Advanced Science
·
2018
·Vol. 5
·期 7
·1800062
·
IF 12.441
Ke-Xin Zhang,Hui Su,Hong-Hui Wang,Jun-Jun Zhang,Shu-Yu Zhao,Weiwei Lei,Xiao Wei,Xin-Hao Li,Jie-Sheng Chen
Heterojunction photocatalysts at present are still suffering from the low charge separation/transfer efficiency due to the poor charge mobility of semiconductor-based photocatalysts. Atomic-scale heterojunction-type photocatalysts are regarded as a promising and effective strategy to overcome the drawbacks of traditional photocatalysts for higher photoenergy conversion efficiencies. Herein, an atomic-scale heterojunction composed of a boron nitride monolayer and graphene (h-BN-C/G) is constructed to significantly shorten the charge transfer path to promote the activation of molecular oxygen for artificial photosynthesis (exemplified with oxidative coupling of amines to imines). As the thinnest heterojunction, h-BN-C/G gives the highest conversion, which is eightfold higher than that of the mechanical mixture of graphene and boron nitride monolayers. h-BN-C/G exhibits a high turnover frequency value (4.0 mmol benzylamine g −1 h −1 ), which is 2.5-fold higher than that of the benchmark metal-free photocatalyst in the literature under even critical conditions.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Chen Fan,You Liang,Hongqiang Dong,Jiale Yang,Gang Tang,Wenbing Zhang,Dandan Kong,Jianqiang Li,Yongsong Cao
The massive release of rhodamine B (RhB) to water system is an emerging problem, which dramatically threaten environment and human health. The development of an adsorbent with enhanced removal efficiency for RhB is urgently needed. Herein, we report an environment-friendly synthesis of high quality zeolitic imidazolate framework-8 (ZIF-8) and functional ionic liquid@ZIF-8 in water-based system without heat treatment for improving its adsorption property. Guanidinium ionic liquids (ILs) could not only act as greener agents instead of volatile bases and toxic surfactants to efficiently control the nucleation and growth rate of ZIF-8, but also were incorporated as shell material to add specific adsorption sites. The relationship between nanoparticle structure and adsorption performance for RhB was systematically investigated. Due to high surface area (1167 m 2 g −1 ), high porosity (0.79 cm 3 g −1 ), high crystallinity , nano size (about 100 nm) and monodispersity, the as-obtained ZIF-8 showed improved adsorption capacity toward RhB (80% removal efficiency). Heteropolyanion-based guanidinium IL@meso-ZIF-8 (HPAIL@meso-ZIF-8) exhibited the high RhB uptake capacity of 278 mg g −1 (higher than most of the reported adsorbents) and effectively removed 99% of RhB within 15 min. The results showed that the adsorption process of prepared materials fitted well with pseudo-second-order kinetics and Langmuir isotherm model. The existence of mesopores in ZIF-8 facilitated the diffusion of RhB and the incorporated guanidinium IL played a significant role in enhancing the adsorption affinity. Moreover, the reusability results revealed the HPAIL@meso-ZIF-8 as a highly efficient adsorbent for RhB removal with satisfactory performance and structural stability. Therefore, HPAIL@meso-ZIF-8 is one of the most promising adsorbents for organic dye removal from water.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2018
·Vol. 135
·期 32
·46569
·
IF 1.901
Yongming Li,Qiang Ren
A nonionic surfmer (MAA-EO 23 C 12 ) was prepared and reacted with acrylamide, acrylic acid, and a double tailed hydrophobic monomer (BTMAM) to synthesize a surface-active hydrophobically associating copolymer (SHAP) through photoinitiated free radical copolymerization in aqueous solution. Fourier transform infrared and 1 H-nuclear magnetic resonance spectroscopy were used to characterize the functional monomer and the SHAP. Several performance evaluations, such as viscosification property, temperature resistance, salt tolerance, and shear resistance, were also conducted. Experiment results demonstrated that the introduced nonionic surfmer and hydrophobic monomer could endow the copolymer with excellent temperature resistance, salt tolerance, and shear resistance capability at low concentration. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 46569.
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Scientific Reports
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2018
·Vol. 8
·期 1
·1-11
·
IF 4.122
Sun Xia,Shi Junpeng,Fu Xiaoyan,Yang Yi,Zhang Hongwu
Near-infrared (NIR) persistent luminescence nanoparticles (NPLNPs) have become one of the most promising candidates for bioimaging. Different from the other fluorescence nanoprobes, the NIR persistent luminescence of NPLNPs can last for a long time after excitation, double exposure that is nanoparticles and light exist during the long-term bioimaging. However, to date, the potential risk of nanoparticles and NIR persistent luminescence of NPLNPs is still unknown. In this study, Cr3 + -doped zinc gallate, Zn 1.1 Ga 1.8 Sn 0.1 O 4 :Cr 3+ (ZGO), the most promising NPLNPs in bioimaging, was chosen as a representative for potential risk assessment. We evaluated the potential risk of nanoparticles and NIR persistent luminescence of ZGO for a long period of time. In vitro study showed that the ZGO possessed a low cytotoxicity. In vivo biodistribution results showed that the ZGO mainly accumulated in the reticuloendothelial system after intravenous injection and could be gradually cleared from the body by digestive system. In addition, the ZGO did not exhibit appreciable toxicity in mice over a period of 60 days. It’s also worth mentioning that long-term NIR persistent luminescence of ZGO did not exhibit obvious toxicities both in vitro and in vivo . Our results provide important information with regards to the risk of NPLNPs in long-term bioimaging.
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ACS Catalysis
·
2018
·
IF 11.384
Shuai Lyu,Li Wang,Jianghao Zhang,Chen Liu,Junming Sun,Bo Peng,Yong Wang,Kenneth G. Rappé,Yuhua Zhang,Jinlin Li,Lei Nie
In order to understand the role of Co catalysts with different phases on Fischer–Tropsch synthesis, single-phase face-centered-cubic (fcc) and hexagonal-close-packed (hcp) Co were synthesized via a two-step approach, involving the formation of single-phase CoO materials followed by reduction in H2. The physicochemical properties of Co catalysts were thoroughly characterized by XRD, SEM, TEM, TPR, and H2 chemisorption. It was found that hcp-Co exhibits higher activity on hydrocarbon formation than fcc-Co in Fischer–Tropsch synthesis. For both catalysts, CO dissociation was suggested as the rate-determining step, on which hcp-Co presents ca. 40 kJ mol–1 lower activation energy than fcc-Co, in agreement with a reported computational study. As a result, hcp-Co is concluded to be the preferable phase for rational catalyst design.
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BIOPOLYMERS
·
2018
·Vol. 110
·期 4
·e23243
·
IF 1.99
Xiaohui Fu,Jiliang Tian,Zheng Li,Jing Sun,Zhibo Li
A series of pegylated polypeptoids have been readily synthesized by a strategy combining ring-opening polymerization (ROP) and thiol-yne photoaddition. The polypeptoids simultaneously incorporated branched oligo(ethylene glycol) (OEG) units and thioether bonds in the side-chains. All the polypeptoids are readily soluble in aqueous solution and show reversible thermo-responsive properties. The cloud points (CPs) were demonstrated to be readily tunable in the range of ~25 °C-60 °C by varying the chemical composition, OEG chain length and the degree of polymerization. Attractively, the chemical compositions of the side chains are readily tunable via adjusting the molar ratios of a mixture of thiol terminated OEG molecules, which avoid synthesizing new monomers or copolymerization of different monomers. Further, the oxidation/reduction of thioether groups shows significant influence on the CPs, providing a second stimulus to tune the phase transition behaviors. Considering the biocompatibility and degradability, the dual-responsive polypeptoids are potential candidates for various biomedical or biotechnological applications. Graphical
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2015
·
IF 2.495
Chao Xu,Yong Chen,Heng-Yi Zhang,Yu Liu
A crown ether-based supramolecular gel with a three-dimensional network structure was successfully constructed via a hierarchical induced assembly strategy and characterized by UV/vis NMR, viscometry and DLS. Therein, the coordination linkage of bis(terpyridyl)dibenzo-24-crown-8 1 with Zn 2+ produces the 1 /Zn 2+ supramolecular polymer as the primary assembly. Then, the anthryl-dibenzylammonium guest 2 was grafted to the 1 /Zn 2+ supramolecular polymer via the non-covalent association of dibenzylammonium moieties on guests with the dibenzo-24-crown-8 rings on supramolecular polymer. Furthermore, the supramolecular polymer with anthryl grafts underwent a photo-induced secondary assembly to produce the supramolecular gel, which could be reversibly disassembled by a thermo-induced dissociation of anthracene dimers. These photo/thermo-induced hierarchical assembly/disassembly behaviors will provide a potential way to construct degradable hierarchical supramolecular assemblies employing environment-friendly external stimuli, such as light and heat, as controlling method.
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ANALYST
·
2014
·Vol. 140
·期 1
·162-173
·
IF 3.906
Chao Han,Jiannan Sun,Jinhua Liu,Heyong Cheng,Yuanchao Wang
To improve repeatability and efficiency and to simplify the operation procedure of capillary electrophoresis (CE), a pressurized CE system (p-CE) with injection valve sampling was developed. It consisted of one high-pressure pump, a six-port injection valve, a PEEK cross, a separation and back pressure capillary, an ultraviolet-visible detector and a high voltage power supply. The pressure-driven flow ranging from 4.5 nL min−1 to 0.81 μL min−1 in the separation capillary was produced by splitting to the flow from the high-pressure pumps (0.005–0.4 mL min−1). Nano-volume sample injection (<10 nL) was conducted by a micro-volume rotary injector (0.5–5 μL) with flow splitting. In the p-CE system, the new commercial capillary could be directly used without any wash, and the capillary-flush process between runs was also eliminated. In this case, the analytes were driven toward the outlet of the separation capillary by the pressurized flow, the electric field force and minute electroosmotic flow, and they were separated owing to the electrophoretic mobility. The p-CE system allows for the independent variation of the pressurized flow rate and electrical field and electrophoretic separation of good repeatability (below 3%) under high electrical fields (500–1000 V cm−1) and flow rate gradient modes. The feasibility of the p-CE system in real analysis was demonstrated by iodate quantification in iodized table salts. The separation of iodide and iodate was realized within 0.3 min, proving its high analytical speed.
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APPLIED SURFACE SCIENCE
·
2015
·
IF 2.711
Jun Dai,Juan Yang,Xiaohan Wang,Lei Zhang,Yingjie Li
Wirelike catalysts of mixed-phase TiO 2 (B)/anatase TiO 2 , bare anatase TiO 2 and TiO 2 (B) are synthesized via calcining precursor hydrogen titanate obtained from hydrothermal process at different temperatures between 450 and 700 °C. Under visible light irradiation, mixed-phase TiO 2 (B)/anatase TiO 2 catalysts exhibit enhanced photocatalytic activity in comparison with pure TiO 2 (B) and anatase TiO 2 toward selective oxidation of benzylamines into imines and the highest photocatalytic activity is achieved by TW-550 sample consisting of 65% TiO 2 (B) and 35% anatase. The difference in photocatalytic activities of TiO 2 samples can be attributed to the different adsorption abilities resulted from their crystal structures and interfacial charge separation driven by surface-phase junctions between TiO 2 (B) and anatase TiO 2 . Moreover, the photoinduced charge transfer mechanism of surface complex is also proposed over mixed-phase TiO 2 (B)/anatase TiO 2 catalysts. Advantages of this photocatalytic system include efficient utilization of solar light, general suitability to amines, reusability and facile separation of nanowires catalysts.
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RSC Advances
·
2015
·Vol. 5
·期 25
·19048-19057
·
IF 3.84
JiaQin Sun,Wei Wei,YaZhen Xu,JieHao Qu,XiangDong Liu,Takeshi Endo
Five commercially available amines: m-phenylenediamine (A1), m-xylylenediamine (A2), isophorone diamine (A3), trimethylhexamethylenediamine (A4), and 4,4′-diaminodiphenyl sulfone (A5), were examined as nucleophilic hardeners for bis-benzoxazine monomers based on aniline paired with bisphenol-A (BA-a) or bisphenol-F (BF-a). The reactivities and reaction mechanisms of their mixtures with BA-a were investigated using FTIR and NMR spectroscopy, DSC, and HPLC techniques. It was found that BA-a rapidly cured with the amines upon heating at 120 °C or 150 °C. The cure rate was similar to the amine/epoxy curing process in practical uses, and significantly faster than the ring-opening polymerization of bulk BA-a. The possible reaction mechanism was supported by the experimental results and includes three successive steps: (i) nucleophilic substitution at the carbon atom (O–C–N) in the oxazine ring by the amine, (ii) thermal decomposition of the resulting aminomethanaminium structure, and (iii) electrophilic addition of the newly formed iminium ion with the aromatic ring to form stable aminomethylphenol structures. These findings are helpful to improve the thermosetting resins in terms of their chemical structure, material properties, and processability.
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Reaction Kinetics Mechanisms and Catalysis
·
2013
·Vol. 109
·期 2
·551-562
·
IF 1.104
Cui Wenjing,Zhu Huaiyong,Jia Meilin,Ao Wulan,Zhang Yulin,Zhaorigetu Bao
Imines were synthesized from benzyl alcohol and amines by using catalysts of gold nanoparticles supported on ZrO 2 (Au/ZrO 2 ). The effects of reaction time, temperature, gold loadings and base were investigated. High yields were achieved under moderate conditions (60 °C) in the presence of KOCH 3 . For instance, the yield of N -benzylidenebenzylamine produced from benzyl alcohol and benzylamine on 3 wt% Au/ZrO 2 is 87 %. The synthesis of imine involves two reaction steps: selective oxidation of benzyl alcohol to benzaldehyde and the coupling reaction of amines with benzaldehyde. In the first step, the base promotes the selective oxidation. The reactions of benzyl alcohol with three different amines, aniline, n -butylamine and benzylamine, were conducted to produce corresponding imines. The results show that the amine with stronger nucleophilicity has better ability to react with benzaldehyde in the second step, resulting in higher yield of the corresponding imine. We proposed a tentative mechanism for the synthesis process.
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JOURNAL OF CATALYSIS
·
2017
·
IF 6.844
Kewei Wang,Zhifang Jia,Xuekang Yang,Ling Wang,Yanlong Gu,Bien Tan
Heterogeneous microporous acid (sulfonic acid) and base (benzylamine) catalysts with high surface areas were synthesized using simple aromatic compounds through one-step external cross-linking reaction. The direct induction and control of catalytic sites were achieved by functionalized monomers using an appropriate amount of acid/base monomers. This strategy provides an easy approach to produce highly stable and acid/base functionalized microporous organic polymers. The structure and composition of the catalysts were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), nitrogen sorption, Fourier transform infrared spectroscopy (FT-IR), solid-state 13 C cross polarization magic angle spinning (CP/MAS) NMR, thermogravimetric analysis (TGA), and element mapping analysis. The stable porous skeleton and the accurate manipulation of the catalyst structure allowed us to use the obtained polymers as compatible and efficient acid/base co-catalysts for one-pot cascade reactions. We demonstrated the use of these microporous heterogeneous catalysts for the cascade deacetalization/Henry and deacetalization/Knoevenagel reactions. The results demonstrated that preparing microporous materials from simple aromatic compounds through one-step external cross-linking reaction is indeed a cost-effective and easy-to-handle method to produce functionalized heterogeneous catalysts. The microporous heterogeneous catalysts produced by this method are highly stable and the amount of catalytically active sites can easily be controlled to form a catalytic system with two antagonistic centers.
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