ANALYTICA CHIMICA ACTA
·
2018
·
IF 5.123
Shi-Fan Xue,Jing-Fei Zhang,Zi-Han Chen,Xin-Yue Han,Min Zhang,Guoyue Shi
A novel type of stimuli-responsive fluorescent polymers has been developed via the self-assembly of riboflavin-5′-phosphate (RiP) as ligand and europium (III) (Eu 3+ ) as central metal ion coordinated with the ligand. The as-prepared RiP/Eu 3+ coordination polymers (RiP/Eu 3+ CPs) are smart and multifunctional for respectively responding to chemical and physical stimuli, in which RiP acts as the stimuli-responsive fluorescent signal indicator. For sensing chemical stimuli, 2,6-pyridinedicarboxylic acid (DPA, an anthrax biomarker) having higher bonding force towards Eu 3+ can grab it from smart RiP/Eu 3+ CPs through competition reaction, resulting in the release of RiP for highly sensitive and selective DPA monitoring in a mix-and-read fluorescent enhancement format, and the detection limit is as low as 41.5 nM. Density functional theory (DFT) calculations has been also performed to verify the DPA sensing principle. For sensing physical stimuli, the smart RiP/Eu 3+ CPs can be acting as a novel sensory probe for the determination of temperature from 10 °C to 40 °C based on the thermal-induced disruption of the binding between Eu 3+ and RiP and the disassembly of the smart RiP/Eu 3+ CPs accompanying with the recovery of the fluorescence of RiP. This work establishes an effective platform for multifunctional sensing of chemical and physical stimuli utilizing both smart lanthanide nanoscale coordination polymers (LNCPs) and novel sensing strategies.
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REACTIVE & FUNCTIONAL POLYMERS
·
2024
·
IF 4.5
Yaxue Xie,Pingxiong Cai,Huining Xiao,Yuanfeng Pan
In this work, a dual-responsive hydrogel for sustainable release of drug was prepared using chitosan grafted with PBA as substrate to form semi-interpenetrating polymer networks (S-IPN) via free-radical crosslinking polymerization of acrylic acid in the presence of MBAA as a crosslinker and KPS as an initiator as well as Fe 3+ .ions introduced. The results from comprehensive characterization indicated that the as-prepared hydrogel possesses cavity structure with the pores of varying sizes, thus facilitating the accommodation of 5-fluorouracil as a model drug. In addition, the swelling behavior of the hydrogels in different pH buffers and glucose solutions was also investigated. As expected, the prepared hydrogels are pH and glucose responsive due to PAA and phenylboronic acid incorporated into the hydrogel, which enables the slow or sustainable release of drug. Moreover, the release processes were fitted with various kinetic models whereas the release was better described by Korsmeyer-Peppas model or the drug release is mainly governed by the release mechanism of the hydrogel is primarily driven by Fickian diffusion from a mechanical point of view. Hydrogel loaded with drug was found to have good antibacterial effects against E. coli and S. aureus, leading to the potential for various medical-related applications.
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APPLIED CLAY SCIENCE
·
2024
·
IF 5.3
Yanan Wei,Yunlei Zhang
A novel halloysite (Hal) based acidic catalyst was synthesized by anchoring functional alkyl group and Cr site and catalyzed the selective conversion of mannose to 5-hydroxymethylfurfural (HMF) in NaCl-H 2 O/dimethyl sulfoxide/methyl isobutyl ketone (MIBK) biphasic system. Herein, adjusting the hydrophilicity/hydrophobicity of catalyst by modifying the octyl group can facilitate the HMF yield. The density functional theory (DFT) calculation and in-situ FT-IR results revealed that increasing the hydrophobicity of catalyst surface weakened the interaction between HMF, water molecule and acid sites and inhibited the rehydration of HMF. Moreover, the synergistic effect between Cr and sulfonic group active sites remarkedly promoted the isomerization of mannose to fructose and the dehydration of fructose to HMF, and the 48.1% yield of HMF was obtained. This study provides references for the high value conversion of hemicellulose with the high efficiency reaction system.
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FUEL
·
2025
·
IF 7.5
Mingfu Li,Pingjun Zhang,Shuanglan Hu,Douyong Min,Jingjie Tang,Yingchuan Zhang,Liqun Jiang
The green synthesis of 5-hydroxymethylfurfural (HMF) from carbohydrates is a significant step for the production of sustainable fuels and fine chemicals, where the solvent plays an important role in terms of conversion efficiency and process sustainability. This work reports the bifunctional use of ternary deep eutectic solvents (TDESs), as both the solvent and catalyst, in the dehydration of fructose to HMF. A series of phenolic acids are used as hydrogen bond donors (HBDs) in TDESs. The combination of choline chloride–1,4-butylene glycol– p -hydroxybenzene propanoic acid (ChCl–BDO–PH) catalysed the quantitative conversion of fructose to obtain the highest HMF yield of 90.2%. Nuclear magnetic resonance and 3D-fluorescence spectroscopy analysis indicated that there were no humins polymers accumulation and it possibly formed the soluble micro-molecules humins byproducts. Moreover, HMF could be readily separated from TDESs, which allowed the stable recycling of TDESs for five recycles. Density functional theory calculations implied that a lower energy of hydrogen bond between TDESs and fructose promoted the fructose conversion and HMF formation, which is due to the methoxy group and side chain structure of phenolic acid that may reduce the ionization activity of hydrogen ions in the carboxyl group, thus reducing the hydrogen bond between TDESs and fructose. This work provides a novel alternative to traditional Brønsted acid towards the greener production of HMF.
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Inorganic Chemistry Frontiers
·
2024
·Vol. 11
·期 8
·2479-2488
·
IF 6.1
Yiwei Zhao,Chao Zhang,Shuangxi Xing,Zuhang Jin,Tingting Xiao
Biomass upgrading by electrochemical means is of great scientific significance due to the environmentally friendly procedures and low energy consumption costs. Herein, electro-oxidation (ECO) of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) and electro-reduction (ECR) to 2,5-furandimethanol (BHMF) with high yield have been studied on CuNi-based bimetallic catalysts. Ni(OH)2-NCF and Cu-NCF achieved 99% and 96.5% yields at a HMF concentration of 10 mM in ECO and ECR, respectively. During ECO, the presence of Cu2O in the catalyst facilitated the adsorption of HMF, and the formed NiOOH in its vicinity promoted the proton coupled electron transfer process and thus resulted in the fast capture and removal of H protons. The presence of Cu–O–Ni linkages in the Ni(OH)2-NCF electrocatalyst was beneficial for the formation of Ni3+ active sites. During ECR, the synergistic effect between Cu and Ni species also contributed to the generation and spillover of Hads species and then enhanced the reactivity.
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Cell Reports Medicine
·
2024
·
IF 11.7
Huidi Wang,Jie Li,Guangyan Wu,Xiaofei Lin,Jiaying Chen,Jingru Liang,Jiahui Zhang,Xiaoxia Luo,Hongyun Mao,Jiahui Xie,Zhuang Li,Hongwei Zhou,Kaiyu Xu,Jia Yin,Yan He
The gut permeability significantly increases after ischemic stroke, partly due to disrupted mucosal barrier, but the mechanism remains elusive. Here, we found that the mucus disruption starts at 2 h post stroke, whereas goblet cell functions remain intact. Meanwhile, the flagellated bacteria Helicobacter thrives and penetrates in the mucus layer. Elimination of the mucosal microbiota or transplantation of Helicobacter in germ-free mice reveals an important role of the mucosal microbiota in mucus disruption. The bacterial invasion is due to downregulated Toll-like receptor 5 (TLR5) and its downstream products flagellin-specific IgA and antimicrobial peptides. Knockdown of intestinal TLR5 increases the abundance of flagellated bacteria and exacerbates mucus injury. Intestinal TLR5 is downregulated by the activation of sympathetic nerve. Serum noradrenaline level is positively associated with flagellin level in patients with stroke and patients’ prognosis. These findings reveal a neural pathway in which the sympathetic nerve disrupts the mucosal barrier, providing potential therapeutic targets for stroke injury.
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Molecular Catalysis
·
2024
·
IF 3.9
Yifei Chen,Xinnan Zhao,Chen Xin,Xiuqin Dong,Hao Gong
This work explored the role of defective sites on the hydroformylation of n-butene through ligand regulation. The investigation examined the effect of modulator properties on defect sites and rhodium loading, and optimized the H 2 BDC/modulator ratio to improve catalyst activity. Atomically dispersed Rh is anchored to these highly dispersed defect sites, effectively preventing aggregation and thereby enhancing hydrogenation ability. Under optimal conditions, the catalyst achieved a conversion of 96.9 %, with an overall aldehyde selectivity of 90 %. DRIFTS analysis provided compelling evidence that Rh(CO) 2 and HRhCO species were formed on 1Rh/MOF-5-HBC, improving CO insertion capability. This study highlights the significance of MOFs as catalyst supports in enhancing performance through defect engineering. The ability of the modulator to induce defect formation was measured by p K a. Meanwhile, it has been discovered that the length differences between the modulator and the MOF organic ligand can have a significant impact on the stability of defective MOFs.
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
·
2024
·
IF 3
Zhang Cong,Guo Yan,Xiao Libai,Gao Hongxu,Zhao Fengqi,Huang Jie,Lü Xingqiang,Ma Haixia
Three 4-(1 H -tetrazole-5-yl-amino)-1,2,4,5-tetrazine-1-one (TATzO) metal salts, K 2 (TATzO)(H 2 O) ( 1 ) and Mg(TATzO)(H 2 O) 6 ·2H 2 O ( 2 ) and Sr(TATzO)(H 2 O) 4 ( 3 ), were synthesized and characterized using Fourier transform infrared (FTIR), elemental analysis, single-crystal X-ray diffraction, and powder X-ray diffraction patterns. The crystal structure and hydrogen bonding interactions have been analyzed. It turns out that 1 and 3 crystallize into a three-dimensional topological network and have strong π – π stacking and hydrogen bonding interactions. Furthermore, the geometric optimization of 1 – 3 was performed using B3LYP-D3/def2svp in Gaussian 16 software package and then analyzed by reduced density gradient. The thermal behavior was conducted using differential scanning calorimetry and thermogravimetric (TG). The decomposition temperature of the three complexes exceeds 250 °C, much higher than that of TATzO (230 °C). The thermal decomposition products of 1 were further studied using thermogravimetric-Fourier transform infrared-mass spectrometry (TG/FTIR/MS). The impact sensitivity test indicated that making complexes can help decrease the sensitivity of the original energetic ligand. Graphical abstract
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TALANTA
·
2024
·
IF 5.6
Xianhong Wang,Jiuying Cui,Qinghua Gong,Lu Zheng,Dandan Liu,Guangming Nie
A novel electrochemiluminescence (ECL) sensor for the detection of Hg 2+ is constructed based on the synthesized cerium stannate/poly(5-formylindole) (Ce 2 Sn 2 O 7 /P5FIn) composite and multiple DNA signal amplification techniques, including strand displacement amplification (SDA) reaction and hybridization chain reaction (HCR). On the one hand, the combination of Ce 2 Sn 2 O 7 and P5FIn improves the electrochemical reaction rate between Ce 2 Sn 2 O 7 and the co-reactant, and significantly enhances the ECL signal. On the other hand, compared to P5FIn, Ce 2 Sn 2 O 7 /P5FIn has a larger specific surface area to facilitate the effective fixation of hairpin DNA H1. The target Hg 2+ is bound to the DNA strand (mDNA) rich in thymine bases (T) by T-Hg 2+ -T. Subsequently, with the assistance of polymerase (phi29 DNA) and restriction endonuclease (Nt. Bbv CI), strand displacement amplification (SDA) reaction is triggered to generate a large number of simulated target (MT). Hairpin DNA H1 captures MT, which then further triggers a hybridization chain reaction (HCR) to produce long strand DNA (dsDNA) rich in cytosine. Finally, a large amount of Ag + is introduced through C–Ag + -C, which is used as a co-reaction accelerator of Ce 2 Sn 2 O 7 –K 2 S 2 O 8 system to significantly enhance the ECL signal strength. Under optimal conditions, the constructed ECL sensor can detect Hg 2+ in a wide linear response range of 1.0 fM-100 nM, with a detection limit of 0.30 fM. The sensor also has high sensitivity and good applicability in the detection of seawater samples.
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Nano Research
·
2024
·
IF 9.5
Jiang Xiaoqian,Qu Aihua,Xu Xinxin,Kuang Hua,Liu Liqiang,Xu Chuanlai
Paclitaxel (PTX), methotrexate (MTX), and 5-fluorouracil (5-FU) are commonly-used small molecule anti-tumor drugs for breast cancer. Unfortunately, drug resistance occurs with long-term treatment or excessive use, and the high concentrations of PTX, MTX, and 5-FU in patients may lead to side effects with dose-limiting toxicities, such as myelosuppression, hepatotoxicity, and peripheral neuropathy. Therefore, concentration monitoring of PTX, MTX, and 5-FU in clinical treatment is very important. We prepared highly sensitive and specific monoclonal antibodies using several haptens, and established a multiple paper-based sensor utilizing optical signals of gold nanoparticles, which simultaneously detected PTX, MTX, and 5-FU in human plasma or urine with 10 min. A portable scanner for quantitative detection in plasma and urine samples was used, and the calculated limit of detection (cLOD) values were 0.002 and 0.142 µg/mL for PTX, 0.187 and 0.976 ng/mL for MTX, and 0.057 and 0.128 µg/mL for 5-FU, respectively. In the recovery test, the recovery rates and the coefficient of variation were 85.84%–108.81% and 1.23%–8.80%, respectively, indicating the reliability and accuracy of the multiple gold immunochromatographic strip (GIS). In addition, for the determination of collected clinical plasma samples, the correlation between the test data of the multiple GIS and liquid chromatography–tandem mass spectrometry (LC–MS/MS) was good. Therefore, the developed multiple GIS could be applied to the rapid detection of PTX, MTX, and 5-FU in different clinical samples.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Kaijun Dong,Jun Zhang,Weimin Luo,Lin Su,Zhilin Huang
An acid functionalized porous organic hyper-cross-linked polymer (HCP) derived from benzene monomer was prepared for catalytic dehydration of carbohydrates into 5-hydroxymethyl furfural (HMF) in a DMSO solvent. Systematic characterizations of the HCP catalysts including essential structural properties, sulfur content and acid amount, were identified by XRD, XPS, FESEM, Raman, NH 3 -TPD, TGA, nitrogen physisorption and elemental analysis. Optimization of reaction parameters such as acid amount, solvent, substrate type, temperature and catalyst dosage, and comparison with reported solid acids were systematically investigated. The results showed that sulfonated HCP materials were highly active in fructose dehydration, which could afford a highest HMF yield of 96.7% at almost 100% fructose conversion in 30 min. Furthermore, the catalyst presented satisfied performance and stability during recycling tests. More importantly, the sulfonated HCP catalysts also exhibited promising activity in hydrolytic reaction, esterification and transesterification for platform chemicals production in biomass transformation.
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Waste and Biomass Valorization
·
2017
·Vol. 9
·期 4
·657-668
·
IF 1.337
He Rong,Huang Xiaolin,Zhao Peng,Han Bin,Wu Tinghua,Wu Ying
Phosphotungstic acidified titanium–zirconium dioxide catalysts with different loading of phosphotungstic acid (HPA) were synthesized by a precipitation-impregnation method. The phosphotungstic acidified solid acids were characterized by fourier transform infrared spectrometer (FT-IR), X-ray diffraction (XRD), ammonia temperature programmed desorption (NH 3 -TPD), X-ray photoelectron spectroscopy (XPS) and transmission electron microscope (TEM) techniques. And the catalytic performance of HPA/TiO 2 –ZrO 2 was explored for glucose degradation to 5-hydroxymethylfurfural (5-HMF) in biphasic system, such as the loading of HPA, the molar ratio of TiO 2 to ZrO 2 , reaction time, temperature, amount of catalyst, the volume ratio of V
NaCl(aq) / V
THF and magnetic stirring speed. It was found that activity of the catalyst was related to the amount and density of acid site. The optimized yield of 51.3% for 5-HMF and the optimum conversion rate of 95.4% for glucose were achieved by 5% HPA/TiO 2 –ZrO 2 . Meanwhile, recycling performance of the catalyst was investigated. And the catalyst had good thermal stability, the yield of 5-HMF was 41.2% and the conversion rate of glucose remained at 85.4% after five cycles.
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