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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Frontiers in Bioengineering and Biotechnology
·
2021
·
IF 5.89
Wang Yujie,Hu Kang,Yang Zhiyu,Ye Chenlu,Li Xin,Yan Kai
Bisphenol A (BPA) produced from biomass is a typical endocrine disrupting compound that is carcinogenic and genotoxic and can be accumulated in water due to its extensive use and difficult degradation. In this study, the porous ZnO photocatalyst with core-shell structure and large surface area was successfully developed for the efficient photocatalytic degradation of BPA. The various effects of calcination temperatures, BPA concentrations, ZnO dosages, pH and inorganic ions on the degradation performance were systemically studied. The results showed that 99% degradation of BPA was achieved in 1 h using the porous ZnO calcined at 550°C under the conditions of 30 mg/L BPA, 1 g/L ZnO, and pH of 6.5. Besides, the inhibition effects of anions for the photocatalytic removal of BPA decreased in the order of H2PO4- > HCO3- > SO42- > Cl−, while the cations K+, Ca2+, and Na+ had little effect on the photocatalytic degradation of BPA. The results of scavenging experiments showed that h+, ·O2-, and e− played the key role in the photocatalytic degradation process. Finally, the main pathways of BPA degradation were proposed based on ten intermediates found in the degradation process. This work may provide a good guideline to degrade various endocrine disrupting compounds in wastewater treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
·
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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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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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xin Li,Shengxiao Zhang,MingMing Zhang,Mingwu Yu,Hou Chen,Huawei Yang,Qiang Xu
A novel FeO X nanoparticles supported biomass activated carbon (BAC/FeO X ) composite was prepared through one-pot calcination method with FeCl 3 and cherry stone powder as precursors. The carbonization of biomass, reduction of Fe 3+ , and FeO X anchored on carbon substrate could be achieved at the same time. Characterization with transmission electron microscope (TEM) and scanning electron microscope indicated that nanoscale FeO X distributed uniformly on carbon substrate, and X-ray photoelectron spectroscopy, X-ray diffraction, and high resolution TEM characterization proved that the loaded FeO X was high crystallinity of Fe 3 O 4 and α-Fe 0 . Bisphenol A (BPA) was used to investigate the degradation performance of BAC/FeO X activating peroxydisulfate (PDS). The ratio of raw materials affected degradation efficiency of BPA intensively through the content, valence state, and dispersibility of FeO X nanoparticles, and the optimal material could degrade 20 mg/L BPA completely in 5 min at 0.1 g/L in the presence of 1 g/L PDS. Free radical determination and quenching experiments indicated that both SO 4 •− and •OH were involved in BPA degradation. The degradation pathway was proposed based on the identification of degradation intermediates. The facile synthesis method, high activation efficiency, and low-cost and environmental friendly raw materials made the BAC/FeO X -50 an alternative catalyst for organic pollution water treatment .
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MACROMOLECULES
·
2020
·
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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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
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.
Graphical abstract
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jun Wang,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Yuanzhi Zhu,Wenchao Peng
In this work, γ-Al2O3-supported CuO (c-CuO/Al2O3) materials are successfully synthesized using a novel impregnation–precipitation–decomposition method. The obtained c-CuO/Al2O3 catalyst shows excellent catalytic activities for bisphenol A (BPA) degradation with sodium persulfate (PDS) as an oxidant. Radical quenching tests and electron paramagnetic resonance (EPR) studies indicate that PDS activation is a combined mechanism involving both free radical and nonfree radical pathways. In a continuous large-scale degradation process, about 1.78 L of 20 ppm BPA can be completely removed within 480 min. Although c-CuO/Al2O3 can be deactivated after several reaction cycles, the catalytic activity can be regenerated after simple aerobic calcination. X-ray photoelectron spectroscopy (XPS) and Raman analysis confirm that the deactivation of c-CuO/Al2O3 should be attributed to the conversion of Cu(II) to Cu(I). The aerobic calcination could oxidize Cu(I) back to Cu(II), thus recovering the catalytic activity. In addition, the density functional technology (DFT) and temperature-programmed oxidation (TPD) results reveal that γ-Al2O3 can not only serve as a carrier to anchor the CuO particles but also can adsorb and activate PDS by introducing more basic sites on the surface. c-CuO/Al2O3 has high activity and can be regenerated easily, thus having great potential applications for wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Ningjie Du,Ying Liu,Qiuju Li,Wei Miao,Dandan Wang,Shun Mao
Single-atom catalysts have drawn increasing attention in advanced oxidation due to their unique structure and significant promise in heterogeneous catalysis. Herein, single-atom iron anchored on nitrogen-doped carbon (SAFe-N-C) was synthesized with iron phthalocyanine (FePc) and metal-organic framework (ZIF-8). With thermal treatment and acid leaching, atomically-dispersed Fe-N x sites were successfully formed on the surface of N-C support derived from ZIF-8. The prepared catalyst was demonstrated to activate peroxydisulfate (PDS) for chloramphenicol (CAP) degradation. Compared with N-C, the SAFe-N-C shows 6 times enhanced removal efficiency (from 15.3% to 93.1%) for CAP. Moreover, the catalyst shows high catalytic activity in a wide pH range of 5 to 9 and good resistance to inorganic anions, in which a singlet oxygen-dominated process is found. This study reveals the role of single-atom site in singlet oxygen evolution and offers a new catalytic approach for selective removal of organic pollutants in complex water matrix.
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MACROMOLECULES
·
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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CHEMOSPHERE
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2020
·
IF 5.778
Xiaoping Liao,Caixiang Zhang,Chao Nan,You Lv,Zenghui Fan,Lisong Hu
Manganese oxides (MnO 2 ), important environmental oxides, have drawn significant attention in areas such as detoxification of micro-hazardous organic contaminants with electron-donating functional groups such as –OH. However, studies on whether these oxidized processes might further impact the fate of some esters like organophosphorus pesticide (OPPs) remain poorly understood. Herein, we propose a new mechanism involved in the enhanced removal of methyl parathion in mixtures of MnO 2 and phenol. Specifically, the removal of methyl parathion (up to 73.7%) was significantly higher for a binary system than for MnO 2 alone (approximately 9.3%) and was primarily due to adsorption rather than degradation. The extent of methyl parathion adsorption was dependent significantly on pH, reactant loading and metal ion co-solutes (such as Ca 2+ , Mg 2+ , Fe 3+ and Mn 2+ ). Both spectroscopic (FT-IR, SEM-EDX and XPS) and chromatographic (LC/HRMS) analyses showed that the remarkable increase in the number of organics (e.g., polymers) onto the MnO 2 surface dominated methyl parathion adsorption via hydrogen bonding, n-π and π-π interactions, van der Waals forces and pore-diffusion. The results from this study provided evidence for the role of manganese oxides in adsorption of methyl parathion in soil-aquatic environments involving phenolic compounds .
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VIBRATIONAL SPECTROSCOPY
·
2021
·
IF 2.507
Lei Zhang,Yingshan Chen,Qin Zhu,Wenjin Ji,Suqing Zhao
Bisphenol A (BPA) is a typical endocrine-disrupting chemical (EDC), which has been banned for food packing and baby bottle material due to its potential endocrine harm to human body. In this paper, an easy and rapid immunochromatographic assay (ICA) combined with the technology of surface-enhanced Raman spectroscopy (SERS) was fabricated to improve the sensitivity and rapidity for quantitative determination of BPA. After 10 min of a quick chromatographic process, the specific Raman signal on T line of the test strip was measured. Compared with the traditional ICA, the SERS-ICA realized quantitative test and showed the limit of detection (LOD) was 0.1 ng/mL, getting approximately 300-fold lower. The method displayed high specificity and precision with RSD of 4.1%, and the test strip indicated favorable stability for two weeks without loss of activity. For river, tap and commercial drinking water sample, the SERS-ICA results were confirmed by HPLC, and the recoveries of spiked BPA were from 90.80-117.80%. It was shown that the proposed method takes advantages both of SERS and ICA, exhibiting high sensitivity, precision, stability, quantification and rapidity for field test, expecting a widely useful method for various small molecules in food safety, medical diagnosis and environmental samples.
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