Catalysts
·
2019
·Vol. 9
·期 10
·869
·
IF 3.444
Xinyu Liu,Meihuan Lu,Xuan Wang,Juyou Lu,Jianxin Yang
For decades the steric effect was still ambiguously understood in catalytic benzylation reactions of arenes with benzyl alcohol, which limited the green synthesis of phenylmethane derivates in industrial scale. This research applies a series of silica–alumina beta zeolites to systematically evaluate factors like catalyst porosity, reactants molecule size, and reaction temperature on catalytic benzylation. First, a suitable hierarchical beta zeolite catalyst was screened out by X-ray powder diffraction, N2adsorption−desorption, and probe benzylation withp-xylene. In the following substrates expanding study, for a typical benzylation of benzene, it showed extraordinary performance among literature reported ones that the conversion was 98% while selectivity was 90% at 353 K only after 10 min. The steric effect of aromatics with different molecular sizes on benzylation was observed. The reaction activities of four different aromatics followed the order: benzene > toluene >p-xylene > mesitylene. Combined with macroscopic kinetic analysis, this comprehensive study points out for the first time that the nature of this steric effect was dominated by the relative adsorption efficiency of different guest aromatic molecules on the host zeolite surface.Keywords:benzylation;benzyl alcohol;hierarchical zeolite;steric effect;green catalysis
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JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Rui Chen,Changjun Yang,Quanquan Zhang,Bingguang Zhang,Kejian Deng
A new iron tetra(2,3-bis(butylthio)maleonitrile)porphyrazine (FePz(SBu) 8 ) has been synthesized, then it was loaded on H-ZSM-5 zeolite to obtain a supported biomimetic photocatalyst H-ZSM-5/FePz(SBu) 8 . Using H 2 O 2 as oxidant, the photocatalytic selective oxidation of glucose in water under visible light (λ ≥ 420 nm) irradiation was carried out in presence of H-ZSM-5/FePz(SBu) 8 . Under such conditions, the glucose can be efficiently converted into value-added chemicals such as glucaric acid, gluconic acid, arabinose, glycerol and formic acid . More importantly, in comparison with pure FePz(SBu) 8 and pure H-ZSM-5 zeolite, the H-ZSM-5/FePz(SBu) 8 exhibited a higher photocatalytic activity for glucose oxidation and the formation of glucaric acid was observed only when H-ZSM-5/FePz(SBu) 8 was used, deriving from the synergistic effect between FePz(SBu) 8 and H-ZSM-5 zeolite. Some reaction parameters of glucose oxidation catalyzed by the H-ZSM-5/FePz(SBu) 8 were discussed, such as loading amount of FePz(SBu) 8 , H 2 O 2 :glucose ratio, glucose concentration, and so on. It was demonstrated that the Soret-band of FePz(SBu) 8 contributed more to the visible light photocatalytic activity than the Q-band during the photocatalytic process. The stability of H-ZSM-5/FePz(SBu) 8 during the photocatalytic process was further evaluated by the reusability test. In addition, the generation of reactive oxygen species was determined by electron spin resonance (ESR) technology and scavenger experiments. A possible reaction pathway of glucose oxidation was also discussed.
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PHYTOMEDICINE
·
2024
·
IF 6.7
Zhenxiu Liu,Lin Chen,Mingyun Chen,Lang Linghu,Zhihua Liao,Min Chen,Guowei Wang
Background Farnesoid X receptor (FXR) is a vital receptor for bile acids and plays an important role in the treatment of cholestatic liver disease. In addition to traditional bile acid-based steroidal agonists, synthetic alkaloids are the most commonly reported non-steroidal FXR agonists. Sarmentol H is a nor-sesquiterpenoid obtained from Sedum sarmentosum Bunge, and in vitro screening experiments have shown that it might be related to the regulation of the FXR pathway in a previous study. Purpose To investigate the therapeutic effects of sarmentol H on cholestasis and to determine whether sarmentol H directly targets FXR to mitigate cholestasis. Furthermore, this study aimed to explore the key amino acid residues involved in the binding of sarmentol H to FXR through site-directed mutagenesis. Methods An intrahepatic cholestasis mouse model was established to investigate the therapeutic effects of sarmentol H on cholestasis. In vitro experiments, including Co-Ip and FXR-EcRE-Luc assays, were performed to assess whether sarmentol H activates FXR by recruiting the receptor coactivator SRC1. CETSA, SIP, DARTS, and ITC were used to determine the binding of sarmentol H to FXR protein. The key amino acid residues for sarmentol H binding to FXR were analyzed by molecular docking and site-directed mutagenesis. Finally, we conducted in vivo experiments on wild-type and Fxr −/− mice to further validate the anticholestatic target of sarmentol H. Results Sarmentol H had significant ameliorative effects on the pathological conditions of cholestatic mice induced with ANIT. In vitro experiments suggested that it is capable of activating FXR and regulating downstream signaling pathways by recruiting SRC1. The target validation experiments showed that sarmentol H had the ability to bind to FXR as a ligand (K D = 2.55 μmol/L) and enhance the stability of its spatial structure. Moreover, site-directed mutagenesis revealed that THR292 and TYR365 were key binding sites for sarmentol H and FXR. Furthermore, knockout of the Fxr gene resulted in a significantly higher degree of ANIT-induced cholestatic liver injury than that in wild-type cholestatic mice, and the amelioration of cholestasis or regulatory effects on FXR downstream genes by sarmentol H also disappeared in Fxr −/− cholestatic mice. Conclusion Sarmentol H is an FXR agonist. This is the first study to show that it exerts a significant therapeutic effect on cholestatic mice, and can directly bind to FXR and activate it by recruiting the coactivator SRC1.
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高影响因子
Current Protocols
·
2022
·Vol. 2
·期 6
·e432
·
IF 0
An-Di Liu,Zhao-Li Wang,Li Liu,Liang Cheng
The photoredox synthesis of C-5 (hetero)arylated uracil and uridine substrates with the corresponding diazonium salts is described. The coupling proceeds efficiently without protection of the hydroxyls at the ribose or pre-functionalization of the C5 position at the nucleobase. No transition-metal catalyst is used in this transformation, thereby avoiding metal contamination in the final products. The use of water as the medium also eliminates the impurities caused by the use of organic solvents. © 2022 Wiley Periodicals LLC. Basic Protocol 1 : Synthesis of 5-aryl and 5-heteroaryl uracil derivatives Basic Protocol 2 : Synthesis of 5-aryl uridine and deoxyuridine uridine derivatives
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Wei Shen,Liang Qiao,Juan Ding,Yongming Sui
Tailoring tantalum disulfide (TaS 2 ) electrocatalysts with tunable stacking architecture and phase structure is of great importance for advancement of hydrogen evolution reaction (HER). In this work, stacking architecture- and phase- modulated tantalum disulfide nanosheets are reported through a facile liquid phase synthesis strategy. Accordion-like nanosheets , vertical nanosheets and ultrathin nanosheets are named according to their obvious stacking architecture, and 1 T-2 H mixed phase structures containing different degrees of 2 H phases are realized. High-resolution transmission electron microscopy shows that there are obvious lattice defects in the nanosheets. Tantalum disulfide nanosheets synergistically integrate multiple advantages of nanostructure engineering, phase engineering and defect engineering. In the HER process, the ultrathin tantalum disulfide nanosheet structure is conducive to the in-plane electron transfer , and its close contact with the electrode surface makes the charge transfer faster and has the best HER activity. The overpotential of the ultrathin nanosheet electrocatalyst at 10 mA cm −2 is 280 mV. After 10,000 CV cycles and over 40 h of i-t test, the catalyst still has high stability in acidic media. Theoretical calculations show that the addition of 2 H phase structure and rich defects improves the intrinsic activity and active sites, and jointly promotes the improvement of HER performance. Our work integrates a variety of optimal regulation methods into TaS 2 nanosheets, providing a new idea for the construction of advanced electrocatalysts for water electrolysis.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Yibo Huo,Zhiqiang Wang,Xu Zhu,Yuting Lu,Siran Jin,Xiaodan Wu,Hui Zhang,Guanghui Tan,Yingxue jin
Immune checkpoint blockade (ICB) therapy faces major challenges including low clinical response rates, while traditional chemodynamic therapy (CDT) is highly dependent on intratumoral hydrogen peroxide (H₂O₂) levels. To address these limitations, we constructed a pH-responsive hyaluronic acid (HA)-based nanosystem (HA-Fc@ART) for targeted cancer therapy. This nanoplatform achieves tumor-specific delivery through the specific interaction between HA and CD44 receptors overexpressed on tumor cells. Upon accumulation in the acidic tumor microenvironment (TME), the nanosystem undergoes Schiff base bond hydrolysis to precisely release artemisinin (ART) and ferrocene (Fc), avoiding off-target toxicity. Fc catalyzes the cleavage of the endoperoxide bridge in ART to generate singlet oxygen ( 1 O₂) in an H₂O₂-independent manner. It simultaneously converts endogenous H₂O₂ into hydroxyl radicals (•OH) via the Fenton reaction. These dual pathways synergistically induce a reactive oxygen species (ROS) burst that efficiently eliminates cancer cells. Notably, HA-Fc@ART exhibits a high photothermal conversion efficiency of 35 ± 3%. The photothermal effect accelerates ROS production, and Fe(III) generated during the reaction depletes intracellular glutathione (GSH) to amplify oxidative damage. In vitro and in vivo experiments demonstrated that HA-Fc@ART possesses strong tumor-targeting ability. It effectively induces tumor immunogenic cell death (ICD) by releasing damage-associated molecular patterns (DAMPs). This process activates dendritic cell (DC) maturation, promotes macrophage M1 polarization, and enhances T cell infiltration into the TME. In the 4 T1 bilateral tumor model, the combination of HA-Fc@ART with photothermal therapy and anti-PD-L1 (αPD-L1) achieved complete ablation of primary tumors and significant inhibition of distant metastatic tumors. Histological analysis and hemolysis tests confirmed the nanosystem's excellent biosafety profile. This study provides a novel and efficient platform for improving the response rate of ICB therapy, offering new insights into the treatment of metastatic cancers.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Simin Wang,Huijuan Xiu,Dingwen Yin,Jinbao Li,Gengmei Liu,Yuxin Qin,Feiguo Hua,Qingjun Meng,Minzhe Wu,Mengxia Shen
Achieving high shielding effectiveness in electromagnetic shielding materials relies heavily on high conductivity, yet simultaneously enhancing the absorption loss remains a persistent challenge. Consequently, the study successfully creates efficient electromagnetic shielding composite films with a unique grape-like bunch structure of hollow nanosilver (HCAF) through layer-by-layer assembly. The utilization of poly(dopamine) (PDA) to anchor nanosilver granules (AgNPs) onto cellulose nanofibers (CNF) results in the formation of CNF@PDA@AgNPs. Subsequently, a surface protection etching method is employed to etch the AgNPs, resulting in hollow nanosilver (H-AgNPs) and the generation of CNF@PDA@H-AgNPs. A composite film featuring a grape bunch structure is fabricated by interweaving high aspect ratio CNF with CNF@PDA@H-AgNPs. A substantial quantity of H-AgNPs creates an abundant interface, while the grape bunch structure establishes an efficient conductive network. That enables the composite film to exhibit excellent impedance matching, excellent conductivity loss, abundant polarization loss, and multiple reflection loss. Therefore, the conductivity of the composite film with a thickness of 148.8 μm reaches 212660 S/m, with SET, SEA, and SER 89.56, 79.03, and 10.53 dB in the X band, significantly better than the 76.9, 55.55, and 21.41 dB of the solid AgNPs composite film. The composite film also exhibits remarkable thermal conductivity (The coefficients of in-plane and out-plane thermal conductivity are 4.61 and 0.17 W/(m·K), respectively), mechanical properties, and strain sensing capabilities, making it significant potential for applications in flexible electronics and other related fields.
研究领域:
材料科学
·
纳米技术
·
电磁干扰屏蔽
·
柔性电子
·
热管理
·
传感器
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2020
·Vol. 21
·期 15
·5347
·
IF 4.556
Xiao-Ran Jing,Huan Liu,Yao Nie,Yan Xu
Fe(II)/2-ketoglutarate-dependent dioxygenase (Fe(II)/2-KG DO)-mediated hydroxylation is a critical type of C–H bond functionalization for synthesizing hydroxy amino acids used as pharmaceutical raw materials and precursors. However, DO activity requires 2-ketoglutarate (2-KG), lack of which reduces the efficiency of Fe(II)/2-KG DO-mediated hydroxylation. Here, we conducted multi-enzymatic syntheses of hydroxy amino acids. Using (2s,3r,4s)-4-hydroxyisoleucine (4-HIL) as a model product, we coupled regio- and stereo-selective hydroxylation ofl-Ile by the dioxygenase IDO with 2-KG generation from readily availablel-Glu byl-glutamate oxidase (LGOX) and catalase (CAT). In the one-pot system, H2O2significantly inhibited IDO activity and elevated Fe2+concentrations of severely repressed LGOX. A sequential cascade reaction was preferable to a single-step process as CAT in the former system hydrolyzed H2O2. We obtained 465 mM 4-HIL at 93% yield in the two-step system. Moreover, this process facilitated C–H hydroxylation of several hydrophobic aliphatic amino acids to produce hydroxy amino acids, and C–H sulfoxidation of sulfur-containingl-amino acids to yieldl-amino acid sulfoxides. Thus, we constructed an efficient cascade reaction to produce 4-HIL by providing prerequisite 2-KG from cheap and plentifull-Glu and developed a strategy for creating enzymatic systems catalyzing 2-KG-dependent reactions in sustainable bioprocesses that synthesize other functional compounds.Keywords:Fe(II)/2-ketoglutarate-dependent dioxygenase;2-ketoglutarate generation;regio- and stereo-selective synthesis;hydroxy amino acids;sequential cascade reaction
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 28
·6963-6972
·
IF 5.16
Yanji Zhu,Huaiyuan Wang,Kai Jin,Jinlong Gong
A graphene-wrapped polyaniline nanoparticles film embedded in carbon cloth (CC/PANI/G) was fabricated and used as a 3D anodic electrocatalyst for oxidation of toluene methyl C−H groups. The methyl C−H bonds can be oxidized effectively at the CC/PANI/G anode with 99.9 % toluene conversion at a low applied voltage of only 1.0 V, which implies low energy input. Importantly, 86.6 % of toluene methyl C−H groups were converted to benzoyl groups (C=O), and hydrogen was produced efficiently at the cathode. The electrocatalytic efficiency at the CC/PANI/G anode was higher at lower voltage (1.0 V) than at higher voltage (1.5 V), and more hydrogen was produced at the corresponding cathode. The synergistic effect between the dynamic redox chemistry of nanoPANI and the excellent conductivity and anticorrosive action of graphene determined the high electrocatalytic efficiency of the oxidation of toluene methyl C−H groups at the CC/PANI/G anode. Owing to the chemical bonding between graphene and PANI, the anticorrosive CC/PANI/G anodic electrocatalyst was durable and effective for oxidation of toluene methyl C−H groups in acidic environment. This approach provides advanced electrode materials for transforming stable chemical bonds (C−H) into useful functional groups (C=O), which will be beneficial for the synthesis of organic intermediates with coupled hydrogen production. Graphical It's a wrap : A graphene-wrapped polyaniline nanoparticles film embedded in carbon cloth was fabricated and used as an anodic electrocatalyst for oxidation of toluene methyl C−H groups (see figure). A toluene conversion of 99.9 % at a low applied voltage of only 1.0 V with 86.6 % conversion of toluene methyl C−H groups to benzoyl groups is coupled with efficient hydrogen production at the cathode.
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Journal of Materials Research and Technology-JMR&T
·
2023
·
IF 6.4
Jianwei Gao,Xiaoqing Si,Hanyue Ding,Xiaoyang Wang,Mushi Zheng,Chun Li,Junlei Qi,Jian Cao
Glass/Glass-ceramic sealing is always accompanied by issues of high porosity and brittle joints. To migrate these problems, an Ag foam was innovatively induced as an interlayer in the process of glass sealing the yttria-stabilized zirconia (YSZ) ceramic to Mn–Co spinel-coated Crofer 22 H stainless steel. Interlayer-added joints showed a significant reduction in porosity, and the shear strength was improved to 52.3 MPa, with an enhancement of 37.8 %. The influence of interlayer on the microstructure of the joint has been investigated and the formation process of the joint is illustrated. The Ag interlayer expels gases from the sealant material through expansion at high temperatures and promotes finer nucleation grains of crystallites integrating with the interlayer, reducing the porosity and alleviating the brittleness as well.
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LANGMUIR
·
2026
·Vol. 42
·期 31
·22950-22957
·
IF 4.4
Chen Nannan,Yuan Qingle,Liu Qin,Zhang Chao,Wu Zhengcui,Bi Wentuan
Single-atom catalysts (SACs) hold great promise for the
electrochemical
reduction of CO 2 to CO; however, the high selectivity is
typically restricted within a narrow potential window, limiting their
practical implementation. In this study, Ni–N–C catalysts
were supported on ordered and disordered carbon nanofiber membranes
(denoted as o-NiNC and d-NiNC, respectively) via electrospinning to
elucidate the effect of nanofiber alignment on CO 2 reduction
activity. The results demonstrate that o-NiNC catalysts allow for
spatially uniform H + /CO 2 delivery and consumption,
thereby mitigating the selectivity variations arising from uneven
spatial distribution of reactants. As a result, the o-NiNC catalysts
achieve a CO Faradaic efficiency (FE) of 98.5% at −1.0 V and
maintain an FE above 90% across a broad potential range (−0.6
to −1.6 V). This work provides new insights into the rational
design of high-performance CO 2 reduction electrocatalysts
through geometric engineering.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122410
·
IF 7.5
Jun Wan,Zhaozhe Zhan,Xinchi Wang,Tingyang Li,Yan Wu,Zhiyong Yan
The effective degradation of persistent and potentially toxic glyphosate in water remains a challenge. Herein, we report an engineering strategy of chloride-modulated synthesis to fabricate illite-modified CuFe₂O₄ composite (CuFe₂O₄/Illite) as robust heterogeneous Fenton-like catalysts. The optimized catalyst exhibited outstanding glyphosate removal efficiency (98.6% in 60 min), wide pH adaptability (pH 3–11), and excellent stability (87.85% efficiency after four cycles). Chloride ions were found to slightly promote degradation, whereas common anions like HCO₃ - , NO₃ - , and SO₄² - showed mild inhibition. Quenching experiments and electron paramagnetic resonance (EPR) analysis identified •OH and O₂• - as the primary reactive oxygen species, with a minor contribution from ¹O₂ contribution. X-ray photoelectron spectroscopy (XPS) results revealed that the facilitated Cu²⁺/Cu⁺ and Fe³ ⁺/Fe²⁺ redox cycles served as an efficient electron-transfer highway, dramatically enhancing the heterolytic cleavage of H 2 O 2 and the sustained generation of reactive species. Based on liquid chromatography-mass spectrometry (LC-MS) analysis, a degradation pathway involving C-P bond cleavage and side-chain oxidation was proposed, leading to the mineralization of toxic intermediate Aminomethylphosphonic acid (AMPA) into CO₂, NH₄⁺, and PO₄³ - . This work provides a promising catalyst and elucidates the underlying mechanism for glyphosate wastewater remediation.
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