SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yuhui Liu,Yonggao Chen,Xiangzhu Liu,Sitong Chen,Tao Bo,Chao Chen,Yingcai Wang,Hao Jiang,Xiaoyan Li,Shuang Zhang
The reduction and removal of uranyl ions (UO 2 2+ ) using highly active zero–valent iron (Fe⁰) are crucial for efficient uranium capture in environmental and nuclear waste management. However, the reported utilization efficiency of Fe⁰ for uranyl reduction remains limited due to surface passivation and inadequate electron transfer. Herein, we demonstrate an advanced approach by introducing boric acid to reconstruct the surface charge on oxygen–rich Fe⁰, effectively repelling oxygen adsorption and enhancing uranium capture efficiency. Combining theoretical calculations with modern characterization techniques, the interaction process between UO 2 2+ and surface boric acid–modified Fe⁰ was studied. Surface modification with boric acid can alter the isoelectric point of Fe⁰, increasing the adsorption of U(VI). Additionally, the empty p orbitals of boron can promote delocalization of electron clouds around shell iron atoms and oxygen atoms, thereby facilitating the outward transfer of electrons from the iron core within Fe⁰ and enhancing the reduction of U(VI). Furthermore, the surface boric acidification of Fe⁰ can enhance the removal of U(VI) through improved adsorption and reduction pathways. Density functional theory calculations revealed that the interfacial electron transfer pathway provided by surface boric acid enhances the reduction capability and inhibits the adsorption of oxygen molecules. This effect reduces the ineffective consumption of Fe⁰ electrons and increases the proportion of U(IV) in the products. This charge redistribution effectively prevents surface passivation while promoting stronger interaction with uranyl ions.
研究领域:
环境科学
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材料科学
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核废料管理
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Zhiwei Zhao,Renchan Lei,Yizhe Zhang,Tingting Cai,Bing Han
Highly effective extraction of uranium from seawater calls for the development of adsorbents with both high capacity and selectivity. Defective Zr-based metal–organic frameworks (MOFs) are potential candidates for uranium sequestration due to their high surface area and tunable active sites. In this work, MOF-808 samples with adjustable missing linker defects were successfully prepared by manipulating the concentration of the carboxylic acid modulator. Impressively, MOF-808 with the highest defect density, namely M808-4, showed excellent selectivity towards uranium in comparison with coexisting competitive ions in seawater. Moreover, M808-4 exhibited remarkable uranium extraction performance in real seawater with an uptake capacity of 5.83 mg/g in 28 d, which is 10.41 times higher than that for vanadium. The results indicated that the abundant Zr unsaturated active sites formed by defect inducing strategy are the key to the efficient capture of uranyl ions. This study highlighted the advantages of defect engineering in MOF based materials for highly selective uranium extraction from seawater.
研究领域:
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Shiqi Lyu,Zurina Zainal Abidin,Thomas Choong Shean Yaw,Mohamad Faiz Mukhtar Gunam Resul
Since solar assisted sorption strategy presented a promising prospect in the capture of aquatic pollutants, the design of an environmental-friendly and low-cost photothermal conversion sorbent would be highly sustainable. Herein, hydrophilic porous oxygen-modified polysulfide/multi-walled carbon nanotubes were prepared via the inverse vulcanization by integrating palm oil, sulfur, sodium chloride, sodium citrate and carbon nanotubes. By adjusting the filling content of carbon nanotubes, the evolution of microstructure, porosity, contact angle, photothermal effect, and mechanical property were systematically studied. Sorption behaviors of U(VI) under various hydrochemical conditions including contact time, solution pH, and initial U(VI) concentration were studied under simulated sunlight illumination and dark respectively. An enhancement of 28.6 %–90.2 % for maximum sorption capacity (208.7–335.1 mg/g) was achieved under sunlight comparing with that in dark. Beside a favorable recycling use, the practical sorption of U(VI) from natural seawater was evaluated. Moreover, hydrophobic polysulfide/multi-walled carbon nanotubes prepared without adding sodium citrate were applied to adsorb toluene and phenol under sunlight and dark. Sorption capacity improvements of 8.8 %–28.3 % for toluene and 9.6 %–28.5 % for phenol were presented under sunlight. This study provided new insights for the cost-effective and scalable capture of radionuclides and organic pollutant using solar-assisted polysulfide sorbents.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Xinyue Zhao,Dingyang Chen,Minsi Shi,Rui Zhao
Capacitive deionization (CDI) technology holds great potential for rapid and efficient uranyl ion removal from wastewater. However, the related electrode materials still have much room for research. Herein, chitosan/phytic acid complexes were anchored on polypyrrole nanotubes (CS/PA-PPy) to fabricate the electrode for the electrosorption of uranyl ions (UO 2 2+ ). In this system, polypyrrole nanotubes provided specific channels for ion and electron diffusion, and chitosan/phytic acid complexes offered selective sites for UO 2 2+ binding. The results demonstrated that CS/PA-PPy via electrosorption showed faster kinetics and higher uranium uptake than those via physicochemical adsorption. The maximum adsorption capacity toward UO 2 2+ via electrosorption (1.2 V) could reach 799.3 mg g −1 , which was higher than most of the reported CDI electrodes. Electrochemical measurements and experimental characterizations showed that the electrosorption of UO 2 2+ by CS/PA-PPy was a synergistic effect of capacitive process and physicochemical adsorption, in which the capacitive mechanism involved the formation of an electric double layer from hollow polypyrrole nanotubes, whereas the coordination of phosphate, amino and hydroxyl groups with UO 2 2+ was attributed to physicochemical adsorption. With the rational design of material, along with its excellent uranium removal performance, this work exhibited a novel and potential composite electrode for uranium capture via CDI from wastewater.
研究领域:
环境科学
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材料科学
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纳米技术
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水处理
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Shipeng Chen,Qiang Luo,Wei Wang,Linqian Li,Yilan Li,Ning Wang
Materials capable of capturing environmentally mobile uranium from various sources, including nuclear waste and bio-aggressive seawater, are critical for energy and environmental sustainability. Unfortunately, the stability and reusability of existing absorbents is limited in seawater due to the ubiquitous and notorious biofouling, and therefore, developing high-performance materials with antibiofouling activity is of great importance for uranium capture. Here we report a tungstate exchanged layered double hydroxide composite (MgAl-LDH-NO 3 - -WO 4 2- ) that exhibits a significant uranium removal efficiency of 98.8 % in 240 ppm uranium-containing wastewater and a maximum uptake capacity of 409.6 mg g −1 . More importantly, MgAl-LDH-NO 3 - -WO 4 2- displays an excellent antibiofouling ability in bio-aggressive seawater by mimicking natural haloperoxidase in marine algae, enabling the excellent cyclic stability for uranium capture from seawater. This work provides an effective strategy to develop highly efficient LDH-based materials for uranium capture.
研究领域:
环境科学
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材料科学
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核工程
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Shuya Liu,Xinjie Ma,Yuxin Liu,Weiwei Chen,Yuejie Ai,Kexin Li,Xiushen Ye,Ming Fang,Xiaoli Tan
To fully utilize the customizable characteristics of metal-organic framework (MOF) materials in environmental applications, it is important to precisely modulate the branching groups of MOFs for improved performance. In this work, MIL-53(Al) was modulated by different numbers of nitrogen atoms and carboxyl groups/phosphite groups (MOF-N 2 -(COOH) 3 , MOF-N 3 -(COOH) 4 , and MOF-N 2 -(PO(OH) 2 ) 3 ) via a post-synthesis modification method, and the influence of functional groups and chain length on adsorption and the mechanism of modified groups on the adsorption of uranium (U) are demonstrated. Batch experiments suggest the removal of U(VI) reaches 37%, 27%, and 90% for MOF-N 2 -(COOH) 3 , MOF-N 3 -(COOH) 4 and MOF-N 2 -(PO(OH) 2 ) 3 , respectively (pH = 4.0, T = 25 ℃, I = 0.01 M NaNO 3 ). The surface complexation between UO 2 2+ and the surface of functional groups on the modulated MOF dominates the adsorption. Nevertheless, the steric hindrance in MOF porous structure can explain the inferiority of U(VI) adsorption on MOF-N 3 -(COOH) 4 (27%) to MOF-N 2 -(COOH) 3 (37%). MOF-N 2 -(PO(OH) 2 ) 3 is more conducive to uranyl adsorption than MOF-N 2 -(COOH) 3 or MOF-N 3 -(COOH) 4 , which is due to better affinity of U(VI) to phosphate group than the carboxyl group by density functional theory (DFT) calculation. Moreover, the excellent regeneration performance and U(VI) adsorption of MOF-N 2 -(PO(OH) 2 ) 3 in natural water or wastewater further confirmed the practical application of modulated MOFs in practical application.
研究领域:
环境科学
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材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Xiaopeng Lv,Jingwen Xiong,Yanqiu Hao,Weixing Chen,Peng Yang,Qingmin Yang,Facui Yang
Biomimetic strategy-derived protein-based materials for uranium adsorption exhibit outstanding selectivity, but corresponding high cost and complicated preparation limits their scale-up application. This study utilizes in situ mineralization to incorporate nano-hydroxyapatite (HAP) into soy protein isolate (SPI) coating, thereby achieving a low-cost and facile strategy to leverage the selective uranium adsorption properties mediated by phosphate groups in HAP. The network structure of SPI facilitates the uniform dispersion of HAP, while the rigid HAP nanoparticles enhance the mechanical properties of the protein film. This synergistic design enables a dual-mechanism adsorption process: HAP first electrostatically preconcentrates U(VI) ions near the interface, followed by strong multidentate coordination with carboxyl and amino groups from SPI. The integrated adsorption mechanism significantly improves uranium capture efficiency while maintaining the cost-effectiveness and process simplicity. Based on this design, the SPI/HAP hybrid coating effectively remove uranium across a pH range of 3.5–9.0, achieving a rejection ratio over 99.1 % and a maximum adsorption capacity of 587.1 mg/g. Moreover, the hybrid material achieved a uranium rejection ratio exceeding 90 % in both simulated salt lake and seawater, while demonstrating exceptional selectivity for uranium over vanadium. Its precision in uranium/vanadium discrimination and interception uranium sequester performance significantly surpass conventional membranes and adsorbents. Furthermore, the SPI/HAP coating is easily regenerated and retained 94.1 % reusability after five cycles. The superior rejection ratio, low cost, environmentally benign nature, and facile preparation of the material, highlight SPI/HAP to be a promising biomass-based material for practical uranium capture in scale-up application.
研究领域:
环境科学
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材料科学
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核工程
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生物技术
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化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Zhen Li,Zhiqun Yu,Yundi Wu,Xilong Wu,Yi Wan,Yihui Yuan,Ning Wang
Nowadays, marine bacteria are abundant in marine ecosystems and considered to be one of the main causes of biofouling. Microbial films formed on adsorbent surfaces play a vital role in marine biofouling and lead to a decrease in uranium extraction. Therefore, developing efficient antibacterial and antibiofilm sorbents for uranium enrichment is an urgent demand. In this work, a novel composite nanofibrous adsorbent, comprising of amidoximated polyacrylonitrile (AOP) and poly(ethylene glycol) methyl ether- b -poly( l -arginine) (PPLA), was prepared via solution blow spinning for potential uranium seawater recovery. The effect of initial pH, adsorbent composition, sorbent dose and contact time on the sorption of uranyl ions and antibacterial assay were investigated. The introduced polycationic diblock PPLA with guanidines not only showed improved shrinkage deformations from negatively charged AOP fibers and excellent antibacterial and antibiofilm activities, but also enhanced the adsorption capacity of the adsorbents, even after eight cycles of adsorption–desorption in uranium-spiked seawater. The adsorption equilibrium could be achieved with a capacity of 10.31 mg/g within 35 d in unfiltered natural seawater. These findings suggest that the blown-spun AOP@PPLA composite nanofibers may be conducive to the evolution of new antifouling adsorbents for uranium separation from seawater.
研究领域:
材料科学
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环境科学
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纳米技术
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 14
·7920-7927
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IF 14.511
Weihua Zhang,Xiao Han,Jun You,Xiaofang Zhang,Danfeng Pei,Stefan Willför,Mingjie Li,Chunlin Xu,Chaoxu Li
The efficient extraction of the aquatic uranium element has drawn growing research interest because of its importance for both nuclear energy acquirement and water environmental remediation. Large-capacity, rapid filtration adsorption is promising, but remains challenging in capturing aquatic uranium ions. Herein, cyanoethyl substitution was found to enable the rapid exfoliation of cyanoethyl cellulose nanofibrils by mild shear (e.g., manual shake and homogenization) within 30 min with a conversion of up to ∼90% and unique re-dispersibility in many organic solvents. After hydrolyzing cyanoethyl into amidoxime, the resultant amidoximated cellulose nanofibrils, serving as a novel type of green absorbent, exhibited rapid kinetics (<5 min) and large reversible capacity (1327 mg g−1) in aquatic uranium adsorption. Their rigid fibrous feature and super dispersibility facilitated the construction of fibrous porous films to capture uranium ions in high capacity in continuous filtration flow. Therefore, this cyanoethyl exfoliation may not only provide an unprecedented route for the rapid and energy-efficient production of cellulose fibrils, but also promises a green and sustainable alternative for the high-efficiency extraction of aquatic uranium element.
研究领域:
材料科学
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环境工程
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核工程
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化学工程
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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）