COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Nanqi Shi,Zhike Li,Xin Li,Hongxin Luo,Shuzhen Dong,Haiyan Li
Hexagonal boron nitride (h-BN), as a two-dimensional lamellar material, has been paid more and more attention in the field of corrosion protection because of its excellent thermal stability, chemical stability and insulation. In order to solve the problem that h-BN is difficult to disperse in resin, inspired by the adhesion ability of mussel secretions, the surface of h-BN was modified with polydopamine (PDA) to improve the dispersion of the fillers in epoxy resin, and the prepared corrosion inhibition CeO 2 nanoparticles were loaded on the surface. A functional filler CeO 2 &PDA/h-BN with corrosion inhibition effect was prepared. The surface morphology , chemical structure and thermal stability of functional fillers were analyzed by SEM, FTIR, XRD and thermogravimetric analysis . The test results show that after 40 days of testing, the low-frequency impedance modulus of the epoxy composite coating is 15 times that of the pure epoxy resin, and the wear resistance properties also significantly improved. The anti-corrosion mechanism of the composite coating is analyzed, and the synergistic effect of h-BN's barrier ability and CeO 2 's corrosion inhibition ability is revealed. This paper provides an idea for the preparation of multifunctional h-BN composite anticorrosive filler.
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高影响因子
ACS Applied Nano Materials
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2024
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IF 5.3
Yuting Li,Jiaming Song,Xin Zhao,Bingda Li,Zhuo Wang,Juanjuan Yang,Guoshuai Ban,Feng Teng,Jialong Ma,Chaoying Meng,Honggang Ye,Guangde Chen,Zhonghua Dai,Yu Cong
With increasing environmental pollution, the utilization of green techniques, such as photocatalysis, is required to degrade harmful sources without secondary pollution. In this study, we synthesized an efficient photocatalyst, i.e., a h-BN/BiPO4 heterostructure modified by Ag nanoparticles at the interface (Ag/BN/BPO) by photodeposition and a hydrothermal method, and investigated photocatalytic degradation performance for rhodamine B dye (RhB). It was found that 95% of RhB was removed by Ag/BN/BPO (optimal ratio) after 60 min of light exposure. Compared to BiPO4 and BN/BiPO4, the removal efficiency was improved by 50 and 30%, respectively. The high photocatalytic degradation activity of Ag/BN/BPO could be possibly attributed to the synergistic effect of the improved separation efficiency of electron–hole pairs by the special heterostructure design and the increased adsorption capacity due to the large specific surface area of the layered h-BN. This study provided a possible route for the development of highly efficient photocatalysts for the degradation of organic pollutants.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Zhisong Liu,Haomiao Xu,Yurui Fan,Wenjun Huang,Feng Yu,Zan Qu,Naiqiang Yan
Ruthenium single-atom catalysts have great potential in ammonia-selective catalytic oxidation (NH3–SCO); however, the stable sp3 hybrid orbital of NH3 molecules makes N(sp3)–H dissociation a challenge for conventional symmetrical metallic oxide catalysts. Herein, we propose a heterogeneous interface reverse atom capture strategy to construct Ru with unique asymmetric Ru1N2O1 coordination. Ru1N2O1/CeO2 exhibits intrinsic low-temperature conversion (T100 at 160 °C) compared to symmetric coordinated Ru-based (280 °C), Ir-based (220 °C), and Pt-based (200 °C) catalysts, and the TOF is 65.4 times that of Ag-based catalysts. The experimental and theoretical studies show that there is a strong d–p orbital interaction between Ru and N atoms, which not only enhances the adsorption of ammonia at the Ru1N2O1 position but also optimizes the electronic configuration of Ru. Furthermore, the affinity of Ru1N2O1/CeO2 to water is significantly weaker than that of conventional catalysts (the binding energy of the Pd3Au1 catalyst is −1.19 eV, but it is −0.39 eV for our material), so it has excellent water resistance. Finally, the N(sp3)–H activation of NH3 requires the assistance of surface reactive oxygen species, but we found that asymmetric Ru1N2O1 can directly activate the N(sp3)–H bond without the involvement of surface reactive oxygen species. This study provides a novel principle for the rational design of the proximal coordination of active sites to achieve its optimal catalytic activity in single-atom catalysis.
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高影响因子
JOURNAL OF CATALYSIS
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2012
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IF 6.002
Xiang Li,Yi Shi,Zhoujun Wang,Yahong Zhang,Yi Tang
In this paper, uniform H-β nanozeolite microsphere (β-ZMS) prepared by polymerization-induced colloid aggregation, combined with an immobilized lipase B from Candida antarctica (commercially available Novozym® 435), is applied as a racemization catalyst to the one-pot dynamic kinetic resolution (DKR) of aromatic sec -alcohols. The DKRs of various aromatic sec- alcohols can be carried out with high selectivity and conversion under optimum conditions. Importantly, it is found that, compared to commercial zeolites β (C-β), β-ZMSs display high selectivity for small sec- alcohol molecules because their shorter microporous channels reduce the diffusion time of substrate/product in the three-dimensional framework, and thereby decrease the possibility of secondary reactions. However, the β-ZMSs show a high racemization rate in the DKR of large sec- alcohol molecules, such as racemic 1-(1-naphthyl)-ethanol, thanks to their abundant accessible active sites. This observation will not only benefit the performance of acidic zeolite catalysts in one-pot DKR systems but also provide a new perspective on the application of nanozeolites in catalysis.
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Journal of the American Chemical Society
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2024
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IF 14.4
Yanliang Zhou,Lili Liang,Congying Wang,Fuxiang Sun,Lirong Zheng,Haifeng Qi,Bin Wang,Xiuyun Wang,Chak-tong Au,Junjie Wang,Lilong Jiang,Hideo Hosono
To date, NH3 synthesis under mild conditions is largely confined to precious Ru catalysts, while nonprecious metal (NPM) catalysts are confronted with the challenge of low catalytic activity due to the inverse relationship between the N2 dissociation barrier and NHx (x = 1–3) desorption energy. Herein, we demonstrate NPM (Co, Ni, and Re)-mediated Mo2CTx MXene (where Tx denotes the OH group) to achieve efficient NH3 synthesis under mild conditions. In particular, the NH3 synthesis rate over Re/Mo2CTx and Ni/Mo2CTx can reach 22.4 and 21.5 mmol g–1 h–1 at 400 °C and 1 MPa, respectively, higher than that of NPM-based catalysts and Cs–Ru/MgO ever reported. Experimental and theoretical studies reveal that Mo4+ over Mo2CTx has a strong ability for N2 activation; thus, the rate-determining step is shifted from conventional N2 dissociation to NH2* formation. NPM is mainly responsible for H2 activation, and the high reactivity of spillover hydrogen and electron transfer from NPM to the N-rich Mo2CTx surface can efficiently facilitate nitrogen hydrogenation and the subsequent desorption of NH3. With the synergistic effect of the dual active sites bridged by H-spillover, the NPM-mediated Mo2CTx catalysts circumvent the major obstacle, making NH3 synthesis under mild conditions efficient.
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FUEL
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2025
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IF 7.5
Shuping Li,Cheng Dong,Xuan Qi,Shiyong Chen,Lixiao Shen,Yinning Zeng,Yan Li,Zhenxin Yi,Lin Zhang,Shunguan Zhu
A novel hollow-structured thermite, n-Al/H-MoO 3 , is designed to enhance the energy release mode and combustion performance of solid propellant. This research comprehensively explores the preparation and structural features of n-Al/H-MoO 3 within solid propellants. Furthermore, a series of rigorous combustion tests, performance assessments, and computational simulations are conducted to investigate its practical application. Experimental results indicate that the significant improvements in combustion performance have been observed by integrating this innovation n-Al/H-MoO 3 in solid propellants as a burning rate modifier. The heat of explosion increases to 6135 J·g −1 , a 41.76 % increase over the blank group (M0). Furthermore, its flame temperature is 494.3°C higher than that of the blank group. These substantial gains are primarily attributed to the unique hollow structure of n-Al/H-MoO 3 , which facilitates the reaction between H-MoO 3 and Al in the gaseous phase region, thereby improving combustion dynamics. The research findings offer theoretical foundations and experimental support for the design of more efficient and stable propellants.
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Lixia Li,Xiuqi Li,Feiyue Li,Xiang Zhen,Mingdong Dong,Jinxing Long,Xiaobing Wang,Zhiyong Jiang
Harnessing photocatalyzed hydrogen atom transfer (HAT) for the precise activation of C–H/O–H bonds is a pivotal yet challenging strategy to selectively drive oxidative C–C bond scission in renewable lignin, yielding value-added chemicals with exceptional selectivity. Herein, we present a metal-free photochemical strategy that enables selective C–C bond scission in lignin via a unique synergistic HAT pathway driven by triplet-excited 2-ethylanthraquinone (EAQ*) and hydroxyl radicals ( • OH) generated in situ from EAQH 2 and O 2 . Under simulated natural conditions, this process achieves a benzaldehyde yield of 146.6 mol% from a lignin-derived phenolic dimer. Mechanistic investigations reveal that preferential activation of the C α -OH in lignin facilitates a tandem HAT process, forming alkoxy radical intermediates that undergo β –scission to produce benzaldehyde, as corroborated by extensive control reactions and density functional theory calculations. Furthermore, this straightforward protocol efficiently cleaves the C–C bonds of technical kraft lignins, providing a rapid, scalable, and metal-free protocol for lignin valorization under mild conditions.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Qisong Yi,Lu Lin,Huawei Geng,Shaohua Chen,Yuanchao Shao,Ping He,Zhifeng Liu,Haimei Xu,Tiehong Chen,Yuanshuai Liu,Valentin Valtchev
The hydrothermal stability of zeolites is essential for their potential applications in biomass conversion, especially in processes involving elevated temperatures alongside the use or generation of H 2 O. In this study, we employed F - ions as mineralizers to synthesize hydrothermally stable ZSM-5 zeolites under acidic conditions. The acidic synthesis system promotes zeolites with fewer silanol-terminated lattice defects (ZSM-5(A)) compared to the traditional basic conditions (ZSM-5(B)), endowing materials with substantially higher structural integrity and hydrophobicity. After 10 days of autoclave treatment at 200 °C in aqueous phase, H-ZSM-5(A) demonstrated nearly unchanged reaction rates in the dehydration of cyclohexanol, while H-ZSM-5(B) lost > 50% of the dehydration activity. Additionally, H-ZSM-5(A) delivered higher initial dehydration rates compared to H-ZSM-5(B). The different measured activation energies further revealed variations in reaction pathways during cyclohexanol dehydration, i.e., the monomer- or dimer-mediated routes depending on the concentration of alcohol molecule within zeolite pores, providing additional evidence for the strengthened hydrophobic nature of H-ZSM-5(A). Beyond this, the zeolite surface properties and the strength of cyclohexanol-zeolite interactions may impose additional transport/adsorption barriers attributed to multi-phase phenomena on the more polar H-ZSM-5(B) zeolite surfaces. More importantly, the hydrothermal treatment did not induce significant desilication and dealumination in H-ZSM-5(A), thereby preserving its active acid sites and ensuring exceptional hydrothermal stability. The present work fundamentally studies the synthesis of hydrothermally stable zeolites in an acidic medium using fluorides and expands the understanding of polar interactions in catalysis, characterized by the dehydration of cyclohexanol, for future application in biomass conversion.
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JOURNAL OF ENZYME INHIBITION AND MEDICINAL CHEMISTRY
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2025
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IF 5.4
Pengtao Yuan,Xi Jiang,Xintong Ni,Xusheng Shao,Xuhong Qian,Qing Yang
Chitinase h (Chi-h) has been identified as a promising pesticide target due to its exclusive distribution in lepidopteran insects and its essential role in the moulting processes. In this study, we leverage OfChi-h from destructive agricultural pest Ostrinia furnacalis (Asian corn borer) as a model target to identify novel chitinase inhibitors. A conformational restriction approach was employed to design a series of novel OfChi-h inhibitors. Among these, compound 6a showed the highest inhibitory activity against OfChi-h, with a Ki value of 58 nM. Molecular docking analysis suggested that 6a tightly bound to three subsites (-3 to −1) of OfChi-h. The binding mode is further confirmed by the co-crystallization data of 6a with the SmChiA, a bacterial homologue of OfChi-h, at a resolution of 1.8 Å. This research presents a novel approach for the development of highly potent insect chitinase inhibitors, offering potential tools for effective pest control.
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高影响因子
RARE METALS
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2025
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IF 11
Wu Yi-Ming,Hou Guo-Yuan,Fan Xin,Zhu Qian-Ye,Cui Ming-Jun,Ren Si-Ming
Polymer materials commonly employed in low Earth orbit (LEO) environments are highly susceptible to atomic oxygen (AO) attack, leading to severe degradation and deterioration of their properties. To address this challenge, 3-glycidyloxypropyltrimethoxysilane-modified hexagonal boron nitride (h-BN@KH560) nanohybrids were synthesized and incorporated into epoxy (EP) composites to enhance their AO erosion resistance. The resulting hexagonal boron nitride-based epoxy nanocomposites (FBN/EP) were systematically evaluated for their tribological performance and AO erosion resistance using a series of characterization techniques. The results demonstrated that the incorporation of h-BN@KH560 nanohybrids significantly improved the wear resistance and AO erosion resistance of the EP matrix. Specifically, the FBN 1.0 /EP nanocomposite exhibited an 86.1% reduction in wear rate compared to pure EP, while FBN 5.0 /EP nanocomposite achieved optimal AO erosion resistance, with a minimal erosion rate of 3.58 × 10 –24 cm 3 atoms −1 at an AO dose of 1.2 × 10 21 atoms cm −2 . These findings indicate that the incorporating content-induced distribution of h-BN@KH560 within the EP matrix strongly influences the wear resistance of FBN/EP nanocomposites, but there is a relatively minor effect on their AO erosion resistance. The enhanced AO erosion resistance is attributed to the synergistic barrier protection provided by h-BN@KH560 and the formed B 2 O 3 and SiO 2 layers under AO irradiation. This study offers a promising strategy for extending the service life of epoxy nanocomposites in harsh LEO environments. Graphical abstract
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PHYTOMEDICINE
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2024
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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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ADVANCED POWDER TECHNOLOGY
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2024
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IF 4.2
Hu Wen,Yuxin Li,Haitao Yin,Wei Wang,Zhengchao Jin,Shunyu Han,Nanzhe Jiang
The conversion of natural clay to crystalline zeolites has been the subject of considerable interest from both academic and industrial circles. We present an effective strategy for converting kaolin to ZSM-5 zeolite, addressing the issue of reduced mesopore formation in conventional nano-ZSM-5 aggregates due to close-packing. This strategy utilizes kaolin as the sole source of silicon and aluminum, and by decoupling the nucleation and growth of ZSM-5 crystals, loosely stacked nano-H-ZSM-5 aggregates with high crystallinity crystals can be synthesized in a solid-like system by employing a tiny amount of TPAOH (TPAOH/SiO 2 = 0.064). The resulting nano-H-ZSM-5 aggregates exhibited high specific surface area (405.66 m 2 /g), high mesopore volume (0.64 cm 3 /g), and superior catalytic activity. This strategy offers a novel approach to the cost-effective synthesis of nano-H-ZSM-5 aggregates suitable for industrial applications.
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