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GREEN CHEMISTRY · 2021 ·Vol. 23 ·期 21 ·8458-8467 · IF 10.182

Dual -functional carbon-based solid acid-induced hydrothermal conversion of biomass saccharides: catalyst rational design and kinetic analysis

Shanshan Xiong,Chao Luo,Zhihao Yu,Na Ji,Lingjun Zhu,Shurong Wang

The isomerization–dehydration cascade conversion on the saccharide platform is a pivotal route for biomass valorization, although it exhibits a specific reaction complexity that makes achieving an efficient conversion a highly technical challenge. The rational design of novel versatile solid acids is deemed to be the key to improving the cascade catalytic performance. In this paper, a dual-functional carbon-based solid acid catalyst (DFCSA) with tunable Brønsted/Lewis acid sites was developed for the cascade conversion of saccharides. The combined modification of H3PO4 and HNO3 on the carbon substrate contributed to the grafting of protonated moieties with a reasonably porous structure. With the aid of AlPO4, which has an orthorhombic crystal structure, the newly developed catalyst was able to achieve good performance for the subsequent hydrothermal conversion. Under optimal conditions, glucose and xylose were transformed with high product yields: 38.2 mol% levulinic acid and 69.7 mol% furfural, respectively. In addition, the catalyst displayed excellent hydrothermal stability, with only a slight degradation in activity after 10 cycles, which was ascribed mainly to the high thermal stability of AlPO4 and the firm grafting of the surface functional groups. As shown by the kinetic analysis, the DFSCA catalyst had a higher conversion rate and lower activation energy in the cascade conversion of xylose than that of glucose, leading to a better yield of furfural.

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BIOSENSORS & BIOELECTRONICS · 2021 · IF 10.618

An integrated and conductive hydrogel-paper patch for simultaneous sensing of Chemical–Electrophysiological signals

Tianyu Li,Bo Liang,Zhichao Ye,Lei Zhang,Shiyi Xu,Tingting Tu,Yiming Zhang,Yu Cai,Bin Zhang,Lu Fang,Xiyu Mao,Shanshan Zhang,Guan Wu,Qifu Yang,Congcong Zhou,Xiujun Cai,Xuesong Ye

Simultaneous monitoring of electrophysiological and biochemical signals is of great importance in healthcare and fitness management, while the fabrication of highly integrated and flexible devices is crucial to these applications. Herein, we devised a multifunctional and flexible hydrogel-paper patch (HPP) that was capable of simultaneously real-time monitoring of electrocardiogram (ECG) signal and biochemical signal (glucose content) in sweat during exercise. The self-assembly of the highly porous PEDOT:PSS hydrogel on paper fiber provided the HPP with good conductivity and hydrophilic wettability for efficient electron transmission and substance diffusion, thereby enabling it to serve as a low-impedance ECG electrode and a highly sensitive glucose sensor . Additionally, the spontaneous capillary flow effect allows the paper patch to be used as microfluidic channels for the collect and analysis of sweat. Moreover, the HPP is integrated with a flexible printed circuit board (FPCB) and works as a multifunctional wearable device mounted on the chest for real-time monitoring of electrophysiological and biochemical signals during exercise.

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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

Catalytic conversion of sucrose to 5-hydroxymethylfurfural in green aqueous and organic medium

Shahi Mulk,Muhammad Sajid,Lei Wang,Feng Liu,Gang Pan

5-Hydroxymethylfurfural (HMF) is one of the promising chemicals, which can serve as a platform chemical to produce various energy chemicals. HMF can be produced from different lignocellulosic biomass derived sugars employing different catalytic processes. In this study, the synthesis of HMF was investigated from excessively available sucrose using environment friendly and cost-effective technology . Among the various solvents applied, dimethyl sulfoxide (DMSO) was found as an efficient organic solvent medium. The results elucidated the combination of p -toluenesulfonic acid ( p TSA) and chromium chloride (CrCl 3 .6H 2 O) as the best dehydrating catalyst. A relatively higher HMF yield of 55% was achieved at a lower temperature (120 ℃) while at 150 ℃ (higher temperature) oxalic acid with higher concentration of CrCl 3 .6H 2 O gave a maximum yield of 59.21%. The time, temperature, and concentrations affected the yields. The positive impact was found with a rise in temperature from 100 to 120 ℃ in p TSA while oxalic acid affected the yield until 150 ℃. HMF yields were reported in descending order as p TSA > oxalic acid > maleic acid > malonic acid > succinic acid > blank at 120 ℃. It was observed that the isomerization of glucose to fructose is the major barrier to achieve the high process yield. Therefore, more efforts should be made to achieve the high rate of isomerization of glucose (part of sucrose disaccharide) in order to improve the HMF selectivity by depressing the humin formation.

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FOOD CHEMISTRY · 2021 · IF 7.514

Effect of high-pressure processing and thermal treatments on color and in vitro bioaccessibility of anthocyanin and antioxidants in cloudy pomegranate juice

Lei Yuan,Fengyun Cheng,Junjie Yi,Shengbao Cai,Xiaojun Liao,Fei Lao,Linyan Zhou

In this study, the effect of high-pressure processing (HPP) and thermal treatments, including pasteurization (PT) and high-temperature short-time sterilization (HTST) on pomegranate juice (PJ) color attributes, anthocyanin (ACNs), vitamin C, and in vitro bioaccessibility of ACNs and antioxidants were investigated. Compared to HPP, thermal treatments significantly changed the CIE color, decreased the total monomeric ACNs and total vitamin C contents, and increased the percent polymeric color (PPC) and browning index (BI). Correlation analysis showed that the generation of polymeric ACNs played a significant role in color change during thermal treatments. The recovery of 7 ACNs in the control sample after in vitro gastrointestinal digestion was ranged from 0.43% to 5.0% and total individual ACNs after digestion showed no significant changes among different treatments. These results contributed to promoting the color quality and health benefits of pomegranate juice rich in ACNs by optimizing the processing conditions in the food industry.

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Journal of Oleo Science · 2021 · IF 1.601

Microwave-assisted Natural Deep Eutectic Solvents Pretreatment Followed by Hydrodistillation Coupled with GC-MS for Analysis of Essential Oil from Turmeric (Curcuma longa L.)

Fang-Xiang Xu,Jing-Yu Zhang,Jing Jin,Zu-Guang Li,Yuan-Bin She,Maw-Rong Lee

In the past decade, natural deep eutectic solvents (NADESs) as green and sustainable extraction solvents with great potential for the efficient extraction of bioactive compounds from the plants are emerging. In this study, a microwave-assisted technology is used to prepare natural deep eutectic solvents. And natural deep eutectic solvents as pretreatment solvents coupled with microwave-assisted hydrodistillation (MAHD) for isolating essential oil (EO) derived from turmeric (Curcuma longa L.) is investigated. To improve the essential oil yield of turmeric (Curcuma longa L.) as a target, various factors affecting extraction efficiency including the type and amount of natural deep eutectic solvents, pretreatment time, pretreatment temperature and hydrodistillation (HD) time are discussed and optimized through central composite design (CCD) of the response surface methodology (RSM). The optimal conditions are as follows: natural deep eutectic solvent composed of choline chloride and oxalic acid (molar ratio with 1:1) as a pretreatment solvent, an amount of 60 g, a pretreatment time of 5 min, a pretreatment temperature of 84 ºC, a hydrodistillation time of 76 min. Under the optimum conditions, the highest essential oil yield of 0.85% is achieved. Additionally, the essential oil is analyzed by using gas chromatography-mass spectrometry (GC-MS), with a total of 49 compounds being identified. Through combining natural deep eutectic solvents with a microwave-assisted hydrodistillation technique, this work provides an eco-friendly extraction way of isolating essential oil, which boosts development in the monitoring other spice quality field.

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Nano Energy · 2021 · IF 17.881

Air-permeable electrode for highly sensitive and noninvasive glucose monitoring enabled by graphene fiber fabrics

Shengying Cai,Changshun Xu,Danfeng Jiang,Meiling Yuan,Qingwen Zhang,Zhaoling Li,Yi Wang

Developing wearable and noninvasive electrochemical devices for glucose monitoring is desirable for diabetes diagnostics and management. However, the adoptions are restricted by their poor reliability due to diluted glucose densities in commonly-used body fluids while lack of highly sensitive electrodes. Graphene fiber fabric, which is macroscopically paper-like and assembled by wet-fused graphene fibers, provides excellent electrical and mechanical properties as well as penetration paths for liquids, showing great potentials for electrochemical monitoring . Additionally, the graphene fiber fabric as a sensing patch provides excellent air-permeability which is necessary for wearing comfort but has rarely been addressed. As a result, the Prussian blue-decorated graphene fiber fabric exhibits a high electrochemical sensitivity to hydrogen peroxide (7298.7 μA mM −1 cm −2 ). After being modified by glucose oxidase and chitosan, it delivers both high selectivity and electrochemical sensitivity to glucose (1539.53 μA mM −1 cm −2 in the concentration range of 2–220 μM, and 948.48 μA mM −1 cm −2 in the concentration range of 220–650 μM). We ascribe these performances to high-speed transfer paths for electrons and electrolytes in resultant electrodes. Additionally, the spontaneous absorption of body liquids by graphene fiber fabric after deposition of hydrophilic Prussian blue improves the utilization of active materials. Finally, the graphene fiber fabric used as a dry sensing patch was applied on human skin for the in vivo noninvasive glucose monitoring with the reverse iontophoresis (RI) technology, which showed good correlation to glucose levels measured by a commercial finger-prick glucometer.

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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 46 ·期 5 ·2526-2533 · IF 3.591

Green and facile synthesis of iron-doped biomass carbon dots as a dual-signal colorimetric and fluorometric probe for the detection of ascorbic acid

Pengfei Fan,Can Liu,Congcong Hu,Feifei Li,Xi Lin,Shengyuan Yang,Fubing Xiao

Iron-doped carbon dots (Fe-CDs) were greenly synthesized via a one-step hydrothermal method using the eco-friendly materials milk powder and FeCl3. It was found that the synthesized biomass Fe-CDs have photoluminescence properties and strong mimetic oxidase activity, which enables catalysis of the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to produce a blue product, oxidized TMB (oxTMB). The presence of ascorbic acid (AA) could reduce the oxTMB and make the solution color lighter to realize the colorimetric determination of AA. In addition, the absorption peak of the oxTMB generated at 370 nm overlaps with the excitation spectrum of Fe-CDs, and oxTMB quenched the fluorescence of Fe-CDs based on the internal filtration effect (IFE). The presence of AA will reduce oxTMB and restore the fluorescence of Fe-CDs, and the change of fluorescence intensity is positively correlated with the concentration of AA. Accordingly, a novel method for colorimetric/fluorometric dual-signal detection of AA was developed. The linear range of the colorimetric assay was 25.0–500.0 μM, and the detection limit was 8.59 μM. The linear range of the fluorometric assay was 20.0–500.0 μM with an LOD of 5.13 μM. The method took advantage of different signals to achieve complementarity and eliminate false positives of single signals and improve the accuracy with great application prospects in the detection of AA.

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MATERIALS & DESIGN · 2021 · IF 7.991

Dynamic biological interfaces functionalized fructose-responsive immunomagnetic beads for high-efficient and high-purity exosome enrichment

Guohao Li,Nanhang Zhu,Jia Cheng,Yujia Zhang,Yue Yu,Xiaolin Zhang,Qiangying Yi,Yao Wu

Enrichment of exosomes with high structural and functional integrity is a critically important step before downstream applications in biological and clinical domains. In this work, dynamic biological interfaces functionalized fructose-responsive immunomagnetic beads (Fr-IMBs) were fabricated by incorporating the dynamic biological interfaces composed of dopamine and 4-carboxyphenylboronic acid with immunomagnetic beads. These fabricated Fr-IMBs were successfully applied to capture the MCF-7 exosomes with a high capture efficacy of 91.0%. After incubation with fructose, the molecular structure of the dopamine-boronic acid complexation can be rearranged and the antibody (anti-CD63) bound exosomes were released competitively, with a yield greater than 79.8%. Those exosomes that underwent both immunomagnetic separation and fructose triggered release remained their good bioactivity to promote MCF-7 cell migration. Better yet, exosomes enriched by Fr-IMBs possessed higher purity and better preservation of tumor-related molecular information of the exosomal proteins than those obtained through the ultracentrifugation approach, as proved by the comparative proteomics. These proposed sugar-responsive immunomagnetic beads may serve as biofriendly candidates in enriching useful biomarkers (e.g., cells, nucleic acids, proteins, etc.) efficiently from complex biological samples with high purity.

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Frontiers in Nutrition · 2021 · IF 6.576

In vitro Prebiotic Properties of Garlic Polysaccharides and Its Oligosaccharide Mixtures Obtained by Acid Hydrolysis

Lu Xiaoming,Li Ningyang,Zhao Renjie,Zhao Meng,Cui Xuanxuan,Xu Yukun,Qiao Xuguang

Fructans and oligofructose are usually used as prebiotics without any limitation in functional food or food ingredients. The degree of polymerization (DP) of polysaccharides affects the utilization of probiotics. Garlic is rich in fructans. The objective of this study was to extract and purify polysaccharides from garlic, analyze its composition, hydrolyze them using HCl, and then evaluate the prebiotic potential of the garlic neutral polysaccharides (GPs) before and after hydrolysis. GPs were 6.57 × 103 Da with a composition of fructose and glucose at a ratio of 4:1. After acid hydrolysis, low molecular weight fraction in garlic oligofructose (GOs) may be eliminated through ultrafiltration. The content of oligosaccharides with an average DP < 10 increased from 15 to 75%. GPs and GOS had a stronger resistance to acid conditions in human stomach than fructooligosaccharide, and GOs showed better prebiotic properties on the growth of lactobacilli than GPs. This study evaluates the prebiotic potential of the garlic frutctans and oligosaccharides mixtures obtained by acid hydrolysis, which may be used as an ingredient in functional food and nutraceutical products.

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JOURNAL OF CHROMATOGRAPHY A · 2021 · IF 4.759

Sustainable hydrophilic ultrasmall carbonaceous spheres modified by click reaction for high-performance polymeric ion chromatographic stationary phase

Yuqing Li,Sha Liu,Qiaoyan Zhang,Wan Gong,Hua Yin,Bo Yang,Luping Qin,Qiming Zhao,Yan Zhu

Novel poly(ethylvinylbenzene-divinylbenzene) (EVB-DVB) agglomerated with ultrasmall carbonaceous spheres (UCSs) anion-exchange packings for ion chromatography (IC) were constructed. Hydrophilic UCSs with mean sizes of 62–98 nm were synthesized in quantity by the polydiallyl dimethyl ammonium chloride aided hydrothermal carbonization of fructose. The green strategy based on the thiol-ene click reaction with cysteamine in aqueous system was first designed for the hyperbranched polyquaternary amine (HPA) grafting of UCSs with negligible damage on their monodispersity. The HPA modified UCSs were evenly distributed on sulfonated EVB-DVB substrate to form one uniform layer of functional nanospheres without observable coagulum. Seven typical anions ( F − , Cl − , NO 2 − , Br − , NO 3 − , SO 4 2- and PO 4 3− ) were baseline separated on constructed packing in 5 min with high efficiencies in the range of 44,800–71,100 plates m   −   1 . The rapid separation of polarizable anions, small organic acids and saccharides could be also accomplished under isocratic elution with competitive peak symmetry and efficiency. Good reproducibility was demonstrated by consecutive injection. Thiosulfate in water reducer was further detected on prepared packing in 4 min with detection limit of 0.04 mg L   −   1 (S/ N  = 3) and good repeatability.

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DYES AND PIGMENTS · 2021 · IF 4.889

A click-induced fluorescence-quenching sensor based on gold nanoparticles for detection of copper(Ⅱ) ion and ascorbic acid

Shijun Lin,Shuwen Liu,Guofei Dai,Xiaojin Zhang,Fan Xia,Yu Dai

Gold nanoparticles (AuNPs), as one of the major tools of fluorescence-quenching sensors, have been widely used in biochemical analysis through fluorescence resonance energy transfer (FRET) effect. With the development of chemistry and biochemistry, reaction-based fluorescent sensors have attracted increasing attention because of their unique selectivity, high sensitivity and rapid detection. Here we report a click-induced fluorescence-quenching sensor based on AuNPs for detection of copper ion (Cu 2+ ) and ascorbic acid (AA). A fluorescent dye Rhodamine B-(CH 2 CH 2 O) 4 -azide (RB-PEG 4 -N 3 ) is conjugated to the surface of AuNPs via Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) in the presence of Cu 2+ and AA, leading to the fluorescence quenching of Rhodamine B. The sensor responds quickly (within less than 3 min). The fluorescent intensity linearly correlates with the concentration of Cu 2+ in the range of 0–108 μM. The limit of detection (LOD) for Cu 2+ is 5.8 μM. The concentration range for detection of AA is 0–3 mM. The LOD for AA is 0.13 mM. In addition, the application of the sensor is verified by performing detection in real samples such as fresh orange, juice, VC tablet, and lake water. This work expands the application of AuNPs-based fluorescence-quenching sensors for multi-component detection.

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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 46 ·期 2 ·877-882 · IF 3.591

Orange-emissive N,S-co-doped carbon dots for label-free and sensitive fluorescence assay of vitamin B12

Pengfei Fan,Can Liu,Congcong Hu,Feifei Li,Xi Lin,Fubing Xiao,Hao Liang,Le Li,Shengyuan Yang

Nitrogen and sulfur co-doped carbon dots (N,S-CDs) with strong orange fluorescence were fabricated through a facile hydrothermal method using o-phenylenediamine and thiourea as precursors. The N,S-CDs exhibited excitation-independent photoluminescent behavior with excellent stability. The largest emission peak at 565 nm occurred at an excitation wavelength of 420 nm, and the quantum yield (QY) was 14.3%. It was found that the absorption spectra of vitamin B12 (VB12) overlaps with the emission peak of the N,S-CDs to a large extent, and based on the inner filter effect (IFE) between VB12 and N,S-CDs, a label-free and sensitive detection method of VB12 in drugs was established. Under optimal conditions, the concentration of VB12 exhibited a satisfactory linear correlation with the fluorescence quenching degree ΔF/F0 of the reaction system at 565 nm in the range of 0.25–20 μM, and the detection limit was 77.5 nM. The N,S-CDs with orange fluorescence emission show huge potential for use in the field of biological analysis.

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