CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2018
·
IF 1.712
Yan Cao,Yafang Chi,Ammar Muhammad,Peng He,liguo Wang,Huiquan Li
A non-phosgene route for the synthesis of hexamethylene-1,6-diisocyanate (HDI) was developed via catalytic decomposition of hexamethylene-1,6-dicarbamate (HDC) over Zn–Co bi-metallic supported ZSM-5 catalyst. The catalyst was characterized by FTIR and XRD analyses. Three solvents dioctyl sebacate (DOS), dibutyl sebacate (DBS) and 1-butyl-3-methylimidazolium tetrafluoroborate (BMIMBF 4 ) were investigated and compared; DOS gave better performance. The catalytic performances for thermal decomposition of HDC to HDI using DOS as solvent were then investigated, and the results showed that, under the optimized reaction conditions, i.e. ,10 wt% concentration of HDC in DOS, 250 °C temperature, 60 min reaction time, 83.8% yield of HDI had been achieved over Zn–Co/ZSM-5. Decomposition of the intermediate hexamethylene-1-carbamate-6-isocyanate (HMI) over Zn–Co/ZSM-5 in DOS solvent was further studied and the results indicated that yield of HDI from HMI reached to 69.6% (98.6% HDI selectively) at 270 °C, which further increased the yield of the total HDI (HDI tol ) to as high as 95.0%. Recycling of catalyst showed that HDI and HMI yield slightly decreased, and by-product yield increased after the catalyst was reused for 4 times. At last possible reaction mechanism was proposed.
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高影响因子
ANALYST
·
2018
·Vol. 143
·期 23
·5744-5753
·
IF 3.864
Wei Yang,Xia Wu,Tingting Liu,Ting Wang,Xiaohong Hou
An attractive triazine-based conjugated microporous polymer (TCMP) was fabricated via the Friedel–Crafts reaction and magnetized by a simple reduction co-precipitation method for the first time. The morphology and textural properties of the as-synthesized materials were characterized by scanning electron microscopy, Fourier transform infrared spectroscopy, powder X-ray diffraction, N2 adsorption measurements, elemental analysis, and magnetic measurements. The resulting magnetic triazine-based conjugated microporous polymer (MTCMP) was introduced as an efficient adsorbent for vortex-assisted magnetic solid phase extraction (MSPE) coupled with ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) for the determination of trace 5-nitroimidazoles (5-NDZs) in environmental water samples. The TCMP has abundant delocalized π-electrons and N-containing triazine that can generate π-interactions, intermolecular hydrogen bonds, and electrostatic interactions with polar 5-NDZs. Extraction parameters affecting the recovery efficiency of five 5-NDZs (metronidazole, ronidazole, secnidazole, tinidazole, and ornidazole), including the amount of the adsorbent, the pH value of the sample, the salting-out effect, the adsorption and elution time, and types and volume of the elution solvents, were investigated. Under the optimal conditions, a wide linear range, acceptable recoveries (ranging from 82.62% to 110.9% with the relative standard deviation lower than 9.58%), and good reproducibility (relative standard deviations less than 8.81% for intra-day and inter-day precision) were obtained. The limits of detection for the five analytes were between 0.012 and 0.035 ng mL−1. The established method is rapid, has high sensitivity and accuracy, and has been successfully applied to the detection of 5-NDZs in real environmental water samples.
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PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 77
·63044-63049
·
IF 3.84
Hualei Hu,Jinghui Lyu,Jie Cen,Qunfeng Zhang,Qingtao Wang,Wenwen Han,Jiayao Rui,Xiaonian Li
The effect of MgO and Pd modification on the catalytic performance of hierarchical porous ZSM-5 for benzene alkylation with methanol was investigated. The results indicated that the introduction of MgO could reduce the Brönsted acid sites which suppressed the side reaction of methanol to olefins and in turn effectively promoted the alkylation of benzene. However, the single modification of MgO could not completely suppress the formation of ethylbenzene and coke. Doping a small amount of Pd had a positive effect on inhibiting the generation of ethylbenzene and coke, which could be attributed to the hydrogenation of ethylene into ethane on Pd. The dual modified catalyst (MgO and Pd) exhibited high benzene conversion (56%) and xylene selectivity (39.1%), and the lowest ethylbenzene selectivity (0.13%) and coke content (0.4 wt%).
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RSC Advances
·
2015
·Vol. 5
·期 78
·63330-63337
·
IF 3.84
Yang Ding,Qiong Wu,Kangdi Zheng,Linkun An,Xiaoying Hu,Wenjie Mei
Two novel ruthenium(II) complexes coordinated with 6-chloro-5-hydroxylpyrido[3,2-a]phenazine (CQM), [Ru(L)2(CQM)]ClO4 [L = 1,10-phenanthroline, (1) and 2,2′-bipyridine, (2)], were investigated as potential fluorescent probes to track dynamic changes in the nuclei of living cells. Confocal laser technology was used to observe their co-location inside the cells. The results showed that both complexes were taken up by HepG2 cells, especially 1, which was localized in the cell nuclei, whereas 2 was distributed in the cell nuclei and mitochondria. Further studies by real-time fluorescence observations revealed that 1 rapidly entered the living cells, namely, HepG2, HeLa and MCF-7 cells, imaged the dynamic changes of the nuclei of living tumor cells, and exhibited low toxicity toward cells. The results demonstrated that 1 may be developed into a novel fluorescent probe for living cell nuclei. This study facilitates the development of fluorescent chemosensors with metal complexes.
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高影响因子
Catalysis Science & Technology
·
2014
·Vol. 5
·期 2
·1314-1322
·
IF 4.76
Zhenzhen Miao,Yibo Zhang,Xiqiang Pan,Tianxiao Wu,Bin Zhang,Jingwei Li,Ting Yi,Zhendong Zhang,Xiangguang Yang
Porous Bi-doped ceria (Ce1−xBixO2−δ solid solution) was prepared by the easy citrate method and then used as a supporting material for Au nanoparticles (NPs) obtained by deposition–precipitation. In the presence of O2, Ce1−xBixO2−δ (0.08 ≤ x ≤ 0.5) efficiently catalyzed the conversion of 5-hydroxymethylfurfural (HMF) to 5-hydroxymethyl-2-furancarboxylic acid (HFCA) and 2,5-bishydroxymethylfuran (BHMF) in alkaline aqueous solution without degradation of HMF. The excellent catalytic activity was attributed to the oxygen activation and hydride transfer enhanced by Bi doping and the large amount of oxygen vacancies. After Au NPs were supported on Ce1−xBixO2−δ (x ≤ 0.2), the presence of Auδ+ facilitated the activation of the C–H bond in the hydroxymethyl group and then the production of 2,5-furandicarboxylic acid (FDCA) as an end product, inhibiting the generation of BHMF.
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高影响因子
JOURNAL OF COORDINATION CHEMISTRY
·
2015
·
IF 2.012
Yan Xie,Junjie He,Tingting Wang,Heping Zeng
Reactions of Zn(II) salts, 5-(4-(1H-imidazol-1-yl)phenyl)-1H-tetrazolate (HIPT) and 2-mercaptobenzoic acid or 2-propyl-1H-imidazole-4,5-dicarboxylic acid (H3PrIDC), result in two mixed-ligand coordination polymers (CPs), [Zn2(IPT)(DSDB)(OH)]n (H2DSDB = 2,2′-disulfanediyldibenzoic acid, 1) and [Zn2(IPT)(PrIDC)(H2O)]n (H3PrIDC = 2-propyl-1H-imidazole-4,5-dicarboxylic acid, 2). Compound 1 possesses a 2-D structure built by 1-D [Zn(IPT)]n chains and DSDB2− connectors, in which the DSDB2− is generated via in situ reaction from 2-mercaptobenzoic acid. It displays a new intricate 4-nodal {3·4·6·7·8·9}{3·6·7·8·9·10}{3·8·9}{4·6·8} topology. Compound 2 displays a 3-D framework with new 3-connected topology with Schläfli symbol of (4·8·10) (8·122), in which the 1-D Zn-carboxylate chains were bridged by 3-connected IPT− ligands. The thermal stabilities and luminescence properties of 1 and 2 have also been studied. The compounds exhibit intense solid-state fluorescent emissions at room temperature.
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高影响因子
INORGANICA CHIMICA ACTA
·
2014
·
IF 2.041
Yong-Peng Xu,Jie Qin,Shi-Min Sun,Tong-Tong Liu,Xiao-Lin Zhang,Shao-Song Qian,Hai-Liang Zhu
Three novel complexes, [Ni II (dpp) 2 (L) 2 ] ( 1 ), [Ni II (eda) 2 (L) 2 ] ( 2 ) and [Ni II (deda) 2 (L) 2 ] ( 3 ) (L = 3-pyridinyl-4-amino-5-mercapto-1,2,4-triazole, dpp = 1,3-diaminopropane, eda = ethanediamine, deda = N,N-dimethyl ethylenediamine), were synthesized by reacting 3-pyridinyl-4-amino-5-mercapto-1,2,4-triazole with diamines and nickel(II) salt. The complexes were structurally determined by single-crystal X-ray diffraction. The inhibitory activity was tested in vitro against jack bean urease. Molecular docking was investigated to insert complexes into the crystal structure of jack bean urease at the active site to determine the probable binding mode. The experimental values and docking simulation exhibited that complexes 1 , 2 , 3 had better inhibitory activity than the positive reference acetohydroxamic acid, showing IC 50 values of 48.16, 32.35 and 15.22 μM, respectively. These complexes exhibited inhibitory activities as potent urease inhibitor.
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高影响因子
RSC Advances
·
2014
·Vol. 4
·期 81
·43029-43038
·
IF 3.708
Heping Gao,Yinxian Peng,Jianming Pan,Jun Zeng,Changhua Song,Yunlei Zhang,Yongsheng Yan,Weidong Shi
Stable water-in-oil (W/O) Pickering high internal phase emulsions (HIPEs) with an internal phase volume fraction of 84.8% were first stabilized by both the hydrophobic silica nanoparticles and span 80. Then, based on the obtained Pickering HIPEs, several macroporous polymerized solid acid (PDVB-SS-X-SO3H, X = 0, 0.2, 0.6) were prepared by polymerizing divinyl benzene (DVB) and sodium p-styrenesulfonate (SS), and were subsequently combined with sulfonation in H2SO4. All the as-prepared PDVB-SS-X-SO3H possessed open-cell structure, interconnecting pores and strong acidity, and were adopted as catalysts to convert cellulose into 5-hydroxymethylfurfural (HMF) in the presence of [Emim]Cl-mediated solvents. The results showed a maximum yield of 29.6% for PDVB-SS-0.2-SO3H, 12.9% for PDVB-SS-0-SO3H and 15.5% for PDVB-SS-0.6-SO3H under the same condition within 2.0 h at 120 °C, suggesting that the pore sizes and strong acidic sites played a key role in cellulose conversion. PDVB-SS-X-SO3H can be very easily recycled at least four times without a significant loss of activity. This research opens up a new method to synthesize porous solid acid catalyst materials through Pickering HIPEs templates.
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ChemPlusChem
·
2015
·Vol. 81
·期 1
·108-118
·
IF 3.026
Yunlei Zhang,Yao Chen,Yating Shen,Yongsheng Yan,Jianming Pan,Weidong Shi,Longbao Yu
Graphical Sweet success : Hierarchically macro-/mesoporous polymer foam has been successfully synthesized and used for the sustainable production of 5-hydroxymethylfurfural (HMF; see figure) from renewable cellulose. The as-prepared catalyst was also effective for the conversion of glucose and fructose to HMF in a DMSO/H 2 O system. Renewable and abundant carbohydrates are being strongly focused upon as a green and sustainable alternative for the production of valuable chemicals and biofuels. In this study, we chemically integrated acid–base bifunctionalized mesoporous silica nanoparticles (MSNs-SO 3 H-NH 2 ) and a macroporous polymer foam poly(HIPE) (PH) matrix that is derived from water-in-oil (W/O) high internal phase emulsion (HIPE) templating. After the subsequent sulfonation process, a SPHs@MSNs-SO 3 H-NH 2 catalyst with a hierarchical porous structure and bifunctional sites was prepared and used for the highly efficient synthesis of top value-added 5-hydroxymethylfurfural (HMF) from renewable cellulose in an ionic liquid (i.e., 1-ethyl-3-methylimidazolium chloride, [EMIM]Cl) based system. Evaluation of the catalytic activity revealed that the designed macropores were favorable for ready mass transfer, whereas the high surface area for active-site anchoring provided by the mesoporous structure was beneficial in enhancing the catalyst performance. A theoretical study also suggested that acidic and basic active sites synergistically work for the transformation reaction. Under the optimized conditions, a remarkably high HMF yield (44.5 %) was obtained efficiently. Furthermore, the as-prepared catalyst was recycled in four consecutive cycles with a total loss of only 4.9 % activity.
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高影响因子
BIORESOURCE TECHNOLOGY
·
2013
·
IF 4.75
Hu Li,Qiuyun Zhang,Xiaofang Liu,Fei Chang,Yuping Zhang,Wei Xue,Song Yang
A series of functional polymeric ionic liquids (FPILs) were prepared by coupling of SO 3 H-functionalized polymeric ionic liquids with different counterpart anions containing or excluding CrCl 3 ·6H 2 O, and characterized by SEM, FT-IR, XRD, NH 3 -TPD, TG, melting point, ICP-AES, and TEM. The catalytic activity of the prepared solid FPILs was investigated for the conversion of biomass including fructose, glucose and cellulose into 5-hydroxymethylfurfural (HMF) with the presence of DMSO-mediated solvents, successively producing moderate to excellent yields of HMF under atmospheric pressure. The FPILs catalysts developed in this study present improved performance on fructose-to-HMF conversion over other solid catalysts, such as functional ionic liquids supported by silica, metal oxides and strong acid ion exchange resin catalysts, and can be very easily recycled at least five times without significant loss of activity. In addition, a kinetic analysis was carried out to illustrate the formation of HMF.
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高影响因子
RSC Advances
·
2013
·Vol. 3
·期 30
·12313-12319
·
IF 2.562
Bing Liu,Zehui Zhang
In this study, prepared silica supported sulfonic acid was used as a heterogeneous catalyst for the production of 5-ethoxymethylfurfural (EMF) from fructose based carbohydrates and the synthesis of ethyl D-glucopyranoside from glucose based carbohydrates in ethanol. EMF was obtained in a high yield of 83.8% from 5-hydroxymethylfurfural (HMF) after 10 h, and a 63.1% yield was obtained from fructose at 100 °C for 24 h. Temperature experiments demonstrated that a higher reaction temperature (in the case of 120 °C) resulted in side reactions such as polymerization of HMF and alcoholysis of HMF into ethyl levulinates. When di- and poly-saccharides (sucrose and inulin) were used, the fructose moieties in sucrose and inulin were also successfully converted into EMF. However, the silica supported sulfonic acid catalyst was inert for the production of EMF from aldose based carbohydrates such as glucose and cellobiose. Ethyl D-glucopyranoside was formed in a high yield of 91.7% from glucose. More importantly, the catalyst could be reused several times without losing its catalytic activity with an average EMF yield of around 60% from a one-pot reaction of fructose. This work provides a good outlook for the conversion of carbohydrates into fine chemicals and biofuel additive.
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GREEN CHEMISTRY
·
2014
·Vol. 17
·期 2
·1308-1317
·
IF 6.852
Zehui Zhang,Judun Zhen,Bing Liu,Kangle Lv,Kejian Deng
A new method for the selective aerobic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) has been developed employing a magnetically separable [γ-Fe2O3@HAP-Pd(0)] catalyst. The catalyst was prepared by the exchange of Pd2+ with Ca2+ in γ-Fe2O3@HAP, followed by reduction of the Pd2+ to Pd(0) nanoparticles, and well characterized by TEM, XRD and XPS. The catalyst showed high activity in the oxidation of HMF to FDCA in water, with 97% HMF conversion and a 92.9% yield of FDCA under optimal reaction conditions. The method developed has demonstrated some advantages, including its sole requirement of a stoichiometric base, and high catalytic performance under atmospheric oxygen, even in air. More importantly, the γ-Fe2O3@HAP-Pd(0) catalyst was readily separated from the reaction solution using an external magnetic field and was successfully reused during five consecutive reaction runs while retaining its catalytic effectiveness. This study provides a green and sustainable method for the production of valuable chemicals from renewable resources.
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