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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Performance of constructed wetlands and associated mechanisms of PAHs removal with mussels

Yan Kang,Huijun Xie,Bo Li,Jian Zhang,Huu Hao Ngo,Wenshan Guo,Zizhang Guo,Qiang Kong,Shuang Liang,Jie Liu,Tingting Cheng,Liwei Zhang

The role of mussels in laboratory-scale constructed wetlands (CWs) where wastewater was contaminated with five typical polycyclic aromatic hydrocarbons (PAHs) (three 3-ring PAHs and two 4-ring PAHs) was investigated in this study. The CWs performance and PAHs removal mechanisms were well studied. Results indicated that these five PAHs improved removal efficiencies of NO 3 -N but in the case of NH 4 -N accumulation occurred. Of the five added PAHs, the 4-ring PAHs were more refractory with higher concentrations in effluent than 3-ring PAHs. By monitoring the five PAHs concentration in water, mussels had excellent removal efficiency of the five PAHs (97%). According to the mass balance calculation, mussels promoted plant uptake of five PAHs, contributing 15.2% of five PAHs removal in CWs. The PAHs could also accumulate in mussels through ingested substrate. Thus, mussels presented a positive correlation with five PAHs purification at a depth of 0–10 cm in substrate, which was 34.7 μg/kg lower than the control group. Due to the purification and enhanced aerated degradation, mussels performed better in removing 3-ring PAHs in substrate, decreasing 8.3% for 3-ring PAHs compared to the control. A positive correlation between five PAHs addition and nirS , nrfA genes was observed. However, PAHs showed negative impact on nitrifying bacteria ( amoA ). The significant correlations between mussels and five PAHs made it possible to improve CWs for PAHs treatment with aquatic faunas.

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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Removal of acetaminophen in the Fe2+/persulfate system: Kinetic model and degradation pathways

Songlin Wang,Junfeng Wu,Xiuqing Lu,Wenxin Xu,Qing Gong,Jiaqi Ding,Bingsong Dan,Pengchao Xie

In this study, the removal of acetaminophen (ACT) in the Fe 2+ /persulfate system has been comprehensively evaluated. A kinetic model has been established based on the principal reactions. Good accordance between the experimental data and the predicted results under different operational conditions including molar ratio of Fe 2+ to persulfate, initial pH, initial ACT concentration, the presence of chloride, under natural water matrices and the mixture of ACT, amoxicillin and pyridine, evidences the validity of the proposed kinetic model. The rate constants for ACT reacting with SO 4 − and HO were determined as (1.80 ± 0.17) × 10 9  M −1  s −1 and (3.26 ± 0.41) × 10 9  M −1  s −1 , respectively. SO 4 − was evidenced to be the primary radical accounting for ACT removal through both kinetic model calculation and the scavenging results, using either methanol or tert -butyl alcohol. The optimum molar ratio of Fe 2+ to persulfate for ACT removal was determined to be 5:4. The removal rate of ACT was little affected by initial pH due to the rapid decrease of solution pH caused by the hydrolysis of iron ions. Cl − has a dual effect on the removal of ACT, and Cl 2 − rather than SO 4 − is proposed as the dominant radical for ACT removal at 10.0 mM Cl − . Possible degradation pathways are also proposed based on the detected intermediates.

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Royal Society Open Science · 2018 ·Vol. 5 ·期 12 · IF 2.504

Synthesis and investigation of physico-chemical properties of dicationic ionic liquids

Yi-Xin Sun,Ying-Ying Wang,Bing-Bing Shen,Bi-Xian Zhang,Xiao-Mei Hu

A series of dicationic ionic liquids (ILs) including [C4(MIM)2][PF6]2, [C5(MIM)2][PF6]2, [C6(MIM)2][PF6]2 and [C4(PYR)2][PF6]2 were synthesized. Their thermal stability and melting points were analysed. It was found that dicationic ILs presented important implications in the design of homogeneous and heterogeneous system with water. A homogeneous system of dicationic ILs with water could be formed at a relatively high temperature and then a heterogeneous system was formed when the solution was cooled to a low temperature. The ILs recovered by altering the temperature were obtained in high percentage yields of [C4(MIM)2][PF6]2 (97.6%), [C5(MIM)2][PF6]2 (97.3%), [C6(MIM)2][PF6]2 (98.0%) and [C4(PYR)2][PF6]2 (94.2%). On the other hand, [C4(MIM)2][PF6]2 and [C5(MIM)2][PF6]2 exhibited good solubility in acetonitrile and acetone. A homogeneous system could be achieved with imidazolium-based ILs with a relatively low amount of water and acetonitrile at room temperature. All of the properties of dicationic ILs have a strong correlation with the nature of dications, the linkage chain and the symmetry of dications. Dicationic ILs may provide a new opportunity for some specific applications in order to enable the effective separation and isolation of products.

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BIORESOURCE TECHNOLOGY · 2019 · IF 6.669

Catalytic fast pyrolysis of corn cob in ammonia with Ga/HZSM-5 catalyst for selective production of acetonitrile

Xin Zhang,Ziguo Yuan,Qian Yao,Ying Zhang,Yao Fu

In this work, corn cob was used as raw material to selectively produce acetonitrile via catalytic fast pyrolysis (CFP) in ammonia over Ga/HZSM-5 catalyst. A series of catalysts with different catalyst carriers (including HZSM-5, USY, MCM-41, HY, and γ-Al 2 O 3 ) and active metals (including Fe, Co, Ni, Cu, Zn, Cr, Ca, Mg and Ga) were prepared and screened. The reaction conditions, such as temperature, ammonia flow rate and residence time were changed to investigate the effect on the product distribution and acetonitrile production. The results indicated that with the desired catalyst (2% Ga/HZSM-5) and optimal reaction conditions (Temperature 700 °C; ammonia flow rate 80 ml/min; residence time 2.4 s), the highest carbon yield of acetonitrile from corn cob with a value of 18.4% could be obtained, and the carbon selectivity in bio-oil was 83.5%. This study provides an economical and environmental-friendly method for the direct production of acetonitrile from abundant biomass.

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JOURNAL OF MATERIALS SCIENCE · 2019 ·Vol. 54 ·期 20 ·13298-13313 · IF 3.442

Nitrophenyl-engaged photocleavage of an amphiphilic copolymer for spatiotemporally controlled drug release

Zhang Liuwei,Qian Ming,Wang Jingyun,Xia Jing,Cui Hongyan,Chen Qixian

Photo-responsive nitrophenyl moieties were proposed to conjugate as pendants of the pullulan backbone through labile carbamate linkage to yield amphiphilic pullulan derivatives. Note that the hydrophobicity of the conjugated nitrophenyl components in the amphiphiles enable facile their self-assembly with the hydrophobic chemotherapeutic drug (doxorubicin) as the internal drug reservoirs, whereas the hydrophilic pullulan segments existed as the biocompatible surroundings. Upon photo-illumination, the carbamate linkage was susceptible to cleavage for departure of the nitrophenyl components from the pullulan backbone owing to the photo-responsive nitrophenyl moieties. Simultaneously, the nitrophenyl components transformed into water-soluble aldehyde-terminalized nitrosophenyl derivatives, leadingly accounting for structural disassembly and liberation of the cytotoxic doxorubicin payloads. Therefore, our proposed photo-responsive strategy could address the reluctant intracellular drug release drawbacks of the conventional amphiphile-based drug delivery systems. Notably, markedly lower IC 50 (half maximal inhibitory concentration) index of our constructed doxorubicin delivery systems was determined to be approximately 1.0 μg/mL upon photo-illumination, in contrast to IC 50 index of 5.6 μg/mL in the absence of photo-illumination (approximate fivefold), thereby representing as a facile spatiotemporal artifice to execute on-demand drug release to the photo-imposed cells.

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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Tumor-Specific Expansion of Oxidative Stress by Glutathione Depletion and Use of a Fenton Nanoagent for Enhanced Chemodynamic Therapy

Qiufang Chen,Jun Zhou,Zhe Chen,Qing Luo,Jian Xu,Guanbin Song

Amplifying intracellular oxidative stress effectively destroys cancer cells. In addition, iron-mediated Fenton reaction converts endogenous H2O2 to produce hypertoxic hydroxyl radical (•OH), resulting in irreversible oxidative damage to combat tumor cells. This method is known as chemodynamic therapy (CDT). Overexpressed glutathione (GSH) in tumor cells efficiently scavenges •OH, significantly reducing the curative effects of CDT. To overcome this challenge and enhance intracellular oxidative stress, iron oxide nanocarriers loaded with β-lapachone (Lapa) drugs (Fe3O4-HSA@Lapa) were constructed and had both Fenton-like agents and GSH depletion properties to amplify intracellular oxidative stress. Release of Lapa selectively increases tumor site-specific generation of H2O2 via NAD(P)H: quinone oxidoreductase 1 (NQO1) catalysis. Subsequently, the iron ions released from the ionization of Fe3O4 in the acidic environment selectively convert H2O2 into highly toxic •OH by Fenton reaction, dramatically improving CDT with minimal systemic toxicity due to low NQO1 expression in normal tissues. Meanwhile, released Lapa consumes GSH in the tumor, amplifying oxidative stress and enhancing the efficacy of CDT. Designed Fe3O4-HSA@Lapa nanoparticles (NPs) exhibit perfect targeting capability, prolonged blood circulation, and increased tumor accumulation. Furthermore, Fe3O4-HSA@Lapa NPs effectively enhance the inhibition of tumor growth and reduce the side effects of anticancer drugs. This work establishes a remarkably enhanced tumor-selective CDT against NQO1-overexpressing tumors by significantly inducing intratumoral oxidative stress with minimal side effects.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

Using Green γ-Valerolactone/Water Solvent To Decrease Lignin Heterogeneity by Gradient Precipitation

Guanhua Wang,Xiaoqian Liu,Bo Yang,Chuanling Si,Ashak Mahmud Parvez,Jinmyung Jang,Yonghao Ni

Lignin heterogeneity, involving complex structure and high polydispersity, is a key challenge that restricts its value-added applications. Fractionation of heterogeneous lignin into several homogeneous subdivisions is an attractive and practical strategy to overcome this limitation. In this work, γ-valerolactone (GVL), a sugar-derived product, was used as a green solvent for lignin fractionation when mixed with water. The enzymatic hydrolysis lignin (EHL) was subdivided into three different fractions (F1, F2, and F3) by dissolving it completely in 60% aqueous GVL and then following gradient precipitation in 40%, 30%, and 5% aqueous GVL solutions, sequentially. Detailed characterization techniques were conducted to provide a comprehensive evaluation of the three obtained lignin fractions. Moreover, the proposed fractionation mechanism was further investigated on the basis of Kamlet–Taft parameters. The gel permeation chromatography (GPC) analyses showed that the three fractions presented lower polydispersity than the parent EHL and, furthermore, a gradual decreasing molecular weight due to the different solubility of various molecular weight lignins in aqueous GVL solvents. The structural analyses revealed that with the decrease of molecular weight, the guaiacyl unit content in lignin fractions decreased, with significant increases of functional groups (i.e., aromatic/aliphatic hydroxyl and carboxyl groups). The solvent recycling study showed that the aqueous GVL had a high recovery, and the recycled GVL had the same lignin fractionation performance as fresh GVL. Overall, compared with traditional fractionation using multiple organic solvents, the present work provides a green and efficient route to fractionate lignin and, therefore, significantly decreases its molecular weight polydispersity and structural heterogeneity.

CAS / MDL: 110-86-1
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Polymers · 2018 ·Vol. 10 ·期 11 ·1284 · IF 2.935

Isothermal Crystallization and Rheology Properties of Isotactic Polypropylene/Bacterial Cellulose Composite

Bo Wang,Fu-hua Lin,Xiang-yang Li,Zhong-wei Zhang,Xiao-rong Xue,Si-xiao Liu,Xu-ran Ji,Qian Yu,Zheng-qiu Yuan,Xin-de Chen,Jun Luo

Bacterial cellulose (BC) is a new kind of cellulose with great potential in enhancing preparation of isotactic Polypropylene (iPP) composites, which have been found with excellent performance. However, the interface compatibility between BC and iPP is poor. In this study, iPP/BC composites were prepared by solution mixing. Esterification modified BC (CO) and Maleic anhydride grafted polypropylene (MAPP) added as a compatibilizer was both used to improve the interfacial compatibility of the iPP/BC composites. The rheology and isothermal crystallization behavior of the composites was tested and discussed. The result shows that the complex viscosity and storage modulus of the composite significantly increase in the rule iPP, iPP/BC2, iPP/CO2, and M-iPP/BC3, which indicates that the compatibility of the composite increases as this rule. According to the isothermal crystallization kinetics result, the crystal growth mode of iPP was not affected by the addition of BC and the interfacial compatibility. The spherulite growth rate of the iPP/BC composite increases with increasing crystallization temperature. Especially, the value decreases as the same rule with the complex viscosity and storage modulus of the composite at the same isothermal crystallization temperature. These results suggest that the interface compatibility of iPP/BC composites is greatly improved and the interface compatibility of the M-iPP/BC3 is better than the iPP/CO2.Keywords:Isotactic polypropylene;bacterial cellulose;rheology;isothermal crystallization

CAS / MDL: 111-64-8 110-86-1
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JOURNAL OF APPLIED POLYMER SCIENCE · 2018 ·Vol. 136 ·期 15 ·47264 · IF 1.901

Electrochromism of novel triphenylamine-containing polyamide polymers

Fuhan Liu,Yaxin Zhang,Guang Yu,Yanjun Hou,Haijun Niu

A series of novel polymers (coded as BCT-1 to BCT-6 (BTC is block triphenylamine)) based on N 1 -(4-aminophenyl)- N 1 -phenyl benzene-1,4-diamine, pyridine-2,6-dicarboxylic acid, 4,4′-(phenyl azanediyl)dibenzoic acid (PDA), and different diamine compounds were synthesized successfully through a polymer condensation reaction. For comparison, model polymers, BCT–2,6-pyridine dicarboxylic acid (PA) and BCT–PDA, were synthesized as well. The electrochromic properties of the BCTs were determined via an electrochemical workstation and a UV–visible spectrophotometer. Through electrooxidation, the polymer films showed reversible redox processes and steady color changes. In a comparision of the electrochromic characteristics of the BCTs, almost all the novel polymer films showed a better electrochromism stability, a higher electrochromic coloration efficiency (CE), and a more rapid switching time than BCT–PA and BCT–PDA. Among these polymers, BCT-1 exhibited the highest CE of 266.7 cm 2 /C, and BCT-4 showed the most rapid switching time (color switching time = 3.08 s and bleaching time = 2.01 s). © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47264.

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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 43 ·21550-21557 · IF 9.931

Mesoporous carbon matrix confinement synthesis of ultrasmall WO3 nanocrystals for lithium ion batteries

Changyao Wang,Yujuan Zhao,Lili Zhou,Yang Liu,Wei Zhang,Zaiwang Zhao,Wael N. Hozzein,Hind M. S. Alharbi,Wei Li,Dongyuan Zhao

Transition metal oxides (TMOs)/carbon nanocomposites are promising for high capacity long life lithium ion batteries (LIBs). Herein, we report a mesoporous carbon matrix confinement growth strategy to synthesize ultrasmall WO3 nanocrystals for lithium storage. In this strategy, WCl6 and phenolic resins (resol) are co-assembled with amphiphilic diblock copolymer PEO-b-PS into ordered mesostructures through an evaporation induced self-assembly (EISA) process. During the pyrolysis process, the resol molecules can be polymerized and carbonized into amorphous mesoporous carbon matrices, which lock the amorphous W species well. Then, WO3 nanocrystals are formed and are uniformly distributed in the ordered mesoporous carbon matrix with the increased pyrolysis temperature; moreover, the particle size is well controlled to ∼3 nm under the confinement effect of the carbon matrices. The resultant ordered mesoporous carbon/WO3 composites show very large pore size (∼11.3 nm), high surface area (∼157 m2 g−1), high pore volume (∼0.25 cm3 g−1), and WO3 content of 84%. As an anode material for LIBs, the obtained composites show excellent cycling stability and rate performance. A high specific capacity of 440 mA h g−1 can be achieved after 100 cycles at a current density of 0.1 A g−1. We believe that such a confinement synthesis strategy is versatile to create TMO-based nanocomposites for outstanding LIBs.

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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2018 · IF 3.235

Three novel donor-acceptor type electrochromic polymers containing 2,3-bis(5-methylfuran-2-yl)thieno[3,4-b]pyrazine acceptor and different thiophene donors: Low-band-gap, neutral green-colored, fast-switching materials

Yan Zhang,Lingqian Kong,Hongmei Du,Jinsheng Zhao,Yu Xie

Three novel donor-accept type electrochromic polymers with very low band gap, namely PMFTTP, PMFBTTP and PMFMOTTP, were prepared via electrochemical polymerization , employing 2,3-bis(5-methylfuran-2-yl)thieno[3,4- b ]pyrazine as the acceptor units and thiophene , butylthiophen and methoxythiophen as the donor units, respectively. All the polymers were comparatively studied by cyclic voltammetry (CV), scanning electron micrographs (SEM), UV–vis-NIR spectroscopy and colorimetry . The results revealed that PMFTTP and PMFBTTP showed obvious color change from green color to brown in the oxidation process , while PMFMOTTP exhibited color change from brick red to dark gray. And the three polymers possessed very low optical band gaps in the following order: PMFTTP (1.23 eV) > PMFBTTP (0.88 eV) > PMFMOTTP (0.74 eV), which demonstrated the different election-donating ability of thiophene or its derivatives. The electrochromic kinetic investigations manifested that the polymers presented satisfactory optical contrasts (ΔT%) in the near infrared region (NIR), which were 35%, 67% and 60% for PMFTTP, PMFBTTP and PMFMOTTP, respectively. Moreover, the polymers also displayed short switching times (lower than 1 s at any wavelengths), high coloration efficiencies (around about 200 cm 2 /C) and outstanding robust stabilities, suggesting the probability of being the promising candidates for the electrochromic devices. In summary, the above positive results, especially the neutral green color and the very low band gap, had important theoretical significance for the application and development of electrochromic polymers.

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ACS Applied Bio Materials · 2018 · IF 0

Visible-Light-Responsive Surface Molecularly Imprinted Polymer for Acyclovir through Chicken Skin Tissue

Lantao Liu,Nan Li,Meijun Chen,Hailin Yang,Qian Tang,Chengbin Gong

The phototoxicity of UV light limits the application of conventional azobenzene-based photoresponsive molecularly imprinted polymers in the biomedical field. This paper reports a tetra-ortho-methoxy-substituted azobenzene, N-(4-((4-amino-2,6-dimethoxyphenyl)diazenyl)-3,5-dimethoxyphenyl)methacrylamide (ADDDM), whose photoswitching is induced by all visible-light irradiation (440 nm for trans form to cis form and 630 nm for cis form to trans form) in N,N-dimethylformamide and tetrahydrofuran (1:9, v/v). Using ADDDM as the monomer, a visible-light-responsive surface molecularly imprinted polymer (VSMIP) on silica microspheres was fabricated for acyclovir (ACV). VSMIP showed a higher drug loading capacity, better specificity, faster drug release rate, and faster photoisomerization rate constant to ACV than the corresponding visible-light-responsive surface molecularly nonimprinted polymer (VSNIP). The selectivity of VSMIP to ACV and competing materials (ganciclovir and triacetylganciclovir) was examined by ultraviolet–visible spectroscopy, and the VSMIP showed excellent specificity of recognition toward ACV. The VSMIP can realize a visible-light-triggered (440/630 nm) release and uptake of ACV through chicken skin tissue (1 mm in thickness).

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