CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Xueli Zhang,Rongxiu Tu,Jinyun Peng,Chuantao Hou,Zonghua Wang
In this paper, a hierarchically porous metal - metalloporphyrin gel (MMPG) based mimic multienzyme system for colorimetric sensing is reported. The synthesis conditions for gel state Fe-MMPG were systematically investigated and the porous structures were readily controlled by varying the reactant concentrations. Based on Fe-MMPG-5 with appropriate mesopores, glucose oxidase encapsulated in Fe-MMPG-5 (GOx@Fe-MMPG-5) with high loading capacity was achieved. The Fe-MMPG-5 provides not only mesopores for enzyme immobilization but also peroxidase-mimic activity in the GOx@Fe-MMPG-5 composite. This multienzyme system was further used for cascade catalysis and colorimetric sensing of glucose with low limit of detection, excellent selectivity and reusability. In additional, this system could also be applied to other oxidases, such as cholesterol oxidase, with intriguing properties. This study combines the advantages of porous gel materials and natural enzymes, providing potential to construct superior biocatalysts for advanced applications in biosensors, industrial catalysis, analytical equipment, and biofuel cells.
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MATERIALS CHEMISTRY AND PHYSICS
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2020
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IF 3.408
Tao Guo,Ting Xu,Wentao Xia,Andrew J. Carrier,Li Wang,Xu Zhang
We report herein, double quantum dot composites of graphene oxide and CuO (GOQD-q-CuO), formed by a low-temperature solution process, possess enhanced haloperoxidase (HPO)-like catalytic activity, which catalyze the oxidation of Cl − by H 2 O 2 to generate reactive chlorine species (RCS). A sensitive and selective colorimetric sensor was then developed via the oxidation of 3,3ʹ,5,5ʹ-tetramethylbenzidine (TMB) by the GOQD-q-CuO catalytic system through the generation of RCS for H 2 O 2 and glucose detection, with detection limits of 0.5 and 2.5 μM and linear ranges between 2.5–200 and 5–400 μM, respectively. This sensor was further applied to glucose detection in clinical serum samples showing no significant differences with the hexokinase method. Additionally, we demonstrate that the GOQD modulates the catalytic activity of q-CuO by reversing its zeta potential , producing an overall negatively charged surface, therefore GOQD-q-CuO has much higher affinity than CuO to the positively charged chromogenic substrate TMB, yielding higher HPO-like activity. Moreover, the presence of Cl − accelerates electron transfer to facilitate Cu 2+ reduction to Cu + on the GOQD-q-CuO surface, speeding up the overall catalytic reaction for the RCS generation, therefore, higher detection sensitivity was achieved.
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ELECTROCHIMICA ACTA
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2020
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IF 6.215
Meizi Chen,Xiaowei Cao,Kang Chang,Huanhuan Xiang,Rong Wang
In this article, a sandwich-type electrochemical sensor for selective determination of glucose based on the formation of glucose-boronic bidentate complex has been developed. 3-aminophenylboronic acid ( m -APBA) was immobilized on the gold nanoparticles modified ITO electrode with the linker molecule 4-mercaptobenzoic acid ( p -MBA). Then, glucose was captured by boronic acid group from m -APBA as the primary receptor and further grafted with an electroactive ferroceneboronic acid (FcBA) as the secondary receptor to form the sandwich-type sensor for selective detection of glucose. For comprehensively understanding the effect of the charge and structure of the terminal boronic acid group of 3-APBA on its binding to glucose, surface p K a was studied by electrochemical titration method, and it was proved the feasibility of examining glucose in physiological condition by the sandwich-type electrochemical sensor. The electrochemical characteristics of the as-prepared sensor were investigated by using electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The electrochemical sensor displayed a linear detection range of glucose from 0.5 mmol L −1 to 30 mmol L −1 , with detection limit of 43 µmol L −1 . The sensor exhibited good performance in selectivity study with the coexistence of galactose, fructose, mannose and other common interferences in physiological environment, such as, uric acid, ascorbic acid and dopamine. The as-prepared electrode with high sensitivity, good stability and reproducibility as well as excellent biocompatibility made it promising for the development of enzyme-free sensors.
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Scientific Reports
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2020
·Vol. 10
·期 1
·1-14
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IF 3.998
Pan Jingjing,Tai Yanni,Qu Haibin,Gong Xingchu
Ethanol precipitation is an important separation and purification process in the traditional Chinese medicines (TCMs) industry. In the present study, a membrane dispersion micromixer was applied to achieve good mixing for the ethanol precipitation process of Astragali radix concentrate. New experimental apparatus was set up to rapidly lower the temperature of ethanol solution before mixing with the concentrate. Ethanol precipitation process was optimized according to Quality by design concept. To identify critical material attributes (CMAs), ten batches of Astragali radix were used to prepare concentrates. Calycosin-7-O-β-D-glucoside content, the sucrose content, and the electrical conductivity were found to be CMAs after the correlation analysis and stepwise regression modelling. Definitive screening design was used to investigate the relationships among critical process parameters, CMAs, and process critical quality attributes (CQAs). Quadratic models were developed and design space was calculated according to the probability of attaining process CQA standards. A material quality control strategy was proposed. High quality and low quality Astragali radix concentrates can be discriminated by the inequalities. Low quality Astragali radix concentrates should not be released for ethanol precipitation process directly. Verification experiment results indicated accurate models and reliable design space. The temperature control method and control strategy are promising for ethanol precipitation process of other TCMs or foods.
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Advanced Materials Technologies
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2020
·Vol. 5
·期 7
·2000138
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IF 5.969
Junjie Hao,Yiwen Li,Xiaoqian Xu,Fenghuan Zhao,Ruikun Pan,Junzi Li,Haochen Liu,Kai Wang,Jiagen Li,Xi Zhu,Marie-Hélène Delville,Ming Zhang,Tingchao He,Jiaji Cheng
Chiral transition metal oxides nanoparticles (NPs) with tunable optical properties are widely accepted as promising toolbox for chiral recognition, stereoselective synthesis, and chiroptical devices. Herein, chirality-based strategy is presented for discrimination of d -glucose from its enantiomer through a cooperative synergy between chiral cysteine capped MoO 2 NPs and the glucose oxidase nanosystem. The valence-state-dependent chirality induced by metal-ligand charge transfer effect is found to be ultrasensitive to its redox environment such as the presence of hydrogen peroxide, which is a key indicator of the stereoselective enzymatic reaction between glucose oxidase and d -glucose. With this know-how, glucose enantiomers can be precisely quantified with a limit of detection of 0.446 µ m . Such a chiral bio-nanosystem would be an ideal platform for a rational design of new types of biosensors, photocatalysts, and chirality-based nanodevices.
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JOURNAL OF CATALYSIS
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2020
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IF 7.888
Junnan Wei,Ting Wang,Huai Liu,Yiqiang Liu,Xing Tang,Yong Sun,Xianhai Zeng,Tingzhou Lei,Shijie Liu,Lu Lin
It is highly desirable but challenging to develop a one-pot process for the transformation of fructose into 2,5-bis(isopropoxymethyl)furan (BPMF), a promising biofuel component, because a cascade sequence involving dehydration, reduction, and etherification requires multifunctional acid catalysts. Herein, we propose a facile and firm assembly of Zr/2-methylimidazole (2-MeIM) coordination polymer over USY zeolite (USY@ZrCP) through N-Al bonds formed by the condensation of 2-MeIM and the hydroxyls on USY surface at room temperature. USY@ZrCP possesses an abundance of strong Lewis acid sites with suitable amount of Bronsted acid sites, which are mainly attributed to the highly dispersed Zr(IV) species and the hydroxyls over USY@ZrCP, respectively. Unexpectedly, USY@ZrCP could offer BPMF yield up to 82.6% from fructose in isopropanol by the integration of dehydration, Meerwein–Ponndorf–Verley reduction and etherification in a one-pot strategy. This work proposes a novel approach to prepare highly efficient and robust solid acid catalyst for the catalytic valorization of biomass-derived carbohydrates and their derivatives.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
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IF 5.162
Tingwei Zhang,Wenzhi Li,Yongcan Jin,Wenhui Ou
A novel sulfonated chitosan-derived carbon-based catalyst was successfully prepared via isoamyl nitrite-assisted sulfanilic acid sulfonation , and its catalytic activity was examined using dehydration of fructose. The structural and chemical properties of sulfonated chitosan-derived carbon were characterized by SEM, FTIR, XRD, XPS , element analysis, N 2 adsorption-desorption experiment, and acid-base titration experiment. KOH was used as activating agent in the synthesizing of carbon supports, and it was found that properly increasing the dose of KOH during activation stage had a positive effect on the subsequent sulfonation of prepared activated carbon. 4KSCC, with the highest sulfonation degree (2.04 mmol/g), exhibited high performance for the conversion of fructose to HMF in various solvent, and an optimal HMF yield of 80.9% was obtained at 140 °C in 40 min. In addition, the reusability of 4KSCC for fructose dehydration was fairly good.
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APPLIED SURFACE SCIENCE
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2020
·
IF 6.182
Yi Zhang,Qi Wang,Dongming Liu,Qian Wang,Tong Li,Zhou Wang
A novel isotype (p-p) heterojunction, on the basis of Cu 2 O coupled with BiOI, has been designed and synthesized via a facile two-step electro-deposition approach at room temperature. The morphology, phase compositions and chemical bonding state were verified by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction measurements (XRD) and X-ray photoelectron spectra (XPS). The optimized Cu 2 O/BiOI hybrid electrode exhibited boosted photoelectrochemical (PEC) H 2 O 2 non-enzymatic sensing performance under visible light illumination, with a phenomenally broad linear range (1.99 µM ~ 17.54 mM), a high sensitivity of 213.87 µA mM −1 cm −2 , as well as a low detection limit of 0.44 µM (S/N = 3). Additionally, the sensor presented satisfying selectivity, repeatability, stability and its feasibility in real samples was corroborated. The photoelectrochemical sensing mechanism was clarified in the view of band structure and p-p heterojunction. Our work would enlighten the perspective research on the application of isotype heterojunction in PEC bio-sensing and provide a promising non-enzymatic biosensor platform for effective detection of H 2 O 2 in food, biomedical and environment analysis.
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Materials
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2020
·Vol. 13
·期 3
·507
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IF 3.057
Hui Wang,Meiyin Wang,Jining Shang,Yuanhang Ren,Bin Yue,Heyong He
In this work various amount of phosphomolybdic acid (PMo) were immobilized on amine functionalized SBA-15 and used as heterogeneous catalysts in the epimerization of glucose in aqueous solution. 13.3PMo/NH2-SBA-15 exhibited the best catalytic performance with a glucose conversion of 34.8% and mannose selectivity of 85.6% within two hours at 120 °C. The activation energy of 80.1 ± 0.1 kJ·mol−1was lower than that of 96 kJ·mol−1over the homogeneous H3PMo12O40catalyst. The catalytic activities of 13.3PMo/NH2-SBA-15 for the transformation of some other aldoses including mannose, arabinose and xylose were also investigated.Keywords:aldose epimerization;phosphomolybdic acid;amino-silanization;SBA-15
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Journal of Cleaner Production
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2021
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IF 9.297
Fengjiao Lai,Feng Yan,Yingqing Wang,Chunyan Li,Jianjun Cai,Zuotai Zhang
Biomass-derived carbohydrates exploited toward the synthesis of alkyl levulinates is very promising, but still limited by the applicable catalyst. In this study, novel metal/Si-pillared montmorillonite supported phosphotungstic acid catalysts (SG-HPW-XSiMt-y, where X = La 3+ , Ce 3+ , Er 3+ , Cu 2+ , Al 3+ , Ti 4+ , Zr 4+ ) were synthesized by sol-gel method. The catalytic performance of SG-HPW-XSiMt-y were comprehensively studied for glucose methanolysis to methyl levulinate (ML), focusing on the effects of metal acidity, HPW contents and reaction conditions. The appropriate Lewis acidity of metal ions effectively facilitated the isomerization of glucose/methyl-glucoside to fructose/methyl-fructoside; the strong Brønsted acidity of incorporated HPW was capable of suppressing the side reactions; and the large specific surface area and hierarchical pores of the mesoporous structure allow the reaction to take place both on surface and inside the porous framework. Among these as-synthesized catalysts, the SG-HPW-ZrSiMt-20 showed the most superior activity and achieved 65.8% yield of ML from glucose at 170 °C for 4 h. Alternative biomass-derived carbohydrates, including fructose, sucrose and cellobiose, also gave excellent ML yields under such catalytic system . The SG-HPW-ZrSiMt-20 had impressively stable reusability with merely loss of catalytic activity after eight cycles, owing to the uniform dispersion and stable bonding of HPW with ZrSiMt support. Generally, this catalyst system realizes an efficient and sustainable conversion of biomass-derived carbohydrates to ML production.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
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IF 6.165
Dongmei Li,Zhiwei Zhu,Da-Wen Sun
Raman spectroscopy has been employed for studying water structures in biomolecular aqueous solutions for decades but challenges remain to quantify the hydrogen bonding strengths in complex aqueous solution systems. In this study, four kinds of saccharide aqueous solutions were employed to investigate the quantitative relationship between the hydrogen bonding strength of water using confocal Raman microscopy and the Raman spectra of these solutions in the range of 3000–3800 cm −1 . Results showed that the enhancement effect of saccharide molecules on the hydrogen bonding strength of water increased with the concentration, and the degree of changes in the strength was related to the hydration capability and partial molal volume of saccharide molecules. An equation based on the average number of hydrogen bonds of water molecule was proposed to quantify the bonding strength in saccharide aqueous solutions with satisfactory accuracy as verified by T 2 relaxation time using nuclear magnetic resonance spectrometer.
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Foods
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2021
·Vol. 10
·期 6
·1391
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IF 4.35
Shiqiang Yang,Zhongfei Zhang,Jiaoyong Li,Yuge Niu,Liangli Lucy Yu
The Maillard reaction (MR) can affect the color, flavor, organoleptic properties, and nutritional value of food. Sometimes, MR is undesirable due to lowering the nutrient utilization, producing harmful neo-formed compounds, etc. In this case, it is necessary to control MR. Some chemical substances, such as phenolic acid, vitamins, aminoguanidine, and thiols extracted from garlic or onion, can effectively prevent MR. In this study, L-cysteine (L-cys) was found to inhibit MR after screening 10 sulfhydryl compounds by comparing their ability to mitigate browning. The inhibition mechanism was speculated to be related to the removal of 5-hydroxymethylfurfural (HMF), a key mid-product of MR. The reaction product of HMF andL-cys was identified and named as 1-dicysteinethioacetal–5-hydroxymethylfurfural (DCH) according to the mass spectrum and nuclear magnetic resonance spectrum of the main product. Furthermore, DCH was detected in the glutamic–fructose mixture afterL-cys was added. In addition, the production of DCH also increased with the addition ofL-cys. It also was worth noting that DCH showed no cell toxicity to RAW 264.7 cells. Moreover, the in vitro assays indicated that DCH had anti-inflammatory and antioxidant activities. In conclusion,L-cys inhibits MR by converting HMF into another adduct DCH with higher safety and health benefits.L-cys has the potential to be applied as an inhibitor to prevent MR during food processing and storage.Keywords:L-cysteine;Maillard reaction;inhibition;HMF;sulfhydryl compound
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