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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Biofouling-resistant polyamidoxime-based natural hierarchical porous bamboo strips prepared by in-situ polymerization for uranium extraction from seawater

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

Effectively extracting uranium (VI) [U(VI)] from seawater requires efficient adsorbents. Generally, there are two major factors that affect the adsorption efficiency of adsorbents, including the biofouling around the adsorbents and the relative density of adsorption active sites. To enhance the practical application value of powdered polyamidoxime-based materials, macro-braidable and hierarchical porous bamboo strips (BS) with antibacterial properties are selected to synthetize polyamidoximized bamboo strips (PAOBS) by in-situ polymerization methods. On the one hand, natural BS have a bamboo quinone structure, and their intrinsic structure is not destroyed during the reaction process, which endows PAOBS with excellent antibacterial properties. In addition, PAOBS retains the hierarchical porous structure of BS, providing channels for the adsorption process, which is beneficial to achieve the maximum utilization of adsorption active sites. On the other hand, PAOBS increases the relative density of amidoxime functional groups, and its adsorption capacity (233 mg g −1 ) is approximately 2.14 times higher than that of pure PAO at pH= 6.0, including electrostatic effect and chelation mechanism. After PAOBS is floated in the Yellow Sea Basin for 30 days, its adsorption capacity for U(VI) reaches 1.03 mg g −1 . Importantly, the addition of BS increases the coordination modes with the uranyl ion, and the single coordination mode of CH(NH 2 )= N - O H from PAO is translated to the three mixed coordination modes of CH(NH 2 )= N - O H, CH( N H 2 )=N - O H, and CH( N H 2 )=N - OH and adjacent CH( N H 2 )=N - OH from PAOBS. Construction of PAOBS plays a role in the design of novel adsorbents with high relative density of adsorption active sites and biofouling-resistant, laying the steady foundation for further realizing sustainable U(VI) extraction from seawater.

研究领域: 材料科学 · 环境科学 · 海洋学
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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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WATER AIR AND SOIL POLLUTION · 2024 ·Vol. 235 ·期 6 ·1-20 · IF 3.8

Accelerated Photocatalytic Degradation of Sulfamethoxazole and Cefixime: A Comprehensive Study of Biotoxicity, Degradation Kinetics and Pathway

Akbari Mohammad Zahir,Xu Yifeng,Liang Chuanzhou,Lu Zhikun,Shen Siyuan,Peng Lai

This study aimed to accelerate photocatalytic treatment of sulfamethoxazole (SMX) and cefixime (CFM) and alleviate the toxicity of photocatalysis effluents to improve further biodegradability. An efficient and fast reactive photocatalyst (Fe 2 O 3 /ZnO@VC) was synthesized, characterized and applied for photocatalytic removal of the targeted compounds. Results further confirmed the complete removal of SMX (1 mgL -1 ) within 30-min photocatalytic treatment. Acidic condition favored SMX removal due to the formation of negative ions, which were attracted by the surface of the catalyst comprising positive charge in pH values below the point of zero charge. The ideal degradation environment for CFM (1 mgL -1 ) was at neutral pH, and 97.2±0.1% of CFM was degraded over 60-min. A quenching test revealed that superoxide radial ( • O 2 − ) and e − played a major role in the photocatalytic degradation of SMX, while hydroxyl radical ( • OH) showed an identical effect during photocatalytic treatment of CFM. The degradation efficiency of SMX was marginally reduced in synthetic wastewater (SWW) and CFM in tap water (TW) due to the quenching effects of phosphates and carbonates anions in SWW and chloride ions in TW, respectively. As a result of the excellent mineralization properties of the photocatalyst, the photocatalysis effluents were highly detoxified, reaching 93.5±11.8% and 87.0±5.1% for SMX and CFM, respectively. Graphical Abstract

CAS / MDL: 79350-37-1
研究领域: 环境科学 · 化学工程 · 生物学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2024 · IF 1.5

Synthesis of novel hyper-cross-linked polymers for efficient uranium(VI) capture from aqueous solution

Yan Huijun,Huo Long,Li Mingxia,Azhati Hayinaer,Bai Jianwei

Uranium extraction from seawater is of great significance for the development of the nuclear industry. However, the adsorption of uranium is limited by selectivity of uranium and recycle performance. In this study, amidoxime-functionalized polymer (BP-AO) was prepared by coupling benzene with phenylacetonitrile to extraction uranium from aqueous solution. Adsorption experiments show that the adsorption progress of BP-AO can reach equilibrium within 5 min and the maximum adsorption capacity is 193.9 mg·g −1 calculated by Langmuir model. The selectivity of BP-AO for U(VI) is excellent and after five adsorption–desorption experiments, the adsorption capacity only decreased about 10%. The adsorption mechanism shows that the sorption is mainly due to the formation of stable chelates between the amidoxime groups and U(VI). These results demonstrate the potential application of the adsorbent for practical utilization.

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

Synergistic cross-linking strategy with oxime-carbamate and hydrogen bonding arrays for excellent damage self-healing and reprocess ability of thermoset polyurethanes

Pengwu Xu,Ning Ding,Hong Wang,Jieyu Guan,Yirui Shen,Deyu Niu,Weijun Yang,Piming Ma

Thermoset polyurethanes face significant deterioration of physical properties after damage self-healing or reprocessing. It is still a great challenge to design the structure of polyurethanes to realize damage self-healing and reprocess ability under mild conditions. In this work, a series of double-crosslinked networked polyurethanes with different crosslinking densities were synthesized by designing a synergistic crosslinking strategy of oxime-carbamate bonding and hydrogen bonding arrays. By regulating the density of the crosslinked network and the content of strong and weak hydrogen bonds, the tensile strength of the polyurethanes was increased from 13.1 to 24.3 MPa, and the toughness was increased from 66.5 to 129.2 MJ/m 3 . Meanwhile, the synergistic effect of the oxime-carbamate with low activation energy and hydrogen bonding arrays enabled the polyurethanes to have an excellent self-healing (97 %) and reprocessing. The polyurethanes could be rapidly reprocessed after only 5 min of hot pressing at 120 °C by virtue of the thermal response of the dual network. More importantly, the tensile strength retention rate can still maintain more than 96 % after reprocessing. Finally, we propose the concept of a wearable device that can intelligently detect changes in resistance values during human movement. Therefore, this work provides a new idea for the preparation of polyurethanes with excellent damage self-healing and reprocessing, which is expected to expand its application.

CAS / MDL: 77-58-7 822-06-0
研究领域: 材料科学 · 高分子化学
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Microorganisms · 2024 ·Vol. 12 ·期 4 ·675 · IF 4.1

Cefotaxime Exposure-Caused Oxidative Stress, Intestinal Damage and Gut Microbial Disruption in Artemia sinica

Huizhong Pang,Kaixuan Zheng,Wenbo Wang,Mingjuan Zheng,Yudan Liu,Hong Yin,Daochuan Zhang

Cefotaxime (CTX) is an easily detectable antibiotic pollutant in the water environment, but little is known about its toxic effects on aquatic invertebrates, especially on the intestine. Here, we determined the oxidative stress conditions ofA. sinicaunder CTX exposure with five concentrations (0, 0.001, 0.01, 0.1 and 1 mg/L) for 14 days. After that, we focused on changes in intestinal tissue morphology and gut microbiota inA. sinicacaused by CTX exposure at 0.01 mg/L. We found malondialdehyde (MDA) was elevated in CTX treatment groups, suggesting the obvious antibiotic-induced oxidative stress. We also found CTX exposure at 0.01 mg/L decreased the villus height and muscularis thickness in gut tissue. The 16S rRNA gene analysis indicated that CTX exposure reshaped the gut microbiota diversity and community composition. Proteobacteria, Actinobacteriota and Bacteroidota were the most widely represented phyla inA. sinicagut. The exposure to CTX led to the absence of Verrucomicrobia in dominant phyla and an increase in Bacteroidota abundance. At the genus level, eleven genera with an abundance greater than 0.1% exhibited statistically significant differences among groups. Furthermore, changes in gut microbiota composition were accompanied by modifications in gut microbiota functions, with an up-regulation in amino acid and drug metabolism functions and a down-regulation in xenobiotic biodegradation and lipid metabolism-related functions under CTX exposure. Overall, our study enhances our understanding of the intestinal damage and microbiota disorder caused by the cefotaxime pollutant in aquatic invertebrates, which would provide guidance for healthy aquaculture.

CAS / MDL: 64485-93-4 63527-52-6
研究领域: 环境科学 · 微生物学 · 毒理学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Bioinspired surface engineering of amidoxime functionalized polyvinylidene fluoride membrane for efficient uranium extraction from seawater and wastewater

Huanhuan Tan,Tianhang Shan,Bingfeng Deng,Jianang Sha,Chuntai Liu,Peipei Yang,Songwei Li,Zhipeng Xie,Zhong Liu

Efficient uranium (VI) extraction from seawater (UES) and wastewater is crucial for environmental remediation and nuclear power generation. Herein, a novel amidoxime functionalized polyvinylidene fluoride (PVDF-AO-4) membrane constructed through reaction of amoximated 2-diaminomaleonitrile (DAMN-AO) with Tannic acid of the Tannic acid (TA)-3-aminopropyltriethoxysilane (APTES) coating (TA-APTES coating) is designed via surface engineering technology. Introducing the amidoxime group with abundant multi-affinity sites endows PVDF-AO-4 with excellent adsorption capacity (q m  = 175.8 mg/g) and selectivity for U(VI). Meanwhile, the PVDF-AO-4 exhibits outstanding recyclability, antifouling capabilities, high flux recovery rate (FRR) of over 90 % and low flux decline rate (FDR) of under 5 % after five cycles in the dynamic adsorption and great elution efficiency (nearly 80 %) after 10 cycles. PVDF-AO-4 can effectively capture 9.84 mg/g U(VI) in 3 weeks period from natural seawater. The membrane material designed in this work can be used for efficient, selective of uranium from seawater and wastewater.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Fabrication of amidoxime grafted polyacrylonitrile for iodine vapor capture from off-gas

Ling Zhang,Mengfang Li,Xuan Liu,Jiaqi Feng,Yujia Liu,Yazhu Tu,Shuyang Li,Tao Duan

The exploration of effective gaseous iodine adsorbents is an interesting and challenging task in the field of radwaste disposal. In this study, amidoxime groups (AO) were successfully grafted onto polyacrylonitrile to obtain amidoxime grafted polyacrylonitrile (PAN-AO) for capturing gaseous iodine. The results of the combined characterization analysis have confirmed that the introduction of AO greatly improved its thermostability, porosity and available functional groups of PAN. The impacts of reaction time, iodine concentration and reaction heat on the uptake capacity for gaseous iodine were systematically studied. The PAN-AO exhibited higher iodine capture capacity (1534.4 mg/g) than PAN (72.1 mg/g) at 80 °C and 600 min, which was ascribed to the chemical reaction between electron-rich AO groups and electron-deficient iodine molecules. The studies of kinetic fitting and activation energy (E a  = 44.11 kJ/mol) further confirmed that chemical adsorption was the major fashion during the whole uptake process of PAN-AO for iodine. Besides, PAN-AO still had an iodine uptake capacity of 704.4 mg/g after five recycling, manifesting the remarkable cycle performance of PAN-AO. In brief, this study offered a new reference for radioactive iodine uptake and the synthesized PAN-AO was able to serve as an efficient iodine capture material.

CAS / MDL: 107-13-1 7553-56-2
研究领域: 材料科学 · 环境科学
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ACS Applied Polymer Materials · 2024 · IF 4.4

Preparation of Antibioadhering Materials Containing Quaternary Phosphonium Salt for Uranium Extraction from Seawater

He Li,Shusen Chen,Yan Song,Haiyun Ding,Ziming Li,Haotian Wu,Fengju Wang,Hao Li,Ziteng Gao,Haizhen Wang

In this paper, three antibioadhering materials with quaternary phosphonium salt-modified polyamidoxime (PAO-QPS) for uranium extraction from seawater were prepared using commercial polyacrylonitrile fiber as the base material by the ion-exchange method. Infrared spectroscopy and thermogravimetric analysis were used to verify the correctness of the structure and to test the thermal stability of the synthetic materials. Scanning electron microscopy was used to analyze the microscopic appearance of the material surface. X-ray photoelectron spectroscopy was used to determine the composition of the surface elements before and after modification of the material and after adsorption of uranium. The uranium adsorption and biological adhesion resistance of the materials were tested. Polyamidoxime-modified hexyltriphenylphosphonium bromide (PAO-C6) was the best adsorption material among the three quaternary phosphonium salt-modified materials with different alkyl chains. The adsorption kinetic curve and adsorption isotherm were drawn according to the uranium adsorption results. The results showed that the adsorption time and temperature were positively correlated to the uranium adsorption capacity of PAO-C6. The maximum uranium adsorption capacity of PAO-C6 could reach 23.6 mg·g–1 in the simulated seawater with a uranium concentration of 3.3 mg·L–1. In addition, the inhibition rates of the material to Escherichia coli and Staphylococcus aureus were 87.60 and 90.59%, respectively, and the inhibition rate against marine bacteria reached 80.61%, indicating that PAO-C6 has good antibioadhering properties. PAO-C6 was expected to be used for uranium extraction from seawater.

研究领域: 材料科学 · 环境科学 · 海洋科学
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SYNTHESIS-STUTTGART · 2023 ·Vol. 55 ·期 20 ·3393-3401 · IF 2.6

Copper-Catalyzed Coupling of N-Phenoxyacetamides and 2H-Azirines for Synthesis of α-Amino Oxime Ethers

Yue-Lu Zhu,Jie Yan,Xiu-Xuan Xu,Zong-Yu Sun,Jiao Chen

Copper-catalyzed coupling reaction involving N-phenoxyacetamides and 2H-azirines is described, in which N–O and C–N bonds are broken and restructured. This protocol provides an efficient strategy for the highly regioselective synthesis of racemic α-amino oxime ethers. In addition, this strategy can be used to modify natural products and is gram-scale compatible.

研究领域: 有机化学 · 合成化学
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2019 ·Vol. 94 ·期 8 ·2512-2521 · IF 2.659

Efficient degradation of cefotaxime by a UV+ferrihydrite/TiO2+H2O2 process: the important role of ferrihydrite in transferring photo-generated electrons from TiO2 to H2O2

Qi Jiang,Runliang Zhu,Yanping Zhu,Qingze Chen

Background Developing effective removal processes for antibiotics has attracted increasing interest recently. In this work, a novel strategy involving the combination of photocatalysis with Fenton reaction using ferrihydrite/TiO 2 (Fh/TiO 2 ) nanohybrids was developed to efficiently degrade the antibiotic cefotaxime. Fh/TiO 2 nanohybrids were synthesized by simply growing Fh on the surface of commercially available TiO 2 . We expected that Fh of Fh/TiO 2 could capture photo-generated electrons from TiO 2 , inhibiting the recombination of electron–hole pairs; also, by virtue of Fe(III)/Fe(II) cycle on Fh/TiO 2 , photo-generated electrons could be continually transferred to H 2 O 2 to produce ·OH. Accordingly, high degradation efficiency of cefotaxime could be achieved. Results With UV light and H 2 O 2 , Fh/TiO 2 with a Fe/Ti molar radio of 7% showed high catalytic activity indeed, and its degradation rate for cefotaxime was nearly three times higher than that of TiO 2 . The decomposition of H 2 O 2 and production of ·OH in the UV+7%Fh/TiO 2 +H 2 O 2 system were also increased markedly. The large amount of Fe(II) on 7%Fh/TiO 2 determined in this system supported our hypothesis that Fh of 7%Fh/TiO 2 could capture photo-generated electrons from TiO 2 . Although dissolved iron was observed, the contribution of Fenton reaction by dissolved iron was rather limited. After four consecutive cycles, 7%Fh/TiO 2 still retained good stability. Conclusions The UV+7%Fh/TiO 2 +H 2 O 2 system provides a potential alternative in degradation of cefotaxime for further practical application, and it has the following advantages: high catalytic activity, simple preparation method, good stability and low cost, as well as continued catalytic activity after total consumption of H 2 O 2 . © 2019 Society of Chemical Industry

研究领域: 环境科学 · 化学工程
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2021 · IF 6.158

Thermal hazards of benzaldehyde oxime: Based on decomposition products and kinetics analysis by adiabatic calorimeter

Xiao-Qiao Zhao,Wen-Qian Wu,Hua-bo Li,Zi-Chao Guo,Wang-Hua Chen,Li-Ping Chen

As a self-reactive substance, benzaldehyde oxime (BO) is prone to a highly exothermic runaway reaction and thermal hazard analysis and the reaction kinetics calculation of BO have great significance. In this work, the decomposition products of BO in nitrogen atmosphere were identified by GC–MS and HPLC techniques. The impact of the decomposition products on the decomposition behaviors of BO were analyzed by comparison of the ARC test results of pure BO and mixture of BO and decomposition products. It was found that N-benzylidene benzylamine was the intermediate decomposition product and benzoic acid , benzamide, N-benzyl benzamide, and 2,4,5-triphenylimidazole were the final products of BO. A two-step continuous autocatalytic reaction model was established to depict the decomposition process of BO. The kinetic parameters of the model were calculated by applying the nonlinear optimization method. Finally, thermal behaviors under different process temperature were predicted based on the kinetic model , and the time to maximum rate (TMR ad ) was predicted as 112.04 °C under 24 h, and 122.19 °C of 8 h, which offer crucial safety information to optimize the safety conditions of BO during usage, storage and transportation, which minimizes the industrial disasters.

研究领域: 化学工程 · 安全科学
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