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Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu NPs@MOFs catalyst under mild conditions

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Science China Chemistry 2024年第5期67卷 1561-1568页

作者： Peng-Fei Guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao Key laboratory of advanced Energy material Chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,*** studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1,2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali ***,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction ***,a novel framework 1 was synthesized,exhibiting 1D channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(NPs)to form Cu NPs@1-x(x=1,2,3,and 4)with varying loading amounts of Cu NPs at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,*** NPs@1-3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1 h-1under eco-friendly mild *** corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale ***,the efficient preparation of DHIQ catalyzed by Cu NPs@1-3 could be realized even under air ***,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@*** investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu NPs and Co metal *** importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu NPs@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

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Exploring the Core-shell Structure of BaTiO3-based Dielectric Ceramics Using Machine Learning Models and Interpretability Analysis

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Journal of Wuhan University of Technology(materials Science) 2024年第3期39卷 561-569页

作者：孙家乐 XIONG Peifeng 郝华 LIU Hanxing State Key laboratory of advanced Technology for materials Synthesis and Processing School of Material Science and EngineeringInternational School of Material Science and EngineeringWuhan University of TechnologyWuhan 430070China Sanya Science and Education Innovation Park Wuhan University of TechnologySanya 572000China Foshan Xianhu laboratory of the advanced Energy Science and Technology Guangdong laboratory Xianhu Hydrogen ValleyFoshan 528200China

A machine learning(ML)-based random forest(RF)classification model algorithm was employed to investigate the main factors affecting the formation of the core-shell structure of BaTiO_(3)-based ceramics and their interpretability was analyzed by using Shapley additive explanations(SHAP).An F1-score changed from 0.8795 to 0.9310,accuracy from 0.8450 to 0.9070,precision from 0.8714 to 0.9000,recall from 0.8929 to 0.9643,and ROC/AUC value of 0.97±0.03 was achieved by the RF classification with the optimal set of features containing only 5 features,demonstrating the high accuracy of our model and its high *** the interpretability analysis of the model,it was found that the electronegativity,melting point,and sintering temperature of the dopant contribute highly to the formation of the core-shell structure,and based on these characteristics,specific ranges were delineated and twelve elements were finally obtained that met all the requirements,namely Si,Sc,Mn,Fe,Co,Ni,Pd,Er,Tm,Lu,Pa,and *** the process of exploring the structure of the core-shell,the doping elements can be effectively localized to be selected by choosing the range of features.

关键词： machine learning BaTiO_(3) core-shell structure random forest classifier

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Mussel-inspired Methacrylic Gelatin-dopamine/Ag Nanoparticles/Graphene Oxide Hydrogels with Improved Adhesive and Antibacterial Properties for Applications as Wound Dressings

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Journal of Wuhan University of Technology(materials Science) 2024年第2期39卷 512-521页

作者：宿正楠 HU Yanru MENG Lihui OUYANG Zhiyuan LI Wenchao ZHU Fang XIE Bin 吴庆知 State Key laboratory of advanced Technology for materials Synthesis and Processing Biomedical Material and Engineering Center of Hubei ProvinceWuhan University of TechnologyWuhan 430070China

A novel strategy was developed to prepare the methacrylic gelatin-dopamine(GelMA-DA)/Ag nanoparticles(NPs)/graphene oxide(GO) composite hydrogels with good biocompatibility,mechanical properties,and antibacterial ***-inspired DA was utilized to modify the GelMA molecules,which imparts good adhesive performance to the ***,interfacial enhancer,not only improves mechanical properties of the hydrogels,but also provides anchor sites for loading Ag NPs through numerous oxygencontaining functional groups on the *** experimental results show that the GelMA/Ag NPs/GO hydrogels have good biocompatibility,and exhibit a swelling rate of 202±16%,the lap shear strength of 147±17 kPa,and compressive modulus of 136±53 kPa,in the case of the Ag NPs/GO content of 2 mg/*** activity of the hydrogels against both gram-negative and gram-positive bacteria is dependent on the Ag NPs/GO content derived from the release of Ag^(+).Furthermore,the GelMA/Ag NPs/GO hydrogels possess good adhesive ability,which is resistant to highly twisted state when stuck on the surface of *** results demonstrate promising potential of the GelMA-DA/Ag NPs/GO hydrogels as wound dressings for biomedical applications in clinical and emergent treatment.

关键词： GelMA dopamine,graphene oxide adhesion antibacterial ability

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Optimizing Electrocatalytic Hydrogen Evolution Stability via Minimal Bubble Adhesion at Electrodeposited Crack-Structured NiPx Catalysts

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Energy & Environmental materials 2024年第5期7卷 248-258页

作者： Qian Sun Xiaoyu Hao Dina Zhang Tianyi Zhang Yuanfang Zhao Xiaolei Huang Xuqing Liu State Key laboratory of Solidification Processing Center of Advanced Lubrication and Seal Materials Northwestern Polytechnical University College of Art and Design Shenzhen University Institute of material and Chemistry Ganjiang Innovation Academy Chinese Academy of Sciences Shandong laboratory of Yantai advanced materials and Green Manufacture

In response to the ongoing energy crisis, advancing the field of electrocatalytic water splitting is of utmost significance, necessitating the urgent development of high-performance, cost-effective, and durable hydrogen evolution reaction catalysts. But the generated gas bubble adherence to the electrode surface and sluggish separation contribute to significant energy loss, primarily due to the insufficient exposure of active sites, thus substantially hindering electrochemical performance. Here, we successfully developed a superaerophobic catalytic electrode by loading phosphorus-doped nickel metal （NiPx） onto various conductive substrates via an electrodeposition method. The electrode exhibits a unique surface structure, characterized by prominent surface fissures, which not only exposes additional active sites but also endows the electrode with superaerophobic properties. The NiPx/Ti electrode demonstrates superior electrocatalytic activity for hydrogen evolution reaction, significantly outperforming a platinum plate, displaying an overpotential of mere 216 mV to achieve a current density of-500 mA cm-2in 1 M KOH. Furthermore,the NiPx/Ti electrode manifests outstanding durability and robustness during continuous electrolysis, maintaining stability at a current density of-10 mA cm-2over a duration of 2000 h. Owing to the straightforward and scalable preparation methods, this highly efficient and stable NiPx/Ti electrocatalyst offers a novel strategy for the development of industrial water electrolysis.

关键词： electrocatalyst gas bubble adhesion hydrogen evolution reaction long-term durability superaerophobic surface

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Porous organic cages as a novel platform for second harmonic generation

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Science China Chemistry 2024年第11期67卷 3669-3674页

作者： Feng Shui Yunqin Zhang Mao Yi Xiongli Liu Lin Li Shuo Zhang Yongshen Zheng Yongtao Yao Qiao Zhao Baiyan Li Xianhe Bu School of materials Science and Engineering National Institute for Advanced Materials TKL of Metal and Molecule-Based Material Chemistry Nankai University National Key laboratory of Science and Technology on advanced Composites in Special Environments Harbin Institute of Technology

Second harmonic generation(SHG) is one of the most extensively applied nonlinear optical phenomena. Compared to traditional inorganic SHG materials, organic SHG materials, including non-centrosymmetric small molecular crystals and organic polymers, have been extensively explored for SHG optics due to their advantageous properties, including high light-induced damage threshold, ultrafast response speed, high polarization ratio, wide transparency range, and elevated dielectric constant. However,in organic SHG materials, most small molecular crystals often show poor thermal stability(material with high thermal stability, large-size crystals,excellent processability, high homogeneity, and a well SHG effect. In the contribution, we developed herein porous organic cages(POCs) as a novel platform for SHG optics. Thanks to its inherent macromolecular composition and zero-dimensional discrete structures, POCs can not only solve the instability problem of small molecule crystals but also overcome the drawbacks in growing large-size crystals for organic polymer. The obtained two POCs with chiral asymmetric centers(CPOC-R-5 and CPOCS-7) display advantageous features for SHG optics including well SHG performance, large-size crystal(5 mm×3 mm×1 mm),high thermal stability(≥250 °C), wide transparency window(750–2,000 nm) and high polarization ratio(up to 94.5%). This work thus develops POCs as a new platform toward the construction of organic NLO materials with the potential application in sorts of SHG optics.

关键词： porous organic cages second harmonic generation novel SHG platform high thermal stability large-size single crystal

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Degradation and biocompatibility of one-step electrodeposited magnesium thioctic acid/magnesium hydroxide hybrid coatings on ZE21B alloys for cardiovascular stents

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Journal of Magnesium and Alloys 2024年第1期12卷 120-138页

作者： Zhao-Qi Zhang Bing-Zhi Li Pei-Duo Tong Shao-Kang Guan Li Wang Zheng-Hui Qiu Cun-Guo Lin Rong-Chang Zeng School of material Science and Engineering&Henan Key laboratory of advanced Magnesium Alloy&Key laboratory of materials Processing and Mold Technology(Ministry of Education) Zhengzhou University100 Science RoadZhengzhou 450001China State Key laboratory for Marine Corrosion and Protection Luoyang Ship Material Research InstituteQingdao 266101China Corrosion laboratory for Light Metals College of Material Science and EngineeringShandong University of Science and TechnologyQingdao 266590China

Constructing a functional hybrid coating appears to be a promising strategy for addressing the poor corrosion resistance and insufficient endothelialization of Mg-based ***,the steps for preparing composite coatings are usually complicated and ***,a novel composite coating,composed of bioactive magnesium thioctic acid(MTA)layer formed by deposition and corrosion-resistant magnesium hydroxide(Mg(OH)_(2))layer grown in situ,is simply fabricated on ZE21B alloys via one-step *** electron microscopy(SEM)shows that the electrodeposited coating has a compact and uniform *** the high adhesion of the MTA/Mg(OH)_(2)hybrid coating is also confirmed by the micro-scratch *** test,scanning kelvin probe(SKP),and hydrogen evolution measurement indicate that the hybrid coating effectively reduces the degradation rate of Mg *** experiment and cell culture trial detect that the composite coating is of fine ***,the preparation mechanism of MTA/Mg(OH)_(2)hybrid coatings is discussed and *** coating shows a great potential application for cardiovascular stents.

关键词： Magnesium alloy Corrosion resistance Hybrid coating Endothelialization Biocompatibility

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Bio-inspired barnacle cement coating of biodegradable magnesium alloy for cerebrovascular application

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Rare Metals 2024年第10期43卷 5164-5185页

作者： Hang Li Fei Wang Xiao-Jing Sun Liu-Jie Qi Jing-An Li Mujahid Iqbal Shao-Kang Guan School of material Science and Engineering Zhengzhou University Henan Key laboratory of advanced Magnesium Alloy&Key laboratory of materials Processing and Mold (Ministry of Education) Zhengzhou University Department of Physics University of Agriculture Faisalabad

Ischemic stroke is increasing worldwide, and stent intervention has gradually become one of the effective treatments. Owing to its good mechanical properties and biocompatibility, biodegradable Mg-Zn-Y-Nd alloy(ZE21B) has good application prospects in vascular ***, too fast degradation and delayed endothelialization are the bottleneck problem to limit its further application. In this study, the bio-inspired coating barnacle cement cp19k is constructed on ZE21B surface through electrostatic spraying to improve the corrosion resistance and pro-endothelialization ability. The coating was evaluated through electrochemistry, static immersion corrosion,in vitro blood experiments and cell experiments. Cp19k effectively improved the corrosion resistance of the substrate ZE21B, reduced the degradation rate, improved endothelial cell proliferation and migration capabilities,inhibited smooth muscle cells proliferation and regulated contractile phenotype, inhibited macrophage adhesion,regulated macrophage M2 phenotype, and reduced the expression of inflammatory factor of TNF-a and inhibited fibroplasia in vivo. Our data indicated that the barnacle cement cp19k coating had potential application on the surface modification of Mg alloy cerebrovascular stent.

关键词： Barnacle cement cp19k Biodegradable magnesium alloy Cerebrovascular stent M2 phenotype Pro-endothelialization

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Efficient guiding and focusing of intense laser pulse using periodic thin slits

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Matter and Radiation at Extremes 2024年第4期9卷 29-39页

作者： L.Xu T.W.Huang K.Jiang C.N.Wu H.Peng P.C.hen R.Li H.B.Zhuo C.T.Zhou Shenzhen Key laboratory of Ultraintense Laser and advanced material Technology Center for Intense Laser ApplicationTechnologyand College of Engineering PhysicsShenzhen Technology UniversityShenzhen 518118People’s Republic of China

Slits have been widely used in laser-plasma interactions as plasma optical components for generating high-harmonic light and controlling laser-driven particle ***,we propose and demonstrate that periodic thin slits can be regarded as a new breed of optical elements for efficient focusing and guiding of intense laser *** fundamental physics of intense laser interaction with thin slits is studied,and it is revealed that relativistic effects can lead to enhanced laser focusing far beyond the pure diffractive focusing *** addition,the interaction of an intense laser pulse with periodic thin slits makes it feasible to achieve multifold enhancement in both laser intensity and energy transfer efficiency compared with conventional *** results provide a novel method for manipulating ultra-intense laser pulses and should be of interest for many laser-based applications.

关键词： laser pulse intense

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Enhanced preparation of dendritic metallic vanadium in recyclable NaCl-KCl-VCl_(2) molten salt by V_(2)CO electrolysis

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Rare Metals 2024年第8期43卷 3961-3973页

作者： Jia-Liang An Ming-Yong Wang Yong-Zheng Jia Jin-Tao Zhang Bao-Yan Feng Shu-Qiang Jiao State Key laboratory of advanced Metallurgy University of Science and Technology BeijingBeijing 100083China College of material Science and Engineering Hebei Province Laboratory of Inorganic Nonmetallic MaterialsNorth China University of Science and TechnologyTangshan 063210China

A promising method for the preparation of pure metallic vanadium via V_(2)CO anode electrolysis was proposed and *** simple and controllable synthesis of a molten chloride salt containing VCl_(2) by an insitu reaction between VCl_(3) and metallic vanadium was verified through thermodynamic analysis and ***-KCl-VCl_(2) molten salt exhibited excellent recycling performance and could be repetitively used to prepare metallic vanadium by V_(2)CO *** V^(2+) ions remained in the molten salt after *** electrolysis conditions,such as the cathode diameter,current density,V^(2+) ion concentration,and temperature,were optimised to maximise the current *** was also simulated to reveal the regulatory *** highest current efficiency was 85%.The purity of metallic vanadium was up to 99.8%.In this study,an easy and efficient preparation of pure metallic vanadium was achieved.

关键词： V_(2)CO Metallic vanadium Current efficiency Molten salt electrolysis

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Atomic-resolution Interfacial Microstructure and Thermo-electro-magnetic Energy Conversion Performance of Gd/Bi0.5Sb1.5Te3 Composites

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Energy & Environmental materials 2024年第4期7卷 355-363页

作者： Chengshan Liu Wenjie Xu Ping Wei Shaoqiu Ke Wenjun Cui Longzhou Li Dong Liang Xianfeng Ye Tiantian Chen Xiaolei Nie Wanting Zhu Wenyu Zhao Qingjie Zhang State Key laboratory of advanced Technology for materials Synthesis and Processing Wuhan University of Technology Foshan Xianhu laboratory of the advanced Energy Science and Technology Guangdong laboratory

Thermo-electro-magnetic materials with simultaneously large magnetocaloric(MC) and thermoelectric (TE) effects are the core part for designing TE/MC all-solid-state cooling *** MC phase with TE material is an effective ***,the elemental diffusion and chemical reaction occurring at the two-phase interfaces could significantly impair the cooling performance.

关键词： interfacial reaction magnetocaloric performance thermoelectric performance thermo-electro-magnetic materials

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