CHEMOSPHERE
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2019
·
IF 5.108
Zifen Luo,Hongyi Chen,Shichuan Wu,Cao Yang,Jianhua Cheng
Aluminum-based metal-organic framework/sodium alginate-chitosan (Al-MOF/SA-CS) composite beads were synthesized and employed as an adsorbent for the removal of bisphenol A (BPA). Several methods, including X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscope (SEM), nitrogen adsorption-desorption isotherms and X-ray photoelectron spectroscopy (XPS), were used to characterize the prepared adsorbents. Results demonstrated that the introduction of CS could change the porosity of the beads and the obtained Al-MOF/SA-CS composite beads possessed higher surface area and total pore volume comparing with the beads without CS. Batch experiments were carried out to explore the adsorption performance and the results displayed that the enhanced adsorption capacity was achieved by Al-MOF/SA-CS beads compared to the Al-MOF/SA ones. It is also found from the fitting results that the adsorption process fitted well with the pseudo-second-order kinetics model and followed the Freundlich isotherm model. Importantly, the composite beads could be easily recycled and regenerated by methanol and the adsorption efficiency still maintained as high as 96% even after five cycles. Furthermore, it can be inferred from the experimental results that the π-π stacking, hydrogen bonding and cation-π interaction could be the primary adsorption mechanisms. Considering the high adsorption properties, good water stability, especially easy separation, and excellent recyclability , Al-MOF/SA-CS composite beads could be a promising adsorbent for the removal of BPA from contaminated water .
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2019
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IF 2.931
Xianmei Piao,Zhongrui Liu,Yangyang Li,Dahong Yao,Liwen Sun,Baihui Wang,Yan Ma,Libo Wang,Yan Zhang
Bisphenol A (BPA) as a chemical raw material, is widely used in the manufacturing process of daily necessities. It was reported that BPA could induce oxidative stress , and catalase (CAT) can protect the body from oxidative stress. In this paper, the effect of BPA on CAT was carried out in vitro and in vivo. Firstly, we studied the effects of BPA on oxidative stress, cell viability and CAT activity in human hepatocytes, and the results of vitro experiments show that the survival rate of hepatocytes significant decreased along with the increase of BPA concentration. And when the BPA concentration was 100 μM, the hepatocyte survival decreased by 13.2%, ROS levels in the cells increased by 85%. However, the activity of intracellular CAT increased with the increasing concentration of BPA in 24 h. The results of vivo experiments showed that the activity of CAT in the high-dose group decreased by 29.1% compared with the control group. The long-term effects of BPA on rats reduced the CAT activity in liver, which reduced the resistance to oxidative stress. Meanwhile, the interaction mechanism between BPA and CAT at the molecule level was performed via multiple spectra methods and molecular docking, and the results illustrated that the structural change of CAT is mainly due to the strong combination of BPA with the residues of Trp185. In addition, the interaction mechanism between BPA and CAT were hydrophobic and electrostatic effect. This study provided experimental evidence for better understanding the toxicity of BPA.
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JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
Gang Chu,Jing Zhao,Yang Liu,Di Lang,Min Wu,Bo Pan,Christian E.W. Steinberg
Biochar, a carbon-rich material, has attracted immense attention owing to its applications in soil remediation. However, the mechanisms by which heterogeneous carbon structures of biochars immobilize organic contaminants are not yet fully understood. In this study, the noncondensed aromatic components in biochars were selectively removed through bleaching. Different techniques, such as 13 C nuclear magnetic resonance, were applied to characterize the biochar compositions, and thus the role of the different carbon structures in organic contaminant sorption was discussed. The aromatic carbon structures in biochars were gradually developed and evolved from noncondensed to condensed structure with increasing pyrolytic temperatures from 300 to 700 °C. Based on elemental analysis, the carbon removed by bleaching decreased from 43.9% to 5.92% with increasing temperatures. After the surface area normalization of the apparent sorption, bleaching increased the sorption of carbamazepine and bisphenol A on biochars produced at 500 °C, but not for those produced at 300 and 700 °C. Bleaching removed noncondensed aromatics and enriched condensed aromatics, which resulted in increased sorption. However, bleaching also resulted in the blockage of micropores in biochars with abundant condensed aromatics, causing decreased sorption. The apparent sorption was determined by the balancing of these two opposite effects.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2019
·
IF 5.589
Aijiao Zhou,Wangwei Chen,Lei Liao,Pengchao Xie,Tian C. Zhang,Xumeng Wu,Xiaonan Feng
The magnetic poly( N -isopropylacrylamide)/chitosan hydrogel with interpenetrating network (IPN) structure was designed based on the functional groups of targeted emerging contaminants , represented by hydrophilic sulfamethoxazole (SMZ) and hydrophobic bisphenol A (BPA). The average particle size, specific surface area, and total pore volume of the hydrogel were turned out to be 103.7 μm, 60.70 m 2 /g and 0.0672 cm 3 /g, respectively. Adsorption results indicated that the maximum adsorption capacity occurred at the pH where SMZ was anionic and BPA was uncharged. When the adsorption temperature increased from 25 °C to 35 °C, the amount of adsorbed SMZ hardly changed, but that of BPA increased by two times. The adsorption capacity of the binary system (i.e., with both SMZ and BPA) was almost the same as that of the single system, indicating that simultaneous adsorption of SMZ and BPA was achieved. The adsorption equilibrium was reached quickly (within 5 min) for both SMZ and BPA. For adsorption isotherm, the Freundlich model fitted well for SMZ at 25, 35 and 45 °C. However, the adsorption of BPA exhibited the sigmoidally shaped isotherm at 25 °C with the Slips model fitting well, and both the Freundlich isotherm and the Slips isotherm fitted the data well at 35 °C and 45 °C, suggesting that the adsorption force was initially weak but greatly enhanced with an increase in adsorbate concentration or ambient temperature. The main adsorption mechanism was inferred to be electrostatic interactions for SMZ, and hydrophobic interactions as well as hydrogen bonding for BPA. The hydrogel adsorbent maintained favorable adsorption capacity for BPA after five adsorption-desorption cycles. These findings may provide a strategy for designing high performance adsorbents that can remove both hydrophilic and hydrophobic organic contaminants in the aquatic environment.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Xin Li,Pengfei Lv,Yixin Yao,Quan Feng,Alfred Mensah,Dawei Li,Qufu Wei
Enzymatic biofuel cell (EBFC) uses enzymes to convert the chemical energy of renewable biofuels into electrical energy, which shows great promise in the continuous power supply of implantable devices. Meanwhile, integrating carbon nanotubes (CNTs) with high conductivity and superior structural properties of bacterial cellulose (BC) as backbone to construct CNTs-BC based nanocomposites has proven to be an effective strategy. Herein, a highly flexible electrode of amidoxime-modified BC (AOBC)/carboxylated multi-walled CNTs (c-MWCNTs) were prepared by vacuum filtration with excellent laccase (LAC) immobilization. Subsequently, we developed a novel EBFC that intramolecular electron transfer was achieved by an alternative pathway for generating electricity within a single enzyme molecule of LAC. Sufficient power was efficiently extracted from unconventional fuels in single-LAC biofuel cells, including persistent pollutants (e.g., bisphenol A, hydroquinone and pyrocatechol). The open circuit voltage generated by EBFC was 0.14 V and the power density reached 1.897 W m −3 . This novel single-enzymatic biofuel cell exhibited a potential for recycling of waste water as fuel.
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POLYMER COMPOSITES
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2019
·Vol. 41
·期 1
·134-141
·
IF 2.268
Mehdi Derradji,Abdeldjalil Zegaoui,Aboubakr Medjahed,Wenbin Liu,Abdelkhalek Henniche
Phthalonitrile resins as one of the leading high performance polymers are currently used in highly exigent applications. Herein, aiming to achieve the best combination of mechanical, thermal, and nuclear shielding performances, we prepared hybrid materials based on the typical phthalonitrile resin and the silane surface modified chopped carbon fibers and tungsten carbide nanoparticles. The obtained results suggested that a synergistic combination between the three constituent was clearly achieved leading to excellent mechanical and gamma rays shielding properties. For instance, the tensile and bending strengths reached up to 505 and 584 MPa for the composite containing 20 and 30 wt% of carbon fibers and tungsten carbide nanoparticles, respectively. Similarly, the gamma rays screening ratio also reached the exceptional value of 39% for the same 2 cm thick hybrid. Finally, the as such described hybrid materials proved that a multi-approach strategy is often the best solution to achieve the requirements of highly exigent applications.
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WATER AIR AND SOIL POLLUTION
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2019
·Vol. 230
·期 6
·1-9
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IF 1.774
Pu Hongbin,Huang Zhibin,Sun Da-Wen,Xie Xiaohui,Zhou Weibiao
Pollution of environmental endocrine disruptors has caused increasing concern globally. In the current study, a simple colorimetric method with high sensitivity and good selectivity for 17β-estradiol (E2) detection was developed, which employed gold nanoparticles (AuNPs) as colorimetric probe for specific recognition of shortening DNA aptamer. Visible color change from bright red to violet was observed for aggregation of AuNPs without the protection of DNA aptamer. After optimization, the method exhibited great performance for E2 detection with good linearity between E2 concentrations from 0.2 to 5 nM and the absorbance ratio at 620 and 523 nm, with the limit of detection of 0.1 nM. The method was also successfully applied to E2 determination in different spiked water samples including fishpond water, lake water, and tap water, in which good recoveries from 93.1 to 108.9% and acceptable relative standard deviations from 3.4 to 8.9% were obtained. This technique showed great potential for on-site fast determination of E2 in environmental water samples.
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Nanomaterials
·
2019
·Vol. 9
·期 3
·402
·
IF 4.034
Hongyu Wang,Chaohai Wang,Junwen Qi,Yubo Yan,Ming Zhang,Xin Yan,Xiuyun Sun,Lianjun Wang,Jiansheng Li
Prussian blue and its analogues (PBA) based nanomaterials have been widely applied to removing pollutants in the recent years. However, easy aggregation and poor recycling largely limit their practical applications. In this work, spiderweb-like Fe-Co Prussian blue analogue/polyacrylonitrile (FCPBA/PAN) nanofibers were prepared by electrospinning and applied to degrading bisphenol-A (BPA) by activating peroxymonosulfate (PMS). Detailed characterization demonstrated that a high loading of FCPBA (86% of FCPBA in FCPBA/PAN) was successfully fixed on the PAN nanofibers. 67% of BPA was removed within 240 min when 500 mg·L−1PMS and 233 mg·L−1FCPBA/PAN were introduced in 20 mg·L−1BPA solution at initial pH of 2.8. Electron paramagnetic resonance (EPR) and radical inhibition experiments were performed to identify the possible degradation mechanism. For comparison, a low loading of FCPBA nanofibers (0.6FCPBA/PAN nanofibers, 43% of FCPBA in FCPBA/PAN) were also prepared and tested the catalytic performance. The results showed that the activity of FCPBA/PAN was much higher than 0.6FCPBA/PAN. Furthermore, a FCPBA/PAN packed column was made as a reactor to demonstrate the reusability and stability of FCPBA/PAN nanofibers, which also exhibited the bright future for the industrial application. This work makes it possible to fabricate efficient PBA nanocatalysts with excellent recyclability and promotes the application of PBA in industrial areas.Keywords:Fe-Co Prussian blue analogues;electrospinning;peroxymonosulfate;BPA
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Liying Wu,Yongbo Yu,Qian Zhang,Junming Hong,Ji Wang,Yuecheng She
Through direct and indirect radical mechanism of peroxymonosulfate (PMS) activation, novel CoFe 2 O 4−x catalysts were successfully developed via hydrogen calcination to overcome popular disadvantages of the dependence on pH. Bisphenol A (BPA) was selected as the model pollutant to decipher the mechanism of catalysts for peroxymonosulfate (PMS) activation. Possible degradation pathways of Bisphenol A were proposed via analysis of liquid chromatograph mass spectrometer (LC-MS). The findings indicated that catalytic activation of CoFe 2 O 4−x was not dependent upon the initial pH, as the direct and indirect radicals seemed to be generated in parallel. FTIR analysis confirmed that surface hydroxyl groups were actively involved in the activation of PMS under alkaline conditions. During the reaction, the oxygen defects promoted electron transfer and participated in the redox cycle from Co 3+ /Fe 3+ to Co 2+ /Fe 2+ to generate 1 O 2 and O 2 − . Hydroxyl (OH ) and sulfate (SO 4 − ) radicals were generated on the surface of CoFe 2 O 4−x by the synergistic interactions among oxygen defects, transition metal, and surface hydroxyl groups. To the best of our knowledge, this combined mechanism of direct and indirect radical generation for advanced oxidation was a first-attempt study to be disclosed in public domain.
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JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
Xiaolin Zhu,Guanlan Wu,Yi Xing,Chengzhi Wang,Xing Yuan,Baikun Li
Bisphenol analogues have been developed as alternatives to bisphenol A (BPA), a common chemical with potential adverse effects on human health. It is imperative to perform a fast and sensitive evaluation for the toxicity of these bisphenol analogues. This study introduces a label-free electrochemical biosensor based on a screen-printed electrode modified with the carboxylated multi-walled carbon nanotube/rhodamine B/gold nanoparticle. Ctenopharyngodon idella kidney (CIK) cells were used as the biological recognition agent to detect changes in electrochemical signals and indicate the cell viability. Only 20 μL of sample was required for detection, which was much lower than that of other conventional electrochemical methods (≥ 1 mL). This biosensor was examined for the cytotoxicity of BPA, bisphenol AF (BPAF), bisphenol B (BPB), bisphenol F (BPF), and bisphenol S (BPS) to CIK cells. The half inhibition concentration (IC 50 ) values after 48 h of exposure indicated that the rank order of cytotoxicities was BPAF > BPB > BPA > BPF > BPS. The morphological changes in CIK cells after treatment with various bisphenols were investigated, and the combined toxicities of the binary bisphenol mixtures were determined. Potentially synergistic and additive effects were observed. These findings provide new insights into the cytotoxicity of bisphenol analogues.
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ENVIRONMENT INTERNATIONAL
·
2019
·
IF 7.943
Min Sun,Yu Zhang,Hui-Hui Liu,Feng Zhang,Lin-Feng Zhai,Shaobin Wang
Oxygen (O 2 ) in air is an eco-friendly and economical oxidant. However, its activation is an energy-intensive process requiring high operation temperature. Herein, we report the synthesis of nanoscaled Co-CoO on a graphite felt (GF) as an anode material for electrocatalytic wet air oxidation (ECWAO) of water contaminants at room temperature. Such an ECWAO process shows extensive effectiveness in mineralizing a variety of biorefractory organic pollutants. A probe pollutant, bisphenol A (BPA), is rapidly degraded in 180 min with mineralization efficiencies higher than 85% over a wide pH range from 3.0 to 11.0. The Co-CoO/GF electrode exhibits excellent stability in the ECWAO process, without loss of activity and leaching of metal. The ECWAO process is confirmed to be initiated by the electrochemical activation of O 2 through a non-radical pathway. The CoO on the surface of Co nanoparticle is identified as the catalytically active site, at which O 2 molecules are first converted to chemisorbed oxygen species and then electrochemically oxidized to their activated states. The ECWAO process with the Co-CoO/GF electrode presents the merits of high efficiency, low energy input and environmental friendliness, and has a great potential for practical wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xiaojie Qiu,Shengjiong Yang,Mawuli Dzakpasu,Xiaoping Li,Dahu Ding,Pengkang Jin,Rongzhi Chen,Qionghua Zhang,Xiaochang C. Wang
Mn 0.8 Fe 2.2 O 4 magnetic nanocrystals (Mn 0.8 Fe 2.2 O 4 MNCs) are synthesized by thermal treatment of a metal-organic framework (MOF) template, and their physicochemical properties are characterized in detail. The Mn 0.8 Fe 2.2 O 4 MNCs exhibited highly efficient performance for the catalytic degradation of Bisphenol A (BPA) by peroxymonosulfate (PMS) activation at various initial pH, catalyst dosage, and PMS concentration. A leaching solution experiment evidenced that PMS activation by the Mn 0.8 Fe 2.2 O 4 MNCs is a heterogeneous process. Interestingly, scavenging experiments and electron paramagnetic resonance (EPR) analysis demonstrated that HO is the dominant radical for BPA degradation, rather than SO 4 − . The scavenger experiment indicated that the surface-bound radicals may play the crucial role for BPA degradation. Increasing Cl − or decreasing bicarbonate concentrations in solution enhanced the catalytic degradation process significantly through non-radical pathways. The Mn 0.8 Fe 2.2 O 4 MNCs exhibited desirable stability and reusability, that the spent Mn 0.8 Fe 2.2 O 4 MNCs could be significantly regenerated by thermal treatment at 450 °C in open air. Findings from this study would expand the applications of MOFs and also provide new insights into the enhancement of degradation efficiency during PMS activation processes.
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