Tailored covalent organic framework with phosphorylation for boosting typical actinide adsorption under acidic conditions

Zhang, Huidi; Wang, Shuai; Yu, Jipan; Li, Zijie; Lan, Jian‐Hui; Zheng, Lirong; Liu, Siyan; Yuan, Liyong; Xiu, Taoyuan; Wang, Jindong; Wang, Xinpeng; Shi, Wei‐Qun

doi:10.1016/j.cej.2023.142408

Cited by 29 publications

(5 citation statements)

References 47 publications

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“…For L1, the peaks at 1634 and 1479 cm –1 represent the stretching vibration peaks of the CO bond and CN bond on the ligand, respectively. , After extraction, the two peaks became weaker and blue-shifted by 24 and 19 cm –1 , respectively, indicating that the CO and CN bonds in the ligand participated in the coordination. The blue-shift of the infrared spectrum may be caused by π–π stacking. , In addition, two new peaks formed at 1383 and 922 cm –1 , matching the free nitrate anion and UO bond peaks, − which indicates that U(VI) entered the organic phase from the aqueous phase and that the nitrate ion was engaged during the process. L2 changes similarly to L1, with the peaks of the CO and CN bonds becoming weaker and blue-shifted by 23 and 19 cm –1 , respectively.…”

Section: Resultsmentioning

confidence: 99%

Selective Separation of U(VI) from Pu(IV) by 2,9-Diamide-1,10-phenanthroline Ligands at High Acidity: Extraction and Coordination Chemistry

Liu,

Xiu,

Shehzad

et al. 2024

Inorg. Chem.

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During the PUREX process, the separation between U(VI) and Pu(IV) is achieved by reducing Pu(IV) to Pu(III), which is complicated and energy-consuming. To address this issue, we report here the first case of separation of U(VI) from Pu(IV) by o-phenanthroline diamide ligands under high acidity. Two new o-phenanthroline diamide ligands (1,10-phenanthroline-2,9-diyl)bis(indolin-1-ylmethanone) (L1) and (1,10-phenanthroline-2,9-diyl)bis((2-methylindolin-1-yl)methanone) (L2) were synthesized, which can effectively separate U(VI) from Pu(IV) even at 4 mol/L HNO3. The highest separation factor of U(VI) and Pu(IV) can reach over 1000, setting a new record for the separation of U(VI) from Pu(IV) under high acidity. Furthermore, extracted U(VI) can be easily recovered with water or dilute nitric acid, and the extraction performance remains stable even after 150 kGy gamma irradiation, which provides solid experimental support for potential engineering applications. The results of UV–vis titration and single-crystal X-ray diffraction measurements show that the 1:1 complex formed by L1 with U(VI) is more stable than all of the previously reported phenanthroline ligands, which reasonably reveals that the ligand L1 designed in this work has excellent affinity for U(VI). The findings of this work promise to contribute to the facilitation of the PUREX process by avoiding the use of reducing agents. It also provides new clues for designing ligands to achieve efficient separation between U(VI) and Pu(IV) at high acidity.

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Section: Resultsmentioning

confidence: 99%

Selective Separation of U(VI) from Pu(IV) by 2,9-Diamide-1,10-phenanthroline Ligands at High Acidity: Extraction and Coordination Chemistry

Liu,

Xiu,

Shehzad

et al. 2024

Inorg. Chem.

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“…The first pair of peaks of Fe 2p3 and Fe 2p1 are located at 710.52 eV and 723.76 eV, respectively, which were characteristic peaks of iron oxides, and the other pair of peaks of Fe 2p3 and Fe 2p1 are located at 712.7 eV and 726.1 eV, respectively, which were the peaks of a type of ferric phosphate salt [50,51]. Meanwhile, fitting the P 2p region yielded two different chemical states (Figure 6d), with the peak at 133.0 eV being the P-O-C bond in phytate, while the peak at 134.2 eV corresponded to the P-O-Fe bond [52,53]. The above analysis showed that PA and MPTS formed a PA/MPTS condensate by connecting through Si-O-P bonds.…”

Section: Surface Analysis By Xpsmentioning

confidence: 99%

The Formation of Phytic Acid–Silane Films on Cold-Rolled Steel and Corrosion Resistance

Duan,

Fan,

Shu

et al. 2024

Metals

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In this work, phytic acid (PA) and 3-mercaptopropyltrimethoxysilane (MPTS) underwent a condensation process to produce a phytic acid–silane (abbreviated PAS) passivation solution. Additionally, it was applied to the surface of cold-rolled steel to create a composite phytic acid–silane film. The functional groups of the passivation solution were analyzed by Fourier transform infrared spectroscopy (FT-IR). The composite film was evaluated using an electrochemical workstation, scanning electron microscope (SEM), energy dispersive spectrometer (EDS), X-ray photoelectron spectroscopy (XPS) and pull-off test. These techniques allowed for the characterization of the film’s micromorphology, oxidation, chemical composition and adhesion strength. The results show that the PAS composite film provides higher protection efficiency compared to cold-rolled steel substrates, low phosphorus passivation films, single phytate passivation films and commercial phosphate films. This composite film also has a higher adhesion strength, which is beneficial for subsequent coating, and a possible corrosion resistance mechanism was proposed as well. The PAS layer successfully prevents the penetration of corrosive media into the cold-rolled steel surface utilizing P–O–Fe bonds, thus improving the corrosion barrier effect of the substrate.

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“…However, there might be risks for humans if radioactive elements are unintentionally released into the environment . Nuclear wastewater that contains a variety of radionuclides, with unreacted uranium consistently being one of the most important radioactive wastes . A significant amount of nuclear waste streams also contains other typical radionuclides, including 99 Tc and 137 Cs, which are byproducts of nuclear fission between 235 U and 239 Pu .…”

Section: Treatment Of Inorganic Pollutantsmentioning

confidence: 99%

“…77 Nuclear wastewater that contains a variety of radionuclides, with unreacted uranium consistently being one of the most important radioactive wastes. 78 A significant amount of nuclear waste streams also contains other typical radionuclides, including 99 Tc and 137 Cs, which are byproducts of nuclear fission between 235 U and 239 Pu. 79 Radionuclide absorption by MOFs is a significant area of environmental protection and nuclear waste management.…”

Section: ■ Treatment Of Inorganic Pollutantsmentioning

confidence: 99%

Recent Development of Metal–Organic Frameworks for Water Purification

El-Sewify,

2024

Langmuir

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Water contamination is an increasing concern to mankind because of the increasing amount of pollutants in aquatic ecosystems. To purify the polluted water, various techniques have been used to remove hazardous components. Unfortunately, traditional cleanup techniques with a low uptake capacity are unable to achieve water purification. Metal−organic frameworks (MOFs) have recently shown potential in effective water pollutant isolation in terms of selectivity and adsorption capacity over traditional porous materials. The high surface area and versatile functionality of MOFs allow for the development of new adsorbents. The development of MOFs in a range of water treatments in the recent five years will be highlighted in this review, along with assessments of the adsorption performance relevant to the particular task. Moreover, the outlook on future opportunities for water purification using MOFs is also provided.

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Tailored covalent organic framework with phosphorylation for boosting typical actinide adsorption under acidic conditions

Cited by 29 publications

References 47 publications

Selective Separation of U(VI) from Pu(IV) by 2,9-Diamide-1,10-phenanthroline Ligands at High Acidity: Extraction and Coordination Chemistry

Selective Separation of U(VI) from Pu(IV) by 2,9-Diamide-1,10-phenanthroline Ligands at High Acidity: Extraction and Coordination Chemistry

The Formation of Phytic Acid–Silane Films on Cold-Rolled Steel and Corrosion Resistance

Recent Development of Metal–Organic Frameworks for Water Purification

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