Nano Research
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2020
·Vol. 14
·期 7
·2383-2389
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IF 8.183
Zhang Yuwei,Liu Fei,Yang Zhichao,Qian Jieshu,Pan Bingcai
In the pursuit of heterogeneous catalysts with high reactivity, metal organic framework (MOF) nanomaterials have received tremendous attentions. However, many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature, because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules. Here, we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel (GA), generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use. Compared to MIL-101-Fe, GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in Fenton-like reaction, attributing to smaller MIL-101-Fe particle size, presence of active Fe(II) sites, and abundant defects in GA. Strikingly, the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature, by resisting the entrance of water molecules and helping to exclude water molecules. This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component, but also overcome its intrinsic drawback by taking advantage of the properties of host. We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Dapeng Liu,Yongliang Chen,Toan Trong Tran,Ganwei Zhang
Non-polyamide (non-PA) thin-film composite nanofiltration (TFC-NF) membranes have received tremendous attention in recent years, but their development is strongly hindered by the complicated fabrication process and the trade-off between permeability and selectivity. Here, we report a highly perm-selective non-PA TFC-NF membrane through 2-minute rapid assembly of tannic acid (TA) on hydrolyzed polyacrylonitrile (PAN) substrate via Fe 3+ intermediated regulation and coordination. The optimized membrane with a molecular weight cut off of ~390 Da showed high rejections for salts in a sequence of Na 2 SO 4 (90.2%) > MgSO 4 (83.4%) > NaCl (50.0%) > MgCl 2 (35.2%) and desirable rejections for organic pollutants (e.g. >99.0% dyes, 92.2% streptomycin and 81.8% chloramphenicol) while maintaining a pure water permeability of as high as 13.6 L·m −2 ·h −1 ·bar −1 , which clearly outperforms the reported non-PA membranes. In addition, the assembled TFC membrane showed excellent antifouling performance and reasonable structural stability against operation pressure and solution alkalinity. These results are highly promising and indicate a great potential for the membrane to be used in practical nanofiltration application, e.g. water purification and wastewater reclamation. Our work outlines the production of novel high-performance non-PA membrane with a fast fabrication process in a green chemistry context.
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RSC Advances
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2020
·Vol. 10
·期 72
·44551-44570
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IF 3.119
Yirui Shu,Pan Zhang,Yanjun Zhong,Xiangyang Xu,Genkuan Ren,Wei Wang,Hengli Xiang,Zhiye Zhang,Xiushan Yang,Xinlong Wang
A new low-cost composite of ZnCoxFe2−xO4 loaded on rice hull carbon (ZnCoxFe2−xO4-RHC) was synthesized via waste ferrous sulfate (the industrial waste produced in the process of producing titanium dioxide) and rice hull as raw materials, which was applied for the degradation of bisphenol A (BPA) by heterogeneous activated peroxodisulfate (PS). A series of characterizations including XRD, SEM, FTIR, and BET analysis were carried out to analyze the structure and morphology of the materials. It is confirmed that the ZnCoxFe2−xO4-RHC composites show better catalytic activity and performance than other control samples, which can be attributed to the synergistic effect of Fe and Co, ZnCoxFe2−xO4 and RHC based on these analyses. The degradation rate of BPA by ZnCo1.3Fe0.7O4-50%RHC reached 100% within 15 min, and it can still maintain good catalytic efficiency after 5 cycles. ESR test and XPS results showed that free radical and non-free radical processes were involved in BPA degradation. These findings offer a novel, low cost and simple strategy for rational design and modulation of catalysts for the industrial degradation of organic pollutants, and provide a new idea for the utilization of waste ferrous sulphate in titanium dioxide industry.
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ACS Applied Bio Materials
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2020
·
IF 0
Xunyuan Jiang,Yitong Yao,Weiming Tang,Dongmei Han,Li Zhang,Ke Zhao,Shuanjin Wang,Yuezhong Meng
Metal-based implants possess excellent mechanical strength, corrosion resistance, and biocompatibility and can deliver favorable performances in clinic treatments. However, modulus mismatching is considered a common defect for metal-based materials, while polymer-based materials with a bonelike elastic modulus have been regarded as one of the most promising candidates for bone replacement implants. In this work, a phosphonic acid- and fluorine-containing poly(aryl ether) (PAE) resin is designed and synthesized, which is determined to be an amorphous polymer with excellent thermostability. The elastic modulus of composites is improved to 15.7 GPa by reinforcing with 60 wt % hydroxyapatite (HA), which demonstrates admirable protein adsorption and hydrophilicity. After 14 days of immersion in simulated body fluid, a layer of HA deposition can be observed, indicating favorable bioactivity in advance, and the preliminary in vitro cell experiments also suggest that PAE-HA composites possess favorable cell responses on adhesion, proliferation, and differentiation, which reveal the feasibility of synthesized polymers to be employed as bone replacement materials, while the adjustability in molecular chains also leaves room for further investigations.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Yongfeng Mu,Han Feng,Shengdao Wang,Shuling Zhang,Jiashuang Luan,Mei Zhang,Zhenxiang Yu,Guibin Wang
Ultrafiltration (UF) membranes blended with hydrophilic nanomaterials usually exhibit preferable overall performance including the membrane permeability and antifouling capability. However, the improvement in antifouling performance may be not outstanding due to the small amount of nanomaterial distributed near the membrane surface and the limited improvement in membrane hydrophilicity. Notably, excess addition of nanomaterials may lead to the decline in membrane permeability. In order to solve the above problem, we integrated the strategy of blending and surface modification to construct novel hybrid UF membranes. Novel nanohybrid was prepared via tannic acid (TA) coating on hydroxyapatite nanotubes (HANTs) and the subsequent grafting of zwitterionic polyethylenimine (ZPEI). The prepared nanohybrid (HANTs@TA-ZPEI) was incorporated with the polysulfone containing tertiary amine groups to fabricate hybrid membranes via the solution blending and the subsequent immersion-precipitation phase inversion process. Then the matrix was modified with zwitterions via the reaction of tertiary amine group with 1, 3-propane sultone. UF tests were conducted using the bovine serum albumin (BSA) and humic acid (HA) as the representative foulants. Results showed that both the permeability and the antifouling performance of the membranes achieved favorable promotion. Thereinto, the water flux of M-B0.4-Z membrane (pre blended with 0.4 wt% HANTs@TA-ZPEI in the casting solution and post-surface modified) exhibited 2.6 times that of the pristine membrane and the flux recovery ratio (FRR) for BSA and HA attained 93.4% and 96.1%, respectively. By the combination of blending and surface modification, both the membrane permeability and fouling resistant properties could attain remarkable promotion, which exerted the advantages of two methods and made up the deficiency of single blending method.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2020
·Vol. 413
·期 2
·389-401
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IF 3.637
Lu Yi Chen,Xiao Wei Wei,Wang Jun Yun,Xiong Xiao Hui
Because of its widespread distribution in the environment, bisphenol A (BPA) has become a global concern as an endocrine disruptor and a threat to human health through the food chain. Thus an efficient determination method is urgently needed for monitoring the levels of BPA. Herein, a novel electrochemical technique for the detection of BPA was performed by synchronous extraction and pre-concentration of BPA onto magnetic molecularly imprinted polymer (BMMIP), with subsequent readout on a magneto-actuated glassy carbon electrode (MGCE) by differential pulse voltammetry. Compared to the current methods of BPA determination, this BMMIP-based electrochemical sensor (BMMIPs@MGCE) not only simplifies the sample handling procedures substantially, without filtration, centrifugation, or other complex operations, but also can be easily renewed by a controllable magnetic field. As a sensor component, the core–shell BMMIPs exhibited excellent binding capacity (Q e = 82.5 mg g −1 ), short adsorption equilibrium time (30 s), and outstanding selectivity (k′ = 7.239) towards BPA, as well as stability and recyclability. Importantly, the BMMIPs@MGCE sensor was successfully applied for the on-site monitoring and rapid detection of BPA in complicated real-world specimens, with good recoveries (81.31–119.77%) and a low limit of detection (0.133 μmol L −1 ). Therefore, the stable and low-cost BMMIPs@MGCE sensor provides a new approach for the rapid determination of BPA in the field of environmental control and food safety.
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JOURNAL OF MOLECULAR LIQUIDS
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2020
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IF 5.065
Lijun You,Ke Xu,Guanjun Ding,Xinming Shi,Jumei Li,Shaoyun Wang,Jiabin Wang
Magnetic covalent organic framework modified by Fe 3 O 4 nanoparticles (Fe 3 O 4 @COF) were facile synthesized and used as adsorbent for the adsorption of bisphenols from aqueous solutions. The Fe 3 O 4 @COF is synthesized by catalyst-free Schiff base reaction of melamine and terephthalaldehyde, and synthesis strategy is flexible and controllable. The as prepared Fe 3 O 4 @COF was characterized by TEM , PXRD , TGA and BET analysis. The Fe 3 O 4 @COF possessed large specific surface area (335.2 m 2 /g), high chemical and thermal stability, and high saturation magnetization (49.6 emu/g), which in favor of rapid magnetic separation and efficient adsorption in the adsorption process. The effects of temperature, adsorbent dosage, pH and salt concentration on the adsorption of bisphenols (BPA and BPAF) were studied. The as-prepared adsorbent showed an excellent adsorption ability for BPA and BPAF , and the max adsorption capacity of BPA and BPAF could reach 140 and 290.4 mg/g. The adsorption kinetic fitted the pseudo-second-order kinetic model and the adsorption isotherm followed the Freundlich isotherm equation. Moreover, the Fe 3 O 4 @COF presented favorable re-use performance, which kept over 81.4% removal efficiency of bisphenols after five consecutive recycles. The high adsorption performance and reusability make the Fe 3 O 4 @COF a promising adsorbent for the removal of bisphenols.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Shi-Wen Lv,Jing-Min Liu,Ning Zhao,Chun-Yang Li,Fei-Er Yang,Zhi-Hao Wang,Shuo Wang
Photocatalysis is a promising strategy to remove contaminants from wastewater. Herein, a novel g-C 3 N 4 @CoFe 2 O 4 /Fe 2 O 3 composite was synthesized via a feasible hydrothermal and calcination method. Benefiting from the Z-scheme heterojunction formed between MOF-derived CoFe 2 O 4 /Fe 2 O 3 and g-C 3 N 4 , the recombination of photoinduced electrons and holes could be inhibited effectively. Meanwhile, doping a little amount of MOF-derived CoFe 2 O 4 /Fe 2 O 3 could remarkably enhance visible light absorption ability of g-C 3 N 4 and reduce band gap of g-C 3 N 4 . Then, the resulting hybrid photocatalysts were employed as a high-efficient mediator to activate persulfate for degrading emergent organic contaminants under visible light irradiation. Significantly, TC of 99.7%, BPA of 98.1%, SMX of 94.8%, DFC of 97.0%, IBP of 96.1% and OFX of 96.5% could be removed within 80 min. Some important factors influencing photocatalytic degradation process were also investigated. The trapping experiments and EPR tests revealed that both SO 4 − and OH were involved in photocatalytic reaction. Besides, the introduction of MOF-derived CoFe 2 O 4 /Fe 2 O 3 provided a new approach for generating radical species. More importantly, obtained g-C 3 N 4 @CoFe 2 O 4 /Fe 2 O 3 -2 composites with good stability exhibited great application potential in the actual degradation tests. To sum up, current work provided novel ideas for photocatalytic oxidation technology in the organic pollution degradation.
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CRYSTAL GROWTH & DESIGN
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2020
·
IF 4.089
Jin-Xia Yang,Xin Zhang,Ye-Yan Qin,Yuan-Gen Yao
A 2D network of {[Zn(Hbcpt)(H2O)3]·7H2O} (1) was hydrothermally synthesized and structurally characterized. By employing different N-donor ligands into the system of 3,5-bis(4′-carboxyl-phenyl)-1,2,4-triazole (H3bcpt) and Zn(II) cations, six novel entangled coordination polymers, namely, {[Zn2(bcpt)(μ2-OH)(H2O)]·(py)·4H2O} (2), {[Zn2(Hbcpt)2(bpa)2]·2H2O} (3), {[Zn(Hbcpt)(bpp)]·[Zn(Hbcpt)(bpp)]·2.5H2O} (4), {[Zn5(bcpt)2(biimpy)2(μ2-OH)4]·5H2O} (5), {[Zn2(bcpt)(bib)(μ2-OH)]·H2O} (6), and {[Zn2(bcpt)(bix)4(μ2-OH)]·3H2O} (7) (H3bcpt = 3,5-bis(4′-carboxyl-phenyl)-1,2,4-triazole, bpa = 1,2-bis(4-pyridyl)ethane, bpp = 1,3-bi(4-pyridyl)propane, biimpy = 2,6-bis(imidazole-1-yl)pyridine, bib = 1,4-bis(N-imidazolyl)butane, bix = 1,4-bis(imidazol-1-ylmethyl)-benzene, py = pyridine), were obtained. Single-crystal X-ray diffraction analysis reveals that, with the different N-donor ligands, the resulting compounds present entangled structures with different topologies. Compound 1 shows a 2D (4, 4) network, and the adjacent sheets are extended into a 3D supramolecular framework via hydrogen-bonding interactions. Interesting, by introducing a series of ditopic N-donor ligands into the reaction system, compounds 2–7 with entangled structures were harvested. Compound 2 exhibits a 3D self-penetrating network with an 8-connected bcu topology. Compound 3 features an 8-fold dia network showing an unusual [4 + 4] mode of interpenetration. Compound 4 is comprised of two parts of undulated 2D 44-sql networks, and the adjacent undulated layers are parallel interpenetrated to each other to give a 2D → 3D polycatenated framework. Compound 5 presents an unusual 3D self-penetrating network with a novel 4,6,6-connected trinodal network with the point symbol of (32·4·52·6)(32·4·56·66}{32·56·66·7}. Compound 6 shows a 2-fold interpenetrating 3D architecture with 6-connected sxd topology. Compound 7 displays an unprecedented self-penetration derived from abnormal [3 + 2] 5-fold interpenetrating dia subnets. Structural diversity of these compounds suggests that different N-donor ligands can induce the organic ligand to present different conformations and coordination modes, and the influence on the final structures. Furthermore, the luminescent properties of compounds 1–7 have been investigated in the solid state.
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CHEMOSPHERE
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2020
·
IF 5.778
Xiaoqi Li,Xiaofan Liu,Zhenzhen Jia,Tian Wang,Hongyan Zhang
Vitellogenin (VTG) is typically produced by females but when present in males can indicate contamination with estrogenic endocrine-disrupting chemicals (EDCs). Here we used primary hepatocytes isolated from male crucian carp uncontaminated with estrogenic EDCs as a culture model. Nine EDCs were used for validation, and an enzyme-linked immunosorbent assay (ELISA) was used to quantify VTG production by primary hepatocytes. The lower limit of detection of 17β-E2, DES, and HES using the method was 10 −12 M. Fresh pork was roasted, and non-hydrolytic acetonitrile-vortexing was used to extract potential estrogenic EDCs. The extracted substances were separated by thin-layer chromatography (TLC), and dimethyl terephthalate present in roast pork was found to induce high VTG concentrations. Therefore, the detection of VTG by ELISA provides a sensitive and reliable method for detecting known and unknown estrogenic EDCs in food products.
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TALANTA
·
2020
·
IF 5.339
Weiwei Ma,Shuangfeng Wan,Chenchen Lin,Xucong Lin,Zenghong Xie
Highly specific sample pretreatment for the sensitive detection of trace bisphenol A (BPA) in compliacted samples is critical. Herein, a new protocol towards online specific recognition and sensitive detection of BPA was proposed by using [email protected] affinity monolith coupled with LC-MS. Optimization of polymerization conditions and characterization such as the morphology, energy spectrum, mechanical stability, aptamer coverage density and specific performance of the affinity monolith were studied. Nano-gold particles (AuNPs) densely distributed on the rigid hybrid-silica substrates, and an unusually high aptamer coverage density reached 3388 pmol/μL, which was favorable to fulfill the effective identification of BPA with high selectivity and inhibit the interference of analogs including BPB and BPC. A highly sensitive recognition of BPA was obtained with the limit of detection (LOD) as low as 0.02 ng/mL. Applied to dairy milk products and serum samples, trace BPA could be sensitive detected by this strategy, while the poor response was achieved by using traditional non-specific SPE column for sample pretreatment. Satisfactory recoveries of fortified BPA were measured as 97.45 ± 2.24%–98.03 ± 4.36% (n = 3) in powdered infant formulas, 96.64 ± 3.37% ~ 99.42 ± 3.22% (n = 3) in bottled milk, 94.69 ± 2.15% ~ 100.96 ± 1.94% (n = 3) in boxed milk, and 93.71 ± 1.53% ~ 96.73 ± 2.56% (n = 3) in children serum samples, respectively. This protocol lights a new access to online specific identification of trace BPA from complex matrix with good detection sensitivity by using aptamer-affinity monolithic column.
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FOOD CHEMISTRY
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2020
·
IF 6.306
Huihuang Xiong,Lan Guo,Xuejin Mao,Ting Tan,Hao Wan,Yiqun Wan
A magnetic hydrophilic molecularly imprinted material (MIM) with multiple stimuli-responses was prepared for efficient recognition of bisphenol A (BPA). MIM consisted of a magnetic core, an inner silica dioxide shell and an outer hydrophilic polymer shell, responsive for rapid magnetic separation, protection of the magnetic core and pH-/thermo-sensitivity to BPA, respectively. Controlled adsorption and release of BPA by pH/temperature regulation were realized through the reversible components of poly[N-isopropylacrylamide- co -2-(dimethylamino)ethyl methacrylate (NIPAM-DMAEMA)] (PND). The resultant MIM possessed superior affinity, selectivity and kinetics to BPA in aqueous solution. MIM was successfully applied to detect BPA in beverages via dispersive solid-phase extraction (d-SPE) coupled with high performance liquid chromatography (HPLC), exhibiting satisfactory recoveries of 80.70–108.18% with relative standard deviations (RSD) below 6.08%. The limit of detection of BPA was obtained as low as 3.75 nmol/L. The versatile MIM could be a promising alternative for extraction/removal of BPA in complicated samples by multiple-stimuli regulations.
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