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Low-cost and fluoride-free synthesis of MFI zeolite nanosheets with enhanced stability for benzene alkylation with ethanol

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Journal of Energy Chemistry 2025年第1期100卷 458-468页

作者： Peng Zhu Cun Liu Yiren Yu Guoshu Gao Yumeng Zhao Xiongfu Zhang Guodong Liu Guohui Yang state key laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology state key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented *** obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.

关键词： MFI zeolite ZSM-5 Nanosheets Scale-up synthesis Aromatic alkylation

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Fabrication of carbon-supported Al2O3 nanoparticles via spontaneous cross-linking to enhance selective hydrogenation of furfural

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Journal of Energy Chemistry 2025年第1期100卷 612-620页

作者： Weiwei Yu Xinbao Zhang Hongyu Chen Yanan Wang Shaoguo Li Fucun Chen Zhenni Liu Xiujie Li Xiangxue Zhu state key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=***,a novel Al2O3/C-u hybrid catalyst,composed of N-modified dendritic carbon networks supporting Al2O3nanoparticles,was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate,Al3+and *** obtained carbon-supported Al2O3hybrid catalyst has a high ratio （31%） of Al species in pentahedral-coordinated *** introduction of urea enhances the surface N content,the ratio of pyrrolic N,and specific surface area of catalyst,leading to improved adsorption capacity of C=O and the accessibility of active *** the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor,Al2O3/C-u catalyst achieved a 90%conversion of furfural with 98.0% selectivity to furfuryl alcohol,outperforming that of commercial γ-***,Al2O3/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on *** work provides an innovative and facile strategy for fabrication of carbon-supported Al2O3hybrid catalysts with rich AlVspecies,serving as a high selective hydrogenation catalyst through MPV reaction route.

关键词： Selective hydrogenation Furfural Furfuryl alcohol Cross-linking MPV route

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Construction of Ni single-atom coordinated with doped N and S elements for mild hydrogenation of methyl acrylate to methyl propionate

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Nano Research 2025年第1期18卷 217-224页

作者： Taolue Sun Chen Jian Gang Wang Hui Zhao Guoliang Zhang Zengxi Li Chunshan Li state key laboratory of Mesoscience and Engineering CAS Key Laboratory of Green Process and EngineeringBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Huizhou Institute of Green Energy and Advanced Materials Huizhou 516081China Advanced Energy Science and Technology Guangdong laboratory Huizhou 516081China

Although the nickel-based catalyst is able toexhibit comparative catalytic activity to noble metal formethyl acrylate hydrogenation,it requires strict reactioncondition,which can be improved by regulation ofcoordination *** this study,we constructed akind of Ni single-atom coordinated with N and S(Ni-NSC)through the pyrolysis of organic Ni-based precursors at600℃.The existence and fine structure of Ni single-atom were confirmed by the spherical electron microscopicobservation in combination with the X-ray absorption spectroscopy(XAS)*** addition,the catalytichydrogenation assessment suggested that the as-prepared Ni-NSC catalyst exhibited higher activity and stability than theNi/NSC supported catalyst prepared by incipient wetness impregnation *** remarkable catalytic activity was dueto the high dispersion and density of Ni single-atom and weak adsorption energy of intermediates on these Ni sites.

关键词： methyl acrylate mild hydrogenation Ni single-atom coordination environment adsorption energy

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Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy Chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia key laboratory of Chemistry and physics of Rare Earth Materials School of Chemistry and Chemical Engineering Inner Mongolia University state key laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Institute of Catalysis Department of Chemistry Zhejiang University National key laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Oxygen vacancy Hydrocarbon production Reaction mechanism

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A surface engineering strategy for the stabilization of zinc metal anodes with montmorillonite layers toward long-life rechargeable aqueous zinc ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 94-105页

作者： Wenbo Wang Ruifeng Xu Xu Zhang Peiyu Wang Bao Yang Bingjun Yang Juan Yang Kailimai Su Pengjun Ma Yanan Deng Xianfeng Fan Wanjun Chen key laboratory for Electronic Materials College of Electrical Engineering Northwest Minzu University Resource Chemistry and Energy Materials Research Center State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Institute for Materials and processes School of Engineering University of Edinburgh

Rechargeable aqueous zinc-ion batteries （AZIBs） exhibit appreciable potential in the domain of electrochemical energy ***,there are serious challenges for AZIBs,for instance zinc dendrite growth,hydrogen evolution reaction （HER）,and corrosion side ***,we propose a surface engineering modification strategy for coating the montmorillonite （MMT） layer onto the surface of the Zn anode to tackle these issues,thereby achieving high cycling stability for rechargeable *** results reveal that the MMT layer on the surface of the Zn anode is able to provide ordered zincophilic channels for zinc ions migration,facilitating the reaction kinetics of zinc *** functional theory（DFT） calculations and water contact angle （CA） tests prove that MMT@Zn anode exhibits superior adsorption capacity for Zn2+and better hydrophobicity than the bare Zn anode,thereby achieving excellent cycling ***,the MMT@Zn||MMT@Zn symmetric cell holds the stable cycling over 5600 h at 0.5 mA cm-2and 0.125 m A h cm-2,even exceeding 1800 h long cycling under harsh conditions of 5 m A cm-2and 1.25 m A h *** MMT@Zn||V2O5full cell reaches over 3000 cycles at 2 A g-1with excellent rate ***,this surface engineering modification strategy for enhancing the electrochemical performance of AZIBs represents a promising application.

关键词： Surface engineering strategy Montmorillonite layer Protection mechanism of Zn anode Cycling stability Aqueous zinc ion batteries

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Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle

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Journal of Energy Chemistry 2025年第1期100卷 286-308页

作者： Yuhao Peng Yuefeng Song Ihar Razanau Juanxiu Xiao Wei Xiao Di Hu Guoxiong Wang College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University state key laboratory of Catalysis Dalian National Laboratory for Clean Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences laboratory of Physical-Chemical Technologies SSPA Scientific and Practical Materials Research Centre of NAS of Belarus state key laboratory of Marine Resources Utilization in South China Sea Collaborative Innovation Center of Marine Science and Technology School of Marine Science and Engineering Hainan University Department of Chemical and Environmental Engineering University of Nottingham Ningbo China

Methane, an abundant one-carbon（C1） resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO2emissions and coke deposition. Electrochemical conversion of methane（ECM） using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO2emission.

关键词： Methane Electrochemical conversion Reaction mechanism Catalyst design Electrode Electrocatalysis

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Preparation and Luminescent Characteristics of LaPO_4∶Eu Nanoparticles and Nanowires

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Journal of Rare Earths 2004年第1期22卷 57-62页

作者：于立新宋宏伟吕少哲孙宝娟张晓波王铁 key laboratory of excited state physics

Nanoparticles and nanowires of LaPO 4: Eu phosphors were synthesized by hydrothermal method. Their luminescent properties including electronic transition, surface effect, and temperature-dependent luminescent characteristics were systemically studied and compared to the bulk powders. It can be concluded that in comparison with the bulk powders, the fluorescence intensity decreases in nanoparticles and nanowires, while the lifetime increases, indicating that the radiative transition rate decreases. The nonradiative transition rate in nanowires decreases than that in nanoparticles due to its decreased surface to volume ratio. The temperature-dependent experiments indicate that the thermal quenching in nanopowders becomes weaker than that in the bulk powders.

关键词： optics lanthanum phosphate europium ion nanoparticle nanowire transition rate thermal quenching rare earths

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Microstructural evolution during the progressive transformation-induced plasticity effect in a Fe-0.1C-5Mnmedium manganese steel

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 369-379页

作者： Mei Zhang Wenhao Li Yangfei Chen Yang Jiang Xiaofei Guo Han Dong School of Materials Science and Engineering Shanghai UniversityShanghai 200444China state key laboratory of Advanced Special Steel Shanghai UniversityShanghai 200444China

The microstructural evolution of a cold-rolled and intercritical annealed medium-Mn steel(Fe-0.10C-5Mn)was investigated during uniaxial tensile ***-situ observations under scanning electron microscopy,transmission electron microscopy,and X-ray diffraction analysis were conducted to characterize the progressive transformation-induced plasticity process and associated fracture initiation *** findings were discussed with the local strain measurements via digital image *** results indicated that Lüders band formation in the steel was limited to 1.5%strain,which was mainly due to the early-stage martensitic phase transformation of a very small amount of the less stable large-sized retained austenite(RA),which led to localized stress concentrations and strain hardening and further retardation of *** small-sized RA exhibited high stability and progressively transformed into martensite and contributed to a stably extended Portevin-Le Chatelier *** volume fraction of RA gradually decreased from 26.8%to 8.2%prior to *** the late deformation stage,fracture initiation primarily occurred at the austenite/martensite and ferrite/martensite interfaces and the ferrite phase.

关键词： medium-Mn steel retained austenite progressive transformation-induced plasticity effect local strain fracture initiation

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Investigation of bubbles escape behavior from low basicity mold flux for high-Mn high-Al steels using 3D X-ray microscope

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 102-110页

作者： Qiang Liu Xiang Li Shen Du Ming Gao Yanbin Yin Jiongming Zhang state key laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China

During the continuous casting process of high-Mn high-Al steels,various types of gases such as Ar need to escape through the top of the *** which,the behavior of bubbles traversing the liquid slag serves as a restrictive link,closely associated with viscosity and the thickness of liquid *** contrast to two-dimensional surface observation,three-dimensional(3D)analysis method can offer a more intuitive,accurate,and comprehensive ***,this study employs a 3D X-ray microscope(3D-XRM)to obtained spatial distribution and 3D morphological characteristics of residual bubbles in mold flux under different basicity of liquid slag,different temperatures,and different holding *** results indicate that as basicity of slag increases from 0.52 to 1.03,temperature increases from 1423 to 1573 K,the viscosity of slag decreases,the floating rate of bubbles *** addition,when holding time increases from 10 to 30 s,the bubbles floating distance increases,and the volume fraction and average equivalent sphere diameter of the bubbles solidified in the mold flux gradually *** one word,increasing the basicity,temperature,and holding time leading to an increase in the removal rate of bubbles especially for the *** findings of bubbles escape behavior provide valuable insights into optimizing low basicity mold flux for high-Mn high-Al steels.

关键词： mold flux low basicity bubbles three-dimensional X-ray microscope viscosity

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Anomalous quality factor evolution of induced transparency in a virtualized coupled-oscillator system

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Science China(physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 148-155页

作者： Yunhan Yang Han Jia Tuo Liu Yuzhen Yang Jun Yang key laboratory of Noise and Vibration Research Institute of Acoustics Chinese Academy of Sciences University of Chinese Academy of Sciences state key laboratory of Acoustics Institute of Acoustics Chinese Academy of Sciences

The phenomenon of induced transparency, characterized by a high quality(Q) factor, holds significant importance in the fields of high-precision sensing, energy storage and wave manipulation. Conventional transparency systems are often constrained by the limited experimentally accessible parameter space and the lack of independent control over intrinsic parameters, thereby hindering advanced research on high-Q effects. Here we propose a virtualized coupled-oscillator system that enables reconfigurable induced transparency in the reflection spectrum. By virtually incorporating a pair of coupled oscillators into an individual acoustic meta-atom, we achieve the manipulation of induced transparency in a decoupled, wide-ranging, and elaborate manner. Exploiting the diverse evolutions across the intrinsic parameter space, we show experimentally a counter-intuitive increase in the Q-factor of the transparency window, which is attributed to the enhanced dissipation of the bright ***, a constant group delay at the center frequency is observed accompanying this evolution. Our work demonstrates an intriguing platform as well as a novel strategy to engineer high-Q induced transparency phenomenon, and paves the way towards applications in programmable acoustic sensors, filters and slow-wave devices.

关键词： induced transparency acoustic meta-atom high quality-factor scattering programmable intrinsic parameter

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