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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： Aspect ratio

Spin-modulated near-infrared-Ⅰ emission in a xanthene-decorated Fe(Ⅱ) spin-crossover complex

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Science China Chemistry 2025年

作者： Cheng Yi Duyong Chen Shihui Zhang Rui Cai Chunying Duan Yinshan Meng Tao Liu State Key Laboratory of Fine Chemicals Frontier Science Center for Smart Materials and Chemical Engineering School of Chemical Engineering Dalian University of Technology Instrumental Analysis Center Dalian University of Technology school of Chemistry Dalian University of Technology Liaoning Binhai Laboratory

Molecular materials showing synergetic coupling of near-infrared （NIR） fluorescence and spin-crossover （SCO） are promisingly applicable in in-vivo bioimaging,temperature sensing,and spintronic *** the related study faces formidable *** this work we graft the NIR fluorophore xanthene onto the dipyridyl substituted triazole ligand and construct a new Febased SCO material,{FeⅡ（ddxc-abpt）2[N（CN）2]2}(1,ddxc-abpt:（E）-4-(((3,5-di（pyridin-2-yl）-4H-1,2,4-triazol-4-yl)imino)methyl)-N,N-diethyl-2,3-dihydro-1H-xanthen-6-amine).Magnetic studies indicate that compound 1 exhibits thermally induced SCO property in both the solid and solution ***-temperature fluorescence emission spectra reveal a remarkable 7-fold increase in photoluminescence intensity upon the transition from the low-spin state at 110 K to the high-spin state at 280 K,which is the record of all reported coupled fluorescence-SCO ***-temperature ultraviolet-visible （UV-Vis）absorption spectra show a significant change in absorption intensity within the fluorescence emission window,consistent with the F?rster resonance energy transfer （FRET） ***-dependent density functional theory （TD-DFT） calculations demonstrate that the strong coupling is attributed to disrupted energy transfer between the xanthene fluorophore and high-spin *** work provides a feasible approach for expanding the synergetic SCO-fluorescence materials to the NIR-Iwavelength region,and hopefully contributes to the applications of tunable NIR-SCO molecule-based sensors and devices.

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Spontaneous Orientation Polarization of Anisotropic Equivalent Dipoles Harnessed by Entropy Engineering for Ultra‑Thin Electromagnetic Wave Absorber

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Nano-Micro Letters 2025年第1期17卷 424-438页

作者： Honghan Wang Xinyu Xiao Shangru Zhai Chuang Xue Guangping Zheng Deqing Zhang Renchao Che Junye Cheng Liaoning Key Lab of Lignocellulose Chemistry and BioMaterials Liaoning Collaborative Innovation Center for Lignocellulosic BiorefinerySchool of Light Industry and Chemical EngineeringDalian Polytechnic UniversityDalian 116034People’s Republic of China school of Life Science and Biotechnology Dalian University of TechnologyDalian 116024People’s Republic of China Department of Mechanical Engineering Hong Kong Polytechnic UniversityHung HomKowloonHong Kong 999077People’s Republic of China school of Materials Science and Engineering Qiqihar UniversityQiqihar 161006People’s Republic of China Laboratory of Advanced Materials Shanghai Key Lab of Molecular Catalysis and Innovative MaterialsAcademy for Engineering&TechnologyFudan UniversityShanghai 200438People’s Republic of China Department of Materials Science Shenzhen MSU-BIT UniversityShenzhen 517182People’s Republic of China

The synthesis of carbon supporter/nanoscale high-entropy alloys(HEAs)electromagnetic response composites by carbothermal shock method has been identified as an advanced strategy for the collaborative competition engineering of conductive/dielectric *** migration modes within HEAs as manipulated by the electronegativity,valence electron configurations and molar proportions of constituent elements determine the steady state and efficiency of equivalent ***,enlightened by skin-like effect,a reformative carbothermal shock method using carbonized cellulose paper(CCP)as carbon supporter is used to preserve the oxygencontaining functional groups(O·)of carbonized cellulose fibers(CCF).Nucleation of HEAs and construction of emblematic shell-core CCF/HEAs heterointerfaces are inextricably linked to carbon metabolism induced by O·.Meanwhile,the electron migration mode of switchable electronrich sites promotes the orientation polarization of anisotropic equivalent *** virtue of the reinforcement strategy,CCP/HEAs composite prepared by 35%molar ratio of Mn element(CCP/HEAs-Mn_(2.15))achieves efficient electromagnetic wave(EMW)absorption of−51.35 dB at an ultra-thin thickness of 1.03 *** mechanisms of the resulting dielectric properties of HEAs-based EMW absorbing materials are elucidated by combining theoretical calculations with experimental characterizations,which provide theoretical bases and feasible strategies for the simulation and practical application of electromagnetic functional devices(e.g.,ultra-wideband bandpass filter).

关键词： high-entropy alloys Carbothermal shock Switchable electron migration modes Emblematic shell-core heterointerfaces Ultra-thin thickness

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A bio-inspired optical imaging method for robotic perception in turbid water

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Science China Technological Sciences 2025年第1期 79-81页

作者： Xudong SUN Yafeng LI Peng LIN Xiaodi SHANG Xianping FU school of Information Science and Technology Dalian Maritime University College of Computer Science and Technology Qingdao University

In the realm of underwater robotics, optical imaging plays a pivotal role in many scientific researches. Due to the effects of absorption and scattering,images captured in turbid water are severely degraded. Therefore, enhancing the quality of underwater optical images stands paramount in ensuring the continued advancement and efficacy of underwater robots across its multifarious applications.

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Visible-light-responsive homologous heterostructure of oxynitrides constructed to boost charge separation and water splitting

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Science China Chemistry 2025年第01期 186-191页

作者： Hai Zou Yunfeng Bao Xueshang Xin Yu Qi Tengfeng Xie Fuxiang Zhang State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences school of Chemistry and Chemical Engineering Liaoning Normal University College of Chemistry Jilin University

Constructing type II heterostructures represents a widely recognized strategy for enhancing charge separation and photocatalytic efficiency,but it remains challenging to fabricate homologous heterostructures based on visible-light-responsive semiconductors,especially for popularly investigated （oxy）nitrides with low thermal ***,we synthesized a homologous heterostructure （denoted as YTON＿H） based on the oxynitrides of YTaO4-xNyand YTa *** heterostructure exhibits type II band structure alignment and intimate interface achieved through a magnesium （Mg） powder-assisted nitridation *** with widely reported heterologous heterostructures,the as-obtained YTON＿H homologous heterostructure could similarly exhibit enhanced charge separation as well as photocatalytic water splitting performance with respect to its counterparts(YTaO4-xNyand YTaON2).Meanwhile,detailed structural characterizations and spectroscopy analysis have been made to confirm the formation of heterostructure and promotion of spatial charge separation.

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The Curative HCV Treatments in China

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Journal of Biosciences and Medicines 2018年第8期6卷 42-59页

作者： Yifan Fei Jiawen Jiang China Agricultural University Beijing China dalian no.24 high school Dalian China

Hepatitis C disease is caused by hepatitis C virus (HCV) which causes chronic infections in about 180 million individuals worldwide. HCV has been identified as the etiologic agent of hepatitis C in 1989 and for the longest time it is very difficult to treat chronic carriers who are at risk of developing severe liver disease. Now there are three main combined treatments which can increase curative ratio from 10% to more than 90%. The advents of so called directly, acting antivirals (DAAs) in the last few years has revolutionized HCV treatment as these drug combinations can effectively cure HCV in the great majority of patients. The impact of DAAs on global disease burden has been limited, however, by the very drug prices. In this paper the situation was analyzed in China, Europe and Australia. DAAs have been made available to patients in Europe and Australia for several years and are generally accessible. The treatment is highly subsidized by the government, thereby making it possible for all patients in need to access therapy. DAAs have only been very recently been adopted for treatment of chronic hepatitis C in China. In our research, only the method of literature search from both Chinese websites and Foreign websites including journals, magazines and internet search is used. We analyze and compare the solutions that each of these countries is providing to their respective patient populations. Given the large number of chronic HCV carriers in China and other less developed countries solutions have to be found to produce DAAs most cost effectively.

关键词： HCV DAA China Australia Europe

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： Activation energy

Controllable synthesis of biomimetic wood stem nanoporous high entropy oxides catalysts for oxygen evolution reaction

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Nano Research 2025年第1期18卷 107-117页

作者： Wei Wang Weiqi Wang Huihui Wang Xing Lu Jinwen Zhang Yunzhuo Lu school of Materials Science and Engineering Dalian Jiaotong UniversityDalian 116028China school of Intelligence and Electronic Engineering Dalian Neusoft University of InformationDalian 116023China Guangdong Key Laboratory of Materials and Equipment in Harsh Marine Environment Guangzhou Maritime UniversityGuangzhou 510725China

Bubbles generated during the oxygen evolution reaction(OER)in water splitting readily adhere to the electrode surface,thereby impeding contact between the electrolyte and the active sites,thereby increasing the ***,it is imperative to elucidate the bubble release behavior and engineer electrodes that facilitate faster bubble *** this study,inspired by the wood stem of the Norway spruce,we synthesized a gradient nanoporous high-entropy oxide(GNP-HEO)electrode with a controllable pore *** GNP-HEO,featuring a well-controlled gradient in pore size,is achieved through a straightforward strategy combining selective laser melting with selective phase *** unique gradient nanoporous structure not only facilitates bubble release but also diminishes the bubble shielding effect in OER,thereby enhancing electrocatalytic *** affect interaction of Al,Co,Cr,Fe,and Ni,coupled with the gradient nanoporous structure,yields exceptional OER performance,evidenced by an overpotential of 250 mV at a current density of 50 mA/cm^(2) and a Tafel slope of 38.0 mV/dec in 1 M *** functional theory calculations confirm that the GNPHEO adheres to the adsorbate evolution mechanism reaction pathway and exhibits significant *** work highlights a promising approach for the design and synthesis of high-performance OER electrocatalysts.

关键词： oxygen evolution reaction high-entropy oxides selective phase dis-solution selective laser melting gradient nanoporous

Surrogate model uncertainty quantification for active learning reliability analysis

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Chinese Journal of Aeronautics 2024年第12期37卷 55-70页

作者： Yong PANG Shuai ZHANG Pengwei LIANG Muchen WANG Zhuangzhuang GONG Xueguan SONG Ziyun KAN State Key Laboratory of high-performance Precision Manufacturing School of Mechanical EngineeringDalian University of TechnologyDalian 116024China

Surrogate models offer an efficient approach to tackle the computationally intensive evaluation of performance functions in reliability ***,the approximations inherent in surrogate models necessitate the consideration of surrogate model uncertainty in estimating failure *** paper proposes a new reliability analysis method in which the uncertainty from the Kriging surrogate model is quantified *** method treats surrogate model uncertainty as an independent entity,characterizing the estimation error of failure *** upon the probabilistic classification function,a failure probability uncertainty is proposed by integrating the difference between the traditional indicator function and the probabilistic classification function to quantify the impact of surrogate model uncertainty on failure probability ***,the proposed uncertainty quantification method is applied to a newly designed reliability analysis approach termed SUQ-MCS,incorporating a proposed median approximation function for active *** proposed failure probability uncertainty serves as the stopping criterion of this *** benchmarking,the effectiveness of the proposed uncertainty quantification method is *** empirical results present the competitive performance of the SUQ-MCS method relative to alternative approaches.

关键词： Reliability analysis Kriging model Uncertainty quantification Active learning Monte Carlo simulation