APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Libo Sun,Qingtai Xie,Heshun Jing,Xueqing Liu,Lijun Zhao,Xun Sun,Baorong Duan,Caixia Qi,Huijuan Su
Here, Au/polydopamine (Au/PDA) catalysts were prepared by gold sol adsorption (Au/PDA(Sol)), PDA in situ reduction (Au/PDA(PDA reduction)) and DA in situ reduction (Au/PDA(DA reduction)). The factors that influence the performance of Au-PDA on the reduction of 4-nitrophenol (4-NP), were systematically studied for the first time. The catalytic performance of Au/PDA(Sol) is the best because of the uniform and small size of Au nanoparticles (NPs) (3.2 ± 0.7 nm), with a turn over frequency (TOF) of 10125 h −1 , a mass-normalized rate constant ( k’ ) of 33360 min -1 g Au -1 and an apparent activation energy (Ea) of 11.39 KJ/mol. It is confirmed that there are electronic interactions between Au and the catechol hydroxyl groups and imino groups of PDA. Some unreduced Au 3+ ions can be reduced in situ by NaBH 4 during the catalytic reaction, forming ultra small Au NPs and leading to a good initial catalytic activity, especially for Au/PDA(DA reduction). This work systematically studied the influencing factors in catalysis for Au/PDA, providing guidance for the preparation and industrial application of PDA supported noble metal catalysts.
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Polymers
·
2025
·Vol. 17
·期 3
·318
·
IF 4.9
Linyi Shui,Xianxin Guo,Jinrong Li,Zimeng Li,Qinghua Zhao,Guohua Chen,Xiaomin Zhao
Long-chain hyperbranched polyesters (LHBPx, x = 1, 2, 3) with varying lengths of branched chains were synthesized through a thiol-ene click reaction. Subsequently, LHBPx was incorporated into PA4 via the solution method to prepare a LHBPx/PA4 polymer blend, aiming to address the limitations of PA4, such as its narrow thermal processing window (△T = Td5−Tm) and high brittleness. The results demonstrated that the addition of LHBPx enhanced the △T of PA4 from 1.6 °C to 14.5 °C (LHBP3/PA4), increasing the rheological properties of LHBPx/PA4 polymer blends, thereby improving its thermal processability. Compared with PA4, the elongation at the break of the LHBP3/PA4 polymer blend was increased by 20.4%, and the brittle fracture was changed into a ductile fracture. The crystallinity of PA4 was greatly decreased, from 54.41% to 37.42%, owing to the incorporation of LHBPx, whereas Tmof PA4 had almost no change. It was explained that LHBPx hindered the crystal growth stage, whereas it promoted the nucleation stage of PA4, resulting in no significant change in crystal type. Moreover, the longer the branched chain of LHBPx was, the more pronounced the improvement in the thermal processability and toughness of PA4 became. Above all, this work was meaningful for the potential application of PA4 in industrial plastics.
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IONICS
·
2024
·
IF 2.4
Yan Qiang,Zhu Wenxu,Ma Xiaoxue,Liu Na,Liu Yucheng,Xia Meichen
A series of ether-functionalized paramagnetic ionic liquids, 1-(2-methoxyethyl)-3-alkylimidazolium tetra thiocyanate cobalt [C n 2O1IM] 2 [Co(NCS) 4 ] ( n = 1, 2, 3), was synthesized and characterized. The density, surface tension, refractive index, and electrical conductivity of these ionic liquids were measured at 293.15 to 343.15 K at intervals of 5 K, and their thermal expansion coefficients α were calculated. The molecular volume was obtained by measuring the pore volume and porosity. Based on Glasser theory, the standard entropy S 0 (298 K), lattice energy U POT , surface entropy S a , and surface enthalpy, H of the ionic liquids were calculated, and the reason why the ionic liquid is in a molten state at room temperature was explained from the perspective of lattice energy. The molar surface Gibbs energy was introduced to improve the traditional Eötvös equation, which was combined with the refractive index to estimate the surface tension, obtaining a fitting index exceeding 0.99. Finally, the relationship between the electrical conductivity of the ionic liquids and temperature was investigated, and the activation energy, molar electrical conductivity, and electrical conductivity diffusion coefficient of the ionic liquids were obtained. The relationship between their properties was summarized. Compared with previously reported ionic liquids using 1-(2-methoxyethyl)-3-methylimidazolium as a cation, this type of ionic liquid has higher density and a smaller coefficient of thermal expansion.
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INORGANICA CHIMICA ACTA
·
2024
·
IF 2.7
Junhong Gu,Zongyong Zhang,Hao Wu,Lijuan Luo,Min Zhao,Shuchang Wu
Copper (Cu)-based materials attract considerable attentions to replace noble-metal based catalysts in the aqueous reduction of highly toxic 4-nitrophenol (4-NP). However, the reported catalysts generally owned well-defined shapes and structures that commonly rely on special synthesis condition. In contrast, the randomly dispersed and sintered Cu-based counterparts were neglected. Herein, irregular and coalesced Cu catalyst was fabricated and evaluated in 4-NP reduction. The as-synthesized CuBNC800 catalyst performed best among all the prepared materials, and the aggregated Cu nanoparticles was identified as the active centers. It showed that the pre-adsorption of 4-NP played positive role in the reaction. The reaction could be completed within 12 min at 25 °C over CuBNC800 without any treatment, while the elimination of the dissolved oxygen in solution significantly reduced the reaction time to only about 2 min. Moreover, full conversion of 4-NP was even realized within 30 min when the reaction temperature reduced to only 6 °C. Different from previously reported first order reaction kinetics over Cu-based catalysts, zero order reaction kinetics was recognized over CuBNC800 in this work, which could be attributed to the limited exposed active centers.
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Small Methods
·
2024
·
IF 10.7
Yijia Kang,Zhilan Qian,Haishuang Yu,Jian Lu,Qing Zhao,Xue Qiao,Min Ye,Xiangshan Zhou,Menghao Cai
Previous data established 4′-deoxyflavone glycosides (4′-DFGs) as important pharmaceutical components in the roots of rare medical plants like Scutellaria baicalensis Georgi. Extracting these compounds from plants involves land occupation and is environmentally unfriendly. Therefore, a modular (“plug-and-play”) yeast-consortium platform is developed to synthesize diverse 4′-DFGs de novo. By codon-optimizing glycosyltransferase genes from different organisms for Pichia pastoris , six site-specific glycosylation chassis are generated to be capable of biosynthesizing 18 different 4′-DFGs. Cellular factories showed increased 4′-DFG production (up to 18.6-fold) due to strengthened synthesis of UDP-sugar precursors and blocked hydrolysis of endogenous glycosides. Co-culturing upstream flavone-synthesis-module cells with downstream glycoside-transformation-module cells alleviated the toxicity of 4′-deoxyflavones and enabled high-level de novo synthesis of 4′-DFGs. Baicalin is produced at the highest level (1290.0 mg L −1 ) in a bioreactor by controlling the consortium through carbon-source shifting. These results provide a valuable reference for biosynthesizing plant-derived 4′-DFGs and other glycosides with potential therapeutic applications.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Shukai Zhang,Linghui Cao,Aijuan Xie,Shiping Luo
4-Nitrophenol (4-NP), a hazardous chemical compound, presents significant risks to ecological balance, public well-being, and the integrity of the food supply chain. Consequently, the development of detection techniques characterized by both efficiency and precision is of utmost importance. In the present work, ZnCo(OH)F/multi-walled carbon nanotubes (MWCNTs) composite was synthesized through a hydrothermal approach, followed by a high-temperature annealing process to transform them into ZnCo 2 O 4 /MWCNTs tailored for electrochemical sensing of 4-NP. The integration of MWCNTs during the fabrication process induced a pronounced synergistic interaction between ZnCo 2 O 4 and MWCNTs, leading to a substantial enhancement in the electrochemical performance of the composite. The ZnCo 2 O 4 /MWCNTs-based sensors exhibit notable benefits, including an expanded electrochemically active surface area, superior electrical conductivity, and exceptional selectivity. Under optimized experimental parameters (S/N = 3), the sensor exhibited a broad linear detection range (0.5–600 μM), coupled with a lower limit of detection of 0.026 μM. When used on real samples, the sensor showed recovery rates of 98.79 %–100.47 %, indicating its feasibility for practical use in environmental monitoring and food safety evaluation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Bei Jiang,Mengya Xu,Ling Zhang,Wenjing Wang,Xin Qin,Shenyan Xu,Chunyu Che,Chuanqi Zhang,Wenzhong Wang
Open-shell organic radicals, characterized by their unique spin states, typically exhibit exceptional photothermal conversion efficiency. However, the development of open-shell organic radical materials with stability and high photothermal properties remains a challenge. Among these radicals, the stable and commercialized 4-OH-TEMPO radical molecule has garnered considerable attention in various organic synthesis reactions owing to its unique redox advantages, but it shows less application comparing with the other open-shell organic radicals in photo-thermal conversion. In this study, 4-OH-TEMPO exhibits favorable photothermal properties upon combination with Cu 2 + , thus it is capable of enhancing the reaction rate of HMF oxidation to DFF by a factor of 10 under LED (400 nm). Under illumination of LED, leading to the complete conversion of HMF and the generation of DFF with a yield of 99.7 % within 30 min. Mechanism study shows that the photothermal effect facilitates the kinetic process of the reaction, and accelerated conversion of 4-OH-TEMPO to the oxidatively active species 4-OH-TEMPO + under light-induced action further increased the reaction rate. This research proffers novel insights and references for 4-OH-TEMPO mediated organic synthesis reactions and the design of free-radical photothermal materials.
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PROPELLANTS EXPLOSIVES PYROTECHNICS
·
2025
·
IF 2
Liang Zhang,Chen Zhao,Zuohui Xu,Yuhuai Shi,Erhai An,Jinhu Liang,Xiong Cao
Al is widely used in solid propellants for its high energy density. (C 6 H 14 N 2 )[NH 4 (ClO 4 ) 3 ]（DAP-4）, a novel energetic material, exhibits excellent detonation performance, thermal stability, oxidizing capacity, and cost efficiency, making it a promising high-energy oxidizer. This study investigated the ignition and combustion properties of DAP-4/nano-Al mixtures. DAP-4 was synthesized via a one-pot molecular self-assembly strategy, and mixtures with varying Al ratios (10%–30%) were prepared through mechanical mixing. X-ray diffraction (XRD) confirmed that the mixed powders retained their original crystalline structures without the formation of new phases. Scanning electron microscopy (SEM) revealed that nano-Al particles adhered effectively to DAP-4 surfaces, with higher Al content increasing the particle coverage. Elemental mapping and EDS were used to further characterize the surface morphology changes. Thermogravimetry-Differential Scanning Calorimetry（TG–DSC） indicated good compatibility between DAP-4 and nano-Al, with minimal mutual interference during thermal decomposition. Ignition experiments were conducted in a shock tube under temperatures (2200–3100 K) and pressures (0.1 and 0.5 MPa). The results showed that in the DAP-4/nano-Al mixtures, an increase in the Al fraction caused a decrease in the ignition delay time and an increase in the burn time. Simultaneously, the reaction in the presence of Al changed qualitatively, as is apparent from the changed activation energies. Compared to the combustion of neat DAP-4, both the ignition delay and burn times could be longer or shorter, depending on the Al fraction. This study demonstrated that the addition of nano-Al effectively enhanced DAP-4 combustion. In practice, DAP-4's ignition and combustion can be controlled by adjusting the nano-Al mass fraction.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Jianshuo Cheng,Feng Yang,Xianfeng Wang,Shaijie Jiang,Ming Lu,Yuangang Xu
High-energy-density materials (HEDMs) based on five-membered nitrogen heterocycles functionalized with dinitromethyl groups hold significant potential but face challenges in balancing energy and stability. While dinitromethyl derivatives of azoles and oxadiazoles exhibit high enthalpies of formation and detonation performance, their inherent acidity, mechanical sensitivities, and poor stability limit practical applications. Energetic salts have been widely explored to enhance stability, yet most reported salts suffer from reduced densities compared to their neutral analogs. Herein, we report the synthesis and characterization of a novel meta-substituted dinitromethylpyrazole derivative, 4-dinitromethyl-1-nitropyrazole ( 5 ), and its ammonium ( 6a ), hydrazinium ( 6b ), and hydroxylammonium ( 6c ) salts. Remarkably, all three salts exhibit superior densities (1.81–1.89 g cm −3 ), surpassing that of neutral 5 (1.74 g cm −3 ), while maintaining enhanced thermal stabilities and reduced mechanical sensitivities. Single-crystal X-ray diffraction and theoretical calculations jointly reveal that the structural transformation from a twisted neutral molecule to a planar dinitromethyl anion, driven by deprotonation, induces a synergistic interplay of intermolecular forces. This transition fosters robust hydrogen-bond networks, intensified π-π stacking interactions, and elevated packing coefficients, while simultaneously enhancing aromaticity and conjugation effects. Concurrently, destabilizing O···O repulsions are significantly reduced. These combined structural and electronic modifications collectively contribute to superior density and thermochemical stability, overcoming the typical density loss observed in analogous systems. This work challenges the conventional limitations of ionic HEDMs and provides a strategic approach to designing high-density, low-sensitivity energetic salts through rational substitution and crystal engineering. The results highlight the critical role of molecular geometry and counterion selection in achieving balanced energetic performance, offering new avenues for advancing HEDM development.
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PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
·
2025
·
IF 4
Sishi Huang,Xiaoyue Yang,Jing Zhao,Muhammad Zeeshan,Chunjuan Wang,Desong Yang,Xiaoqiang Han,Guoqiang Zhang
Rhizoctonia solani is a significant soil-borne pathogenic fungus that poses a significant threat to the economically important agricultural crops. 4-(Diethylamino)salicylaldehyde (DSA) is a secondary metabolite produced by Streptomyces sp. KN37, which has antifungal activity, meanwhile its inhibitory mechanism is still unclear. In this study, we explored the antifungal efficacy of DSA and its potential mechanism of inhibiting R. solani . It was found that DSA exhibited significant antifungal activity against six tested plant pathogenic fungi, with R. solani being the most sensitive (EC 50 = 26.904 μg/mL). Notably, DSA effectively reduced the mycelial mass and inhibited sclerotia germination, demonstrating a good control efficacy of cucumber damping-off disease. Morphological observation showed that DSA significantly disrupted the shape and ultrastructure of the mycelium. Transcriptomic and metabolomic analyses revealed that DSA impacted the integrity of the cell membrane, redox processes, and energy metabolism in R. solani . The results of fluorescence staining, relative conductivity, H 2 O 2 content, and antioxidant enzyme activity showed that the accumulation of ROS in hypha cells after DSA treatment possibly resulted in damage to cell membrane integrity. Furthermore, the reduction in ATP content, along with decreased ATPase and citrate synthase activity, indicates that energy production may be inhibited. Molecular docking analysis further showed that DSA may competitively inhibit citrate synthase, thereby inhibiting cell energy production and ultimately inducing apoptosis. Our study provides new insights into the potential mechanism by which DSA inhibits the mycelial growth of R. solani .
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JOURNAL OF NATURAL PRODUCTS
·
2023
·
IF 5.1
Ci-Qin Li,Jin-Hui Shi,Jie Mu,An-Qi Wang,Li-Wei Zou,Guang-Bo Ge
A set of 22 analogs of licochalcone A was designed and synthesized to explore their potentials as dipeptidyl peptidase 4 (DPP4) inhibitors with anti-inflammatory effects. The anti-DPP4 effects of these analogs were evaluated using the fluorescent substrate Gly-Pro-N-butyl-4-amino-1,8-naphthalimide (GP-BAN). The nitro-substituted analogue 27 exhibited the most potent activity (Ki = 0.96 μM). A structure–activity relationship investigation revealed that 4-hydroxyl and 5-chloro substituents are essential for DPP4 inhibition, while the 3′-nitro substituent improved both DPP4 inhibition and microsomal stability. Furthermore, compound 27 demonstrated good selectivity for DPP4 over other proteases, including dipeptidyl peptidase 9 (DPP9), thrombin, prolyl endopeptidase (PREP), and fibroblast activation protein (FAP). The cytotoxic effect of 27 was evaluated in cancer cell lines HepG-2 and Caco-2 and in somatic RAW264.7 cells and RPTECs. Compound 27 showed no toxicity to normal cells and weak toxicity to cancer cells. In a living cell imaging assay, 27 blocked the dipeptidase activity of DPP4 in both Caco-2 and HepG-2 cells. This compound also dose-dependently suppressed the expression levels of the chemokines tumor necrosis factor-α (TNF-α), interleukin-6 (IL-6), and interleukin-1β (IL-1β).
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高影响因子
Current Protocols
·
2021
·Vol. 1
·期 10
·e274
·
IF 0
Jingyi Wang,Jiachen Shang,Yu Xiang,Aijun Tong
Functionalized oligonucleotides (ONs) are widely applied as target recognition molecules for biosensing and gene regulation. Herein, we describe a general method for post-synthetic modification of ONs based on the oxidative amination of 4-thio-2′-deoxyuridine (4SdU) with sodium periodate and several amines. Alkyne-/azide-, biotin-, and fluorophore-modified ONs were prepared by modifying 4SdU-containing ONs with the corresponding amines and characterized for their bioorthogonal reactivity, streptavidin-binding affinity, and fluorescence properties, respectively. We synthesized three fluorophore-modified ONs with and without the aromatic fluorophores conjugated to modified nucleobases and investigated their emission properties. © 2021 Wiley Periodicals LLC. Basic Protocol 1 : Post-synthetic modification of ONs Supporting Protocol : Preparation of dansyl ethylenediamine Basic Protocol 2 : Quantification of ON reaction yields Basic Protocol 3 : Characterization of modified ONs
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