RSC Advances
·
2014
·Vol. 4
·期 94
·52402-52409
·
IF 3.708
Yong Liu,Lungang Chen,Tiejun Wang,Ying Xu,Qi Zhang,Longlong Ma,Yuhe Liao,Ning Shi
Non-edible cellulose has attracted considerable attention to be converted into valuable platform chemicals. Direct transformation of cellulose to C6 alditols (mannitol and sorbitol) provides a sustainable route. A productive approach is presented in this work using a Ru/C catalyst combined with H+-released boron phosphate in an aqueous phase. A yield of C6 alditols as high as 74.9% with a 91% conversion of cellulose is achieved. By adding silica–alumina materials, the yield of C6 alditols can be improved to 93.5% with complete conversion. The acid sites gradually released from boron phosphate under hydrothermal conditions could promote the hydrolysis of cellulose without significant degradation of glucose. Furthermore, the interaction of boric acid with C6 alditols may form borate–polyol complexes, which can enhance the stability of the C6 alditols to avoid further hydrogenolysis and dehydration of the C6 alditols formed. Due to the adsorption ability of the substrate, the addition of silica–alumina materials with a high content of silica leads to improved performance.
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MEDICINAL CHEMISTRY RESEARCH
·
2015
·Vol. 24
·期 8
·3327-3333
·
IF 1.402
Ye Lianbao,Wu Jie,Yang Jiebo,Chen Weiqiang,Luo Yan,Zhang Yanmei
Abstract HGF/c-Met signaling pathway has come into the spotlight as a promising therapeutic target for inhibiting tumor growth and has become one of the leading molecular targets in cancer. Various strategies are currently in development to disrupt the HGF–Met signal transduction pathway, in which small molecular inhibitors have been a particularly active field. On the basis of the structures of two c-Met inhibitors, PF-04217903 and JNJ-38877605, some novel 7-[(quinolin-6-yl)methyl] purines ( 4a – 4e ) were rationally designed on the principle of bioisosterism strategy. These compounds were synthesized and evaluated as novel c-Met inhibitors. Molecular docking experiments analyzed the results and explained the molecular mechanism of eminent activities to c-Met. The results showed that all the title compounds were active against c-Met enzyme to some extent. Though these compounds did not demonstrate inhibition as we expected, this study provided important information for building diversification of chemical library and molecular docking experiment supplied the basis for further research works. Graphical Abstract Some novel
7-[(quinolin-6-yl)methyl] purines as potential c-Met inhibitors have been designed and prepared. Their synthesis and spectral characterization are reported here.
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GREEN CHEMISTRY
·
2014
·Vol. 16
·期 6
·3305-3312
·
IF 6.852
Yuhe Liao,Qiying Liu,Tiejun Wang,Jinxing Long,Longlong Ma,Qi Zhang
The selective transformation of cellulose to C6 alditols provides a feasible route towards the sustainable synthesis of chemicals and fuels. Herein, the catalytic performance of amorphous zirconium phosphate (ZPA) combined with 5 wt% Ru/C was evaluated in the direct conversion of cellulose to C6 alditols (sorbitol and mannitol) under hydrothermal conditions. The yield of C6 alditols reached 63.5% and 85.5% with microcrystalline cellulose and ball-milled cellulose as the feedstock, respectively. This hybrid catalyst was developed to convert concentrated cellulose to obtain C6 alditols with a high concentration of 68.8 mg mL−1 in the final products. The high yield of C6 alditols from cellulose was ascribed to the fact that ZPA favoured the adsorption of cellulose and promoted its depolymerization to cellobiose and glucose, which was hydrogenated immediately to C6 alditols over Ru/C. The weak adsorption of C6 alditols over ZPA inhibited the dehydration of C6 alditols to sorbitan. Furthermore, ZPA exhibited excellent hydrothermal stability and could be reused for several runs.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY B-BIOLOGY
·
2015
·
IF 2.96
Junhui Pan,Langhong Wang,Guowen Zhang,Deming Gong
The characteristics of binding of 2-tert-butyl-4-methylphenol (TBMP), a synthetic phenolic antioxidant with hydroxypropyl-β-cyclodextrin (Hp-βCD) and calf thymus DNA (ctDNA) were investigated by multi-spectroscopic techniques and molecular simulation. The results indicated that TBMP preferred to form a 1:1 inclusion complex with Hp-βCD, with an inclusion constant of determined to be 7.15 × 10 3 L mol −1 . The intercalative mode of TBMP to ctDNA was supported by ctDNA melting temperature and relative viscosity studies, salt quenching effect, competitive binding with methylene blue and molecular modeling. The changes in Fourier transformed infrared (FT-IR) and circular dichroism (CD) spectra suggested that TBMP mainly bound to the G–C rich region with inducing a significant perturbation in B-like DNA structure. It was also found that Hp-βCD decreased the binding ability of TBMP with ctDNA, but did not affect the interactive mode between TBMP and ctDNA, and the formed inclusion complex of TBMP–Hp-βCD decomposed in the presence of ctDNA. This study may provide insights into the mechanism of binding of TBMP with ctDNA and the role of Hp-βCD in the TBMP–ctDNA interaction.
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PubMed
高影响因子
EUROPEAN JOURNAL OF LIPID SCIENCE AND TECHNOLOGY
·
2015
·Vol. 117
·期 10
·1636-1646
·
IF 1.812
Lingyi Liu,Meirong Pang,Ying Zhang
AOB-w is a water-soluble antioxidant extracted from bamboo leaves, containing four flavone C-glucosides (orientin, isoorientin, vitexin, and isovitexin) as functional components. Flavone C-glucoside esters were firstly synthesized by three lipases (CALB, RM IM, and TL IM) in organic solvent system or solvent-free system. Results indicated that C12 fatty acid ester exhibited the optimal antioxidant capacity, CALB was the most efficient lipase in both systems, and higher conversion yields were achieved in solvent-free system. Highest conversion was obtained with 1% water content for CALB and 2% water content for RM IM and TL IM. All lipases displayed absolute 6″-regioselectivities with monoester. It is required to consider both of hydrophobicity and antioxidant capacity to prepare high-efficiency oil-soluble antioxidant. Regression equations were built up to illuminate the relationship between conversion yield of flavone C-glucoside and antioxidant capacity of its corresponding ester. Highest antioxidant capacity could be achieved when conversion yield was nearly 60% for flavone C-glucosides. Based on reaction parameters of flavone C-glucosides, high-efficiency eAOB-o was prepared, which could be expected as an excellent oil-soluble antioxidant in lipids. Practical applications: Water-soluble antioxidant of bamboo leaves (AOB-w) is a natural food antioxidant extracted from bamboo leaves, with four flavone C-glucosides (orientin, isoorientin, vitexin, and isovitexin) as functional components. This study aimed to provide a practical procedure to prepare high-efficiency lipid antioxidant by enzymatic acylation. Based on the optimal parameters from the synthesis of flavone C-glucoside esters, high-efficiency oil-soluble antioxidant of bamboo leaves (eAOB-o) was prepared. eAOB-o exhibited higher antioxidant capacity than cAOB-o, which has been approved as food antioxidants in China. High-efficiency acylation products were obtained by consideration both of lipid solubility and antioxidant capacity. Based on the rule, flavone C-glucoside ester and eAOB-o were prepared.
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RSC Advances
·
2014
·Vol. 4
·期 49
·25625-25632
·
IF 3.708
Hua-Jun Zhu,Wei Zhai,Meng Yang,Xiao-min Liu,Yun-Chao Chen,Hui Yang,Xiao-dong Shen
Compared with LiFePO4, LiMnPO4 offers 20% higher energy density, but suffers from several orders lower electronic and ionic conductivity. The strategy usually adopted to overcome these intrinsic drawbacks is particle nanosizing mainly achieved by wet chemical methods or solid-state reactions in molten hydrocarbon, but which are not suitable for scale-up. A novel, economic and scalable method is proposed, using a T type micro-channel reactor to continuously precipitate nano-Mn3(PO4)2·3H2O for the first time. With the characterization of X-ray diffraction (XRD), transmission electron microscopy (TEM) and inductively coupled plasma (ICP), the generated Mn3(PO4)2·3H2O is proved to have an orthorhombic structure, a lath shape and possesses very high purity. The optimized temperature to prepare LiMnPO4/C nano-composites from the obtained Mn3(PO4)2·3H2O via a solid state reaction is proved to be 650 °C. The resulting sample is characterized by XRD, field emission scanning electron microscopy (FESEM), carbon/sulfur analysis, galvanostatic charge–discharge tests and alternating current impedance measurements. With 4.54 wt% of in situ carbon coating, this sample exhibits 137 mA h g−1 at 0.05 C and relatively good capacity retention. Moreover, by minimizing the impurities, the LiMnPO4 obtained from this novel method presents much improved Li+ diffusion coefficient due to less blocked [010] channels for Li+ migration.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2016
·Vol. 408
·期 14
·3867-3874
·
IF 3.125
Chen Lingfan,Shan Yichu,Weng Yejing,Yuan Huiming,Zhang Shen,Fan Runlong,Sui Zhigang,Zhang Xiaodan,Zhang Lihua,Zhang Yukui
The analysis of protein C-termini is of great importance, because it not only provides valuable information about protein function, but also facilitates the elucidation of proteolytic processing. However, even with the recent methods for the global profiling of protein C-termini, the identification of C-termini is still far behind that of N-termini due to the lack of basic residue and low reactive carboxyl group. Therefore, an unbiased and complementary method for C-termini profiling is imperative. In this work, we developed a negative enrichment strategy to achieve the in-depth analysis of C-terminome. Proteins were firstly amidated to block carboxyl groups, followed by lysyl endoproteinase (LysC) digestion to generate C-terminal peptides with α-amines and internal peptides bearing both α- and ε-amines. After the α-amines were blocked by site-selective dimethylation or succinylation, the remaining ε-amines on internal peptides were labeled with phosphate groups. Finally, internal peptides were depleted by TiO 2 , leaving exclusively the fraction of C-terminal peptides for LC-MS/MS analysis. With Escherichia coli ( E. coli ) digests as the sample, the efficiency of amidation, dimethylation/succinylation, phosphate labeling and TiO 2 depletion was proved high. With the combination of dimethyl and succinic blocking strategy, our method enabled the identification of 477 unique C-terminal peptides in E. coli . In comparison with the C-terminal amine-based isotope labeling of substrates (C-TAILS) method, 83 C-termini were identified by both methods, whereas 369 C-termini were unique to C-TAILS and 394 to our dataset. The method proposed is therefore efficient and possibly promotes the comprehensive profiling of C-termini.
Negative isolation of C-terminal peptides with combination of site-selective blocking, phosphate labeling, and TiO 2 adsorption
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 21
·10495-10509
·
IF 8.867
Jiying Long,Yun Gong,Jianhua Lin
Through an annealing method, Co9S8@CoS@CoO@C nanoparticles (NPs) of 5–20 nm size were synthesized using a metal–organic framework (MOF) as the precursor. The Co9S8@CoS@CoO@C NPs exhibited excellent electrocatalytic activity for the oxygen evolution reaction (OER) with a lower overpotential than RuO2 (0.37 V) and Pt NPs (0.60 V). The better electrocatalytic activity of the hybrid material is associated with its heterojunction structure, in which the strong electron coupling interactions between Co9S8, CoS, CoO and C give rise to a superior synergistic effect. The interconnected amorphous carbon not only anchored the active Co compounds to avoid aggregation, but also afforded conducting channels for electron transfer. Furthermore, the cobalt compounds were the active species in the sample during the OER process; they were converted into CoOOH and Co(OH)2 in the KOH electrolyte, and the S elements in the sample entered the solution. The Co9S8@CoS@CoO@C NPs can exhibit the best OER activity with minimum overpotential (0.028 V) to afford a stable OER current after activation in a KOH aqueous solution. The sample also showed obvious photoresponse to visible light irradiation with enhanced OER current and lowered onset potential, which was probably associated with the semiconducting characteristics of the spin-polarized CoO and the quantum confinement effect of the nanoparticles.
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Nano Energy
·
2016
·
IF 11.553
Peng Sun,Rui Lin,Zilong Wang,Meijia Qiu,Zhisheng Chai,Bodong Zhang,Hui Meng,Shaozao Tan,Chuanxi Zhao,Wenjie Mai
As an emerging energy storage device for wearable electronics , fiber supercapacitors (FSCs) have distinguished themselves from two dimensional SCs. Herein, TiN@C nanotube-based fiber electrodes are designed through a one-step nitridation and complete carbon coating process . They exhibit 260% higher capacitance than the samples obtained by traditional two-step nitridation and carbonization method. The carbon shell and the fabrication method are critical for the performance of the electrodes. The carbon shell remarkably protects the polycrystalline TiN core from mechanical cracking and chemical oxidation . FSCs based on these fiber electrodes demonstrate excellent electrochemical performance and mechanical stability. High capacitance of 2.4 mF cm −1 (19.4 mF cm −2 and 1.9 F cm −3 ) at a scan rate of 10 mV s −1 with an energy density of 2.69 μW h cm −2 and a power density of 809 μW cm −2 can be achieved. Moreover, nearly 80% capacitance retention after 10,000 cycle tests can be realized and the novel FSC can be bent for 2000 times with capacitance decay of 7.2%. Interestingly, our FSCs show almost no decay when cut into two segments due to the adoption of solid state electrolyte , demonstrating excellent tailorability. Finally, they can be also used as electric cables while store energy, demonstrating their bi-functionality.
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HIGH PERFORMANCE POLYMERS
·
2016
·
IF 1.045
Bei Liu,Zheng Chen,Liming Lin,Yuntao Han,Jinhui Pang,Zhenhua Jiang
3,6-Diphenyl-9H-carbazole pendants are grafted herein to poly(arylene ether ketone)s (PAEKs) via the Ullmann C–N coupling reaction. To the best of our knowledge, this is the first time that PAEKs containing a carbazole pendant (Cz) have been synthesized through the Ullmann C–N coupling reaction. The high molecular weights of PAEK-Cz (PAEKs with 3,6-diphenyl-9H-carbazole pendants) are inherited from their precursors, owing to the high reactivity of their monomers. The obtained PAEK-Cz-x polymers exhibit good solubility in most common organic solvents and excellent thermal stabilities, with the 5% weight loss temperatures for all products being above 598°C under a nitrogen atmosphere. The glass transition temperatures are all above 199°C and can be controlled by adjusting the feed ratio of monomers. The polymer membranes obtained by the casting method are tough and thus have strong potential for practical applications.
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JOURNAL OF NANOPARTICLE RESEARCH
·
2017
·Vol. 19
·期 6
·1-15
·
IF 2.02
Qin Xin,Shi Penghui,Liu Haolin,Fan Jinchen,Min Yulin,Xu Qunjie,Yao Weifeng
Metal nanoparticles have been combined with magnet metal–organic frameworks (MOFs) to afford new materials that demonstrate an efficient catalytic degradation, high stability, and excellent reusability in areas of catalysis because of their exceptionally high surface areas and structural diversity. Magnetic M
x
O
y
@N-C (M = Fe, Co, Mn) nanocrystals were formed on nitrogen-doped carbon surface by using 8-hydroxyquinoline as a C/N precursor. The Co@N-C, MnO@N-C, and Fe/Fe 2 O 3 @N-C catalysts were characterized by X-ray diffraction (XRD), Raman, scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), N 2 adsorption/desorption, and X-ray photoelectron spectroscopy (XPS). The catalytic performances of catalysts were thoroughly investigated in the oxidation of aniline solution based on sulfate radicals (SO 4
−. ) toward Fenton-like reaction. Magnetic M
x
O
y
@N-C exhibits an unexpectedly high catalytic activity in the degradation of aniline in water. A high magnetic M
x
O
y
@N-C catalytic activity was observed after the evaluation by aniline degradation in water. Aniline degradation was found to follow the first-order kinetics, and as a result, various metals significantly affected the structures and performances of the catalysts, and their catalytic activity followed the order of Co > Mn > Fe. The nanoparticles displayed good magnetic separation under the magnetic field.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2016
·Vol. 28
·期 1
·949-957
·
IF 1.798
Qiu Qingchao,Yang Weihua,Zhan Yangfan,Wang Hao
The development of non-noble metal catalysts is of great interest due to their significant potential application in both fuel cell system and metal-air batteries, particularly when considering long term commercial deployment. Fe/N/C is a promising non-Pt electrocatalyst for the oxygen reduction reaction (ORR), but its catalytic activity is considerably inferior to that of Pt in acidic medium. In this paper, an improved Fe/N/S/C catalyst (denoted as Fe–N–S/C) is presented. Nitrogen-sulfur-iron-doped porous carbon material is synthesized by the pyrolysis of dicyandiamide, a kind of abundant and inexpensive compound, with thiourea as additional sulfur source in argon atmosphere. The Fe–N–S/C shows excellent performance for the ORR with the onset and half-wave potential at 0.89 and 0.78 V (vs.RHE) in 0.1 M H 2 SO 4 solution, respectively, which are significantly higher compared to those of the catalysts derived from only dicyandiamide (0.85 and 0.75 V). Our results indicate that as compared to the commercial 20 % Pt/C catalyst, the synthesized catalyst exhibits not only higher current density and long-term durability but also higher tolerance to methanol poisoning. More importantly, the synthetic method is simple and inexpensive.
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