MACROMOLECULES
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2020
·
IF 5.918
Fan Zhang,Tiantian Li,Wanting Chen,Xiaoming Yan,Xuemei Wu,Xiaobin Jiang,Yang Zhang,Xiaozhou Wang,Gaohong He
As critical triggers, both the electron-withdrawing links and neighboring cationic groups induce and accelerate the aryl ether cleavage in the widely used aryl ether containing anion exchange membranes (AEMs). Herein, a novel alkaline stable polyelectrolyte is proposed by converting the electron-withdrawing C═O links in the widely used poly(aryl ether ketone) backbone into the electron-donating C–NH2 links, and then grafting faraway para-type cations by Leuckart-Menshutkin reaction without using noble metal catalysts. Contributions of the elimination of electron-withdrawing C═O links and graft of para-type cations to the excellent alkaline stability of the aryl ether containing polyelectrolytes are demonstrated through density functional theory, as the increasing electron cloud density on the ether-connected carbon atom elevates the activation energy barrier to OH– initiated aryl ether cleavage, and the para-type cation is more stable than the conventional ortho-type cation due to the sterical protection and low electrophilicity to benzylic carbon. By converting C═O to C–NH2 groups and then tuning the quaternization degree, the remaining C–NH2 groups in the polymer backbone could form hydrogen bonding networks to reinforce the membranes. The novel quaternized poly(aryl ether amine) membrane exhibits high conductivity (92.2 mS cm–1 at 80 °C), excellent mechanical properties (48.2 MPa, 51.3%), and suppressed swelling ratio (12.8% at 80 °C). Excellent alkaline stability is also confirmed experimentally with no polymer backbone degradation even in harsh conditions (4 M KOH, 80 °C, 400 h), which is at the top level among the state-of-the-art side chain and aryl ether-free types of AEMs.
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ENVIRONMENT INTERNATIONAL
·
2020
·
IF 7.577
Miaoling Lin,Rui Hua,Jing Ma,Yao Zhou,Pei Li,Xiya Xu,Zhiqiang Yu,Song Quan
Background Bisphenol A (BPA) is a widespread endocrine-disrupting chemical with estrogen like effects, which could interfere with the human reproductive system by disrupting the normal function of granulosa cells (GCs) leading to abnormal ovarian function. However, the mechanism of its toxicity on human GCs has not been clearly described thus far. Methods 106 normogonadotropic infertile women undergoing their first in-vitro fertilization-embryo transfer (IVF-ET) cycle were recruited. Urinary BPA level and the early outcomes of IVF-ET were analysed. Patients were divided to low and high BPA exposure groups using the median urinary BPA concentration as the cut-off value. In-vivo and in-vitro studies were conducted using mice and human granulosa cell line (KGN cells). Female Kunming mice approximately 6–8 weeks of age were poisoned with BPA at different dosages (1, 10 or 100 μg/kg) by oral gavage once daily for 2 weeks, while KGN cells were exposed to BPA at the concentration of 1, 10 or 100 nM for 24 h, 48 h or 72 h. BPA-induced ovarian morphologic changes were analysed by histopathology investigation. Cell viability and apoptosis were evaluated using CCK-8, TUNEL and flowcytometric, respectively. Hormone levels were determined using ELISA and the molecular mechanism studies were conducted using immunofluorescence, RT-PCR and western blots. Results The oocyte retrieval rate, maturation rate and embryo implantation rate significantly decreased with the higher level of urinary BPA concentration. Peak E2 level was lower in high BPA group, but no statistical significance could be observed. In BPA treated mice, cystic dilation of the follicles with a decreased number of GCs could be observed histopathologically. Decreased E2, P4 and AMH level and GCs autophagy could be detected both in-vivo and in-vitro with the activation of AMPK/mTOR/ULK1 signalling pathway. As being confirmed in KGN cells, phosphorylated AMPK and ULK1 increased while phosphorylated mTOR decreased, and by inhibition autophagy using knockdown of AMPK or 3-MA, adverse effects of BPA exposure in-vitro could be reversed. Conclusion BPA exposure might abnormally influence human ovarian functions leading to abnormal folliculogenesis by activation of autophagy in GCs through AMPK/mTOR/ULK1 pathway.
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FOOD CHEMISTRY
·
2020
·
IF 6.306
Min Jia,Shuang Chen,Tingting Shi,Chunyang Li,Yanping Wang,Hongyan Zhang
A plasmonic biomimetic enzyme-linked immunosorbent assay (PBELISA) method was developed for ultrasensitive and on-site visual detection of bisphenol A (BPA). The PBELISA was an enzyme-linked immunoassay using molecularly imprinted polymer (MIP) film as biomimetic antibody combined with catalase (CAT)-mediated growth of plasmonic gold nanoparticles (AuNPs). With the BPA concentration increased, a distinguished color change was observed from colorless to blue and then red. Therefore, the proposed method could be employed with naked-eye observation to detect BPA with visual limit of detection (LOD) of 40 pg/mL. For quantitative analysis, this method also exhibited a good dynamic linear response to the logarithmic BPA concentrations ranged from 10 pg/mL to 1.024 × 10 4 pg/mL with a correlation coefficient of R 2 = 0.9922 and LOD of 6.20 pg/mL. The recovery rates in tap water, milk and orange juice ranged from 91.83% to 107.39%. In brief, the developed PBELISA method is sensitive, cost-effective and easy-to-use for BPA detection.
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高影响因子
Journal of Water Process Engineering
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2020
·
IF 3.465
Zhuang Lin,Wenlei Qin,Lei Sun,Xiangjuan Yuan,Dongsheng Xia
The degradation of Bisphenol A (BPA) in the vacuum ultraviolet/ ultraviolet/ peroxymonosulfate (VUV/UV/PMS) process based on a mini-fluidic VUV/UV photoreaction system has been comprehensively investigated focusing on the degradation performances and kinetics in this study. With 20 min reaction at pH 7.0 in VUV/UV/PMS process, the removal efficiency and the apparent degradation rate constant ( k app ) of BPA were > 95.2 % and 0.145 min −1 (R 2 = 0.9935). In addition, the impacts of operational parameters and co-existing constituents on BPA degradation are systematically evaluated. Importantly, the effective degradation of BPA (> 96.1 % at least) achieved at the test pH conditions (5–11) after 30 min reaction and achieved the highest BPA removal rate at pH = 11 (0.243 min −1 , R 2 = 0.9952). The electron paramagnetic resonance and radical scavenger experiments confirmed that both hydroxyl radical ( OH) and sulfate radical (SO 4 − ) are the predominant reactive radicals in VUV/UV/PMS process. The second-order reaction rate constants of BPA with OH and SO 4 − under different pH conditions were determined to be 0.74–1.86 × 10 10 M −1 s −1 and 2.92–5.01 × 10 9 M −1 s −1 via the competition kinetics. Meanwhile, the relative contribution rate of OH decreased from 97.2 %–33.1 % with the increasement of pH from 5.0 to 11.0, while the relative contribution rate of SO 4 − rose from 1.7 % to 48.9 %. The present study demonstrated that the VUV/UV/PMS process, as a new advanced oxidation process, has potential applications for micropollutants removal in water.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Jingjing He,Yu Wan,Wenjun Zhou
Developing high-efficient hybrids carbon catalysts for PMS-based advanced oxidation process (AOPs) are crucial in the field of environmental remediation. In this work, novel carbon nanocubes (xFe‒N‒C) with three-dimensional porous structure and abundant well-dispersed FeN x sites were obtained via a skillful cage-encapsulated-precursor pyrolysis strategy. The as-synthesized xFe‒N‒C exhibited superb activity for phenol degradation by activating peroxymonosulfate (PMS). Besides, the catalytic system not only possessed good recycling performance, wide pH adaptation and relatively low activation energy, but also had high resistance to environmental interference. Singlet oxygen ( 1 O 2 ) dominated non-radical process was responsible for phenol degradation rather than traditional radical pathways. Impressively, the doping level of Fe could regulate FeN x contents in catalysts, and the catalytic activity of xFe‒N‒C was greatly enhanced with increasing FeN x contents. Based on density functional theory calculations (DFT), the introduction of FeN x sites regulated the electronic structure of catalysts. Such electron-deficient Fe center acted as electron acceptor to receive electrons transmitted by the adsorbed PMS , thus generating highly reactive 1 O 2 for rapid phenol oxidation. This work provides a new insight into the innovation in transition metal-nitrogen hybrid carbon catalysts and highlights the pivotal roles of FeN x sites in 1 O 2 generation during PMS activation process.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Xiaohong He,Kun Jia,Yun Bai,Zhongyuan Chen,Yiyao Liu,Yumin Huang,Xiaobo Liu
Simultaneous detection of multiple heavy metal ions (HMI) is of great importance for the environmental monitoring, and the analytical tools based on multiband emissive fluorescent probes have been regarded as one of the most promising candidate for multiple HMI detection. Herein, the rod-coil amphiphilic block copolymer (BCP) with intrinsic blue fluorescence emission has been synthesized and subsequently employed to encapsulate two types of hydrophobic quantum dots (QD) with green and red fluorescence emission via the three dimensionally confined emulsion self-assembly, leading to the generation of white-emitting superparticles showing good colloidal stability and stable aqueous phase fluorescence. Furthermore, it was found that the fluorescence emission intensity of obtained superparticles can be selectively quenched by Ag + , Hg 2+ , Cu 2+ and Fe 3+ ions via different mechanisms, and the four metal ions can be further discriminated according to their distinct combinational quenching effects onto three fluorescent bands of white-emitting superparticles. In addition, an analytical model was built to enable the simultaneous detection of Cu 2+ , Hg 2+ and Fe 3+ in the real sample. Basically, the current work opens the new way to fabricate fluorescent probes with multiple emission bands, which can be easily adapted to prepare more complicated QD encoded fluorescent probes for high throughput detection.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Xiaoye Geng,Yan Gao,Ning Wang,Na Han,Xingxiang Zhang,Wei Li
In this study, a series of reversible thermochromic MicroPCMs (RT-MPCMs) were synthetized through encapsulating ternary thermochromic mixtures via in-situ polymerization, and presented outstanding stable light-to-thermal conversion capability (η = 86.9%), excellent latent thermal energy storage-release performance (ΔH m = 171.9 J·g −1 , ΔH c = 171.4 J·g −1 ) and color-changing monitoring the states of energy storage or release, satisfactory thermal reliability and thermal cyclic durability. The RT-MPCMs with spherical integrity, smooth surface morphology and obvious core-shell microstructure were obtained by emulsifying with the solution (1.2 wt%–3.1 wt%) of sodium salt of styrene maleic anhydride copolymer. The crystallization of RT-MPCMs was mainly affected by the structure of methyl stearate (MeS). The crystallization changes and coloration inside capsules was observed real-timely via microscope at different temperature ranging from 1 to 40 °C. In addition, based on these excellent performances, the actual application value of RT-MPCMs was further discussed. The narrow-disperse composite macrocapsules containing RT-MPCMs was prepared and further encapsulated by real non-woven fabrics substrate for the intelligent adjustment-based garment to research practical value in thermoregulation field. The experimental results show that it can absorb the latent thermal energy from the skin or environmental heat, which is beneficial for keeping constant and comfortable body surface temperature, and showing great application value in the fields of temperature regulation and thermal management.
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JOURNAL OF MEMBRANE SCIENCE
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2020
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IF 7.183
Songxue Wang,Jiayu Tian,Linran Jia,Jialin Jia,Sujie Shan,Qiao Wang,Fuyi Cui
CuO catalyst dispersed in the feed water (CDF) and CuO catalyst immobilized on the ceramic hollow fiber membrane (CIM) for peroxymonosulfate (PMS) activation were developed and employed in the submerged membrane filtration systems for drinking water treatment , respectively. The performance of the CDF and CIM systems was systematically investigated and compared. The result indicated that BPA concentration, PMS dosage and CuO content exerted much less influence on BPA degradation in the CIM system as compared with that in the CDF system. The CIM system exhibited a greater advantage in the performance of BPA degradation and TOC removal when treating a large volume of feed (>300 mL). In addition, the effect of actual water matrix on the two systems was evaluated. The CIM system showed higher resistance to the adverse influence and better anti-fouling performance than the CDF system. The comparative study on the performance of CDF and CIM systems provides meaningful information for developing the process of membrane filtration coupled with PMS oxidation .
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Lanbo Bi,Zhonglin Chen,Linghan Li,Jing Kang,Shengxin Zhao,Binyuan Wang,Pengwei Yan,Yabin Li,Xiaoxiao Zhang,Jimin Shen
In the paper, molecularly imprinted TiO 2 was prepared by surface molecularly imprinted technology and liquid phase deposition method for preferential removal of persistent toxic pollutants from complex environmental water. Diclofenac was selected as the template molecule and target for photodegradation study. The characterization results of SEM , TEM, FTIR and XRD showed that the TiO 2 film with imprinted diclofenac was successfully synthesized on the surface of TiO 2 particles. Meanwhile, the adsorption and photodegradation experiments also indicated that the molecularly imprinted TiO 2 had larger adsorption capacity, better selectivity and higher photodegradation performance for diclofenac than non-imprinted TiO 2 . The primary active species and degradation pathways during photodegradation process were also elucidated according to radical capture experiments and UPLC-MS-TOF technology. The prepared molecularly imprinted TiO 2 has the advantages of efficient removal ability, high stability and environmental protection, so it has a wide application value in water treatment and water environmental restoration, especially when involved persistent toxic pollutants.
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AUSTRALIAN JOURNAL OF CHEMISTRY
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2020
·Vol. 74
·期 4
·261-267
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IF 1.073
Chaoqiang Pan,Jianmin Qiu,Lumei Wang,Zhiyu Yan,Weiwen Huang,Dongwei Zhang,Xuejia Zhan,Guoqing Shen,Chaoqiang Pan,Jianmin Qiu,Lumei Wang,Zhiyu Yan,Weiwen Huang,Dongwei Zhang,Xuejia Zhan,Guoqing Shen
This paper proposes a colorimetric aptasensor for the detection of testosterone (TES) in environmental water, using TES-specific aptamer (apT5) as a sensing probe, gold nanoparticles (AuNPs) as indicator, and hexadecyltrimethylammonium bromide (CTAB) as inducer, respectively. Based on competition between TES and CTAB for apT5, the aptamer can form an aptamer–TES complex, leaving CTAB free to aggregate AuNPs in the presence of TES. Dispersed and aggregated AuNPs have different absorption wavelengths and the signal of absorption intensity is associated with the concentration of TES, so TES can be detected quantitatively based on the signal absorption intensity. This sensitive aptasensor for TES detection has a wide linear range (R = 0.998) from 1.91–800 nM and a limit of detection (LOD) of 1.91 nM. In addition, this aptasensor has high selectivity over some interferents. The method detects TES in tap water samples with recoveries in the range of 98.9–102.6 % (RSD ≤ 7.35 %). This biosensor presents a good and potential application to rapidly detect TES in actual environmental water samples.
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MACROMOLECULES
·
2020
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IF 5.918
Ziqin Li,Jing Guo,Jifu Zheng,Tauqir A. Sherazi,Shenghai Li,Suobo Zhang
A novel microporous anion exchange membrane containing a spirobiindane segment and cardo moiety is successfully synthesized through superacid-catalyzed Friedel–Crafts-type polymerization. The developed polymer showed good solubility in common polar aprotic solvent and exhibited excellent ionic conductivity (163 mS cm–1 at 80 °C). A series of poly(spirobiindane-aryl ether sulfone) copolymers P(SBI/AES)-X with variable SBI/AES molar ratios were synthesized, and each copolymer exposed different free volumes that increases by increasing the content of spirobiindane in the copolymers. In turn, this free volume of copolymer causes the construction of well-developed ion channels in the developed anion exchange membranes (AEMs). The resulting QP(SBI/AES)-0.5 AEM, with an ion exchange capacity (IEC) of 1.59 mmol g–1, exhibited a high hydroxide conductivity of 110 mS cm–1 at 80 °C as well as good mechanical robustness. The peak power density achieved using a single cell fuel cell test is 593 mW cm–2. The results depicted the excellent potential of the resultant microporous anion exchange membrane in the progress of anion exchange membrane fuel cells.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Hao Guo,Zijun Min,Ying Hao,Xu Wang,Jinchen Fan,Penghui Shi,Yulin Min,Qunjie Xu
Increasing demand and waste of lithium-ion batteries (LIBs) has adversely affected resources and the environment. Multistage utilization of spent LIBs is essential to their sustainable development. Here, we propose a simple recycling method of LiCoO 2 cathode scrap, based on the first use of the cathode scrap as a catalyst to degrade organic pollutants via peroxymonosulfate activation , and subsequent recovery of valuable metals from the used catalyst. Compared with pristine LiCoO 2 , the LiCoO 2 cathode scrap exhibits excellent catalytic performance due to the active sites generated, such as the vacancy generation and electronic structure modulation by the degradation of LiCoO 2 during the continuous lithiation and delithiation processes. The removal efficiency of cathode scrap to the o -phenylphenol exceeds 98% within 60 min, and the degradation efficiency is still above 95% after the 10th use because its unique sandwich and porous structure ensure the stability and recyclability . After multiple catalytic reactions, due to the generation of crack, the separation of the sandwich structure, and further degradation of active materials, the leaching efficiency of transition metals from the cathode scrap in deep eutectic solvent is promoted. 86% of lithium and 95% of cobalt are leached from the used catalyst respectively. This study provides a promising strategy for the sustainable development of LIBs and promotes the utilization of spent LIBs in multiaspect.
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