DALTON TRANSACTIONS
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2018
·Vol. 47
·期 13
·4508-4517
·
IF 4.099
Hang Huo,Xianzhu Xu,Tingting Zhao,Yudong Li,Yanqiu Jiang,Kaifeng Lin
Hybrid molecularly imprinted mesoporous silicas were synthesized by co-condensation of tetraethoxysilane and functional organosilica precursors of HQP and BPAP, in which hydroquinone (HQ) and bisphenol A (BPA) were linked as imprinting molecules. Owing to the existence of a thermally reversible covalent bond of carbamate (–NH–COO–), the imprinting molecules could be eliminated under thermal treatment and molecularly imprinted cavities were formed in the framework wall. All of these materials were used to catalyze heterogeneous Knoevenagel reactions and proved to exhibit higher catalytic conversion and turnover frequency (TOF) number compared with the materials with imprinting molecules, which is attributed to the presence of amino groups with higher basicity and molecularly imprinted cavities. Importantly, compared with amino functionalized SBA-15 materials, the decisive role of molecularly imprinted cavities in the enhanced accessibility of amino groups in a mesoporous framework was further confirmed. Moreover, the size of imprinting molecules has an influence on the catalytic conversion and TOF values: imprinting molecules with relatively bulkier size tend to provide higher accessibility to the active sites. The amino groups in the framework are extremely stable during the reaction procedure and recycling process.
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高影响因子
TALANTA
·
2018
·
IF 4.244
Lei Chen,Yanting He,Zhixian Lei,Chenling Gao,Qing Xie,Ping Tong,Zian Lin
Core-shell structured magnetic covalent organic framework (Fe 3 O 4 @COF) nanocomposites were synthesized via a facile approach at room temperature and explored as an absorbent for magnetic solid-phase extraction (MSPE) of bisphenols (BPs) from human serum sample. The as-prepared Fe 3 O 4 @COF nanocomposites with core-shell structure possessed high specific surface area (181.36 m 2 /g), uniform mesoporous size (~ 3.6 nm), high saturation magnetization (42.7 emu/g), and excellent thermal and chemical stability, rendering it as an ideal adsorbent with high adsorption efficiency and size selectivity. The experimental parameters influencing extraction efficiency, including adsorbent dosage, extraction time, pH and ion strength, desorption solvent and time, were investigated in detail. Taking these advantages together, a simple, fast, effective and sensitive method that MPSE followed by HPLC-MS, was proposed to detect five BPs, which exhibited good linearity (r > 0.9982) within the concentration ranges of 0.1–50 μg/L. Moreover, the low detection limits (1.0–78.1 ng/L), signal-to-noise ratio (S/N = 3), the high enrichment factors (56–95 fold), and good recoveries (93.0–107.8%) with relative standard deviations (RSDs) less than 3.4% for inter-day and 6.9% for intra-day were achieved. The developed method was also successfully applied to the analysis of trace BPs in human serum sample, which demonstrated the most promising potential of the Fe 3 O 4 @COF nanocomposites as good adsorbent in sample pretreatment.
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高影响因子
CARBON
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2018
·
IF 7.082
Yanbin Wang,Man Liu,Xu Zhao,Di Cao,Tao Guo,Bo Yang
Sulfate radicals and/or hydroxyl radicals (SO 4 − ∙ or ∙OH) have been generally demonstrated as the primary oxidative species in the activation of peroxymonosulfate (PMS). Recently, the role of singlet oxygen ( 1 O 2 ) on the degradation of pollutants has attracted increasing research attention. In this study, boron-doped ordered mesoporous carbon (B-OMC) was prepared and used to activate PMS for the removal of bisphenol A (BPA). Compared with the pristine OMC, the catalytic activity of B-OMC was greatly increased, which resulted from the enhanced adsorption capacity for BPA and the increased catalytic activity for PMS activation. On the one hand, B doping promoted the BET surface area and pore size of OMC; on the other hand, Lewis acid sites were introduced on the surface of OMC and acted as catalytic sites for PMS activation. Influencing factors, such as PMS concentration, catalysts dosage, reaction temperature and initial pH, on the removal of BPA were investigated. Combining the results of radical quenching experiments with electron spin resonance , it was verified that superoxide radical (O 2 − ·) and 1 O 2 instead of SO 4 − ∙ and ∙OH were the dominated oxidative species in B-OMC-PMS system. Electrochemical analysis demonstrated that the boron doping benefited from the electron transfer from B-OMC to PMS.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2018
·
IF 5.667
Jing Zhang,Xiaojian Xu,Lu Chen
This work constructed an ultrasensitive electrochemical bisphenol A (BPA) sensor using hierarchical Ce-metal-organic framework (Ce-MOF) modified with cetyltrimethylammonium bromide (CTAB) as a sensing platform. Ce-MOF had been successfully prepared and conveniently modified with a cationic surfactant (CTAB) via the electrostatic interaction. Ce-MOF and CTAB/Ce-MOF were characterized by scanning electron microscopy, X-ray diffraction, infrared spectrum, thermogravimetric analysis and zeta potentials analysis. CTAB/Ce-MOF suspension was dropped onto glassy carbon electrode (GCE) surface to fabricate CTAB/Ce-MOF/GCE. Combined with preconcentration of BPA of the long alkane chain in CTAB via hydrophobic interaction and electrocatalytic activity of Ce-MOF, the dual amplification made CTAB/Ce-MOF/GCE exhibit high electrochemical response toward the oxidation of BPA, and an electrochemical BPA sensor was constructed based on CTAB/Ce-MOF/GCE by differential pulse voltammetry. The designed BPA sensor had a wide linear range from 0.005 to 50 μmol L −1 and a low detection limit of 2.0 nmol L −1 (S/N = 3). The proposed sensor had excellent reproducibility, stability and anti-interference, and was successfully employed for BPA detection in real samples. This convenient and sensitive sensor proved to be a promising and reliable tool for detecting BPA in food and environmental pollution.
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IONICS
·
2018
·Vol. 24
·期 10
·3053-3063
·
IF 2.347
Qaisrani Naeem Akhtar,Ma Yanjiao,Ma Lingling,Liu Jiafei,Gao Li,Li Lv,Gong Shoutao,Yan Xiaoming,Zhang Fengxiang,He Gaohong
A new type of composite anion-exchange membrane is fabricated using benzoxazine (Bz) monomer and polytetrafluoroethylene (PTFE) via a green and facile method. Membrane fabrication is achieved via in situ ring-opening polymerization of Bz within the PTFE matrix, followed by quaternization and ion-exchange reactions. The quaternized PBz works as a self-cross-linked and anion conductive polymer. The synthesized membranes show improved conductivity (26 to 70 mS/cm) at a reasonable water uptake and a low swelling ratio; they also show improved alkaline stability for 150 h at 60 °C in 1 M KOH solution, the decrease in conductivity being only ca. 10%. Our method of AEM fabrication is advantageous over conventional ones due to facile process and the avoidance of chloro- or bromomethylation as well as the self-cross-linked structure; the resulting membranes show relatively good performance as compared with some of those obtained from conventional techniques.
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高影响因子
ENVIRONMENTAL POLLUTION
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2018
·
IF 4.358
Lun Lu,Baoliang Chen
A high-efficient, low-cost, and practical biochar implementation method is desired to extend biochar's powerful adsorption performance for environmental remediation. This study presents novel results with advanced biochar application by integrating biochar with biofilter for the removal of bisphenol A (BPA) from stormwater . Biochars derived from wood dust (BC0) at different pyrolytic temperatures (300, 500, and 700 °C, referred as, BC300, BC500, and BC700, respectively) were characterized and investigated for their adsorption of BPA under different pH levels and humic acid (HA) concentrations by batch sorption and fixed-bed column experiments. Microcosm biofilters vegetated with phragmites australis and amended with different biochars were constructed and used for BPA removal under different hydraulic loading rates (HLRs). Compared with other biochars, BC700 showed a high adsorption rate and capacity due to high specific surface area and pore volume. As a consequence, fixed-bed columns amended with BC700 can remove BPA more efficiently than columns with BC0, BC300, and BC500 from synthetic stormwater, though the treatment performance was affected relatively by pH change and HA concentration. A high correlation ( r 2 = 0.899) between the breakthrough time and the product of adsorption rate ( k 2 ) and capacity ( Q max ) was found, which suggests that batch sorption experiments could be an efficient tool for prediction of breakthrough time. The BPA removal efficiency of microcosm biofilters amended with BC0, BC300, BC500 and BC700 for real stormwater containing 200 μg/L BPA at HLR of 40 cm/h averaged 4.1, 10.8, 80.3, and 98.4%, which were about 6, 15, 115, and 141 times, respectively, compared to bilfitlers without biochar amendment. Moreover, biochar amendment not only enhanced the BPA removal but also promoted phragmites australis growth, elevated nutrients and increased the E. coli removal efficiency. Hence, biochar-amended biofilters could be a promising approach for enhancing the elimination of endocrine-disrupting chemicals such as BPA from aqueous environments.
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高影响因子
ANALYTICA CHIMICA ACTA
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2018
·
IF 5.123
Kunhao Yang,Zhongqiu Li,Yueguang Lv,Chuyi Yu,Peilong Wang,Xiaoou Su,Li Wu,Yujian He
An electrochemical aptasensor for ultrasensitive detection of hydroxylated polychlorinated biphenyl (OH-PCB) was developed. In this work, the sulfydryl aptamer selected for OH-PCB was easily immobilized on the surface of the modified glassy carbon electrode via Au-S bond due to incorporation of gold nanoparticles/poly dimethyl diallyl ammonium chloride-graphene composite. The fabrication process of the electrochemical aptasensor was characterized by electrochemical impedance spectroscopy and cyclic voltammetry . The peak currents obtained by differential pulse voltammetry decreased with the increasing of OH-PCB concentrations. The current responded approximately logarithmically to the OH-PCB concentration ranging from 2.9 × 10 −11 M to 2.9 × 10 −7 M with excellent linear correlation performance. The detection limit of OH-PCB was estimated as low as 5.3 × 10 −12 M. The developed method had been successfully applied to analyzing lake water. Particularly, the method of the electrochemical aptasensor opens up a new perspective in environmental monitoring by the aptamer identification.
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TALANTA
·
2018
·
IF 4.244
Zhenzhen Fan,Lifang Fan,Shaomin Shuang,Chuan Dong
A facile and sensitive photoelectrochemical (PEC) sensing platform based on zinc phthalocyanine (ZnPc) sensitized TiO 2 nanorodarrays (NRAs) was successfully fabricated for detection of bisphenol A (BPA). The vertically aligned TiO 2 NRAs with one-dimensional (1D) nanostructure was synthesized in-situ on fluorine-doped tin oxide-coated glass (FTO) substrate by simple one-step hydrothermal method , and then the TiO 2 NRAs/FTO surface was covered with ZnPc. 1D nanostructure of TiO 2 NRAs could provide not only more spaces for the load of ZnPc, but direct pathways to reduce the recombination of electron-hole pairs, improving the photocatalytic efficiency. The combination of ZnPc with TiO 2 NRAs extended effectively the absorption of TiO 2 to visible region and improved greatly the charge transfer ability of TiO 2 NRAs. With the addition of BPA, BPA was oxidized by photogenerated holes during PEC reaction so that the photocurrent of the PEC sensing platform increased. BPA could be quantified by measuring the photocurrent change. The developed PEC sensor exhibited outstanding analytical performance with high sensitivity, excellent stability and good reproducibility. A wide linear work range from 0.047 to 52.1 μM was obtained with a low detection limit of 8.6 nM. Meanwhile, the sensor was also used to evaluate the level of BPA in plastic products and food.
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CHEMOSPHERE
·
2018
·
IF 4.427
Shanshan Yang,Pingxiao Wu,Quanyun Ye,Wen Li,Meiqing Chen,Nengwu Zhu
Novel Fe 0 -vermiculite (Fe-Ver-C-H 2 ) composite was synthesized by thermal reduction and acted as catalysts to remove bisphenol A (BPA) in photo-Fenton system. In term of activation ability toward H 2 O 2 , separation ability and stability, Fe-Ver-C-H 2 presented obvious advantages over other kinds of Fe 0 -vermiculite composite (Fe-Ver-NaBH 4 ), which obtained by traditional liquid reduction. The reason was that iron oxide shells on the surface of Fe 0 were α-Fe 2 O 3 and Fe 3 O 4 for Fe-Ver-NaBH 4 and Fe-Ver-C-H 2 , respectively. And for Fe-Ver-C-H 2 , the synergistic effect between iron core (Fe 0 ) and iron oxide shell (Fe 3 O 4 ) is beneficial to catalytic performance. The mechanism and plausible pathway of BPA degradation were also proposed according to the results of radical scavenger studies and gas chromatography-mass spectrometry (GC-MS), respectively. In addition, factorial effects for Fe-Ver-C-H 2 in photo-Fenton system were also investigated and optimized as: pH of 5, dosage of 0.2 g L −1 and H 2 O 2 concentration of 20 mM. This study presented a facile method to synthesize novel Fe 0 -vermiculite composite and provided a new sight to investigate the effect of iron oxide shell on the catalytic performance when Fe 0 -vermiculite composite acted as catalyst to remove contaminants from the environment in photo-Fenton system.
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高影响因子
HIGH PERFORMANCE POLYMERS
·
2018
·
IF 1.047
Yongjun Liu,Ming Zhong,Chen Song,Shouri Sheng,Xiaoling Liu,Haoqing Hou
Novel alternating poly(aryl ether ketone)s (PAEKs) were prepared from a multiple aromatic difluoroketone monomer, that is, containing six aromatic rings via nucleophilic substitution polycondensation with various bisphenols. Each chain segment of the synthesized poly aryl ether ketone alternating copolymer was regularly separated by bisphenol units, which resulted in improvements in their thermal stability and solubility in common organic solvents. All glass transition temperatures of the alternating PAEKs were above 179°C, and the temperatures at 5% weight loss were above 446°C under nitrogen atmosphere. Wide-angle X-ray diffraction patterns confirmed that the resulting PAEKs were amorphous. PAEKs can form strong, transparent, and flexible films by solution casting, with a tensile strength of 72–79 MPa, Young’s modulus of 1.5–2.0 GPa, and elongation at break of 7–17%.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2018
·
IF 6.434
Lingshuai Kong,Guodong Fang,Ya Kong,Meng Xie,Vinothkumar Natarajan,Dongmei Zhou,Jinhua Zhan
Wastewater systems contain a large number of compounds, such as anthropogenic aromatic pollutants and natural organic matter (NOM), and usually have pH higher than 4. Fenton-like reaction is the most widespread method for removal of organic pollutants, but their reactivity with H 2 O 2 may be inhibited by NOM due to the competition of hydroxyl radicals and chelating agents. In this work, Cu 2 O@β-cyclodextrin was developed to achieve the collaboration between molecular recognition and Fenton-like catalysis to destruct aromatic pollutants at neutral pH. In Cu 2 O@β-CD, covalent Cu O C bond was topotaxially converted from CuCl assisted by β-CD at room temperature. Covalently linked β-CD could keep humic acid from interfering catalytic performance of Cu 2 O surfaces and inhibit the leaching of copper. A higher catalytic ability was observed for Cu 2 O@β-CD with rate constant 0.0331 min −1 than Cu 2 O (0.0064 min −1 ) at neutral pH. A mechanism of synergistic catalysis was proposed on the basis of Cu + , β-CD and phenoxo-Cu 2+ complexes in the Cu 2 O@β-CD/BPA/H 2 O 2 system. The strategy of coupling molecular recognition into Fenton-like reaction provides an efficient and promising approach to the destruction of aromatic pollutants at neutral pH.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 9
·6770-6777
·
IF 3.201
Kai Luo,Shi-Xi Zhao,Yi-Feng Wang,Shu-Jin Zhao,Xi-Hui Zhang
Petal-like δ-MnO2 microspheres were successfully synthesized by a very simple hydrothermal method with potassium permanganate (KMnO4) as the only raw material. By adjusting the initial concentration of KMnO4 solution and the time of the hydrothermal reaction, the morphology and crystallinity of δ-MnO2 can be controlled. The synthesized δ-MnO2 microspheres were characterized by XRD, SEM, TEM, TG/DSC, BET, ICP-AES and XPS. The catalytic ozonation performance of δ-MnO2 prepared by a hydrothermal reaction at 160 °C for 24 h using 0.1 mol L−1 KMnO4 solution was tested. Its catalytic activity is excellent. The degradation efficiencies of bisphenol A and ibuprofen using 0.1 g L−1 δ-MnO2 as the catalyst were 68.2% and 68.5% in 20 min reaction time. The results were much better than those of individual ozone treatment and with commercial MnO2 as the catalyst. The formation of hydroxyl radicals was not the main reason for the rapid degradation of organic compounds in the catalytic reaction with δ-MnO2 as the catalyst. The strong interaction among the catalyst surface, ozone and organic molecules was the important reason for catalysis based on the related experimental results.
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