …”

Section: Photocatalysismentioning

confidence: 76%

Highly selective removal of U(VI) from aqueous solutions by porous nanomaterials

Li,

Wang,

Wang

2024

EcoEnergy

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With the fast development of nuclear energy peaceful utilization, large amounts of U(VI) are not only required to be extracted from solutions for sustainable nuclear fuel supply but also inevitably released into the environment to result in pollution, which is hazardous to human health. Thereby, the selective extraction of U(VI) from aqueous solutions is crucial to U(VI) pollution treatment and also to nuclear industry sustainable development. In this minireview, we summarized the selective extraction of U(VI) from solutions by porous nanomaterials (i.e., porous carbon nanomaterials, covalent organic frameworks, metal organic frameworks, and other nanomaterials) using different techniques, that is, sorption, electrocatalysis, photocatalysis, and other strategies. The efficient high extraction ability is dependent on the properties of porous nanomaterials and the used techniques. The high surface areas, abundant active sites, and functional groups are efficient for the high sorption of U(VI), but the special functional groups such as amidoxime groups are more critical for high selective extraction. The electrocatalytic extraction is related to the active sites, especially the single atom sites, of the porous nanomaterials as electrode. The special functional groups, bandgap, electron transfer pathway and electron donor–acceptor structures of photocatalysts contribute the high photocatalytic extraction of U(VI). The interaction mechanisms are discussed from spectroscopic analysis and computational simulation at molecular level. In the end, the challenges and prospectives for the efficient extraction of U(VI) are described.

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Section: Photocatalysismentioning

confidence: 76%

Highly selective removal of U(VI) from aqueous solutions by porous nanomaterials

Li,

Wang,

Wang

2024

EcoEnergy

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Section: Uranium Enrichment and Separation From Wastewatermentioning

confidence: 99%

“…(g) EPR spectra of imine or amide COFs TFPPY-DP in aqueous solution at 10 min light irradiation, trapping agent: TEMPO. Reproduced with permission from ref . Copyright 2022, American Chemical Society.…”

Section: Uranium Enrichment and Separation From Wastewatermentioning

confidence: 99%

“…The separation of excitons and photoelectrons are both influenced by the bond connections in COFs, which also play a role in determining the substance's physicochemical properties. The amide and imine 2D COF TFPPY-DP were effectively synthesized by Kang et al, 107 and both of them have shown excellent visible light utilization and U(VI) catalytic reduction. Amide TFPPY-DP has a bigger band gap and higher negative CB in terms of photoelectric characteristics, which is advantageous for catalytic reduction.…”

Section: Photocatalytic Extractionmentioning

confidence: 99%

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Photocatalytic and Electrocatalytic Extraction of Uranium by COFs: A Review

Wen,

Yao,

Meng

et al. 2023

Ind. Eng. Chem. Res.

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The highly selective and effective enrichment of U(VI) from seawater and nuclear industry wastewater is important not only for nuclear power development and dependable energy source, but also for reducing the potential threat of radionuclides to the environment and human health. Covalent organic frameworks (COFs) are ideal materials for trapping U(VI) ions in aqueous solutions because of their advantages such as inherent porosity, strong skeleton, chemical stability, and good structural regularity. Herein, the most recent developments in the investigation of COFs for efficient preconcentration and separation of U(VI) by adsorption, photocatalysis, and electrocatalysis from seawater and radioactive wastewater are reviewed. The performance and related mechanisms of U(VI) interaction with COFs are carefully analyzed from the results of batch sorption experiments, the advanced spectroscopy analysis, and theoretical calculations. The potential and challenges of the present regarding the use of functional COFs for U(VI) extraction are described. Our aim is to provide insight and advice for the creation of innovative functional COFs for U(VI) extraction with high efficiency and selectivity in the future.

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“…However, from the perspective of green chemistry, if this method needs further development, some of the shortcomings need to be solved. First, as far as we all know, toxic reaction solvents such as 1,4-dioxane, mesitylene, N , N -dimethylformamide, dichlorobenzene, or the mixture of these solvent are commonly used reaction solvents in the solvothermal synthesis method. − These solvents have typical characteristics of high toxicity and high pollution. Thus, green, low toxic, or even nontoxic solvents need to be developed to replace these organic solvents.…”

Section: Introductionmentioning

confidence: 99%

A General Synthetic Strategy for the Synthesis of Imine-Linked Covalent Organic Frameworks in Choline Chloride–Hexafluoroisopropanol-Based Deep Eutectic Solvents

Deng,

Wang,

Liu

et al. 2023

Macromolecules

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The imine-linked covalent organic frameworks (COFs) have garnered significant attention in various fields due to exceptional stability and polyamide structures, etc. However, the conventional synthetic protocols for the high-crystallinity iminelinked COFs often necessitate the use of harmful organic solvent and extra catalyst, rendering their synthesis environmentally detrimental. Therefore, it is imperative to develop facile methods for COF preparation that employ green solvents without the need of extra catalyst. Herein, an environmentally friendly, efficient, general synthetic strategy was developed to synthesize five iminelinked COFs with high yield and high crystallinity by using choline chloride (ChCl)−hexafluoroisopropanol (HFIP) linked deep eutectic solvents (DESs) as general solvents for the first time. Unlike other reactions that required repeated exploration of the types of solvents to synthesize COFs with high crystallinity, the as-developed method only required changing the molar ratio of ChCl and HFIP in DES; various imine-linked COFs with high crystallinity can be synthesized. To further elucidate the formation of iminelinked COFs in ChCl-HFIP-based DESs, COF-CH-1, which was prepared using 1,3,5-tris(4-aminophenyl)benzene (TPB) and terephthalaldehyde (TPDD) as precursors, was regarded as an example. The formation process of COF-CH-1 was preliminarily deduced linked on the changes of morphology, functional groups, element compositions, etc., with the change of reaction temperature and reaction time in optimal DES. Finally, according to the results, we also preliminarily speculated on the possible role of DESs in COFs' formation.

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Amide Linkages in Pyrene-Based Covalent Organic Frameworks toward Efficient Photocatalytic Reduction of Uranyl

Cited by 15 publications

References 59 publications

Highly selective removal of U(VI) from aqueous solutions by porous nanomaterials

Highly selective removal of U(VI) from aqueous solutions by porous nanomaterials

Photocatalytic and Electrocatalytic Extraction of Uranium by COFs: A Review

A General Synthetic Strategy for the Synthesis of Imine-Linked Covalent Organic Frameworks in Choline Chloride–Hexafluoroisopropanol-Based Deep Eutectic Solvents

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