MICROCHIMICA ACTA
·
2016
·Vol. 183
·期 10
·2823-2830
·
IF 4.831
Zhong Yaping,Deng Chun,He Yu,Ge Yili,Song Gongwu
The authors describe a method for increasing the peroxidase-like catalytic properties of copper nanoclusters (Cu-NCs) that are used in non-enzymatic assays. The Cu-NCs were prepared by utilizing 6-thio-β-cyclodextrin as both the template and as effective modulators for increasing the peroxidase-like properties of the Cu-NCs. The β-CD-coated Cu-NCs have an average diameter of 2 nm, are stable in aqueous solutions, display strong fluorescence with excitation/emission peak wavelengths of 360/450 nm, and possess peroxidase-like catalytic activity which makes them a useful enzyme mimic. We have applied the findings to non-enzymatic photometric determination (at 650 nm) of (a) H 2 O 2 in the concentration range of 0.02 to 10 mM using the β-CD/Cu-NC assisted oxidation of tetramethylbenzidine by H 2 O 2 , and (b) glucose in the concentration range of 0.04 to 20 mM after addition of glucose oxidase and formation of H 2 O 2 . The detection limits (at an S/N ratio of 3) are 0.2 μM for H 2 O 2 and 0.4 μM for glucose. The β-CD coating is found to result in a strong increase in the reaction rate, probably because the cavity of β-CD acts as a pocket for the recognition and catalysis of substrate. Hence, the binding specificity becomes similar to that of natural enzymes.
The peroxidase-like catalytic activity of Cu-NCs in non-enzymatic sensors is strongly enhanced by utilizing mono-6-thio-β-cyclodextrin (mono-6-SH-β-CD) as both the template molecule and the effective rate modulator.
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ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Zhenzhen Yang,Wei Qi,Rongxin Su,Zhimin He
Three-dimensional flower-like Ce–Mo micro/nano composite oxides with different Ce/Mo atomic ratios (f-Ce10-xMoxOδ) were synthesized as effective bifunctional catalysts for one-pot conversion of fructose to 2,5-diformylfuran (DFF) via dehydration and aerobic oxidation. The catalytic activities of f-Ce10-xMoxOδ depended on their structure and physicochemical properties, which were closely related to their elementary compositions. The f-Ce9Mo1Oδ, which possesses polymeric octahedral MoOz species, the highest Oα ratio, BET surface area, and acidity density, exhibited the highest catalytic activity for DFF production. High DFF yields of 94% and 74% were obtained from f-Ce9Mo1Oδ catalyzed HMF oxidation and “one-pot” fructose conversion, respectively. Furthermore, f-Ce9Mo1Oδ is easily prepared, has low cost, and is ecofriendly, which has potential application in industrial production of DFF from fructose.
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AICHE JOURNAL
·
2016
·Vol. 63
·期 1
·257-265
·
IF 2.98
Haizhou Lin,Qingang Xiong,Yuan Zhao,Jingping Chen,Shurong Wang
In this work, a green reaction system of CO 2 -water-isopropanol was developed for 5-hydroxymethylfurfural (HMF) production. The conversion of fructose in a CO 2 -water system was first investigated, and the results showed this system could promote the formation of HMF compared to a pure water system. Then, isopropanol was introduced into the CO 2 -water system and the HMF formation became better because the solvent effect of isopropanol increased the tautomeric composition of fructofuranose, which was easy to form HMF. The existence of isopropanol was found to greatly suppress secondary reactions where HMF was converted to levulinic acid and insoluble humin. Meanwhile, the effects of reaction parameters on the conversion of fructose to HMF in the CO 2 -water-isopropanol system were analyzed, and a high HMF yield of 67.14% was obtained. Finally, to further illustrate the merits of CO 2 -water-isopropanol system, productions of HMF from other carbohydrates were tested and satisfactory yields were achieved. © 2016 American Institute of Chemical Engineers AIChE J , 63: 257–265, 2017
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ANALYTICA CHIMICA ACTA
·
2016
·
IF 4.712
Xiangheng Niu,Yanfang He,Jianming Pan,Xin Li,Fengxian Qiu,Yongsheng Yan,Libo Shi,Hongli Zhao,Minbo Lan
Nanosized materials acting as substitutes of natural enzymes are currently attracting significant research due to their stable enzyme-like characteristics, but some flaws of these nanozymes , including their limited catalytic rate and efficiency, need to be remedied to enable their wider applications. In this work, we verify for the first time the catalytic behavior of uncapped nanobranch-based CuS clews as a peroxidase mimic. XRD , XPS , SEM, and TEM proofs demonstrate that high-purity CuS clews composed of intertwined wires with abundant nanodendrites outside are successfully produced via a facile one-pot hydrothermal synthesis approach, with thiourea as both the sulfion source and the structure-directing agent. The synthesized CuS can catalytically oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) by H 2 O 2 to trigger a visible color reaction with rapid response (reaching a maximum change within 5 min). The proposed CuS nanozyme exhibits preferable catalytic kinetics over natural horseradish peroxidase (HRP). This outstanding activity primarily results from the large surface area and rich sites exposed by the uncapped unique structure. Under optimized conditions, the fabricated sensing system provides linear absorbance (652 nm) changes in the H 2 O 2 concentration range of 0.2˜130 μM, with a detection limit of as low as 63 nM. When coupled with glucose oxidase (GOD), the system is demonstrated to be capable of monitoring glucose in blood samples with excellent performance.
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PubMed
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ELECTROANALYSIS
·
2016
·Vol. 29
·期 3
·730-738
·
IF 2.471
Hui Min,Wenqin Wu,Huimin Wu,Shengfu Wang,Chuanqi Feng,Yu Ding
Pt x Sn/MWCNTs (x=1, 2, 3) nanocomposites were synthesized by chemical reduction. Comparing all of the materials, the results revealed that the best material was Pt 3 Sn/MWCNTs. The sensor based on Pt 3 Sn/MWCNTs exhibited excellent catalytic activities towards glucose and hydrogen peroxide. Sensing of glucose had a double-linear range: one was between 50 μM and 550 μM, the other was between 1.35 mM and 16.35 mM. These were due to the fact that more and more intermediate species were adsorbed onto the electrode surface with increasing concentration of glucose, which limited the following glucose oxidation. Meanwhile, the sensor also had a linear response range between 0.05 mM and 18.95 mM for hydrogen peroxide. Furthermore, the glucose and hydrogen peroxide sensors exhibited excellent selectivity, stability, and reproducibility. Thus the sensors had potential utilities in the detection of glucose and hydrogen peroxide.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2017
·
IF 5.401
Huihui Li,Ling Zhu,Xinyue Zhu,Haixia Zhang
A fluorescent glucose probe designed by a new strategy was reported. The probe consisted of ammonium-modified tetraphenylethylene (TPEA) with the feature of aggregation-induced emission and phenylboronic acid-containing polyanion that induced aggregation of TPEA via electrostatic interaction. With adding glucose and glucose oxidase, the produced H 2 O 2 converted phenylboronic acid into weaker acid phenol, which reduced negatively charges on the polyanion, resulting in the disaggregation of TPEA. This probe well qualified glucose in the range from 4 to 50 μM with detection limit of 2.6 μM. Moreover, it exhibited excellent selectivity and was successfully applied to blood glucose detection. As far as we know, no report has been published on glucose detection based on acidity difference between phenylboronic acid and phenol.
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MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 5
·1389-1396
·
IF 4.58
Jin Jiayi,Wu Wenqin,Min Hui,Wu Huimin,Wang Shengfu,Ding Yu,Yang Shuijin
Iron sulfides with different atomic ratios were synthesized by a hydrothermal method and used to modify a glassy carbon electrode. The various sulfides were compared to each other for their amperometric response to H 2 O 2 . It is found that FeS is the most adequate material. Operated in 0.1 M NaOH solution at 0.4 V (vs. Ag/AgCl), the sensor based on FeS displays a linear response that extends from 0.50 μM to 20.5 mM of H 2 O 2 , with a sensitivity of 36.4 μA mM −1 cm −2 and a detection limit of 0.15 μM (at an S/N ratio of 3). The sensor is selective, stable and reproducible.
Schematic of the synthesis of pomegranate flower-like FeS by a hydrothermal route using ferric chloride and thiourea (SC(NH 2 ) 2 ) as the precursors, and ethanolamine (EA) as the structure-guiding auxiliary agent. A glassy carbon electrode (GCE) modified with this material allows for amperometric sensing of hydrogen peroxide in 0.1 M NaOH solution with a 0.15 μM detection limit.
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JOURNAL OF MOLECULAR LIQUIDS
·
2017
·
IF 3.648
Canghao Ni,Yinyan Gong,Xinjuan Liu,Chang Q. Sun,Zhaofeng Zhou
Low-temperature Raman spectroscopy revealed that sugar solvation depresses the critical temperature for homogeneous ice nucleation ( T N ) whose depression extent follows the order of: trehalose > glucose > fructose at the same concentration and the extent of T N depression for a specific sugar is proportional to its concentration. We attribute the T N depression to the O:H vibration mode redshift induced by the solute dipolar polarization and distortion of the solvent hydrogen bond (O:H O or HB with “:” being the electron lone air of oxygen). The O:H phonon redshift lowers the Debye temperature of the O:H specific heat and disperses the quasisolid-phase boundary and the associated T N .
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Journal of Energy Chemistry
·
2016
·
IF 2.322
Ran An,Guizhuan Xu,Chun Chang,Jing Bai,Shuqi Fang
Butyl levulinate (BL) is a promising new candidate as diesel fuel and fuel additive. In this study, an efficient process for a one-pot synthesis of BL from biomass-derived carbohydrates in butanol medium with the catalysis of metal sulfates was developed. The catalytic activity of a series of metal sulfates for the synthesis of BL from fructose was investigated. Among various metal sulfates, ferric sulfate Fe 2 (SO 4 ) 3 was found to be the most efficient catalyst, which gave a remarkably high BL yield of 62.8 mol% under the conditions of 463 K, 3 h, a catalyst dosage of 5.0 g/L, and fructose concentration of 25 g/L. Different carbohydrates including glucose, cellulose , inulin and sucrose were also used for one-pot synthesis of BL with the catalysis of Fe 2 (SO 4 ) 3 , showing the yields of 39.6, 30.5, 56.6 and 50.1 mol%, respectively. In addition, the recycling and reuse of Fe 2 (SO 4 ) 3 was studied by characterizing them using powder X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS). A plausible reaction pathway for the one-pot synthesis of BL from fructose was proposed. This study provides a facile and feasible way for the synthesis of BL from biomass.
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RSC Advances
·
2017
·Vol. 7
·期 10
·5621-5627
·
IF 3.108
Shan Huang,Kai-Li Yang,Xiao-Fang Liu,Hu Pan,Heng Zhang,Song Yang
MIL-100(Fe) was used for the first time in the catalytic transformation of hexose sugars into lactic acid (LA). The as-synthesized MIL-100(Fe) was systematically characterized, and its superior morphological and textural properties were demonstrated to contribute greatly to the pronounced catalytic performance in fructose-to-LA conversion (up to 32% yield), as compared with other catalysts like Cu-BTC and MIL-100(Cr). The effects of reaction conditions including temperature, reaction time, and substrate loading were explored. In addition, MIL-100(Fe) could be easily reused for 4 cycles with no evident decrease in catalytic activity.
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NEW JOURNAL OF CHEMISTRY
·
2016
·Vol. 40
·期 10
·8459-8464
·
IF 3.277
Qianqian Du,Fei Qu,Beibei Mao,Shuyun Zhu,Jinmao You
An efficient sensor was developed for highly sensitive and selective determination of melamine based on Ag nanoclusters (Ag NCs) capped by hyperbranched polyethyleneimine (PEI) molecules with different molecular weights. The fluorescence of the Ag NCs could be quenched by Hg2+ and recovered by melamine. The molecular weights of PEI had an appreciable effect on the sensitivity, and Ag NCs capped by PEI with a molecular weight of 600 were more sensitive; the linear range of melamine was from 0.1 to 30 μM with a detection limit 30 nM. Moreover, this Ag NCs–Hg2+ system displayed excellent selectivity over common interferences such as metal ions, amino acids, sugars and nitrogen-containing organic molecules. Benefiting from the high selectivity, good recoveries ranging from 96% to 101% were obtained in food samples, including milk, infant formula, and dog food. More importantly, Ag NC-doped agarose hydrogels were fabricated easily to construct a visual device for the detection of melamine in food samples.
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WATER AIR AND SOIL POLLUTION
·
2016
·Vol. 227
·期 9
·1-11
·
IF 1.551
Wu Hailu,Xu Kaiqin,He Xiaojuan,Wang Xinze
Three macrophyte species, Typha augustifolia ( T. augustifolia ), Phragmites australis ( P. australis ), and Acorus calamus L. ( A. calamus L.), have been grown in hydroponic cultivation systems fed with synthetic wastewater. The experiment was designed as 3 × 2 factorial, with three species and two ratios of NH 4
+ /NO 3
− so as to investigate the nitrogen transformation and nitrogen removal capacity of each species. The nitrogen removal mechanism was further disclosed by comparing biomass production, nitrogen mass balance, and root exudates of the three plant species under different NH 4
+ /NO 3
− ratios. The results indicated there exists a linear relationship, with positive significance ( r = 0.946, p < 0.05), between plant biomass and total nitrogen (TN) removal efficiency; in other words, biomass could best reflect plant ability to remove nitrogen. It is also found that NH 4
+ /NO 3
− ratio could influence plant biomass and root exudates significantly. Additionally, the hydrogen donor and source of energy in denitrification happened in this research were mainly organic acids and soluble sugars, accounting for approximately 50 % of the composition in root exudates.
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