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• ZIF-8 was fabricated by stirring at room temperature. • Enhancing the adsorption performance of ZIF-8 through thermal modification. • Surface complexation and electrostatic interaction were main removal mechanisms. • U(VI) formed coordination complexes with the N atoms of ZIF-8-400. Zeolite imidazolium framework materials (ZIFs) had been extensively applied for U(VI) removal because of their superior structure, high porosity and large specific surface area. Nevertheless, ZIF-8 tended to accumulate in aqueous solution and it was hard to detach from water, resulting in a decrease in the removal performance. Therefore, it was necessary to conduct thermal modification treatment to solve the above problems. The U(VI) removal capability of ZIF-8 was investigated in this study by subjecting it to various thermal modification temperatures (0 °C, 200 °C, 400 °C, 600 °C). The effect of thermal modification on the removal of U(VI) from ZIF-8 was investigated by a combination of macroscopic and microscopic experiments. Macroscopic experiments revealed ZIF-8, ZIF-8-200, and ZIF-8-400 showed excellent removal efficiency, reaching reaction equilibrium rapidly (about 60 min). The adsorption kinetic and isotherm datum were more consistent with proposed second-order kinetic model and Langmuir model, confirming that removal process of U(VI) was mainly a single-molecule chemisorption reaction. The maximum removal amounts of ZIF-8, ZIF-8-200 and ZIF-8-400 were 470.5, 474.6 and 606.0 mg/g, respectively. Microscopic spectroscopic analysis revealed that there was a synergistic effect between the combination bonds in ZIF-8 during the adsorption reaction. Surface complexation and electrostatic interaction were the main mechanisms used by ZIF-8-400 to remove U(VI). This research offered theoretical guidance on the design of high-performance materials and the migration and transformation laws of radionuclides, which had significant theoretical significance for the future treatment of radioactive nuclides or other pollutants. [Display omitted] [ABSTRACT FROM AUTHOR]

Efficient containment and capture of uranium (U(VI)) from aqueous solution is an essential component to ensure socially and environmentally sustainable development. Herein, the three-dimensional graphene/titanium dioxide composite (3D GA/TiO 2) was synthesized and applied as an effective adsorbent to remove U(VI) from wastewater as a function of contact time, temperature, pH and ion strength. The 3D GA/TiO 2 material was characterized by X-ray diffraction, Raman spectroscopy, Fourier-transform infrared spectroscopy, and X-ray photoelectron spectroscopy. The batch experiments results indicated that the adsorption of U(VI) on materials were fitted with the pseudo-second order kinetics and Langmuir models. More specifically, 3D GA/TiO 2 (441.3 mg/g) was observed to outperform the GO (280.0 mg/g), rGO (140.9 mg/g) and TiO 2 (98.5 mg/g) at pH 5.0, which was attributable to the excellent cooperative effects. Furthermore, XPS analyses and DFT calculations confirmed the formation of surface complexes between oxygen-containing group and U(VI) with the U–O bonds length of 2.348 Å (U–O1) and 2.638 Å (U–O2). Meanwhile, the adsorption energy was calculated to be 1.60 eV, which showed a very strong chemisorption during the interaction process. It is believed that the 3D GA/TiO 2 revealed good removal performance for uranyl ions, which showed a great potential application to control the nuclear industrial pollution. Image 1 • 3D GA/TiO 2 composite was prepared via a facile and green method. • Synergistic effects improved the capture ability for U(VI) on 3D GA/TiO 2 than GO, rGO and TiO 2. • The adsorption energy of U(VI) onto 3D GA/TiO 2 was calculated to be 1.60 eV. • Interaction mechanism was electrostatic interaction and inner-sphere surface complexation. Three-dimensional graphene/titanium dioxide nanoparticle hybrids (3D GA/TiO 2) were fabricated and revealed excellent removal properties for uranyl ions. [ABSTRACT FROM AUTHOR]

Graphical abstract Highlight • LDH@nZVI composite was prepared via a facile and green method. • Synergistic effects improved the capture ability for U(VI) on LDH@nZVI than single-guest. • O and Fe functional groups play an important role in the immobilization process of U(VI). • Interaction mechanism between U(VI) and LDH@nZVI was adsorption and reduction. Abstract In this study, nanoscale zero-valent iron (nZVI) supported on layered double hydroxide (LDH) composite (LDH@nZVI) was prepared, characterized and applied to U(VI) scavenging in water. Removal of U(VI) as a function of pH, ionic strength, reaction time, initial concentrations of U(VI), and temperature were studied and compared with pure LDH and nZVI, the LDH@nZVI had best U(VI) removal efficiency owning to the excellent synergistic combination of LDH adsorption and nZVI reduction. XPS analysis found that surface oxygen functional groups and surface-bound Fe(II) played a critical role in U(VI) remediation. The large surface areas (334.0 m2/g), abundant functional groups (i.e., M O, C O and OH), rapid kinetics (adsorption equilibrium within 1 h) and excellent adsorption capacities (176 mg/g) indicating that LDH@nZVI can be considered as a potential material for preconcentration of U(VI) from sewage water. [ABSTRACT FROM AUTHOR]

Graphical abstract Highlights • CMN and CCMN were prepared via a single-step hydrothermal technique and calcination process. • The maximal removal capacities of U(VI) on CMN and CCMN were 585.6 and 973.7 mg/g, respectively. • Metal-oxygen functional groups played an important role in the elimination of U(VI). • Interaction mechanism was attributed to strong inner-surface complexation. Abstract Uranium is considered to be a strategic means for the nuclear power as well as a worldwide highly toxic pollutant. For the enhanced U(VI) elimination from wastewater, novel Co-Mo-Ni ternary hydroxide (CMN) and calcined CMN (CCMN) nanocomposites were prepared via a simplistic single-step hydrothermal technique and calcination process. The elimination process and adsorption property of U(VI) on CMN and CCMN were analysed by batch experiment as well as spectroscopy analysis, and the researches showed that U(VI) was formed stable and strong complexes with the surface groups of CMN and CCMN. The maximal removal capacities of U(VI) on CMN and CCMN amounted to be 585.6 and 973.7 mg/g at pH = 5.0 and T = 298 K, correspondingly, that exhibited competitiveness with the majority of the reported adsorbents. The U(VI) uptake was substantially impacted by the tested solution pH and not affected by the ionic strength, which revealed that the interaction mechanism was primarily inner-sphere surface complexation, which received further confirmation by the XPS analysis. Based on the above analyses, the facile synthesis process and excellent U(VI) elimination performance denoted that the ternary (hydr)oxide materials were applicable as an attractive adsorbent for the radionuclides preconcentration and removal from aqueous solutions in natural environmental management. [ABSTRACT FROM AUTHOR]

Uranium mainly exists in the form of uranyl carbonate in seawater. [UO 2 (CO 3) 3 ]4- has strong stability, which increases the difficulty of uranium extraction from seawater. Meanwhile, the complex marine environment, a large number of coexisting competing ions and biological pollution are all non-negligible disturbing factors. Herein, we introduced amidoxime (AO) groups into the surface of Ti 3 C 2 and grafted polyamides (PA) by a simple one-step hydrothermal method to produce an efficient seawater uranium extraction adsorbent Ti 3 C 2 -AO-PA. Owing to the amidoxime groups, the material was highly selective for uranium. And the large number of amino groups in the polyamides gave it ideal resistance to biofouling. The possibility of Ti 3 C 2 -AO-PA as an adsorbent for uranium extraction from seawater was confirmed by various characterization techniques, numerous adsorption batch experiments, simulated seawater experiments and antibacterial performance tests. It was demonstrated that the uptake of [UO 2 (CO 3) 3 ]4- by Ti 3 C 2 -AO-PA showed fast reaction kinetics (about 120 min), brilliant absorption capacity (81.1 mg·g−1 at pH 8.3), significant high selectivity (32.8 mg-U/g-Ads) and outstanding anti-biological contamination performance (92.9% antibacterial rate). XPS and DFT further indicated that the high extraction ability of Ti 3 C 2 -AO-PA for uranium was mainly attributed to the strong complexation of AO and –NH 2 with [UO 2 (CO 3) 3 ]4-. These conclusions showed that Ti 3 C 2 -AO-PA not only had an ideal application prospect for uranium extraction from seawater, but also provided an available strategy for rapid and selective uranium adsorption from real seawater. [Display omitted] • Polyamide enhanced amidoxime-functionalized Ti 3 C 2 nanosheet was constructed. • The uranium extraction capacity was highly enhanced. • Ti 3 C 2 -AO-PA showed excellent selectivity and antimicrobial properties. • Synergistic interactions of amidoxime and polyamide with uranium ions in seawater. [ABSTRACT FROM AUTHOR]

The potential threat of radionuclide uranium from nuclear industry had attracted worldwide attention because both environment and human beings were menaced. Nowadays, modified nanoscale zero valent iron (NZVI) had been reported to be efficient in U(VI) elimination due to its high reactivity, reducibility, and availability. In this study, serial biochar-based sulfide NZVIs (BC-SNZVIs) with different C/Fe and S/Fe were synthesized and applied to the elimination of U(VI) in order to investigate the effect of iron, sulfur, and biochar precursor. The morphological investigations indicated the precursor played an essential role towards BC-SNZVIs on their dispersibility and structure. The XRD analyzes were conducted to study their crystalline structure and the BC 1.0 -S 0.14 NZVI showed outstanding stability after 10-day exposure under atmosphere. The excellent magnetism was confirmed via VSM study, and BC 1.0 -S 0.14 NZVI could be easily and rapidly separated from aqueous solution. The batch kinetic and isothermal studies illustrated the superior performances towards U(VI), and the results revealed the fast kinetics and high capacities of BC-SNZVIs. Finally, the removal mechanism was explored by using XPS technology and pH-effect experiment. U(VI) was adsorbed by BC matrix and SNZVI, while portion of U(VI) was reduced into U(IV) by Fe0 inner core. The elimination process of U(VI) towards BC-SNZVI was confirmed to be a synergistic effect of adsorption and reduction. This study verified the optimal ratio of C/Fe and S/Fe, and explained the removal mechanism in detail, which was beneficial to further investigations of NZVI-based and biochar-based materials. [Display omitted] • The impact of C/Fe and S/Fe ratios on biochar-based SNZVIs were investigated. • BC 1.0 -S 0.14 NZVI showed excellent attraction and outstanding performance to U(VI). • The removal mechanism was a synergistic effect of reduction and adsorption. [ABSTRACT FROM AUTHOR]

Bacteria may change the physicochemical properties of montmorillonite and further effect the disposal of high-level radioactive waste. Therefore, we explored the influence of Shewanella oneidensis MR-1 on the elimination of representative radionuclide U(VI) by montmorillonite (MMT). The batch experiments showed that MR-1 significantly enhanced the removal efficiency of U(VI), the adsorption capacity of MMT improved from 8.4 to 16.1 mg/g after addition of MR-1, and the adsorption type changed from Langmuir to Freundlich. FTIR and XPS analysis revealed that hydroxyl, phosphate, carbonyl and amine in MMT + MR-1 were primary actors in the elimination of U(VI). The U 4f high-resolution XPS spectrum of MMT + MR-1 showed U(VI) and U(IV) peaks at the same time, indicating that the adsorption process was accompanied by the reduction reaction, which may be due to the extracellular respiration of MR-1. These investigations are significant to insight the potential significance of microbial processes for the transport and elimination of U(VI) in repositories, which in return will contribute to their safe disposal. [Display omitted] ● Synergetic effect existed in U(VI) sequestration onto MMT + MR-1. ● Shewanella oneidensis MR-1 enhanced the elimination of U(VI) on montmorillonite. ● The adsorbed U(VI) can be reduced to U(IV) by Shewanella oneidensis MR-1. ● The main mechanisms between U(VI) and MMT + MR-1 were adsorption and reduction. [ABSTRACT FROM AUTHOR]

Both environment and human beings were menaced by the widespread application of radioactive uranium, high-performance and effective elimination of uranium from wastewater is of important meaning for development of environmental sustainability in the future. In this study, the water-stable MOF material and the highly crystalline COF were compounded by a mild hydrothermal strategy, which achieved efficient removal of U(VI) through the synergistic effect. The composites showed the characteristics of both COFs and MOFs, which will possess higher stability, larger surface area and faster adsorption efficiency that cannot be carried out by a single component. Batch experiments and characterizations (SEM, TEM, XRD, FT-IR, BET, XPS, etc.) indicated that UiO-66-NH 2 @LZU1 had more stable and multi-layer pore structure and rich active functional groups. The Langmuir model and the pseudo-second-order kinetics fitting was more suitable for the U(VI) elimination process. The greatest uranium adsorbing capacity of UiO-66-NH 2 @LZU1 (180.4 mg g−1) was observed to exceed the UiO-66-NH 2 (108.8 mg g−1) and COF-LZU1 (65.8 mg g−1), which reached the excellent hybrid effects. Furthermore, FT-IR and XPS analyses confirmed that the most nitrogen-containing group from COF-LZU1 and oxygen-containing group of UiO-66-NH 2 could be combined with U(VI). In addition, electrostatic interaction was also a mechanism during the removal process. This work displayed that UiO-66-NH 2 @LZU1 was a prospective hybrid material for radioactive waste remediation. The compound method and application mentioned in this work had provided a theoretical basis for designing and developing multi-functional composite adsorbents, which contributed to the development of new materials for radioactive wastewater treatment technologies. [Display omitted] • UiO-66-NH 2 @LZU1 composite material was obtained by solvothermal method. • Highly efficient uranium adsorbent, adsorption capacity reached 163.1 mg g−1. • Abundant nitrogen/oxygen functional groups promote uranium removal. • Main removal mechanism included electrostatic interaction and surface complexation. [ABSTRACT FROM AUTHOR]

[Display omitted] • The characteristics of novel nanomaterials for uranium extraction are summarized. • The influencing factors for uranium extraction from seawater are introduced. • The mechanisms mainly include electrostatic, coordination, and chelation. • The opportunities and challenges in seawater uranium extraction are presented. There are abundant uranium resources in the ocean, from the perspective of resource utilization and ecological environmental protection, seawater uranium extraction is a way to regenerate uranium resources with high potential value. Due to the advantages of low cost, simple operation, practicality and environmental friendliness, the adsorption method has become one of the most commonly used and effective techniques for uranium extraction from seawater. This review first introduces commonly used adsorbents, mainly including carbon-based materials, metal organic frameworks (MOFs), covalent organic frameworks (COFs), biopolymers, amidoxime based materials and so on. Then, the main influencing factors of seawater uranium extraction by adsorption are listed, mainly including coexisting metal ions, salinity, pH, temperature and biofouling. Next, some experimental examples of the application of advanced techniques to speculate on reaction mechanisms such as coordination, chelation, electrostatic attraction, and adsorptive photocatalytic synergy are presented. Finally, this review puts forward the opportunities and challenges that still exist in seawater uranium extraction, and looks forward to its development prospects on this basis. The overview will help readers to further understand the key technologies of seawater uranium extraction and to discover more efficient and environmentally friendly materials for seawater uranium extraction, which is significant to support the development of nuclear power industry. [ABSTRACT FROM AUTHOR]

Graphical abstract Rod-like metal-organic framework (MOF-5) nanomaterial for efficient removal of U(VI) from aqueous solutions. Abstract With the widespread application of radionuclide 235U(VI), it is inevitable that part of U(VI) is released into the natural environment. The potential toxicity and irreversibility impact on the natural environment has become one of the most forefront pollution problems in nuclear energy utilization. In this work, rod-like metal-organic framework (MOF-5) nanomaterial was synthesized by a solvothermal method and applied to efficiently adsorb U(VI) from aqueous solutions. The batch experimental results showed that the sorption of U(VI) on MOF-5 was strongly dependent on pH and independent of ionic strength, indicating that the dominant interaction mechanism was inner-sphere surface complexation and electrostatic interaction. The maximum sorption capacity of U(VI) on MOF-5 was 237.0 mg/g at pH 5.0 and T = 298 K, and the sorption equilibrium reached within 5 min. The thermodynamic parameters indicated that the removal of U(VI) on MOF-5 was a spontaneous and endothermic process. Additionally, the FT-IR and XPS analyses implied that the high sorption capacity of U(VI) on MOF-5 was mainly attributed to the abundant oxygen-containing functional groups (i.e., C O and C O). Such a facile preparation method and efficient removal performance highlighted the application of MOF-5 as a candidate for rapid and efficient radionuclide contamination's elimination in practical applications. [ABSTRACT FROM AUTHOR]

Uranium has attracted sustained attention due to its high mobility and biotoxicity. Among various techniques, sorption is considered as the most effective technique to treat the U(VI)-containing wastewater. In serving for low-cost adsorbents, layered double hydroxides (LDHs) have been proved to be promising candidates. However, the interaction mechanism of U(VI) with LDHs is still unclear, although plenty of LDHs have been used in this field. Herein, we developed two novel methods to fabricate ternary LDHs (MgFeAl LDHs and NiFeAl LDHs) and applied the ternary LDHs as adsorbents to investigate their sorption performance towards U(VI). The results showed that the sorption was endothermic and followed the pseudo-second-order kinetics through the formation of inner-sphere surface complexes, and the sorption isotherms were simulated by the Langmuir model well. Furthermore, systematic spectroscopy characterization indicated that the sorption occurred on the surface sites of Mg-OH and Ni 2+ –OH, while the CO 3 2− in the gallery space also played an important role. This work highlighted the synthesis of high-efficient materials and their application in wastewater treatment. [ABSTRACT FROM AUTHOR]

Graphical abstract A novel arginine modified hydroxyapatite carbon microsphere (C@HAp/Arg) composite were synthesized by a facile and green method and exhibited superior adsorption efficiency for removal of U(VI). Abstract Uranium was not only the main source of nuclear energy but also one of the long-lived radionuclide. Herein, a novel arginine modified hydroxyapatite carbon microsphere composites (defined as C@HAp/Arg) obtained promptly via a one-step mild hydrothermal method, was applied to remove U(VI) from aqueous solutions. Based on the characterization of transmission electron microscopy (TEM), scanning electron microscopy (SEM), Fourier transformed infrared spectroscopy (FT-IR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), the synthesized C@HAp/Arg presented globular morphology and abundant functional groups (e.g., COO−), which were beneficial to its combination with U(VI). The interaction mechanism and removal capability of U(VI) on C@HAp/Arg were studied by batch adsorption technique and spectroscopy analysis. The results implied that U(VI) can form strong surface complexes on C@HAp/Arg. The kinetics adsorption of U(VI) followed pseudo-second-order kinetic model with high removal efficiency (∼95% within 5 h at pH 5.0). The adsorption isotherms were well fitted by Langmuir model, implying that U(VI) uptake on C@HAp/Arg was monolayer coverage. It was found that the maximum adsorption capacities of CSs, C@HAp and C@HAp/Arg toward U(VI) were calculated to be 23.16, 72.09 and 569.66 mg/g, respectively, at 298.15 K and pH 5.0, and thermodynamic parameters revealed that the adsorption processes of U(VI) were spontaneous and endothermic. In addition, effect of co-existed ions and CO 3 2− concentrations demonstrated that U(VI) adsorption on C@HAp/Arg was weakly interfered by foreign ions and carbonate concentrations. More importantly, the adsorption performance of U(VI) on C@HAp/Arg was still over ∼87% after five cycles. Therefore, it was noted that the versatile C@HAp/Arg could be potentially used as a powerful building block for the enrichment and disposal of U(VI) from aqueous solutions, which could efficiently reduce the potential toxicity of U(VI) in the U(VI)-contaminated water. [ABSTRACT FROM AUTHOR]

Radioactive uranium removal plays a key role in energy development and environmental security. Sulfide nanoscale zero-valent iron (S-NZVI) has good antioxidant capacity, dispersibility and activity to eliminate U(VI) from wastewater, but the removal efficiency is limited. To improve the reduction and adsorption capacity of S-NZVI, through treating Fe3+ solution by nitro-functionalized UiO-66 (UiO-66-NO 2) with high porosity, UiO-66-NO 2 enhanced S-NZVI adsorbent (S-NZVI/UiO-66) was prepared by liquid phase reduction method. The smaller size and larger specific surface area of S-NZVI/UiO-66 were confirmed by a variety of characterization techniques. Based on the excellent surface structure and reactivity, the U(VI) removal capacity of S-NZVI/UiO-66 (895 mg g−1) was much better than S-NZVI (434 mg g−1) and UiO-66-NO 2 (267 mg g−1). The impacts of pH, background ion strength, coexisting ions and different water environments on adsorption were studied via macroscopic batch experiments. The results showed that S-NZVI/UiO-66 could remove U(VI) adequately in a wide pH range. The removal rate was basically not affected by the concentration of NaNO 3 , demonstrating that the adsorption process of U(VI) on S-NZVI/UiO-66 tended to inner surface complexation. From XPS technique combined with the results of batch adsorption experiments, it was clear that the elimination mechanisms of U(VI) by S-NZVI/UiO-66 were mainly the physical adsorption, electrostatic attraction and complexation of UiO-66-NO 2 , and the reduction and complexation of S-NZVI. Therefore, it is believed that S-NZVI/UiO-66 has a great potential to be an excellent adsorbent in the field of the environment remediation. Moreover, S-NZVI/UiO-66 promises to be a novel nanomaterial for solving the problem of radionuclide contamination in practical environments. [Display omitted] • The pretreatment of UiO-66-NO 2 can effectively reduce the size of S-NZVI. • S-NZVI/UiO had a better specific surface area than the original S-NZVI. • The practical application potential of S-NZVI/UiO was confirmed. • The removal mechanisms were adsorption and reduction. [ABSTRACT FROM AUTHOR]

[Display omitted] • TC-AO were used to adsorb U(VI) and Eu(III). • Abundant functional groups and good selectivity endowed TC-AO excellent property. • The practical application potential of TC-AO was confirmed. • The mechanisms were surface complexation and electrostatic interaction. Although two-dimensional transition metal carbides and carbonitrides (MXenes) are becoming increasingly popular in contaminant remediation field, the preparation of MXene nanosheets that can efficiently eliminate the target pollutants still deserves in-depth investigation. Here we produced amidoxime Ti 3 C 2 T x nanosheets (TC-AO), which were efficient radionuclide adsorbents with high stability and positive affinity, by introducing the amidoxime group into the Ti 3 C 2 T x MXene surface through grafting by diazonium salt. The high stability and abundant functional groups of TC-AO were demonstrated by different characterization techniques such as scanning electron microscope (SEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analyzer (TGA), and X-ray photoelectron spectroscopy (XPS). Multiple factors affecting the radionuclide removal performance were explored, including reaction time, temperature, pH, ionic strength, anions and cations. The experimental results demonstrated that the radionuclide uptake by TC-AO was a heat-absorbing, spontaneous single-molecule chemisorption process and was consistent with the pseudo-secondary and Langmuir models. When pH < 6, the mechanism of uranium removal was inner complexation, and as the pH continued to increase, uranium removal shifted to outer complexation. Furthermore, the results certificated that TC-AO exhibited fast reaction kinetics (reaching equilibrium in about 20 min), excellent removal efficiency (279.57 mg U·g−1 and 73.99 mg Eu·g−1), outstanding selectivity and good stability. The studies showed that TC-AO had good stability and functionality, which was not only valuable for the design of MXene based adsorbents, but also provided a meaningful option for the extraction of radioactive pollutants from wastewater. [ABSTRACT FROM AUTHOR]

Radioactive pollutants have always been the top priority in wastewater, and searching a green and efficient treatment technology remains a significant challenge. In this study, a novel melamine sponge supported sulfurized nanoscale zero-valent iron (MS@S-NZVI) material with high dispersion was firstly designed to effectively capture U(VI) from water environment. The target material could retain its original structure in water due to the excellent mechanical strength of MS, which greatly inhibited the aggregation of S-NZVI. A series of characterization techniques, such as SEM, XRD, FTIR, TGA and XPS, had proved the effective synthesis and excellent structural properties of the MS@S-NZVI. The faster reaction equilibrium (<1 h) and higher maximum adsorption capacity (180 mg/g at pH = 5 and 298 K) exposed the perfect performance of target material in the elimination of U(VI). In addition, further researches in different water systems exhibited that MS@S-NZVI had a significant U(VI) removal rate in simulated wastewater systems. Finally, the removal process of MS@S-NZVI to U(VI) could be divided into three pathways through the XPS technique, adsorption and reduction were the main reaction mechanisms. This study provides a new insight into the utilization of melamine sponge and a prospect for the practical application of S-NZVI in the removal of radionuclide. [Display omitted] • Melamine sponge was used to support S-NZVI for the first time. • The structure of sponge enabled MS@S-NZVI to disperse fully in water. • The practical application potential of MS@S-NZVI was confirmed. • Adsorption and reduction were the main reaction mechanisms. [ABSTRACT FROM AUTHOR]

Highly porous zeolitic imidazolate frameworks (ZIFs), with disparate metal ions (ZIF-8 and ZIF-67), disparate organic ligands (ZIF-9 and ZIF-67), single or double central metal atoms (ZIF-8, Zn/Co-ZIF and ZIF-67) were prepared and used in the elimination of typical radionuclide U(VI). The detailed interaction mechanisms were studied by batch experiments, spectral analyses and DFT calculation. Langmuir isotherms model revealed a decreasing tendency to remove U(VI): ZIF-8 (540.4 mg/g) > Zn/Co-ZIF (527.5 mg/g) > ZIF-9 (448.6 mg/g) > ZIF-67 (368.2 mg/g). Based on the effects of pH and foreign ions, FTIR and XPS spectra analyses, the possible interaction mechanisms of U(VI) onto ZIFs were surface complexation and electrostatic interaction. Among them, ZIF-8 with Zn metal center and 2-methylimidazolate organic ligand had the best elimination capacity for U(VI) because of its large surface area, active metal ion and abundant nitrogen-containing groups (e.g., C–N, Zn–N and C N). Specially, the adsorption energy of ZIF-8-Zn2-UO 2 2+ structure was −2.299 eV obtained by DFT calculation, illustrating that U(VI) and N atoms were formed the most stable bidentate coordination compounds. This paper highlights the effects of the hydroxylated metals, the functional groups of the imidazole ring on the elimination of U(VI), which can provide constructive suggestions for further adsorbent materials amelioration. Image 1 • ZIF-8, ZIF-9, ZIF-67 and Zn/Co-ZIF were fabricated by stirring at room temperature. • Excellent structural performances endowed four ZIFs outstanding sorption capacity. • The differences in adsorption mechanism of four ZIFs were investigated in detail. • The N atoms of ZIF-8 formed bidentate coordination compounds with U(VI). [ABSTRACT FROM AUTHOR]