CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Hao Peng,Xiaoyu Li,Lina Lv,Tingting Deng,He Chen,Lu Wang,Qiang He,Caiping Dang,Lianggui Bao,Yihao You,Fangting Chi
Amidoxime-based polymers have been widely regarded as ideal adsorbents for uranium extraction from seawater. However, significant challenges remain in the efficient utilization of amidoxime groups on the polymers which is closely related to the conformation of molecular chains in complex marine environments. Herein, by integrating multi-scale computational simulation with chain conformation regulation, three representative auxiliary group were designedly introduced to polyamidoxime (PAO) by grafting glycine, aminomethylsulfonic acid and aminomethylphosphonic acid. Firstly, the hydrophilicity of adsorbents was directly observed to increase significantly after modification by contact angle test and swelling test. Furthermore, the chain conformation was investigated by combined SAXS and MD simulation under real factors from seawater. Finally, uranium adsorption performance and mechanism were investigated by XPS and DFT calculation. The minimum contact angle reaches 26.9° and the maximum swelling rate is above 153.4 %. The conformation of the modified PAO was much more stretched than the raw one, with a radius of gyration up to 161.5 nm for PAO-AMP. The uranium adsorption capacity of PAO was only 165.5 mg/g, while that of the modified adsorbents PAO-AMP went up to 375.0 mg/g. The above results indicate that auxiliary groups played a role not only in optimizing the chain conformation of adsorbents but also in enhancing coordination capacity with uranium, which is beneficial for uranium extraction from seawater. This study offers a new point of view to assess adsorption phenomena of polymers, bridging chain conformations in different environment at the mesoscopic level with metal–ligand interactions at the molecular level.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shi-Cheng Liu,Ming-Bang Wu,Hao Ye,Lin Liu,Lu-Lin Ma,Juming Yao
Highly efficient extraction of uranium from seawater is regarded as an important guarantee for the promotion of nuclear electricity generation. Amidoxime based adsorbents are considered as the most promising materials for uranium recovery due to their high selectivity and binding capability to uranyl ions. Herein, natural celluloses with advantages of low cost, biodegradability , renewability were chosen as the raw materials. Moreover, amidoximated cellulose-based adsorbents are fabricated by two steps of homogeneous reactions including the Michael addition and amidoximation reaction. Compared with traditional surface grafting methods, both the grafting density of active adsorption sites and the utilization of raw materials could be greatly improved because of the lower steric hindrance as well as more exposed reactive sites during the homogeneous reactions. The adsorption capacity of our adsorbents can reach as high as 517.07 mg/g at pH = 7, one of the best cellulose-based adsorbents as far as we know. In addition, excellent hydrophilicity of the adsorbents, which is inherited from the natural cellulose, can endow them with enhanced mass transfer as well as resistance to marine pollutants. More importantly, the adsorption microspheres would be filled into filtration column for dynamic adsorption benefited from their aforementioned merits. The average adsorption capacity could maintain above 2.5 mg/g per day when the filtration column was exposed to simulated seawater for 24 days. All these characteristics make the amidoximated cellulose-based adsorbents potentially applicable to the uranium recovery from seawater.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Zhong Zhou,Qi Liu,Jiahui Zhu,Jingyuan Liu,Hongsen Zhang,Jing Yu,Rongrong Chen,Ying Li,Jun Wang
Amidoxime-based materials have made a great contribution to the selective adsorption process in the extraction of uranium from seawater. However, traditional adsorbents with amidoxime groups are limited by adsorption capacity and adsorption rate, which greatly hinder the development of uranium extraction from seawater. Based on this, we combined the amidoxime group with carbon nitride to synthesize the amidoxime group carbon nitride (NCN-AO), which is rich in nitrogen defects. Compared with ordinary carbon nitride (CN), NCN-AO has better selectivity and uranium reduction ability. In the process of extracting uranium from seawater, soluble hexavalent uranium (U(VI)) can be reduced to insoluble tetravalent uranium (U(IV)), to achieve high-efficiency extraction of uranium. The removal rate of uranium by NCN-AO in 100 mg/L uranium solution is 99 %, and NCN-AO has specific and selective adsorption of uranium. The band structure, density of states (DOS), highest occupied molecular orbital (HOMO), and lowest unoccupied molecular orbital (LUMO) of NCN-AO were calculated by Density Functional Theory (DFT) method, and adsorption reduction occurred on the surface and interface of NCN-AO. The above results show that NCN-AO may be a promising material for extracting uranium from seawater.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 333
·期 1
·71-84
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IF 1.6
Du Zhiyuan,Ni Yuran,Peng Hao,Tang Mei,Li Yuanli,Lv Lina,Li Xiaoyu,Chi Fangting
Novel chitosan crosslinked amidoxime polyacrylonitrile aerogel was synthesized and used for adsorption of uranium from seawater. The effects of initial uranium concentration, contact time, and pH value on uranium adsorption were investigated. The simulated uranium solution adsorption experiment shows that under the condition of an initial uranium concentration of 100 mg/L, the maximum adsorption capacity of CTS-g-PAO is 203.4 mg/g. The adsorption process can be well-fitted by Freundlich and Pseudo-second order models. In addition, CTS-g-PAO aerogel has good antibacterial activity against marine bacteria, with the antibacterial activity reaching 94.8%. The results demonstrated that CTS-g-PAO aerogel was an effective adsorbent for extracting uranium from seawater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
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IF 10.383
Hongxia Zhao,Chao Qi,Xuewu Yan,Jinyan Ji,Zhifang Chai,Shuao Wang,Tao Zheng
The material for managing and monitoring waste made from the waste itself is an excellent example of cyclic utilization, which could reduce issues and be more sustainable. A three-dimensional porous uranyl phosphonate MOF (UPF-105) was synthesized via a hydrothermal method. UPF-105 is stable in aqueous solution with pH in the range of 1–11 and maintains crystallinity below 215 °C. The uncoordinated phosphonate groups in the channels act as functional anchors to selectively capture uranyl ions, with a maximum uranium adsorption capacity of 170.23 mg g–1. The fluorescence of UPF-105 makes it a good candidate for a uranyl ion sensor in uranium-contaminated solutions with concentrations in the range of 5–90 ppm.
研究领域:
材料科学
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环境科学
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核化学
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分析化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Hao Li,Ningning He,Chong Cheng,Hao Dong,Jun Wen,Xiaolin Wang
Uranium extraction from seawater is a long-term process, in which biofouling caused by marine bacteria drastically decreases the properties of adsorbents. All reported antimicrobial uranium adsorbents are prepared with inorganic nanoparticles or single-molecule antibiotics, which possess poor antimicrobial, durability and adsorption performances. Herein, an antimicrobial polymer contained uranium adsorbent is prepared for the first time. The introduction of antimicrobial polymer endows the adsorbent with efficient and stable antimicrobial activity, as well as enhanced adsorption performance and good hydrophilicity attributed to plentiful amine groups. It possesses an inhibition rate up to 99.46% against marine bacteria at a high concentration (10 8 CFU mL −1 ), and a saturation uranium adsorption capacity of 684.3 mg g −1 (pH 8.0, 25 °C). Note that negligible degradation is observed in antimicrobial (>99%) and adsorption (>92%) tests after five cycles, indicating its great durability. Furthermore, as the first antimicrobial adsorbent used in marine tests, the kilogram-grade adsorbent performs excellent comprehensive property in 40-day marine tests. These results suggest that antimicrobial polymer contained adsorbent is a promising candidate for efficient uranium extraction from seawater.
研究领域:
材料科学
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环境科学
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海洋科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jiangnan Huang,Shuang Chen,Yingjie Ruan,Hao-Fan Wang,Hongjuan Wang,Hao Yu,Yonghai Cao
The efficient uptake of U(VI) ions from the real seawater as the nuclear energy source was of paramount importance. Here, the three-dimensional (3D) flexible carbon felts (FCFs) with N dopants and oxygen-containing groups (o-NFCF) were prepared via the solvothermal method. The obtained FCFs were used as the adsorbents for the uptake and enrich of U(VI) by a flow-through electro-sorption operation in the laboratory-designed device. The pristine FCF (pFCF) displayed a 5.0 mg/g capacity under the initial conditions of 10 mg/L U(VI), which was improved with the presence of an electric field (7.2 mg/g, 0.6 V). The o-NFCFs with 2.58 at.% N dopant and 11.09 at.% oxygen functionalities on the surface would lead to the enhanced performance (11.8 mg/g). This was facilitated by the aid of an electric field (18.8 mg/g, 0.6 V) with a Q max of 44.6 mg/g as well. The decreased activity was observed in the simulated seawater (16.4 mg/g) and real seawater (10.6 mg/g), respectively, probably ascribed to the coexistence of organisms and complex ions. The uptake stability of U(VI) from the real seawater was then observed, ascribed to the desorption capability of U(VI) from the surface of o-NFCF. In this process, o-NFCF could be in-situ regenerated simultaneously. By doing so, the enrichment of U(VI) to 5.85 mg/L concentration from a real seawater was obtained. Mechanistic studies and DFT simulations indicated that the electrochemical properties of 3D-NFCF materials dominated the electro adsorption of U(VI).
研究领域:
环境科学
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材料科学
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核化学
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电化学
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海洋资源利用
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jianzhang Gao,Jiaqi Chen,Huitao Lv,Shitao Liao,Yongde Yan,Yun Xue,Fuqiu Ma,Shuao Wang
Resource utilization of uranium from the nuclear wastewater is of significance, and the facile strategy to recover high purity uranium oxide directly from wastewater is urgent to develop. Herein, a three-step uranium oxide reduction recovery process (URRP), that is integrated solid–liquid separation (SLS) and electrochemical purification (EP) together with solid-phase uranium re-recovery (SUR), is designed and applied for uranium reduction and purification. The SEM and ICP results were used to determine the carbonate system as the optimal separation system and the Ti electrode as the optimal electrochemical purification electrode. The single electron transfer process of uranyl ions in carbonate was established using cyclic voltammetry. Such three-step recovery process achieves a high-efficient recovery of uranium with a purity of over 99.9% in complex wastewater systems, and an improved return rate of uranium as high as 98.6%. Furthermore, the concentration of metal ions in wastewater is reduced to the standard set by the World Health Organization. Such a URRP offers a very promising solution for the treatment of wastewater and the recovery of high purity uranium.
研究领域:
环境科学
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核能工程
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Ying Wang,Zaiwen Lin,Jiahui Zhu,Jingyuan Liu,Jing Yu,Qi Liu,Rongrong Chen,Ying Li,Jun Wang
Efficiently capturing of uranium (VI) [U(VI)] from seawater elicits unparalleled attraction for sustaining the uplifted requirement for nuclear fuel. However, obtaining the abundant U(VI) resource from seawater has always seriously restricted by competitive adsorption from higher concentrations of competitors, especially vanadium (V) [V(V)]. Herein, based on amidoximized natural bamboo strips with hierarchical porous structure, the molecular-level uranyl-specific “nano-holes” was co-constructed by the intramolecular hydrogen bonds for specifically trapping U(VI) from seawater. Manipulating the branched degrees of amino groups enabled the creation of a series of the molecular-level uranyl-specific “nano-holes” that exhibit ultrahigh affinity and selective adsorption of U(VI) with a adsorption capacity 1.8 fold higher compared to that of V(V) after 30 days floating in the Yellow Sea basin, conquering the long-term challenge of the competitive adsorption of V(V) for amidoxime-based adsorbents applied to extract U(VI) from seawater. The diameter of the molecular-level uranyl-specific “nano-holes” is approximately 12.07 Å, significantly larger than (UO 2 ) 3 (OH) 3 + (10.37 Å) and smaller than HV 10 O 28 5- , thereby exhibiting specifically trapping of U(VI) in a series of adsorption experiments with different U(VI)-V(V) ratios. Besides, the adsorption model based on the combination of experimental and theoretical results is accompanied by "hydrogen bond breaking and coordination bond formation".
研究领域:
环境科学
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材料科学
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核能技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Ying Wang,Zaiwen Lin,Jiahui Zhu,Jingyuan Liu,Jing Yu,Qi Liu,Rongrong Chen,Ying Li,Jun Wang
Amidoxime-based materials are currently the most promising adsorbents for sustainable extraction uranium from seawater. However, in practical applications, the strong affinity of amidoxime-based materials for vanadium seriously interferes with the extraction uranium from seawater. Herein, a novel environmentally friendly and degradable adsorbent is firstly designed through grafting animal protein on natural bamboo strips (BS). In detail, the casein hydrolysates (sodium caseinate, acid hydrolyzed casein and casein phosphopeptide) are grafted with amidoximated bamboo strips (SCAOBS, AHCAOBS and CPPAOBS) by chemical cross-linking and amide reactions to construct biaxial adsorption sites, including amidoxime and amino acid branched chains. The optimal adsorption pH of SCAOBS, AHCAOBS and CPPAOBS were 5, 7 and 7, the adsorption capacities were 186.3, 204.0 and 68.6 mg g −1 , and the attenuation was 23.1%, 17.7% and 20.2% after 5 cycles, respectively. Utilizing the weavability of BS, SCAOBS, AHCAOBS and CPPAOBS adsorbents are woven and floated in the Yellow Sea Basin, exhibiting that the adsorption capacity of uranium is 0.84, 1.21 and 0.81 mg g −1 , respectively, much higher than that of vanadium. Evenly, the adsorption capacity of AHCAOBS for uranium is about 15.3 times that of vanadium (0.077 mg g −1 ). Through DFT spatial structure optimization, there are indeed biaxial dual adsorption sites (–CO O H from amino acid and C = N - O H from amidoxime groups) between amino acids and amidoxime branched chains, and even the spatial structure of biaxial triple adsorption sites (–CO O H from amino acid, O = C-N from amide bond and C = N -OH from amidoxime groups) is more stable, thereby breaking this bottleneck from the vanadium interference for the amidoxime-based adsorption materials.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2022
·Vol. 331
·期 11
·4489-4502
·
IF 1.754
Wu Xuanchun,Zhang Yujing,Nie Xiaoqin,Ma Chunyan,Pan Ning,Dong Faqin,Li Xiaoan
A kind of amino-modified polyvinyl alcohol fibers were prepared to extract uranium from actual uranium-containing laundry wastewater. The Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy confirmed that amino groups were successfully attached to polyvinyl alcohol fibers' surface. The maximum adsorption capacity of uranium is 337.84 mg g −1 (pH 6.0). In the actual uranium-containing laundry wastewater system the modified fibers exhibited a high distribution coefficient for uranium (1.55 × 10 5 mL g −1 ). Given the aforesaid findings, It is an outstanding adsorbent for uranium elimination from actual uranium-containing laundry wastewater. Graphical abstract
研究领域:
环境科学
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材料科学
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核化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2024
·
IF 1.5
Li Qi,Wang Jiaqi,Hou Hairui,Wang Min,Yu Shujun,Xu Huan,Fu Dong,Wang Xiangxue
In this work, an amidoxime functionalized graphitic carbon nitride (g–C 3 N 4 –AO) was prepared by grafting amidoxime groups onto graphitic carbon nitride (g–C 3 N 4 ). The results of the kinetic and isotherm studies conducted on g–C 3 N 4 –AO indicate it exhibits rapid sorption kinetics by achieving equilibrium in 30 min with a homogeneous surface which performed a maximum sorption capacity of 67.1 mg g −1 . The zeta potential values of the g–C 3 N 4 –AO are between 35 to − 44.3 mV in the pH range of 2.0–11.0. It was further observed that it complexes with uranium ions, which act as bidentate ligands, utilizing the lone pairs on O and N atoms. The empirical evidence strongly suggests that the utilization of g–C 3 N 4 –AO in uranium water remediation can be a promising solution. Graphical abstract
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）