CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yong Zhang,Xuan Liu,Yujia Liu,Jiaqi Feng,Kexing Jiang
Lamellar membranes made from 2D materials have garnered significant attention as advanced separation materials for wastewater treatment, particularly for wastewater containing uranium (U(VI)). Nevertheless, it is still a great challenge to obtain assembled lamellar membranes with both high flux and retention rate from 2D materials. In this work, a method of in-situ loading hydroxyapatite nanoparticles onto MXene nanosheets and vacuum filtration to form a novel Ti 3 C 2 T x MXene/hydroxyapatite (MXene/HAP, MXHP) membrane had been developed for separating U(VI) from wastewater. From the characterization results, the MXHP membrane displayed an increasing trend of interfacial pores and interlayer channels for comparison to the pure MXene membrane, which could notably improve water permeability of MXHP membrane. Based on membrane separation experiments, the MXHP-2 membrane achieved a flux of 515.5 L/(m 2 ·h·bar) and a U(VI) retention rate of 98.2 % in the treatment of U(VI)-containing wastewater. Additionally, the MXHP-2 membrane exhibited strong recyclability with a high U(VI) retention rate of 85.3 % after five cycles. The U(VI) separation mechanism of MXHP-2 was photocatalytic reduction assisted dissolution-deposition. The above results could provide valuable insights for developing new composite membranes with high throughput and high uranium retention rate.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Junhan Luo,Qi Qing,Shuang Liu,Bo Liang,Jingyu Wang,Zhe Wang,Jing Chen,Yuexiang Lu
The efficient extraction and recovery of uranium from spent fuel is crucial for the sustainable development of nuclear energy. Pyrochemical reprocessing based on chloride molten salt electrolysis shows promise in addressing this challenge but still has several key issues remain unresolved. The non-contact microplasma gas electrode may be an ideal anode in this system, which can solve the problem of anode corrosion. Herein, we propose combining microplasma anodes with molten salt electrochemistry to explore the feasibility of separating U 4+ and UO 2 2+ from chloride molten salts and to investigate the effects of electrochemical parameters on the separation of U 4+ and UO 2 2+ . Experimental results demonstrate that microplasma anodes exhibit excellent performance in separating U 4+ and UO 2 2+ from molten salts to form Al-U intermetallic and UO 2 solids, respectively. The composition of the products and the deposition rate of the uranium were significantly influenced by electrolysis temperature and current, whereas the initial concentration of reactants had a minimal overall impact on the experiments. Under conditions of prolonged electrolysis, the microplasma anode achieves high separation efficiencies for both U 4+ and UO 2 2+ (>96 %).
研究领域:
核能工程
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 45
·39150-39158
·
IF 3.289
Chiyao Bai,Meicheng Zhang,Bo Li,Xiaosheng Zhao,Shuang Zhang,Lei Wang,Yang Li,Ji Zhang,Lijian Ma,Shoujian Li
Recently, research into functional materials with various desired properties has been ceaselessly promoted. However, the development of convenient and practical strategies for building flexible material platforms to realize multi-functionalization and to prepare various functional derivatives is still a challenge. Herein, we propose for the first time a new strategy that introduces conjugated carbon–carbon triple bonds into the skeleton of covalent organic frameworks (COFs) that can act as both building blocks and active sites to create a versatile platform. Based on the platform, in situ multipurpose functionalization according to diverse real needs can be achieved more easily and efficiently with different addition reactions, compared with current approaches used for the preparation of functional materials. In this paper, a novel COF material (TCD), which contains diynes acting as a skeleton of the material platform, was directly prepared under microwave irradiation. Then, three new functional materials with a cyano group (TCD-CN), an amidoxime group (TCD-AO) and a hydroxyl group (TCD-OH) were obtained by further functionalization of the CC bonds in TCD. The capabilities of the prepared materials for the selective separation of uranium from a simulated nuclear industrial effluent were examined, and TCD-AO was found to exhibit the highest separation efficiency.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Wen He,Zhenglemei Qiu,Qunying Sun,Zhouzhou Li,Zhuting Chen,Lijun Hu,Hongqing Wang
Constructing desirable morphology has been demonstrated to be an effective strategy for enhancing the capabilities of the covalent organic frameworks (COFs) for the processing of uranium. Traditional 3D-COFs only possess a limited number of structural nodes, not being the ideal structure for uranium adsorption, but 2D-COFs with rich structural nodes also suffer from reduced exposure of adsorption sites due to stacking during uranium treatment, which is not beneficial for achieving sustained and efficient adsorption. To this end, by polymerizing COFs on the silica carrier, followed by etching the silica carrier, and utilizing the conversion of nitrile to amidoxime groups as chelation sites, we designed and synthesized a hollow 3D-like structure of 2D-COFs (COF-TD-H-AO, similar to three-dimensional COFs) as adsorbents to capture the radionuclide uranium. Systematic studies were carried out for the adsorption characteristics of this material at different pH values and in the presence of interfering ions, as well as its adsorption thermodynamics and kinetics. Compared with COF-TD-AO (pure 2D-COFs) and SiO 2 @COF-TD-AO (unetched), COF-TD-H-AO exhibited a higher adsorption capacity as well as selective adsorption of uranium. This work provides an innovative perspective on material design and preparation by providing more adsorption sites in an effort to improve the capacity of adsorption and the selectivity of adsorption.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Ying Wang,Bowen Hu,Qing Li,Yijie Wu,Xintong Shang,Pinghua Yang,Yimin Cai,Lihua Yuan,Wen Feng
A challenge in nuclear waste remediation is the construction of extraction systems with exceptional stability and remarkable selectivity under harsh conditions, to achieve efficient uranium separation from nuclear wastewater. In this work, two novel N, O-hybrid extractants, L1 and L2 attaching two or one pyrrolidone groups to the phenanthroline skeleton were synthesized and applied in uranium extraction. Solvent extraction tests showed that these ligands in 3-nitrobenzotrifluoride can extract uranium with fast kinetics, high selectivity over twelve competing ions, and facile stripping. Slope analysis indicated that each uranyl ion binds to one ligand during extraction, and the extraction conforms to the cation exchange mechanism. The effect of temperature on uranium extraction was also carried out to determine the thermodynamic parameters. Notably, outstanding radiation stability was demonstrated for these extractants even after being exposed to 500 kGy γ ray irradiation. In addition, NMR titration and DFT calculations were performed to understand the complexation behaviors between ligands and uranyl ions. This study reveals the potential of these two phenanthroline-based extractants for the use in uranium separation from nuclear wastewater.
研究领域:
核化学与化工
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环境科学
·
计算化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2014
·
IF 3.552
Juan Li,Xiaodan Yang,Chiyao Bai,Yin Tian,Bo Li,Shuang Zhang,Xiaoyu Yang,Songdong Ding,Chuanqin Xia,Xinyu Tan,Lijian Ma,Shoujian Li
A novel COF-based material (COF-COOH) containing large amounts of carboxylic groups was prepared for the first time by using a simple and effective one-step synthetic method, in which the cheap and commercially available raw materials, trimesoyl chloride and p -phenylenediamine, were used. The as-synthesized COF-COOH was modified with previously synthesized 2-(2,4-dihydroxyphenyl)-benzimidazole (HBI) by “grafting to” method, and a new solid-phase extractant (COF-HBI) with highly efficient sorption performance for uranium(VI) was consequently obtained. A series of characterizations demonstrated that COF-COOH and COF-HBI exhibited great thermostabilities and irradiation stabilities. Sorption behavior of the COF-based materials toward U(VI) was compared in simulated nuclear industrial effluent containing UO 2 2+ and 11 undesired ions, and the UO 2 2+ sorption amount of COF-HBI was 81 mg g −1 , accounting for approximately 58% of the total sorption amount, which was much higher than the sorption selectivity of COF-COOH to UO 2 2+ (39%). Batch sorption experiment results indicated that the uranium(VI) sorption on COF-HBI was a pH dependent, rapid (sorption equilibrium was reached in 30 min), endothermic and spontaneous process. In the most favorable conditions, the equilibrium sorption capacity of the adsorbent for uranium could reach 211 mg g −1 .
研究领域:
化学
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环境科学
·
核能技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Yang Li,Lei Wang,Bo Li,Meicheng Zhang,Rui Wen,Xinghua Guo,Xing Li,Ji Zhang,Shoujian Li,Lijian Ma
A new strategy combining a pore-free matrix and cooperative chelating was proposed in the present paper in order to effectively avoid undesired nonselective physical adsorption and intraparticle diffusion caused by pores and voids in porous sorbents, and to greatly enhance uranium-chelating capability based on hyperbranched amidoxime ligands on the surface of nanodiamond particles. Thus, a pore-free, amidoxime-terminated hyperbranched nanodiamond (ND-AO) was designed and synthesized. The experimental results demonstrate that the strategy endows the as-synthesized ND-AO with the following expected features: (1) distinctively high uranium selectivity (SU = qe-U/qe-tol × 100%) from over 80% to nearly 100% over the whole weak acidity range (pH < 4.5); especially, the SU can reach up to unprecedented >91% at pH 4.5, more than 20% of selectivity increment over any analogous sorbent materials reported so far, with a uranium sorption capacity of 121 mg/g in simulated nuclear industry effluent samples containing 12 coexistent nuclide ions; (2) superfast equilibrium sorption time of <30 s; and (3) one of the highest distribution coefficients (Kd) of ∼3 × 106 mL/g for U(VI) as well as a fairly high sorption capacity of 212 mg/g at pH 4.5 in pure uranium solution. The strategy could also provide an optional approach for the design and fabrication of other new high-performance sorbing materials with prospective applications in selective separation of other interested metal ions.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Yanyi Liu,Wenhuan Yuan,Wenli Lin,Shan Yu,Lei Zhou,Qingyi Zeng,Jin Wang,Luoheng Tao,Qunwei Dai,Juan Liu
Even though uranium (U) is considered to be an essential strategic resource with vital significance to nuclear power development and climate change mitigation , U exposure to human and ecological environment has received growing concerns due to its both highly chemically toxic and radioactively hazardous property. In this study, a composite (M-BC) based on Ficus macrocarpa (banyan tree) aerial roots biochar (BC) modified by δ-MnO 2 was designed to separate U(VI) from synthetic wastewater. The results showed that the separation capacity of M-BC was 61.53 mg/g under the solid – liquid ratio of 1 g/L, which was significantly higher than that of BC (12.39 mg/g). The separation behavior of U(VI) both by BC and M-BC fitted well with Freundlich isothermal models, indicating multilayer adsorption occurring on heterogeneous surfaces. The reaction process was consistent with the pseudo-second-order kinetic model and the main rate-limiting step was particle diffusion process. It is worthy to note that the removal of U(VI) by M-BC was maintained at 94.56% even after five cycles, indicating excellent reusability and promising application potential. Multiple characterization techniques ( e.g. Scanning Electron Microscope-Energy Dispersive Spectrometer (SEM-EDS), Fourier Transform Infrared Spectroscopy (FTIR), X-ray Diffraction (XRD), Brunauer-Emmett-Teller (BET) and X-ray Photoelectron Spectroscopy (XPS)) uncovered that U(VI) complexation with oxygen-containing functional groups ( e.g. O–C O and Mn–O) and cation exchange with protonated ≡MnOH were the dominant mechanisms for U(VI) removal. Application in real uranium wastewater treatment showed that 96% removal of U was achieved by M-BC and more than 92% of co-existing (potentially) toxic metals such as Tl, Co, Pb, Cu and Zn were simultaneously removed. The work verified a feasible candidate of banyan tree aerial roots biowaste based δ-MnO 2 -modified porous BC composites for efficient separation of U(VI) from uranium wastewater, which are beneficial to help address the dilemma between sustainability of nuclear power and subsequent hazard elimination.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 47
·23788-23798
·
IF 7.443
Bo Li,Chiyao Bai,Shuang Zhang,Xiaosheng Zhao,Yang Li,Lei Wang,Kuan Ding,Xi Shu,Shoujian Li,Lijian Ma
On the basis of the unusual coordination structure of UO22+ combined with the adaptive nature of supramolecular organic frameworks (SOFs), here we have designed and prepared a novel SOF-based solid phase extraction adsorbent (MA–TMA) using N-donor-containing melamine (MA) and O-donor-containing trimesic acid (TMA) as bifunctional building blocks mutually linked via hydrogen bonds. The as-prepared MA–TMA, with a rich N-/N- and N-/O-heterocyclic structure throughout its framework, provides an accessible coordination geometry and/or ligand environment for the uranyl ion, which builds the crucial structural basis for the pre-organized adaptive frameworks closely related to the “induced-fit” and selective recognition of uranyl ions. The main results are as follows: (1) the highest selectivity of 92%, so far unreported, and a considerable capacity of 324 mg g−1 for uranium adsorption by MA–TMA are observed in weak acidic multi-cation solution (pH 2.5), accompanied by a distribution coefficient Kd value of 16 000 mL g−1, 100-fold or more over other 11 competitive cations; (2) MA–TMA could reach its limiting saturation capacity of 1028 mg g−1 at pH 4.5 in pure-U(VI) solution; (3) noteworthily, the morphology of MA–TMA changed from a ribbon-like structure with a nano-diameter before adsorption into aggregated granules with a size of tens of microns after adsorption, which would be much more favorable for subsequent solid–liquid separation. Furthermore, possible mechanisms for the selective recognition of uranyl ions and the morphological changes of MA–TMA after adsorption are explored based on experimental characterization and chemical rationale.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Tianqi Liu,Zhan Li,Xin Zhang,Hongxin Tan,Ziying Chen,Jinsheng Wu,Jia Chen,Hongdeng Qiu
Design and construction of a membrane that can achieve selective separation of uranium from spent fuel or seawater is a big challenge in the field of separation science. In this work, 1,3,5-benzenetricarboxylic acid (BTC) and three different nitrates (Zn/Ni/Cu) were used to prepare metal–organic frameworks (BTC–MOFs) with different pore sizes, and then, BTC–MOFs were intercalated into the interlayers of graphene oxide (GO) for preparing the composite membranes which presented selective separation of uranium with strong acid resistance. Composite membranes prepared by Zn/Ni/Cu-BTC–MOFs and GO can achieve the separation between ions of different valence states, and their permeability and selectivity depend on the membrane thickness, the acidity of driving solution, and the pore sizes of MOFs. Importantly, Cu-BTC–MOF-intercalated GO membranes can not only achieve the selective separation of Th4+ and UO22+ with a selectivity of ≈6 but also induce the ultra-high selectively separation of UO22+ and Ce3+ because the rejection rate of Ce3+ is about 100%. Moreover, the Zn-BTC–MOF-intercalated GO membrane shows an excellent selectivity of Th4+ and UO22+ with a selectivity of ≈25, and it may also achieve selective separation of uranium from seawater.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Zifan Li,Zhibin Zhang,Xiang Zhu,Cheng Meng,Zhimin Dong,Songtao Xiao,Yingcai Wang,Youqun Wang,Xiaohong Cao,Yunhai Liu
Photocatalytic uranium extraction from nuclear effluent is a promising approach for avoiding environmental damage and recovering uranium resources. Here, a hollow tube-like D-A organic semiconductor photocatalyst consisting of triazine (Acceptor) and carbon ring (Donnor) was synthesized via two cheap monomers , sodium alginate and melamine . The incorporation of carbon ring structure could endow g-C 3 N 4 with unique hollow hexagonal tube-like morphology, modulate the electronic excitation model, lower the energy for exciton dissociation, and promote the adsorption and activation of O 2 . Thus, the D-A photocatalyst established high efficiency of photocatalytic uranium separation under LED light and high concentration of anions and cations interference. More importantly, we propose a novel theory, that photocatalytic-induced-uranyl-coordination-reaction (PIUCR), and highlight that the formation rate and pathway of crystal nucleus is the most crucial step for the surface reaction of photocatalytic uranium separation. This study provides insights and guidelines for the in-depth understanding of the photocatalytic separation of uranium.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
Advanced Science
·
2021
·Vol. 8
·期 7
·2002717
·
IF 16.806
Tong Wu,Zhe Wang,Yuexiang Lu,Shuang Liu,Hongpeng Li,Gang Ye,Jing Chen
Graphene oxide (GO) membranes with unique nanolayer structure have demonstrated excellent separation capability based on their size-selective effect, but there are few reports on achieving ion–ion separation, because it is difficult to inhibit the swelling effect of GO nano sheets as well as to precisely control the interlayer spacing d to a specific value between the sizes of different metal ions. Here, selective separation of uranium from acidic radioactive waste containing multication is achieved through a precise dual-adjustment strategy on d . It is found that GO swelling is greatly restricted in highly acidic solution due to protonation effect. Then the interlayer spacing is further precisely reduced to below the diameter of uranyl ion by increasing the oxidation degree of GO. Sieving uranyl ions from other nuclide ions is successfully realized in pH =3–3 mol L −1 nitric acid solutions.
研究领域:
材料科学
·
环境科学
·
核化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）