GREEN CHEMISTRY
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2019
·Vol. 21
·期 5
·1075-1079
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IF 9.405
Yong Ni,Zhihao Bi,Hui Su,Lifeng Yan
Efficient conversion of furfural to valuable chemicals is attracting attention because it is one of the bulk feedstocks in biomass refinery. Maleic acid (MA) and fumaric acid (FA) are two types of bulk monomers that can be prepared from furfural. Here, a simple method was developed to oxidize furfural to both MA and FA in a green deep eutectic solvent (DES). DES contained oxalic acid and choline chloride (ChCl); oxalic acid worked as both the main content of the solvent and acidic catalyst for the conversion. It was found that the conversion of furfural could reach 100%, while the yield of MA and FA reached 95.7% under a mild reaction temperature of 50 °C, which provided a green and efficient route for the synthesis of valuable monomers from furfural.
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ANALYTICA CHIMICA ACTA
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2019
·
IF 5.256
Mei-Yuan Shi,Ming Xu,Zhi-Yuan Gu
Ultrathin two-dimensional (2D) metal-organic framework (MOF) nanosheets have attracted numerous attention due to their unparalleled advantages such as unique structures, large surface areas, good stability and high catalytic efficiency . In this paper, 2D Cu(bpy) 2 (OTf) 2 nanosheets (Cu-MOF, bpy = 4,4-bipyridine, OTf = trifluoromethanesulfonate) are first utilized to achieve the fluorescent detection for H 2 O 2 and glucose with their intrinsic peroxidase-like activity. The fluorescent biosensor Cu-MOF nanosheets were achieved by the efficient catalysis of non-fluorescent thiamine (TH) to strong fluorescent thiochrome in the presence of H 2 O 2 . With the combination of glucose oxidase , highly selective and sensitive fluorescent detection for glucose could be established with a detection limit of 0.41 μM and two separate linear ranges of 10–100 μM and 100–1000 μM, respectively. Furthermore, the developed method has been applied to human serum for the quantitative determination of glucose as a clinical diagnosis indicator of diabetes mellitus.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 14
·3930-3939
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IF 9.405
Guo Qiu,Chongpin Huang,Xiuliang Sun,Biaohua Chen
Bio-based platform chemical 5-hydroxymethylfurfural (5-HMF) can be converted into large-scale, high value-added compounds generally obtained from petroleum. Hence, developing an efficient catalytic system to transform glucose (a cheap and abundant branch of biomass) into 5-HMF has drawn significant attention. Earlier reports have concentrated on a two-step conversion of glucose to 5-HMF involving glucose isomerization into fructose and subsequent dehydration. In this work, efficient heterogeneous niobium-loaded montmorillonite (Nb-MMT) catalysts containing Lewis and Brønsted acid sites have been synthesized by a readily cation-exchanged synthetic method and were used to convert glucose and showed high selectivity and conversion. An optimum 5-HMF yield of 70.52% with a 99% conversion of glucose was achieved in a biphasic solvent of methyl isobutyl ketone (MIBK)/water at 170 °C for 3 h. The catalytic system also exhibited an excellent activity in the conversion of disaccharides and polysaccharides to 5-HMF with satisfactory yields. In addition, Nb-MMT was effectively reused four times without significant loss of activity. Nb-MMT also featured good catalytic activity and selectivity towards carbohydrate conversion in water. Furthermore, the reaction mechanism for the transformation of glucose to 5-HMF over Nb-MMT was investigated by density functional theory (DFT) calculations, and the results showed that niobium oxyhydroxide species of Nb-MMT played an essential role in glucose conversion, and the catalytic mechanism was a synergetic proton transfer process via hydrogen bonding. This study paves the way for improvements in Nb-containing solid acid catalysts for conversion of carbohydrates.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2019
·Vol. 166
·期 10
·B814
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IF 3.12
Jinlei Huang,Xufei Fang,Xue Liu,Siyuan Lu,Shuxin Li,Zixuan Yang,Xue Feng
Fast and accurate measurement of hydrogen peroxide is essential to glucose monitoring. In this work, we describe a highly efficient H2O2 sensor through the modification of Prussian blue (PB) on the nanoporous gold film (NPG). By de-alloying from Au-Ag film, we prepare the NPG film and characterize it through SEM and AFM. Tests using chronoamperometry and cyclic voltammetry on the Prussian blue modified NPG electrodes show an excellent electrochemical performance of the sensors. Owing to the comparatively huge specific surface area in the nanoporous structure, such electrodes significantly enhance the direct electron transfer from PB nanocrystals to NPG film. Comparing to earlier PB modified electrodes, the sensor fabricated in this work exhibits the widest linearity of 0.001∼17 mM, and produces a high selectivity of 708 μA·cm−2·mM−1.
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FUEL PROCESSING TECHNOLOGY
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2019
·
IF 4.507
Siquan Xu,Donghui Pan,Feng Hu,Yuanfeng Wu,Huazheng Wang,Yuan Chen,Hui Yuan,Lijing Gao,Guomin Xiao
In the presented work, a series of Cr/β zeolites were prepared and used as bifunctional catalysts with Brønsted and Lewis acidity in the conversion of biomass-derived carbohydrates to 5‑hydroxymethylfurfural (HMF). The physicochemical properties of all catalysts were characterized by ICP-AES, N 2 physisorption , solid-state 27 Al NMR, XRD, SEM-EDX, UV–Vis, XPS , Raman, NH 3 -TPD and Py-FTIR techniques. It was found that the catalysts with appropriate total acidity, ratio of Lewis to Brønsted acid sites and acid density appear to be beneficial for HMF formation. Under mild reaction conditions, a superior 72% HMF yield with 83% selectivity was achieved from glucose in the H 2 O/THF biphasic system by using the 0.4-Cr/β zeolite catalyst. Moreover, the results of the stability evaluation showed that the catalytic activity of the 0.4-Cr/β zeolite was not significantly lost after four consecutive cycles, and the framework remained intact. Therefore, the catalytic approach proposed in this study is believed to provide potential prospects for the production of HMF from biomass material refining in the future.
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Materials Research Express
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2019
·Vol. 6
·期 6
·065405
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IF 1.449
Qinghong You,Miaomiao Wan,Xiaoxu Fang,Xiulian Yin,Chuping Luo,Xuejuan Zhang
The process of intermittent microwave extraction (IME) pectin from pomelo peels assisted with EDTA was optimized by response surface methodology. Results showed that the optimal process for intermittent microwave extraction of pectin was as follows: 0.25% EDTA, pH 1.0, solid-to-liquid ratio 1:25 g ml−1, extraction time 125 s, microwave power 550 W, the extraction yield of pomelo peels was (38.48 ± 0.28)%. The structure of three kinds of pectin was verified by IR, SEM, XRD, HPLC and the results showed that pectin obtained from IME had a poor solubility but a good emulsifying activity. The IUEP had the highest scavenging rates of DPPH radicals.
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ACS Omega
·
2019
·
IF 2.584
Meng Li,Haiping Su,Yan Tu,Yazhuo Shang,Yu Liu,Changjun Peng,Honglai Liu
The alkylimidazolium tetrafluoroborate ionic liquids (ILs) ([Cnmim][BF4] n = 2, 4, 6, 8, 10) and anionic surfactant sodium dodecyl sulfate (SDS) were combined together to produce effective mediums for chromogenic catalysis of tetramethylbenzidine (TMB) with horseradish peroxidase (HRP) in the presence of H2O2. The chromogenic performance, kinetic behavior, and the possible influencing mechanism for the chromogenic catalysis of HRP-H2O2-TMB were discussed in detail. Therein, the roles of ionic liquids (ILs) were highlighted by the combination of experiments and theoretical calculations. The SDS/[C4mim][BF4] combination displayed superiority in chromogenic catalysis by improving both the substrate solubility and product stability to the maximum extent possible. Furthermore, SDS/[C4mim][BF4] combination showed uniqueness for TMB in improving the chromogenic performance compared with other chromogenic substrates of HRP. Inspired by the efficient chromogenic system, an enhanced enzyme-linked immunosorbent assay strategy for the detection of human immunoglobulin G was established and the sensitive colorimetric strategies for the detection of H2O2 and glucose were further developed by employing SDS/[C4mim][BF4] combination as the medium of chromogenic catalysis of HRP-H2O2-TMB. This unique chromogenic system is endowed with multitude of potential applications in biological systems.
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Nanoscale
·
2019
·Vol. 11
·期 27
·13126-13138
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IF 6.97
Yurui Zhou,Lu Li,Shenghui Li,Shufei Li,Miao Zhao,Qinghong Zhou,Xiaoqun Gong,Jin Yang,Jin Chang
Diabetic cataracts (DCs) are one of the most common ocular complications of diabetes, and easily causes blindness among diabetics. However, there are limited drugs to delay and prevent DCs. Research studies indicate that oxidative damage of the crystalline lens and nonenzymatic glycosylation of the lens protein play a key role in the pathogenesis of DCs. Hence, we developed a kind of autoregenerative redox nanoparticle, which was CeO2 NPs coated with PEG-PLGA (PCNPs). We first found that PCNPs could work not only as an antioxidant to protect lens epithelial cells from oxidative stress based on the repetitive elimination of reactive oxygen species (ROS), but also as a glycation inhibitor effectively restraining α-crystallin glycation and crosslinking, thereby keeping the lens transparent and alleviating DCs. Experimental results successfully validated the fact that the PCNPs were able to operate in eyes for a long time to attenuate lens opacity. We expect that this strategy will provide promising potential for the treatment of DCs.
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PubMed
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MICROCHIMICA ACTA
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2019
·Vol. 186
·期 6
·1-7
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IF 5.479
Qiao Juan,Liu Qianrong,Wu Han,Cai Huiwu,Qi Li
A fluorescent probe is described for the determination of serum glucose after hepatotoxin-induced liver injury. The probe is based on the use of a water-soluble polymer and has been prepared from a multi-functional azlactone polymer as the linker, amino boronic acid, and Alizarin Red as the signalling moiety. The excitation/emission peaks of the polymeric fluorescent probe are at 468/567 nm. Fluorescence is reduced on addition of glucose. Intensity drops linearly in the 0.1 mM to 14 mM glucose concentration range. The probe was applied to non-enzymatic detection of glucose in rat serum after CCl 4 -induced liver damage.
A polymer based fluorescent probe has been constructed and applied for non-enzymatic monitoring of serum glucose following hepatotoxin induced liver injury.
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CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Jun Zhang,Kaijun Dong,Weimin Luo
A facile and mild method for the catalytic production of 2,5-dimethylfuran (DMF) from 5-hydroxymethylfurfural (HMF) was developed, which utilized commercial PdCl 2 as the catalyst together with the green, non-toxic and low-cost hydride source, polymethylhydrosiloxane (PMHS). A synergistic effect among hydrogen donor, in situ generated metallic Pd 0 species and acid site HCl in the reaction played a key role in DMF formation. Gratifyingly, the desirable yield of hydrodeoxygenation product DMF as high as 89.7% from HMF was attained at room temperature (298 K) in 0.5 h. Meanwhile, biomass derived sugars also could be converted into DMF in relative high efficiency via a one-pot reaction in the present system. A plausible pathway for the hydrodeoxygenation of HMF into DMF in the present system was also proposed. The study thus highlights a new perspective for a simple, green, and efficient hydrodeoxygenation of biomass derivatives under milder conditions, employing a readily available, inexpensive and practical catalytic system of PdCl 2 -PMHS-ethanol, but without any external hydrogen supplies and pre-reduction treatments.
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Analytical Methods
·
2019
·Vol. 11
·期 12
·1697-1706
·
IF 2.378
Zhixia Yao,Zhen Li,Hanmeng Liu,Yaosheng Liu,Yujing Sun,Zhuang Li
A rapid and sensitive colorimetric strategy for the determination of ascorbic acid (AA) is presented, using amino functionalized copper metal–organic framework nanoparticles (Cu-BDC-NH2 NPs) with effective intrinsic peroxidase-like properties. In our design, Cu-BDC-NH2 NPs catalyze the H2O2 oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) generating blue-colored oxidized TMB (ox-TMB) with a significant absorbance at 655 nm in the UV-vis spectrum. AA can reduce ox-TMB, inducing a dramatic blue color fading and a decrease in absorbance. Under the optimal experimental conditions, this proposed system presents a good linear relationship (0.5–60 μM) and the detection limit is 0.15 μM. Repeatability, high selectivity and practicability are also well-studied, proving that the sensing system based on Cu-BDC-NH2 NPs can be successfully applied for colorimetric detection of AA in human serum, food and pharmaceutical samples. The designed method can provide a highly selective and sensitive optical sensing system to detect AA and establish a new platform to develop extensive applications of metal–organic framework nanoparticles with enzyme-mimetic activity in colorimetric biosensing.
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Biomass Conversion and Biorefinery
·
2019
·Vol. 10
·期 2
·277-287
·
IF 2.326
Shi Ning,Liu Qiying,Cen Hu,Ju Rongmei,He Xiong,Ma Longlong
Humins are undesired solids formed during the hydrothermal degradation of carbohydrates. In order to reveal the mechanism of formation of humins, we studied the degradation behavior of 11 model compounds including carbohydrates and furfural derivatives, within water and various pure organic solvents as reaction media. All the studied carbohydrates could generate solid humins in both water and studied organic solvents except ethanol, while the furfural derivatives could generate solid humins in only water. The results could be explained by regarding the formed α-carbonyl aldehydes and α,β-unsaturated aldehydes as primary precursors for formation of humins. Furfural derivatives could generate chain α-carbonyl aldehydes (for example, 6-hydroxy-2,5-dioxohexanal from 5-hydroxymethylfurfural and 2-oxopentanedial from furfural) through hydrolytic ring opening reaction; thus, water is essential for these furfural derivatives to generate humins. As for carbohydrates, they could generate α-carbonyl aldehydes and α,β-unsaturated aldehydes through simple step of β-elimination in all solvents; thus, they could form humins in both water and studied organic solvents except ethanol. Ethanol could react with α-carbonyl aldehydes by acetalization; thus, the condensation between α-carbonyl aldehydes was suppressed in ethanol, leading to few humins formation from carbohydrates. Based on the above analysis, we proposed that the formed α-carbonyl aldehydes and α,β-unsaturated aldehydes should be the primary precursor of humins.
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