RSC Advances
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2015
·Vol. 5
·期 96
·79022-79030
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IF 3.84
Lei Xu,Xiaoqiong Lu,Xiaomin Cheng
A series of novel cotton cellulose-graft-polycaprolactone copolymers with different grafting contents were successfully prepared via ring-opening polymerization (ROP) in an ionic liquid 1-N-butyl-3-methylimidazolium chloride ([Bmim]Cl). The structures of the grafting copolymers were systematically characterized by FTIR, CP/MAS13C-NMR, XRD, SEM and AFM, while thermal properties were investigated by DSC and TGA. Subsequently, Langmuir, Freundlich, Temkin, and Dubinin–Radushkevich (D–R) adsorption isotherms were representative to simulate adsorption isotherms of Cu(II) and Ni(II) ions in aqueous solution. From the comparison of different adsorption isotherm models, it was found that adsorption of Cu(II) by modified cellulose followed Langmuir, Freundlich and Temkin models, while that of Ni(II) followed the Freundlich model. The results of adsorption indicated that the selectivity sequence of metal ions on graft copolymers was Cu(II) > Ni(II) and the maximum removal capacities of Cu(II) and Ni(II) ions were 98.7% and 35.6%, respectively. Hence, the graft copolymers exhibited significant potential to be an environmentally feasible biosorbent for removal of Cu(II) and Ni(II) ions from aqueous solution.
研究领域:
环境科学
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高分子化学
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材料科学
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重金属去除
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吸附技术
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Science China-Chemistry
·
2023
·Vol. 66
·期 3
·853-862
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IF 9.6
Yang Lei,Liu Zenghe,Neisiany Rasoul Esmaeely,Lou Jiaming,Guo Yifan,Zhang Luzhi,Liu Huijie,Chen Shuo,Gu Shijia,You Zhengwei
It is exceedingly desired, but difficult to construct self-healing materials with both excellent mechanical properties and healing efficiency, which are usually realized by using mutually exclusive methods. Here, we reconcile this contradiction by utilizing copper-bis-(imidazole-2-yl)-methane-urea (Cu-BIMU) locked units based on novel designed dynamic imidazole-urea bonds with coupled multiple noncovalent bonds (coordination bonds, π − π stacking bonds, and hydrogen bonds). The coordination of Cu(II) greatly reduces the electron-cloud density of imidazole, which lowers the free energy barrier of imidazole-urea bonds and promotes their reversible dissociation, as demonstrated by the density functional theory and small-molecule model reaction. The topological design of Cu-BIMU polyurethane (Cu-BIMU-PU), which concentrates multiple crosslinking-in-one locked unit to avoid the formation of excessive crosslinking sites to ensure high chain mobility, facilitates self-healing. Accumulative extensive intermolecular interactions endowed excellent mechanical properties to the resulting Cu-BIMU-PU elastomer with a tensile strength of 65.3 MPa, among the highest ever-reported value. This work provides a novel molecular design principle for fabricating high-performance dynamic polymers.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Wei Yang,Mingli Cao
The removal of heavy metal ions from the aqueous environment is an important topic as heavy metal pollution is widely distributed in water bodies, causing serious damage to aquatic ecosystems and worsening the already scarce freshwater resources. In this work, we report the synthesis of novel ZIF-8@GO-COOH composite nanosorbent materials by in situ self-assembly. The physicochemical properties of the composites were investigated using relevant characterisation techniques, and the adsorption capacity of ZIF-8@GO-COOH for copper and lead ions in aqueous solution was tested by batch adsorption experiments. The adsorption behaviour was analysed by combining adsorption kinetics, adsorption isotherm model and Van't Hoff model. The results showed that the adsorption capacities of ZIF-8@GO-COOH for Cu(II) and Pb(II) were 93.26 mg/g and 95.875 mg/g, respectively, when the initial heavy metal ion concentration was 100 mg/L, the adsorption time was 60 min, the temperature was 293 K and the pH conditions were suitable. The high adsorption performance of ZIF-8@GO-COOH was attributed to its surface with abundant oxygen-containing functional groups and excellent specific surface area, which gives it a significant advantage in the removal of heavy metal ions from aqueous solutions.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2022
·
IF 8.025
Liuting Mo,Shifeng Zhang,Fei Qi,Anmin Huang
Water pollution by heavy metal ions is a global concern due to detrimental effects on the ecological environment and human health. To solve the problem of the stability and recyclability of the traditional adsorbents, we proposed three-dimensional lamellar porous cellulose nanofiber/polyacrylamide composite aerogel with outstanding pollutants adsorption, easy regeneration, and multiple recycling. The aerogel adsorbent was prepared by a two-step method via facile in-situ physical/chemical double cross-linking and freeze-drying processes. The resulting aerogels showed good thermal stability , superior water stability and excellent adsorption properties, with a maximum Langmuir adsorption capacity for Cu(II) ions up to 240 mg g −1 due to the in-situ physical/chemical combination of anionic polyacrylamide and carbonylated cellulose nanofibers. The adsorption mechanism was the electrostatic attraction, chelating effect and complex formation driving forces for the fast and efficient adsorption of Cu(II) ions. The removal efficiency of the aerogels for Cu(II) remained above 80% after 10 adsorption/regeneration cycles, suggesting its outstanding recyclability. The proposed aerogel adsorbent shows noteworthy potential for the practical treatment of heavy metal ion wastewater.
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Molecular Catalysis
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2022
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IF 5.089
Pan Pan,Mingming Li,Yuxin Liu,Yisi Feng,Xinglong Li
2,5-diformylfuran (DFF) is a multifunctional intermediate, which can be used in drugs, functional polymers, fluorescent materials and surfactants. In this paper, a TEMPO-assisted magnetic Fe 3 O 4 @SiO 2 @mSiO 2 -NH 2 -Cu(II) catalytic system was developed for the selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran. The structure of Fe 3 O 4 @SiO 2 @mSiO 2 -NH 2 -Cu(II) was double-layer shell-core spherical structure with uniform ordered mesoporous on the surface, amino groups and Cu were evenly distributed in the outer mesoporous. The catalyst was characterized by FT-IR, TEM, EDS, SEM, XRD, BET and VSM. The effects of reaction conditions were investigated in detail. The conversion of HMF was 98.9% and the highest DFF yield was 92.4% under atmospheric oxygen in toluene solvent. The catalytic activity did not decrease significantly after 5 cycles. The catalytic system had good substrate adaptability for benzyl alcohols and aromatic alcohols with satisfactory yield of corresponding aldehydes (91.3–100%). A possible reaction mechanism was also proposed and found that bis(μ-hydroxy) double copper (II) may be the active reactant in oxidation reaction. The system provides a promising industrialized preparation method for DFF.
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APPLIED ORGANOMETALLIC CHEMISTRY
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2022
·Vol. 36
·期 10
·e6833
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IF 4.072
Jing Hu,Yun Luo,Min Hou,Jia Jia Qi,Li Li Liang,Wen Ge Li
Two dinuclear complexes [Cu 2 (LO) 2 ] and [Ni 2 L 2 Cl 2 (C 2 H 5 OH) 2 ] derived from (5-chlorosalicylaldehyde)-4-aminoantipyrine (HL) were synthesized and characterized by infrared (IR) spectroscopy,thermogravimetric analysis, and powder X-ray diffraction. Molecular structures of the Cu (II) and Ni (II) complexes were determined by single-crystal X-ray diffraction. Their cytotoxicity was evaluated by methyl thiazolyl tetrazolium assay against human tumor cells, such as lung carcinoma A549, lung adenocarcinoma H1975, breast carcinoma MDA-MB-231, and nasopharyngeal carcinoma CNE-2Z cell lines. The results showed that the Cu (II) complex had much better anticancer activity than the Ni (II) complex, especially for MDA-MB-231 and CNE-2Z cells. The reason may be that they have different structures. The methyl group on the (5-chlorosalicylaldehyde)-4-aminoantipyrine (HL) was oxidized to the hydroxymethyl group, herein, namely LO, which is difficult to achieve in the normal chemical synthesis process. However, we did it by a solvothermal method at low temperature. It provides a new way of thinking and synthesis. The anticancer activity of the copper complex was next only to cisplatin, and the copper complex was nontoxic for the human normal cell lines. The experiment results also showed that the copper complex could inhibit tumor cell proliferation through the cell cycle and cell apoptosis.
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TALANTA
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2021
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IF 6.057
Rongrong Wang,Yong Cao,Hao Qu,Yanbo Wang,Lei Zheng
Copper sulfate is a widely used agent to control insects, bacteria and algae for fishery. However, excess amount of copper ions in water accumulate in aquatic products through the ecological cycle system, highly threatening food safety and public health. Therefore, it is urgent to develop a rapid and efficient method for the determination of copper content in aquatic products. In this study, we developed a label-free biosensor for Cu(II) based on a graphene field-effect transistor gated by structure-switching aptamer probes (SSA-GFET) against Cu(II) we obtained before. The detection mechanism of the biosensor is attributed to the surface charge shift and the potential change of the gate electrode upon the specific binding of Cu(II). The SSA-GFET biosensor has a low detection limit of 10 nM and a linear range of 10 nM to 3 μM to Cu(II). In addition to the excellent selectivity to Cu(II), the biosensor also showes the advantage of high recovery rate for detection of Cu(II) in real fish samples. Because of the detection characteristics of label-free SSA-GFET, it has great advantages in the field of food safety and environmental detection.
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Journal of the Taiwan Institute of Chemical Engineers
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2021
·
IF 5.876
Wei Zhang,Ping Sun,Desheng Liu,Quanlin Zhao,Binze Zou,Lincheng Zhou,Zhengfang Ye
Herein, a simple and green method to fabricate β-cyclodextrin (β-CD) porous cross-linked polymer modified poly(chloromethylstyrene) (PS-Cl) resin, namely, PS@CM-CDP, for ultrafast and efficient removal of heavy metal ions and organic pollutants from aqueous solution was reported. The selected (PS-Cl) was used as a matrix; meanwhile, the β-CD was formed on the surface of PS-Cl under a rigid cross-linking agent of tetrafluoroterephthalonitrile nitrile. The structure and surface elements distribution of PS@CM-CDP were characterized using FT-IR, TG, SEM, XPS, and BET. The resultant PS@CM-CDP with a relatively high maximum adsorption capacity for Cu(II) and BPA can reach 121.88 and 8.25 mg g −1 , respectively, and the spherical nature of the resin makes conventional β-CD polymers easy to recycle 6 times without significantly decreased. The possible adsorption mechanism was also proposed. Industrial wastewater adsorption methods have been used into practice, and the practice presents considerable prospects in the aspects of column for water treatment.
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Materials
·
2020
·Vol. 13
·期 9
·2033
·
IF 3.057
Yongzhen Lei,Long Mao,Jin Yao,Zhihan Li
Poly(lactic acid) (PLA) represents one of the most promising and attractive bio-based polymers for green packaging. However, toughness, gas barrier and antibacterial properties of pure PLA films cannot compete with those of traditional petroleum-based active packaging plastics. To fill this gap, utilization of excellent chelating properties of phytic acid (PA), functionalized layered double hydroxides (LDHs@PA-Cu(II)) was firstly synthetized via facile deposition and chelation of one-step assembled PA-Cu(II) coordination compounds on the surface of layered clay. Furthermore, LDHs@PA-Cu(II)/PLA nanocomposites were prepared by blending LDHs@PA-Cu(II) and pure PLA via solution casting evaporation process. After adding only 1 wt % LDHs@PA-Cu(II), elongation at break and tensile strength increase by 53.0% and 18.9%, respectively, and the oxygen relative permeability decreases by 28.0%. Due to the strong interface interaction and heterogenous nucleation, the reinforcement effect of LDHs@PA-Cu(II) at low loadings is remarkable. Meanwhile, owing to the antibacterial activity of PA-Cu(II) coatings, the antibacterial rate (against Escherichia coli) of LDHs@PA-Cu(II) exceeds 99.99%. Furthermore, the corresponding LDHs@PA-Cu(II)/PLA nanocomposites also show outstanding antibacterial properties, which will be a promising candidate for active packaging application.Keywords:layered double hydroxides;phytic acid;antibacterial activity;polylactic acid;barrier properties
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BIORESOURCE TECHNOLOGY
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2019
·
IF 6.669
Mingyun Dai,Ying Liu,Benzhi Ju,Ye Tian
A novel polysaccharide-based thermoresponsive hydrogel containing sodium alginate (SA) and 2-hydroxy-3-isopropoxypropyl starch (HIPS) was developed for removing Cu(II) from aqueous solution. HIPS/SA hydrogel showed network and porous structure, as well as the abundant carboxy groups inside the structure, endowed it with sufficient binding sites for adsorption of Cu(II). The reversible thermoresponsive swelling-shrinking behavior of HIPS/SA hydrogel was discussed. The effects of pH and initial Cu(II) concentration on adsorption capacity were investigated. The adsorption isotherms and kinetics of HIPS/SA hydrogel demonstrated that the adsorption of Cu(II) was subjected to Langmuir and pseudo-second-order models respectively, and the maximum adsorption capacity was 25.81 mg/g. Additionally, HIPS/SA hydrogel could be successfully desorbed by only small amounts of dilute hydrochloric acid within a short time for its thermoresponsive property, it also exhibited the feasibility of regeneration, because the adsorption capacity for Cu(II) was still higher than 15.23 ± 0.27 mg/g even after five cycles.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jinjuan Xue,Jiaqian Zhang,Meng Yuan,Yiting Lv,Zhaoxia Chen,Mingxin Wang
The development of novel photocatalytic platform for efficient water purification and sterilization is of utmost importance due to the significant threat of chronic diseases resulting from water pollution and bacterial contamination. Herein, a high-efficiency, easy-recyclable, and environment-friendly photocatalytic fabric was developed as a water disinfection and organic pollutant degradation platform. In which, microamounts of Au nanoparticles (2 wt%) and Cu(II) clusters (2.5 wt%) co-decorated porphyrinic MOF (Au/PCN-224/Cu(II)) coating was applied as photocatalytic surface, and flexible cotton fabric served as stable support. Au/PCN-224/Cu(II) composite photocatalyst was prepared via a facile photo-deposition procedure followed by impregnation method, and further immobilized onto polydopamine (PDA) pre-treated cotton fabric through catechol-amine reaction. The fabricated photocatalytic platform exhibited excellent ability to generate reactive oxygen species (ROS) by multiple routes under low-power visible light irradiation, and achieved efficient photodisinfection effects for causative organism including Gram-negative Escherichia coli ( E. coli ) and Gram-positive Staphylococcus aureus ( S. aureus ) without the obvious leakage of metal ions from the potocatalyst during the reaction. Additionally, the reaction rate constant for organic dye MB photodegradation achieved by Au/PCN-224/Cu(II)@Fabric was 3.73 times higher than that of PCN-224@Fabric, and the degradation intermediates analysis was also conducted. The band alignments of PCN-224, Au/PCN-224, Au/PCN-224/Cu(II) photocatalysts were determined, and the charge transfer mechanism within Au/PCN-224/Cu(II) photocatalyst was elucidated through the utilization of DRS, Mott − Schottky, ESR, EIS, and photocurrent analyses. It is suggested that the deposition of Au and doping of Cu(II) both with small amounts enhanced the light absorption capacity, and also improved the charge separation ability through the surface plasmon resonance (SPR) effect and interfacial electron transfer (IFCT) mechanism. Moreover, Au SPR and Cu doping exhibited a substantial enhancement in photothermal conversion effect, thereby synergistically reinforcing the sterilization performance. This work provides an approach for the development of effective photocatalytic platform based on porphyrinic MOFs combined with trace metal co-catalysts in the application of water disinfection and purification.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Tingting Zhu,Jinhang Yang,Yuxiang Shen,Ting Liang,Songyu Fan,Shiming Zhang,Zebin Yu,Shuangfei Wang,Yanping Hou
Z-scheme heterojunction photocatalysts can restrain carriers’ recombination while retaining high redox capacity. Herein, a novel ZnTe/rGO/WO 3 (ZRW) Z-scheme heterojunction was constructed for simultaneous removal of TC and Cu (II) from wastewater. The highly conductive rGO served as a bridge connecting the ZnTe and WO 3 whereby forming a tight interaction interface, beneficial to carriers transfer and separation. The removals of TC and Cu (II) using the optimized ZRW-10% achieved 90.6% and 89.5% within 150 min of light exposure, which were much higher than those from the ZnTe and WO 3 . Results of free radical trapping experiments and electron spin resonance analysis suggested that·O 2 - and·OH were the key active species for TC oxidation while e - dominated Cu (II) reduction. Based on the identified TC degradation intermediates, two possible degradation pathways for TC were proposed, and the ecotoxicity of most intermediates were less than TC. This study can advance research development of designing efficient Z-scheme photocatalyst and elimination of complex pollutants.
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