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Catalysis Science & Technology · 2018 ·Vol. 8 ·期 17 ·4463-4473 · IF 5.365

Polyoxometalate-based Gemini ionic catalysts for selective oxidation of benzyl alcohol with hydrogen peroxide in water

Pengbo Hao,Mingjie Zhang,Wei Zhang,Zhiyang Tang,Ni Luo,Rong Tan,Donghong Yin

Keggin-type phosphotungstic acid (H3PW12O40, HPW)-based di-imidazolium ionic liquid (IL) hybrids were prepared by exchanging the protons of HPW with PEG-bridged di-imidazolium cations in water. Characterization results suggested that intact Keggin-type [PW12O40]3− anions were incorporated with various PEG-modified di-imidazolium cations through ionic interaction, giving PW-based ionic catalysts with a Gemini structure. PEG-bridged di-imidazolium cations could not only fine-tune the redox properties of PW anions but also enhanced the compatibility of the catalyst in the aqueous system, which in turn improved its catalytic performance. Furthermore, combination of double catalytic sites into a single molecule enforced an intramolecular, cooperative reaction pathway resulting in a further enhanced reaction rate and higher selectivity in the selective oxidation of benzyl alcohol with H2O2 in water. More importantly, the di-imidazolium IL cations imparted a reaction controlled phase transfer function to the PW hybrids. The catalysts were thus precipitated from the aqueous system upon consumption of H2O2 and could be reused several times without loss of activity and selectivity.

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POLYMER DEGRADATION AND STABILITY · 2018 · IF 3.193

Synergistic effects of synthetic phosphonium sulfonates with expandable graphite on flame retardancy for EVA rubber blends

Shijie Hou,Yong Jian Zhang,Pingkai Jiang

Synergistic effects of synthetic phosphonium sulfonates (PhSs) bearing different groups with expandable graphite (EG) on flame retardancy properties in poly(ethylene-co-vinyl acetate) (EVA) rubber blends have been studied by limiting oxygen index (LOI), UL-94 test, cone calorimeter test (CCT), and thermogravimetric analysis (TGA). The EVA/EG/PhS composites revealed excellent flame retardancies. Upon adding 2.5 wt% of PhSs and 20 wt% of EG to EVA matrix, V-0 rating can be achieved. The heat release rate (HRR) and the total heat release (THR) of EVA/PhS-2(2.5 wt%)/EG(20 wt%) and EVA/PhS-4(2.5 wt%)/EG(20 wt%) blends decreased remarkably based on CCT. In addition, the thermal stabilities and mechanical properties of EVA/EG/PhS composites did not deteriorate comparing with those of EVA/EG composites.

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Royal Society Open Science · 2018 ·Vol. 5 ·期 1 · IF 2.504

Nanostructure selenium compounds as pseudocapacitive electrodes for high-performance asymmetric supercapacitor

Guofu Ma,Fengting Hua,Kanjun Sun,Enke Fenga,Hui Peng,Zhiguo Zhang,Ziqiang Lei

The electrochemical performance of an energy conversion and storage device like the supercapacitor mainly depends on the microstructure and morphology of the electrodes. In this paper, to improve the capacitance performance of the supercapacitor, the all-pseudocapacitive electrodes of lamella-like Bi18SeO29/BiSe as the negative electrode and flower-like Co0.85Se nanosheets as the positive electrode are synthesized by using a facile low-temperature one-step hydrothermal method. The microstructures and morphology of the electrode materials are carefully characterized, and the capacitance performances are also tested. The Bi18SeO29/BiSe and Co0.85Se have high specific capacitance (471.3 F g–1 and 255 F g–1 at 0.5 A g–1), high conductivity, outstanding cycling stability, as well as good rate capability. The assembled asymmetric supercapacitor completely based on the pseudocapacitive electrodes exhibits outstanding cycling stability (about 93% capacitance retention after 5000 cycles). Moreover, the devices exhibit high energy density of 24.2 Wh kg–1 at a power density of 871.2 W kg–1 in the voltage window of 0–1.6 V with 2 M KOH solution.

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Journal of Materials Chemistry B · 2018 ·Vol. 6 ·期 42 ·6858-6864 · IF 4.776

Co3O4 nanocrystals as an efficient catalase mimic for the colorimetric detection of glutathione

Wenying Li,Jiayan Wang,Jiacheng Zhu,Yue-Qing Zheng

Nanomaterial-based artificial enzymes (nanozymes), as an emerging generation of artificial enzymes, have received extensive attention in recent years owing to their striking merits. In this study, the obtained Co3O4 nanocrystals exhibited catalase-like activity and could catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2, and a clear absorption peak at 652 nm can be observed. It was verified that the catalytic activity for the oxidation of TMB originated from the oxygen, which is generated by Co3O4 catalyzed H2O2 decomposition. Upon addition of glutathione (GSH), the catalytic ability of the Co3O4 nanocrystals was inhibited. And, the changes of absorbance at 652 nm could be utilized to quantify the concentration of GSH. Under the optimized conditions, the proposed assay showed good linear relationships and a low detection limit towards GSH. Moreover, the Co3O4 nanocrystals had excellent stability and can maintain the catalytic activity for a long time. Thus, a simple, sensitive and selective nanozyme-based biosensor was developed for the colorimetric detection of GSH.

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Journal of Materials Chemistry B · 2018 ·Vol. 6 ·期 42 ·6865-6876 · IF 4.776

A tough and self-healing poly(L-glutamic acid)-based composite hydrogel for tissue engineering

Weijun Zhang,Kunxi Zhang,Shifeng Yan,Jie Wu,Jingbo Yin

A hydrogel with excellent mechanical properties and self-healing ability provides a promising tool for the repair of load-bearing tissues under a dynamic microenvironment. In this study, poly(L-glutamic acid) (PLGA)-based composite hydrogels with good toughness and self-healing ability were fabricated via filling soft self-healing hydrogels into a tough porous hydrogel skeleton. The PLGA-based tough porous hydrogel skeleton was treated by laser ablation to form a uniform porous structure with 85% porosity and 260 μm pore diameter, and the structure formation was reinforced by the hydrophobic assembly mechanism. The resulting hydrogel skeleton possessed good toughness (maximum compressive stress of 0.51 MPa with strain of 80%) and could fully recover after cyclic compression tests. Furthermore, PLGA-based self-healing hydrogels were fabricated based on a Schiff base reaction, followed by being composited with a tough porous hydrogel skeleton. More importantly, the composite hydrogel exhibited a homogenous interpenetrated structure that inherited mechanical strength and the self-healing ability of the two original compositions. These composite hydrogels exhibited a compressive failure stress of 0.21 MPa at a 63% strain, which was 1.3-fold higher than the value of the original porous hydrogel skeleton at 63% strain. The healing percentage gradually reached 81% within 6 h, indicating the good self-healing efficiency. Furthermore, live/dead staining images revealed that 89% of laden cells remained alive after culture for 7 days. Moreover, the composite hydrogel could self-heal even after cell encapsulation. The developed PLGA-based composite hydrogel will be a promising biomaterial for the repair of load-bearing tissues.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2018 · IF 11.698

Constructing a system for effective utilization of photogenerated electrons and holes: Photocatalytic selective transformation of aromatic alcohols to aromatic aldehydes and hydrogen evolution over Zn3In2S6 photocatalysts

Xiangju Ye,Yinghao Chen,Yahui Wu,Xuemei Zhang,Xuchun Wang,Shifu Chen

In a reaction system, the simultaneously efficient utilization of photogenerated electrons and holes to realize the photocatalytic selective redox reactions of organics has been a hot topic. In this paper, the Zn 3 In 2 S 6 samples were synthesized via a simple solvothermal method with different solvents, which could make full use of photogenerated electrons and holes to achieve the photocatalytic selective transformation of aromatic alcohols to aromatic aldehydes and hydrogen evolution under mild conditions. The results show that the Zn 3 In 2 S 6 synthesized with water (Zn 3 In 2 S 6 -W) exhibits the highest photocatalytic performance among the selected samples, with which the yields of benzaldehyde and hydrogen reach up to 732 and 708.8 μmol under light irradiation (λ ≥ 380 nm) for 4 h, respectively. The molar ratios between aldehydes and hydrogen are close to 1: 1. The apparent quantum efficiency is about 6.48% for wavelength λ = 380 ± 10 nm over Zn 3 In 2 S 6 -W sample. A possible reaction mechanism for the photocatalytic selective transformation of benzyl alcohol to benzaldehyde and hydrogen evolution under light irradiation is proposed. This work highlights that a reaction system is developed to effectively make use of the photogenerated electrons and holes for selective transformation of aromatic alcohols to aromatic aldehydes and hydrogen evolution over Zn 3 In 2 S 6 photocatalysts under mild conditions.

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Polymers · 2018 ·Vol. 10 ·期 10 ·1089 · IF 2.935

Bimetallic Gold-Silver Nanoparticles Supported on Zeolitic Imidazolate Framework-8 as Highly Active Heterogenous Catalysts for Selective Oxidation of Benzyl Alcohol into Benzaldehyde

Lili Liu,Xiaojing Zhou,Yongmei Yan,Jie Zhou,Wenping Zhang,Xishi Tai

The metal-organic zeolite imidazolate framework-8 (ZIF-8) supported gold-silver bimetallic catalysts with a core-shell structure (Au@Ag/ZIF-8 and Ag@Au/ZIF-8) and cluster structure (AuAg/ZIF-8) were successfully prepared by the deposition-redispersion method. Energy dispersive X-ray spectroscopy (EDS) elemental mapping images displayed that in the Au@Ag/ZIF-8 catalyst, Ag atoms were deposited on an exposed Au surface, and core-shell structured Au@Ag particles with highly dispersed Ag as the shell were formed. Additionally, the XPS investigation at gold 4f levels and silver 3d levels indicated that the Au and Ag particles of Au@Ag/ZIF-8, Ag@Au/ZIF-8, and AuAg/ZIF-8 were in a zero valence state. Among the resultant catalysts obtained in this study, Ag@Au/ZIF-8 catalysts showed the highest catalytic activity for the selective oxidation of benzyl alcohol, followed by AuAg/ZIF-8 and Au@Ag/ZIF-8. The turnover frequency (TOF) values were in the order of Ag@Au/ZIF-8 (28.2 h−1) > AuAg/ZIF-8 (25.0 h−1) > Au@Ag/ZIF-8 (20.0 h−1) at 130 °C within 1 h under 8 bar O2when using THF as solvent. The catalysts of Au@Ag/ZIF-8 and Ag@Au/ZIF-8 with core–shell structures have higher benzaldehyde selectivities (53.0% and 53.3%) than the AuAg/ZIF-8 catalyst (35.2%) in the selective oxidation of benzyl alcohol into benzaldehyde. The effect of the solvent, reaction temperature, reaction time, and reaction pressure on benzyl alcohol conversion and benzaldehyde selectivity in benzyl alcohol selective oxidation over Au@Ag/ZIF-8, Ag@Au/ZIF-8, and AuAg/ZIF-8 were also investigated. All of the catalysts showed excellent performance at 130 °C under 8 bar O2within 1 h when using THF as the solvent in the selective oxidation of benzyl alcohol to benzaldehyde. Moreover, the catalysts can be easily recycled and used repetitively at least four times.Keywords:metal-organic frameworks;core-shell;bimetallic catalyst;aerobic oxidation;benzyl alcohol

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ENTOMOLOGIA EXPERIMENTALIS ET APPLICATA · 2018 ·Vol. 166 ·期 6 ·483-490 · IF 1.454

Behavioral responses of Anagrus nilaparvatae to common terpenoids, aromatic compounds, and fatty acid derivatives from rice plants

Guofeng Mao,Jiaxin Tian,Ting Li,Hatem Fouad,Hassan Ga'al,Jianchu Mo

The attraction of parasitoids to their hosts is a key issue in efforts to enhance biological control efficiency. This study was conducted to identify which rice plant volatiles are attractive to females of the rice planthopper egg parasitoid Anagrus nilaparvatae Pang et Wang (Hymenoptera: Mymaridae) by using Y-tube olfactometer behavior assays. Our results demonstrated that 10 of 17 selected volatiles – that is, 3-carene, linalool oxide, linalool, benzyl alcohol, benzaldehyde, methyl salicylate, ( E )-2-hexenal, ( E )-2-hexen-1-ol, ( E )-3-hexen-1-ol, and hexanal – from three major groups of rice plant volatiles – terpenoids, aromatic compounds, fatty acid derivatives – attracted female A. nilaparvatae at various doses. Two full-component mixtures of 10 behaviorally active compounds at different ratios were more attractive to wasps compared with individual volatiles. Blends composed of the 10 behaviorally active compounds in their optimally attractive doses (i.e., each in the dose that elicited the strongest response in the wasps) or at equal mass ratio may be considered as attractants for A. nilaparvatae and thus help to control rice planthoppers.

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RSC Advances · 2019 ·Vol. 9 ·期 28 ·15694-15702 · IF 3.049

Comprehensive quali-quantitative profiling of neutral and sialylated O-glycome by mass spectrometry based on oligosaccharide metabolic engineering and isotopic labeling

Lijing Nan,Jiao Li,Wanjun Jin,Ming Wei,Mengjun Tang,Chengjian Wang,Guiping Gong,Linjuan Huang,Ying Zhang,Zhongfu Wang

Mass spectrometry (MS) analysis combined with stable isotopic labeling is of great importance for quantitatively profiling abnormal sialylated O-glycans associated with disease development, but technically hindered by the poor releasing efficiency of O-glycans from glycoprotein or the labile nature of sialic acid residues at glycans. Herein, we developed an isotopic precursor based metabolic amplification and labeling (IPMAL) technique for relative quantitative profiling of the repertoire O-glycans between normal and tumor cells by ESI-MS. Two groups of cells were incubated with peracetylated benzyl-α-N-acetylgalactosamine (Ac3GalNAc-α-Bnd0) or a heavy labeled peracetylated benzyl-α-N-acetylgalactosamine (Ac3GalNAc-α-Bnd5) precursor respectively to amplify the repertoire of O-glycans as Bnd0/d5-O-glycans which could achieve the quantitative O-glycome analysis by ESI-MS after derivatization. The established method demonstrates desirable feasibility, accuracy (relative error (RE) ≤ 4.20%), reproducibility (coefficient of variation (CV) ≤ 7.61%, n = 3) and good quantitation linearity (R2 > 0.99, n = 3) for five Bn-O-glycans with 2 orders of magnitude. Finally, the method has been successfully applied to quantitative analysis of the repertoire O-glycome changes between normal human liver cell line L02 and human hepatoma cell line SMMC-7721. Moreover, the α-2,3/2,6 sialic acid isomers of Bn-O-glycans from these two cells have been further quantitatively distinguished when involved a sialic acid specific derivatization procedure.

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Polymer Chemistry · 2019 ·Vol. 10 ·期 21 ·2666-2673 · IF 4.76

Fabrication of biocleavable crosslinked polyprodrug vesicles via reversible donor–acceptor interactions for enhanced anticancer drug delivery

Xiaolong Zhang,Qi Hua,Ping Meng,Mingqi Wang,Yunfei Wang,Lu Sun,Liwei Ma,Baoyan Wang,Cuiyun Yu,Hua Wei

Incorporation of various dynamic stimuli-responsive bonds to nanocarriers has been repeatedly highlighted to provide an elegant solution to the tradeoff between extracellular stability and intracellular high therapeutic efficiency; however, most of the developed systems still suffer from drug leakage-associated side effects due to insufficient stability and unsatisfactory therapeutic efficiency attributed to low drug loading capacity. To further address these critical issues, herein we reported a coordination-driven formation of biocleavable crosslinked polyprodrug vesicles (CPV) based on the reversible coordination interactions between the electron acceptor-containing polyprodrug and electron donor-based crosslinker, 1,6-hexanediamine. The resulting CPV exhibited a high drug loading content of 34.8%, and simultaneously enhanced extracellular micelle stability and promoted intracellular redox-triggered decrosslinking and drug release. More importantly, a comparison study further revealed that the CPV outperformed the noncrosslinked analogues in terms of greater stability, faster redox-triggered decrosslinking and drug release, a more compact structure with a smaller size toward higher cellular uptake, and greater in vitro cytotoxicity. This work thus developed a robust reversible crosslinking strategy to address high stability vs. sufficient therapeutic efficiency dilemma of polyprodrug-based nanocarriers.

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APPLIED CATALYSIS A-GENERAL · 2018 · IF 4.521

The effect of halogen on BiOX (X = Cl, Br, I)/Bi2WO6 heterojunction for visible-light-driven photocatalytic benzyl alcohol selective oxidation

Fengjiao Wang,Yuyao Gu,Zhenya Yang,Yanyu Xie,Jiangjie Zhang,Xiaotong Shang,Huibo Zhao,Zizhong Zhang,Xuxu Wang

We developed a simple X − -assisted (X = Cl, Br, I) one-pot hydrothermal reaction to successfully synthesize a series of BiOX/Bi 2 WO 6 heterojunction. The effect of different halogens and their addition amount on the photocatalytic performance of BiOX/Bi 2 WO 6 composites was investigated using benzyl alcohol selective oxidation under visible-light irradiation. All BiOX could enhance the photocatalytic activity of Bi 2 WO 6 , but the BiOBr was the optimum for the maximum improvement of Bi 2 WO 6 . The match of energy band structure between BiOX and Bi 2 WO 6 resulted in the highly efficient separation of photogenerated charges, which was mainly attributed to their fundamental distinction of the photocatalytic activity. This work clarified the essential distinction in photocatalytic performance of the different halogen of BiOX/Bi 2 WO 6 heterojunction, and also provided guidance for the construction of efficient heterojunction photocatalysts.

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Nanoscale · 2019 ·Vol. 11 ·期 31 ·14654-14667 · IF 6.97

MnFe2O4-decorated large-pore mesoporous silica-coated upconversion nanoparticles for near-infrared light-induced and O2 self-sufficient photodynamic therapy

Binbin Ding,Shuai Shao,Haihua Xiao,Chunqiang Sun,Xuechao Cai,Fan Jiang,Xueyan Zhao,Ping'an Ma,Jun Lin

The limited light penetration depth and tumor hypoxia are two natural shortcomings of photodynamic therapy (PDT). Overcoming these two issues within a single system is still a great challenge. Herein, photosensitizer (PS)-loaded and PEG-modified MnFe2O4-decorated large-pore mesoporous silica-coated β-NaYF4:20%Yb,2%Er@β-NaYF4 upconversion nanoparticles (UCMnFe-PS-PEG) as excellent PDT agents are successfully prepared for NIR light-mediated and O2 self-sufficient PDT. The large mesoporous structure observably increases PS loading efficiency (11.33 wt%) and the green luminescence from upconversion nanoparticles activated by NIR is able to activate PSs to generate ROS effectively. In addition, sub-10 nm MnFe2O4 nanoparticles work as a Fenton catalyst to generate O2in situ. In vivo experiments further prove that UCMnFe-PS-PEG not only provides magnetic guidance to the tumor, but also overcomes tumor hypoxia and dramatically enhances PDT efficiency. Furthermore, in vivo MR and UCL imaging are performed for accurate cancer therapy. We believe that the successful construction of the multifunctional UCMnFe-PS-PEG provides more revelations for developing advanced nano-drug systems for cancer therapy.

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