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MARINE POLLUTION BULLETIN · 2021 · IF 5.553

Microplastics aged in various environmental media exhibited strong sorption to heavy metals in seawater

Liu Gao,Dongdong Fu,Jinjin Zhao,Wanshan Wu,Zezheng Wang,Yuanyuan Su,Licheng Peng

To date, the degradation of microplastics (MPs; <5 mm) in different environments, particularly their adsorption characteristics for coexisted metal pollutants remains to be elucidated. Thus, this study investigated the effects of aging MPs, including polyamide (mPA), polyethylene terephthalate (mPET), polystyrene (mPS), and polyvinyl chloride (mPVC) for 3 months under UVA irradiation in four environmental media (air, seawater, sand, and soil) and adsorption of heavy metals (Cu, Cd) onto seawater-aged mPS and mPVC. The results showed that surface morphological changes, including cracks, oxidized particles, and wrinkles, appeared on aged MPs. The heavy metal adsorption capacity decreased in the order aged mPVC > aged mPS > unaged mPS > unaged mPVC, and the Cu 2+ and Cd 2+ ions competed for active adsorption sites on the MPs surfaces. Overall, the aging environment affected the physical and chemical properties of MPs and the aging of MPs enhanced their adsorption of coexisting metals tested.

研究领域: 环境科学 · 化学
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JOURNAL OF MOLECULAR LIQUIDS · 2022 · IF 6.633

Amidoxime-modified hypercrosslinked porous poly(styrene-co-acrylonitrile) adsorbent with tunable porous structure for extracting uranium efficiently from seawater

Lien Zhu,Chunhong Zhang,Feifan Qin,Fuqiu Ma,Changlong Bi,Ruiqi Zhu,Lijia Liu,Jianwei Bai,Hongxing Dong,Toshifumi Satoh

To efficiently and economically extract uranium from seawater, novel amidoxime-modified hypercrosslinked poly(styrene-co-acrylonitrile) (SAN) adsorbents with tunable porous structure were synthesized via simple Friedel-Crafts reaction followed by amidoximation. The adsorbent HCPSAN-B-AO obtained by using biphenyl dichlorobenzyl (BCMBP) as an additional crosslinking agent, possessed a larger pore size and higher surface area due to the longer and more rigid molecular structure of BCMBP compared to the original crosslinking agent 1,2-dichloroethane (DCE), resulting in the higher uranium adsorption capacity of HCPSAN-B-AO. Investigations on the adsorption performance in real seawater containing a large amount of interfering ions showed that the adsorbent owned excellent selectivity for uranyl ions, and the removal percentage of uranium could reach 84.4%. Furthermore, the adsorbent maintained good adsorption performance even after 5 adsorption–desorption cycles, indicating a good recyclability. Investigations on adsorption kinetics, thermodynamics, adsorption isotherms and adsorption mechanism manifested that the adsorption was a rapid (adsorption equilibrium within 30 min), spontaneous and chemical adsorption process (maximum adsorption capacity was 228 mg g −1 ), and the mechanism was mainly the interaction between uranyl ions and amidoxime groups. In summary, the as-prepared adsorbent was a feasible adsorbent for uranium extraction from seawater.

研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Fabrication of novel pectin-based adsorbents for extraction of uranium from simulated seawater: Synthesis, performance and mechanistic insight

Haiyan Luo,Haoyu Yao,Min Li,Fanfang Meng,Hui Zhao,Changjiang Yu,Xiangfeng Liang,Huizhou Liu

Efficient extraction of uranium from seawater is of great significance to the stable development of nuclear energy. The graft modification of pectin is expected to realize the efficient extraction of uranium through the dual action of aminoxime and carboxyl groups. In this work, novel biomimetic pectin adsorbents were developed and their performance on the adsorption performance of uranium from seawater was investigated. The physical structure and morphology were characterized by employing FT-IR, BET, SEM and elemental analysis. The skeleton structure and surface functional groups of the pectin-derived adsorbents, which were modified to improve the adsorption selectivity, favored the adsorption of uranium in simulated seawater. The modified apple pectin (MPA) adsorbents exhibited the highest adsorption capacity of 212.27 mg/g at optimal conditions. The thermodynamic results showed that the adsorption of uranium on MPA surface followed the Langmuir single-layer model, and the theoretical maximum adsorption capacity could reach up to 296.25 mg/g. The adsorption process conformed to the pseudo-second-order model. Furthermore, the synergistic mechanism between aminoxime and carboxyl groups of the pectin-based adsorbents was proposed. In conclusion, this work provides a new bio-based adsorbent with high efficiency for uranium extraction from concentrated seawater.

研究领域: 材料科学 · 环境科学
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ANALYTICAL CHEMISTRY · 2022 · IF 8.008

Dual-Modulated Heterojunctions for Anti-Interference Sensing of Heavy Metals in Seawater

Ye Ma,Ming Li,Kun Pang,Minggang Zhao

Trace analyte detection in a complex environment such as in seawater is usually challenging for classic redox-based electrochemical sensors since the matrix effect of high salinity and various interfering species with similar redox properties can generate false positive/negative signals, thus impacting the sensitivity and specificity of the sensors. In this work, unlike redox-based approaches, we propose a novel sensing mode that relies on dual-modulated interfacial energy barriers of heterojunctions. By constructing the hierarchical structure of Ni/TiO2/porous-reduced graphene oxide/chitosan (CS), we introduce interfacial energy barriers of Schottky junctions into the electrochemical sensors for Cu2+. Most importantly, we found that two factors, light and the electrostatic interactions between the heterojunctions and Cu2+, can be coupled to regulate the height of the interfacial energy barrier and at last exponentially magnify the sensing signals in response to Cu2+. Since the electrostatic interaction is inert to redox, the proposed sensor is robust against most interfering species even in seawater. Illumination further enhances its sensitivity by 6.23 times and endows it a limit of detection of 0.22 nM. Such a dual-modulated sensing mode is also valid in other heterojunctions such as in the p–n junctions of Ni/NiO/MoS2/CS, demonstrating its potential in more universal applications.

研究领域: 材料科学 · 环境科学 · 电化学传感
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DESALINATION · 2024 · IF 8.3

Enhanced uranium extraction from seawater using bifunctional-modified molecular sieves with high selectivity and adsorption capacity

Wen Guo,Zixin Lin,Kun Jiang,Hao Li,Xiangfeng Liang,Weizhong An,Huizhou Liu,Haiyan Luo,Haoyu Yao

The extraction of uranium from seawater is not only crucial from a strategic standpoint but also poses significant technical challenges. In this work, a series of novel bifunctionalized mesoporous silicas were prepared through a straightforward method, utilizing the structural characteristics of SBA-15 and synergistic effect of functional groups. The impact of pH value, initial uranium concentration, temperature, and duration on uranium adsorption was investigated through a series of batch experiments. The bifunctional modified SBA-15 demonstrated rapid uranium adsorption, which was a spontaneous endothermic reaction and conformed to the pseudo-second-order model. Thereinto, SBA-15 modified with aldoxime and amino group (SBA-15-SAO-N) exhibited the best uranium adsorption performance, with a maximum adsorption capacity of 701.85 mg·g −1 at 298 K and pH 6, an increase of 146 % compared to SBA-15-SAO. SBA-15-SAO-N exhibits excellent U/V selectivity (selectivity coefficient of 30) in the coexistence of U and V solutions, and it still maintains high adsorption capacity after five adsorption-desorption cycles. In actual seawater conditions, the adsorption capacity of SBA-15-SAO-N was 135.26 μg·g −1 . By combining DFT calculations and characterization, the coordination model and interaction energy between functional groups and uranyl were elucidated, revealing that introducing bifunctional groups can enhance the binding strength of adsorbents to uranium and form more stable complexes, thereby improving adsorption capacity and selectivity. These results indicate that bifunctional modified mesoporous silica offers a promising strategy for recovering uranium resources from seawater.

研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Simple one-step synthesis of woven amidoximated natural material bamboo strips for uranium extraction from seawater

Ying Wang,Zaiwen Lin,Qi Liu,Jiahui Zhu,Jingyuan Liu,Jing Yu,Rongrong Chen,Peili Liu,Jun Wang

The uranium(VI) (U(VI)) extraction from seawater was crucial for future energy problems such as increasingly depleted fossil fuels and serious environmental pollution , and it could improve the current situation of limited U(VI) reserves on land. In this study, the natural material bamboo strips (BS) were utilized due to the flexibility and richness of various functional groups, and the amidoximized bamboo strips (AOBS) could be directly prepared by a simple one-step method. The amidoximation of materials not only adjusted the optimal adsorption pH from 4 to 6, but also advanced the hydrophilicity, speeded up the reaction rate (adsorption equilibrium within 1 h, about 0.17 times of BS), and increased the adsorption capacity (q e  = 268.41 mg g −1 at pH = 6, about 1.7 times of BS). Importantly, the AOBS maintained its initial stitchability through flexibility adjustment, and was woven into a macro-shaped adsorbent (AOBS-M). After being placed in the Yellow Sea basin for 30 days, approximately 44.75 g of crude U(VI) (U(VI) content = 40.45 mg) was obtained (q e  = 0.97 mg g −1 ), and it showed the excellent selectivity for U(VI). The AOBS-M not only overcame the problem that the existing adsorption materials were difficult to achieve macroscopic large-area molding, but also realized the flexibility adjustment during the modification process by controlling the reaction conditions, and promoted the industrial development of U(VI) extraction from seawater.

CAS / MDL: 8013-01-2 91079-40-2
研究领域: 环境科学 · 材料科学
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Frontiers in Marine Science · 2025 · IF 3

UVA-induced weathering of microplastics in seawater: surface property transformations and kinetics

Liu Gao,Yuanyuan Su,Tariq Mehmood,Zezheng Wang,Licheng Peng,Naiming Zhang

During environmental migration, large plastic fragments can undergo degradation into microplastics (MPs), posing a significant threat to ecosystems. A research gap exists in understanding how MPs age in complex environments. We modeled aging by integrating an aging index with degradation kinetics. This study investigated the degradation of MPs (polyethylene (PE), polypropylene (PP), polystyrene (PS) and polyvinyl chloride (PVC)) exposed to ultraviolet radiation in seawater. Aged MPs exhibited cracks, oxidized particles, and wrinkles on their surfaces. The functional groups experienced stretching (e.g., -OH, C-H, C=O) and bending (e.g., X-H in-plane, C-H in-plane), as identified through Fourier transform infrared spectroscopy (FTIR). Meanwhile, the crystallinity of MPs increased initially but decreased over time. The roughness and carbonyl index (CI) of MPs was increased as the weathering time progressed. mPE and mPP exhibited the most pronounced aging. The Elovich kinetic model poorly fitted the CI for aged MPs. A First-order kinetic improvement model fitted well but lacked clear parameter significance. The degradation mechanisms of mPE and mPP were similar. The benzene ring structure in mPS and dechlorination experienced by mPVC render them resistant to degradation. This study provides evidence that that enhances our understanding of the mechanisms underlying the aging process of MPs in seawater.

CAS / MDL: 7758-02-3
研究领域: 环境科学 · 材料科学 · 生态学
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RADIATION PHYSICS AND CHEMISTRY · 2024 · IF 2.8

Design of amidoximized hydroxyapatite for extracting uranium from seawater

Yan Wang,Yong Zhang,Xiaolin Liu,Sen Sun,Bowei Chen

Extracting uranium from natural seawater is a huge challenge because of the complex environment of seawater and extremely low uranium concentration. In this work, amidoximized hydroxyapatite (AO-HAP) was prepared to capture uranium from seawater. The introduction of amidoxime group greatly improved the recognition ability of AO-HAP for uranium in neutral and weakly alkaline environment (pH = 7–8). The uptake process of AO-HAP for uranium was fitted by Langmuir and pseudo-second-order models, suggesting that the capture behavior of AO-HAP for uranium was a homogeneous chemisorption . The saturated uranium uptake capacity of AO-HAP was 865.3 mg g −1 from aqueous solution, which was better than most of other reported uranium extractants. More importantly, AO-HAP had good regeneration ability and excellent adsorption performance in natural seawater (6.25 mg g −1 in 30 days). In sum, AO-HAP is a highly potential candidate as adsorbent material for the efficient extraction of uranium from seawater.

研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Regulation of chain conformation and synergistic effect of auxiliary groups towards polyamidoxime for highly efficient uranium extraction from seawater

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 · 环境科学
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Journal of Materials Chemistry B · 2020 ·Vol. 8 ·期 36 ·8232-8241 · IF 5.344

A high-strength double network polydopamine nanocomposite hydrogel for adhesion under seawater

Min Liang,Chunpeng He,Jidong Dai,Pengfei Ren,Yifu Fu,Faming Wang,Xin Ge,Tianzhu Zhang,Zuhong Lu

Mussel-inspired catechol-based strategy has been widely used in the development of underwater adhesives. Nonetheless, the properties of the adhesives were still severely limited under harsh environments. A facile approach was proposed herein to prepare a double network hydrogel adhesive with low swelling rate and high strength in seawater, where the first network was polyacrylamide (PAM) and the second network was alginate (Alg). Meanwhile, polydopamine (PDA) nanoparticles, which were formed through self-polymerization as adhesion anchoring sites, distributed evenly throughout the double network hydrogel and effectively enhanced the adhesion capability of the hydrogel. The properties of the resulting hydrogel have been fully characterized. The optimal adhesion strength of the hydrogel adhesive in seawater was as high as 146.84 ± 7.78 kPa. Furthermore, the hydrogel also has excellent ability to promote the growth of zooxanthellae. Our studies provide useful insights into the rational design of underwater adhesives with high performances even beyond nature.

研究领域: 材料科学 · 海洋生物学 · 生物材料
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Amidoximated cellulose microspheres synthesized via homogenous reactions for High-Performance extraction of uranium from seawater

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 · 环境科学
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CARBOHYDRATE POLYMERS · 2022 · IF 10.723

Poly(amidoxime)-graft-magnetic chitosan for highly efficient and selective uranium extraction from seawater

Yizhe Zhang,Tingting Cai,Zhiwei Zhao,Bing Han

Adsorbents with highly efficient and selective recovery performance towards uranium are significantly demanded for the sustainable nuclear power production. Herein, poly(amidoxime)-graft-magnetic chitosan (P(AO)-g-MC) was synthesized through functionalizing magnetic chitosan with polyacrylonitrile followed by amidoximation process. Under magnetic field, P(AO)-g-MC can be separated from the solution in 10 s. Owing to the strong affinity of high-density amidoxime groups towards uranium, P(AO)-g-MC showed remarkable adsorption capacity, rapid kinetics and good regeneration performance in uranium spiked aqueous solution. Notably, the 7-day uranium adsorption capacity of P(AO)-g-MC from natural seawater in column mode was up to 5.14 mg/g, 12 times that of vanadium. The excellent uranium uptake performance over vanadium originated from the strong coordination by N and O in amidoxime groups according to theoretical simulation. The advantages of easy separating and high selectivity make P(AO)-g-MC a very potential uranium adsorbent in natural seawater.

研究领域: 材料科学 · 环境科学
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