Frontiers in Chemistry
·
2021
·
IF 5.221
Liu Can,Zhang Liming,Tan Li,Liu Yueping,Tian Weiqian,Ma Lanqing
In this study, we immobilized pectinase preparation on porous zeolite ZSM-5 as an enzyme carrier. We realized this immobilized enzyme catalyst, pectinase preparation@ZSM-5, via a simple combined strategy involving the van der Waals adsorption of pectinase preparation followed by crosslinking of the adsorbed pectinase preparation with glutaraldehyde over ZSM-5. Conformal pectinase preparation coverage of various ZSM-5 supports was achieved for the as-prepared pectinase preparation@ZSM-5. The porous pectinase preparation@ZSM-5 catalyst exhibited ultra-efficient biocatalytic activity for hydrolyzing the β-glycosidic bonds in the model substrate 4-nitrophenyl β-D-glucopyranoside, with a broad operating temperature range, high thermal stability, and excellent reusability. The relative activity of pectinase preparation@ZSM-5 at a high temperature (70 °C) was nine times higher than that of free pectinase preparation. Using thermal inactivation kinetic analysis based on the Arrhenius law, pectinase preparation@ZSM-5 showed higher activation energy for denaturation (315 kJ mol−1) and a longer half-life (62 min−1) than free pectinase preparation. Moreover, a Michaelis–Menten enzyme kinetic analysis indicated a higher maximal reaction velocity for pectinase preparation@ZSM-5 (0.22 µmol mg−1 min−1). This enhanced reactivity was attributed to the microstructure of the immobilized pectinase preparation@ZSM-5, which offered a heterogeneous reaction system that decreased the substrate–pectinase preparation binding affinity and modulated the kinetic characteristics of the enzyme. Additionally, pectinase preparation@ZSM-5 showed the best ethanol tolerance among all the reported pectinase preparation-immobilized catalysts, and an activity 247% higher than that of free pectinase preparation at a 10% (v/v) ethanol concentration was measured. Furthermore, pectinase preparation@ZSM-5 exhibited potential for practical engineering applications, promoting the hydrolysis of β-glycosidic bonds in baicalin to convert it into baicalein. This was achieved with a 98% conversion rate, i.e., 320% higher than that of the free enzyme.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Yun Lin,Xinyi Gong,Yangcan Chen,Xiaoli Wu,Dongfei Lu,Jingjing Yu,Rengui Weng,Yu Zhang,Fanan Wang,Gang Xu
The electrochemical oxidation of HMF (HMFOR) to FDCA presents a promising alternative to the anodic oxygen evolution reaction (OER) in water electrolysis, offering reduced energy consumption and enhanced safety. However, achieving efficient FDCA production is hindered by the instability of HMF in alkaline media and the critical challenge of generating and stabilizing the high-valence metal active centers required for oxidizing the less reactive alcohol group in HMF at practical rates and potentials. This study addresses this challenge by constructing a Co(OH)2/Cu(OH)2 heterostructure on copper foam (CF) via a facile two-step synthesis. Comprehensive characterization, including in situ Raman spectroscopy, reveals significant electron transfer from Co to Cu within the heterostructure. This electronic interaction elevates the oxidation state of Co, thereby facilitating the generation of high-valence CoO2 and enhancing its stability compared to that of pure Co(OH)2. Consequently, the Co(OH)2/Cu(OH)2/CF electrode exhibits a high current density of 200 mA·cm–2 at 1.4 V vs RHE in 20 mmol/L (mM) HMF, along with nearly 100% carbon balance within 60 min. Mechanistic studies confirm that the stabilized CoO2 centers promote strong adsorption of HMF, particularly activating the alcohol group for efficient oxidation to FDCA. This work provides a viable electronic structure modulation strategy for stabilizing high-valent metal centers through interfacial electronic modulation toward efficient biomass electrooxidation.
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Mengchuan Li,You Zhou,Tongsheng Zhang,Rensheng Li
The sluggish advancement in technology for the recovery of rare earth elements from secondary resources can be largely attributed to an inadequate understanding of the thermodynamic properties of cerium oxide-based slag systems. This study systematically investigates the phase equilibrium of the Ce 2 O 3 -CaO-SiO 2 -5 wt% MgO quaternary system at 1500 °C and 1600 °C. High-temperature equilibrium experiments followed by rapid quenching were conducted, and phase assemblages were characterized by XRD, SEM and EPMA. For the first time, the results accurately determined the isothermal liquidus lines for the first time and identified the stable regions of key phases such as SiO 2 , Ce 2 Si 2 O 7 , CaO·2Ce 2 O 3 ·3SiO 2 , CaO·Ce 2 O 3 ·2SiO 2 , the Ce-doped dicalcium silicate (i.e., (Ca, Ce) 2 SiO 4 ), and the monticellite (i.e., CaMgSiO 4 ), as well as their coexistence relationships. Furthermore, the isothermal sections at 1500 °C and 1600 °C were constructed based on experimental data and fundamental thermodynamic principles. This study not only fills a critical gap in the thermodynamic database for rare-earth slag systems but also provides a theoretical basis for optimizing slag design and enhancing cerium recovery from waste slags.
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产品关联
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高影响因子
JOURNAL OF PINEAL RESEARCH
·
2021
·Vol. 71
·期 3
·e12765
·
IF 13.007
Jinpeng Wu,Zengqi Tan,Hongjiao Li,Meixuan Lin,Yazhuo Jiang,Liang Liang,Qilong Ma,Junjie Gou,Lulu Ning,Xiang Li,Feng Guan
Melatonin helps to maintain circadian rhythm, exerts anticancer activity, and plays key roles in regulation of glucose homeostasis and energy metabolism. Glycosylation, a form of metabolic flux from glucose or other monosaccharides, is a common post-translational modification. Dysregulated glycosylation, particularly O-GlcNAcylation, is often a biomarker of cancer cells. In this study, elevated O-GlcNAc level in bladder cancer was inhibited by melatonin treatment. Melatonin treatment inhibited proliferation and migration and enhanced apoptosis of bladder cancer cells. Proteomic analysis revealed reduction in cyclin-dependent-like kinase 5 (CDK5) expression by melatonin. O-GlcNAc modification determined the conformation of critical T-loop domain on CDK5 and further influenced the CDK5 stability. The mechanism whereby melatonin suppressed O-GlcNAc level was based on decreased glucose uptake and metabolic flux from glucose to UDP-GlcNAc, and consequent reduction in CDK5 expression. Melatonin treatment, inhibition of O-GlcNAcylation by OSMI-1, or mutation of key O-GlcNAc site strongly suppressed in vivo tumor growth. Our findings indicate that melatonin reduces proliferation and promotes apoptosis of bladder cancer cells by suppressing O-GlcNAcylation of CDK5.
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高影响因子
ACS Applied Bio Materials
·
2024
·
IF 4.6
Yujun Zhang,Peiling Zhang,Yan Lv,Jing Liu,Yiyu Zhou,Zibin Zhang,Jianying Huang
The increasing number of infections caused by pathogenic bacteria has severely affected human society. More and more deaths were originated from Gram-positive methicillin-resistant Staphylococcus aureus (MRSA) infection each year. The potential and excellent bacteriostatic activity and resistance to biofilm formation of pillar[5]arene with different functional groups attract important attention to further study the relationship between antimicrobial activity and cytotoxicity by varying the length of the hydrophobic chain, the number of positive charges, and the hydrophobic/hydrophilic balance of the molecule. In this work, four pyridinium-based cationic pillar[5]arene (PPs) with linear aliphatic chains of different lengths were synthesized. After systematic characterization, their inhibition activities against S. aureus were investigated. It revealed that PP6 (six methylenes in each linker) exhibited excellent inhibition activity against S. aureus (ATCC 6538) with a minimum inhibitory concentration (MIC) of 3.91 μg/mL and a minimum bactericidal concentration (MBC) of 62.50 μg/mL. As expected, PP6 exhibited the strongest antibiofilm ability and negligible antimicrobial resistance even after the 20th passage. A study of the action mechanism of selected PPs on the bacterial membrane depolarization and permeability by transmission electron microscopy (TEM) disclosed that the cationic pyridine groups of PPs inserted into the negatively charged bacterial membranes, thereby leading to membranolysis, cytoplasmic content leakage, and cell death. Importantly, PPs all showed very low toxicity to mammalian cells (L929 and HBZY-1), which provided a significant reference for the construction of hypotoxic antibacterial biomaterials for multiple drug-resistant bacteria based on pyridinium-grafted cationic macrocycles with controllable hydrophobic chain lengths.
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PubMed
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Jiarong Li,Zhe Liu,Guangfa Hu,Ruimin Gao,Ronglan Zhang,Jianshe Zhao
A series of hybrid catalyst PMoW@HKUST-1@ZSM-5-MCM-41 was prepared in which H 3 PMo 6 W 6 O 40 were supported in the pore of micro/mesoporous materials ZSM-5-MCM-41 and HKUST-1 by one-pot method. Five types of ZSM-5-MCM-41 were prepared and corresponding ODS catalysts PMOW@HKUST-1@ZSM-5-MCM-41 were synthesized. The prepared catalysts were characterized and the most efficient catalyst was selected by XRD, FT-IR, UV–vis, N 2 adsorption-desorption, SEM, TEM. The removal of DBT reached 98.13 % by using PMoW@HKUST-1@ZSM-5-MCM-41−2 under 60 °C with molecular oxygen as oxidant after 150 min. After desulfurization, the catalyst can be simply recovered and reused 7 times with an unnoticeable decrease in catalytic activity, indicating the successful combination of heteropolyacids and micro/mesoporous materials for desulfurization.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Shijie Gu,Yingyue Cui,Kaihua Wen,Shimou Chen,Jianling Zhao
Layered lithium/manganese-rich oxides (LMR) receive much attention due to its high specific capacity (∼300 mAh g -1 ). However, the serious capacity degradation during cycling hinders the commercial application of the LMR. Herein, 3-cyano-5-fluorophenylboronic acid (CFBA) was applied as an electrolyte additive for enhancing the cycling stability of LMR at high voltage. Linear sweep voltammetry (LSV), density function theory (DFT) calculations and the initial charge d Q /d V profiles indicate that the preferential oxidation of CFBA can improve the oxidative stability of electrolyte. By adding 0.7 wt% CFBA into standard (STD) electrolyte (1 M LiPF 6 in EC :EMC:DMC = 1:1:1, by weight), the LMR/Li half-cell delivered a discharge capacity of 245 mAh g -1 with a capacity retention of 88.4% after 200 cycles at 0.5C, while only 68 mAh g -1 with 25.2% retention in STD electrolyte. Further characterizations and theoretical calculation illustrate that CFBA can effectively eliminate the harmful HF, which improve the electrochemical performance . More importantly, the CFBA participates in the formation of a thin and uniform protective cathode-electrolyte interface (CEI) film on the surface of LMR, which effectively suppresses electrolyte decomposition and protects the structural integrity of LMR.
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高影响因子
ENERGY & FUELS
·
2022
·
IF 4.654
Jing Li,Suxia Ma,Rongji Cui,Nuo Xu,Ting Pei
Solid waste fly ash can encroach on land, contaminate the environment, and jeopardize human health. An alkali fusion method combined with a hydrothermal method was adopted to prepare fly ash-derived ZSM-5 molecular sieves, and a series of Fe/ZSM-5 catalysts were also prepared to test their catalytic performance in NO oxidation with H2O2. Moreover, the characteristics of catalysts synthesized by fly ash, as well as the relationship between the structure and the catalytic activity, were analyzed in detail through multiple characterization approaches. The results gave important insights into the active sites of catalytic oxidation. They concluded that 10% Fe/ZSM-5 had the best catalytic activity in which Fe sites and Brønsted acid sites collectively provided the catalytic functionality, and 92% NO removal efficiency was obtained achieved under optimal experimental conditions. This work provided a new way for recycling fly ash and developing low-cost catalysts for NO removal.
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高影响因子
JOURNAL OF COORDINATION CHEMISTRY
·
2018
·
IF 1.703
Zi-Mei Ding,Wen-Li Cao,Xiao-Jing Hang,Xiao Ma,Hui Zheng,Kang-Zhen Xu,Jie Huang
The green nitrogen-rich coordination compound Cd(SCZ)2(AFT)2 (1) (AFT =4-amino-3-(5-tetrazolate)-furazan and SCZ = semicarbazide) was first synthesized and characterized by EA and Fourier Transform Infrared (FT-IR). The single crystal was cultivated and determined with X-ray diffraction. It revealed that 1 crystallizes in the monoclinic space group P21/c. A Cd2+ ion is coordinated by four N atoms and two O atoms to form a distorted octahedral structure. Among them, two nitrogen atoms are from the two AFT ions and the other four atoms are from two SCZ molecules. The thermal decomposition behavior of 1 was studied with DSC and TG-DTG methods. The apparent activation energy (E), thermal stability, and safety parameters (T
SADT, T
TIT, and T
b) were calculated for 1. Moreover, entropy of activation (ΔS
≠), enthalpy of activation (ΔH
≠), free energy of activation (ΔG
≠), specific heat capacity (C
p), and impact sensitivity were also discussed in detail.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Jin Wang,Lin Zhou,Jiali Bei,Mengyuan Xie,Xiting Zhu,Tingting Chen,Xiaomei Wang,Yukou Du,Yong Yao
In this work, the ultrasensitive photoelectrochemical (PEC) sensor for the detection of bovine hemoglobin (BHb) was developed based on water-soluble pillar[5]arenes (WP5) functionalized gold nanoparticles (Au NPs) and bismuth oxybromide (BiOBr) nanoflowers (Au@WP5/BiOBr). The photoelectrical signal of dopamine (DA) was decreased after adding the different concentrations of BHb due to the formation of hydrogen bond between the COOH groups of BHb molecules and the NH 2 group of DA, which could achieve the indirect detection of BHb. Benefiting from the photo-generated electron-holes of BiOBr nanoflowers, the localized surface plasmon resonance (LSPR) effect of Au NPs, the host–guest interaction of WP5 between and DA, the PEC sensor showed a specifically recognize toward BHb with a wide detection range of 1.0 × 10 −11 –1.0 × 10 −1 mg/mL and a detection limit of 4.2 × 10 −12 mg/mL (S/N = 3). Additionally, the proposed PEC sensor also displayed good stability, remarkable selectivity and provided a promising strategy of design pillar[5]arenes functionalized photoelectric activity nanomaterials for PEC sensing application.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Linhuo Gan,Li Lyu,Tianruo Shen,Shuai Wang
Sulfonic acid-functionalized lignin-derived mesoporous carbon (LDM C-S O 3 H) was prepared using phenolation and evaporation induced self-assembly method followed by sulfonation. The obtained LDM C-S O 3 H bearing sulfonic acid density of 0.6528 mmol/g possessed a well-ordered two-dimensional hexagonal mesoporous characteristics. A 5-hydroxymethylfurfural (5-HMF) yield of 98.0% with a full fructose conversion was obtained using LDM C-S O 3 H as catalyst at 140 °C for 2 h in DMSO. Reactive kinetics studies revealed that fructose conversion in DMSO without catalyst or catalyzed by LDMC-SO 3 H may obey pseudo-first-order kinetics, and the activation energy of latter (72 kJ/mol) was much lower than that of former (114 kJ/mol). Adsorption kinetics studies indicated that almost no 5-HMF adsorbed onto LDM C-S O 3 H probably had a great contribution to the high selectivity of up to 98.0%, while the fructose adsorption on LDM C-S O 3 H was a diffusion-controlling adsorption process with more following Bangham kinetic model and Weber-Morris kinetic model owing to the characteristics of ordered mesostructure of LDM C-S O 3 H. Moreover, LDM C-S O 3 H exhibited superior reusability and stability in catalytic performance with a 5-HMF yield higher than 88.0% in six runs probably due to the synergistic effect of mesopore structure with a special surface and -SO 3 H groups with a relatively high content. These research results will contribute to a better understanding of structure-performance relationship of LDM C-S O 3 H used as an efficient catalyst in the fructose-to-5-HMF transformation as well as the high-value utilization of lignin in the field of catalysis.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Deyu Si,Meihua Zhu,Ronghui You,Yuqin Li,Ting Wu,Tian Gui,Na Hu,Izumi Kumakiri,Xiangshu Chen,Hidetoshi Kita
Aluminum-rich ZSM-5 zeolite membranes are prepared on α-alumina support through organic template free precursor gels by secondary hydrothermal synthesis , microstructure of the membrane through the different Si/Al ratio and alkali metal fluoride synthesis gel are discussed in this work. Alkali metal fluorides have a significant influence on the synthesis of aluminum-rich ZSM-5 zeolite membranes without organic template, which are realized by the synergistic reaction of the “bridging” and “salting-out” effects. Sodium fluoride and potassium fluoride could produce dense and needle-like zeolites layer on the supports by an extremely low Si/Al ratio synthesis gel (Si/Al <10). When the Si/Al ratio of the initial synthesis gel is 18.52, the compact and prismatic ZSM-5 zeolites are fully covered on the supports with sodium fluoride, potassium fluoride or lithium fluoride. There are few of ZSM-5 zeolites could form on the support by cesium fluoride containing synthesis gel.
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高影响因子
危险品化学品经营许可证（带存储）