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Applications of in-situ solid-state nuclear magnetic resonance in methanol to olefins reaction

Science China Chemistry 2025年第1期68卷 134-151页

作者： Jing Niu Shutao Xu Yingxu Wei Zhongmin Liu national Engineering Research Center of Lower-Carbon Catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of Sciences State key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

The methanol-to-olefins（MTO） reaction offers an alternative pathway for the production of low-carbon olefins from non-oil feedstocks. Fundamental research has been impeded by a lack of comprehensive understanding of its underlying mechanism,despite the significant progress made in industry. In-situ solid-state nuclear magnetic resonance（ss NMR） spectroscopy has emerged as a pivotal tool, offering crucial insights into key species under real-time operando conditions. Furthermore, the host–guest interaction between zeolites or surface species residing on zeolites and the reactant/active intermediates is revealed by the combination of in-situ13C MAS NMR and 2D correlation spectroscopy. Moreover, recent technological advancements in hyperpolarization（HP） methods, including HP129Xe NMR and dynamic nuclear polarization（DNP）, have significantly improved the sensitivity of ss NMR, enabling detailed structural and kinetic analysis as well as the detection of trace species. In this feature article, we summarized recent advancements in（in-situ） ss NMR spectroscopy applied to MTO reaction processes,encompassing mechanistic investigations at various stages and the intricate host–guest interactions. These theoretical insights into the dynamic evolution of MTO reactions lay a solid foundation for the optimization of catalytic processes and the development of efficient catalysts, thereby advancing the techniques towards more sustainable and economical production route for olefins.

关键词： MTO zeolites in-situ ssNMR reactive intermediates reaction mechanism

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MixerKT:A Knowledge Tracing Model Based on Pure MLP Architecture

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Computers, Materials & Continua 2025年第1期82卷 485-498页

作者： Jun Wang Mingjie Wang Zijie Li Ken Chen Jiatian Mei Shu Zhang key laboratory of Education Informatization for nationalities Ministry of EducationYunnan Normal UniversityKunming650000China Yunnan key laboratory of Smart Education Yunnan Normal UniversityKunming650000China

In the field of intelligent education,the integration of artificial intelligence,especially deep learning technologies,has garnered significant *** tracing(KT)plays a pivotal role in this field by predicting students’future performance through the analysis of historical interaction data,thereby assisting educators in evaluating knowledgemastery and tailoring instructional *** knowledge tracingmethods,largely based on Recurrent Neural Networks(RNNs)and Transformer models,primarily focus on capturing long-term interaction patterns in sequential ***,these models may neglect crucial short-term dynamics and other relevant *** paper introduces a novel approach to knowledge tracing by leveraging a pure Multilayer Perceptron(MLP)*** proposeMixerKT,a knowledge tracing model based on theHyperMixer framework,which uniquely integrates global and localMixer feature *** architecture enables more effective extraction of both long-terminteraction trends and recent learning behaviors,addressing limitations in currentmodels thatmay overlook these key *** evaluations on twowidely-used datasets,ASSIS Tments2009 and Algebra2005,demonstrate that MixerKT consistently outperforms several state-of-the-art models,including DKT,SAKT,and Separated Self-Attentive Neural Knowledge Tracing(SAINT).Specifically,MixerKT achieves higher prediction accuracy,highlighting its effectiveness in capturing the nuances of learners’knowledge *** results indicate that our model provides a more comprehensive representation of student learning patterns,enhancing the ability to predict future performance with greater precision.

关键词： Knowledge tracing multilayer perceptron channel mixer sequence mixer

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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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Unraveling brain aging through the lens of oral microbiota

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Neural Regeneration Research 2025年第7期20卷 1930-1943页

作者： Qinchao Hu Si Wang Weiqi Zhang Jing Qu Guang-Hui Liu State key laboratory of Membrane biology Institute of ZoologyChinese Academy of SciencesBeijingChina Hospital of Stomatology Guanghua School of StomatologyGuangdong Provincial Key Laboratory of StomatologySun Yat-sen UniversityGuangzhouGuangdong ProvinceChina Advanced Innovation Center for Human Brain Protection and national Clinical Research Center for Geriatric Disorders Xuanwu HospitalCapital Medical UniversityBeijingChina Aging Translational Medicine Center International Center for Aging and CancerBeijing Municipal Geriatric Medical Research CenterXuanwu HospitalCapital Medical UniversityBeijingChina CAS key laboratory of Genomic and Precision Medicine Beijing Institute of GenomicsChinese Academy of Sciences and China National Center for BioinformationBeijingChina University of Chinese Academy of Sciences BeijingChina Institute for Stem Cell and Regeneration Chinese Academy of SciencesBeijingChina Aging Biomarker Consortium BeijingChina State key laboratory of Stem Cell and Reproductive biology Institute of ZoologyChinese Academy of SciencesBeijingChina Beijing Institute for Stem Cell and Regenerative Medicine BeijingChina

The oral cavity is a complex physiological community encompassing a wide range of *** of oral microbiota can lead to various oral infectious diseases,such as periodontitis and tooth decay,and even affect systemic health,including brain aging and neurodegenerative *** studies have highlighted how oral microbes might be involved in brain aging and neurodegeneration,indicating potential avenues for intervention *** this review,we summarize clinical evidence demonstrating a link between oral microbes/oral infectious diseases and brain aging/neurodegenerative diseases,and dissect potential mechanisms by which oral microbes contribute to brain aging and *** also highlight advances in therapeutic development grounded in the realm of oral microbes,with the goal of advancing brain health and promoting healthy aging.

关键词： Alzheimer's disease brain aging multiple sclerosis neurodegeneration neurodegenerative diseases oral microbiota Parkinson's disease periodontitis bacteria Porphyromonas gingivalis

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A self-adaptive inorganic in-situ separator by particle crosslinking for nonflammable lithium-ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 469-480页

作者： Jiarui Yang Jiuzhou Liu Wenrui Cai Ziyu Zhao Shan Wang Lu He Shanshan Lv Zhiwei Zhu Zhongfeng Ji Guojiang Wen Hua Li Yuanming Zhai Xuewei Fu Wei Yang Yu Wang College of Polymer Science and Engineering State Key Laboratory of Polymer Materials Engineering Sichuan University

All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.

关键词： Silica nanoparticles

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Ca2+ cation-mediated microenvironment for electrochemical hydrodimerization of furfural

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Science China Chemistry 2025年

作者： Wei Du Shuangshuang Cha Can Lei Mengxin Qu Zhongqiang Deng Ming Gong Xinhe Bao Department of Chemistry and Shanghai key laboratory of Molecular Catalysis and Innovative Materials Fudan University State key laboratory of Catalysis National Laboratory for Clean Energy Collaborative Innovation Center of Chemistry for Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences

Furfural is one of the most important biomass-based platform molecules as sustainable precursors for chemicals and fuels. The electrochemical hydrodimerization of furfural can generate hydrofuroin, which is a promising precursor for gasoline or jet ***, steering the selectivity toward hydrodimerization under near-neutral conditions that suppress polymerization and disproportionation of furfural remains challenging. Herein, we discovered that tuning the electrolyte cations could be an effective and alternative strategy for modulating furfural reduction to the traditional electrocatalyst design. Under the optimal Ca2+cations,hydrofuroin yield could be much improved from other cations with hydrofuroin selectivity of 95.5%. The systematic characterization of the ion-centered double layer reflected the suitable sizes and charges of hydrated Ca2+for suppressing the hydrogen evolution reaction from activation of surrounding water molecules as well as encouraging furfural accumulation via non-covalent interaction for directing the electron transfer to furfurals. Ions with smaller or larger sizes can either activate local water molecules or form a crowded ionic interface that casts an adverse effect on furfural enrichment. This work not only presents an effective strategy for facilitating biomass valorization via hydrodimerization but also emphasizes the essential role of the ion-centered microenvironment for steering the electrocatalytic pathways.

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Reduced mesencephalic astrocyte-derived neurotrophic factor expression by mutant androgen receptor contributes to neurodegeneration in a model of spinal and bulbar muscular atrophy pathology

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Neural Regeneration Research 2025年第9期20卷 2655-2666页

作者： Yiyang Qin Wenzhen Zhu Tingting Guo Yiran Zhang Tingting Xing Peng Yin Shihua Li Xiao-Jiang Li Su Yang Guangdong key laboratory of Non-human Primate Research Key Laboratory of CNS Regeneration(Ministry of Education)Guangdong–HongKong–Macao Institute of CNS RegenerationJinan UniversityGuangzhouGuangdong ProvinceChina

Spinal and bulbar muscular atrophy is a neurodegenerative disease caused by extended CAG trinucleotide repeats in the androgen receptor gene,which encodes a ligand-dependent transcription facto *** mutant androgen receptor protein,characterized by polyglutamine expansion,is prone to misfolding and forms aggregates in both the nucleus and cytoplasm in the brain in spinal and bulbar muscular atrophy *** aggregates alter protein-protein interactions and compromise transcriptional *** this study,we reported that in both cultured N2a cells and mouse brain,mutant androgen receptor with polyglutamine expansion causes reduced expression of mesencephalic astrocyte-de rived neurotrophic *** n of mesencephalic astrocyte-derived neurotrophic factor amelio rated the neurotoxicity of mutant androgen receptor through the inhibition of mutant androgen receptor *** down endogenous mesencephalic astrocyte-derived neurotrophic factor in the mouse brain exacerbated neuronal damage and mutant androgen receptor *** findings suggest that inhibition of mesencephalic astrocyte-derived neurotrophic factor expression by mutant androgen receptor is a potential mechanism underlying neurodegeneration in spinal and bulbar muscular atrophy.

关键词： androgen receptor mesencephalic astrocyte-derived neurotrophic factor mouse model neurodegeneration neuronal loss neurotrophic factor polyglutamine disease protein misfolding spinal and bulbar muscular atrophy transcription factor

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Distributed optimal consensus control for multiagent systems based on event-triggered and prioritized experience replay strategies

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Science China(Information Sciences) 2025年第1期68卷 306-321页

作者： Cuijuan ZHANG Lianghao JI Shasha YANG Xing GUO Huaqing LI Chongqing key laboratory of Image Cognition Chongqing University of Posts and Telecommunications key laboratory of Intelligent Perception and Computing of Anhui Province Anqing Normal University College of Electronic and Information Engineering Southwest University

This study uses event-triggered(ET) and reinforcement learning methods to investigate the optimal consensus control problem for cooperative-competitive multiagent systems. It proposes a novel distributed ET control strategy, which relies on a prioritized experience replay(PER) policy. This strategy not only conserves communication resources but also ensures acceptable system performance. To implement the proposed method, actor-critic(AC) dual-structured neural networks(NNs) are used to approximate the value function and control policy. In the AC NNs, the weight estimates for the NNs are updated at the moment of event triggering, resulting in a nonperiodic weight adjustment pattern. This approach decreases the computational cost in comparison with the traditional ET mechanism. The PER-based ET mechanism makes full use of valid historical data and effectively establishes a balance between system performance and communication resource ***, it does not require the following two conditions in most existing studies:(1) requirement of the system dynamics model to be known, and(2) persistent excitation. In addition, Zeno behavior is excluded from this study. Finally, a simulation is conducted to confirm the validity of the suggested approach.

关键词： multiagent systems event-triggered mechanism prioritized experience replay dual-structured neural networks optimal consensus control

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Double [5]carbohelicene: facile synthesis, chiroptical properties,isomerization study, and lasing application

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Science China Chemistry 2025年第1期68卷 233-240页

作者： Peipei Liu Yantong Li Meng-Xiang Wu Hao Kang Xiao-Li Zhao Lin Xu Linlin Liu Xiaodong Li Junfeng Fang Zhiwei Fang Ya Cheng Hai-Bo Yang Huakang Yu Xueliang Shi State key laboratory of Petroleum Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular Engineering East China Normal University School of Physics and Optoelectronics South China University of Technology Institute of Polymer Optoelectronic Materials & Devices State Key Laboratory of Luminescent Materials & Devices South China University of Technology School of Physics and Electronic Science Engineering Research Center of Nanophotonics & Advanced Instrument Ministry of EducationEast China Normal University State key laboratory of Precision Spectroscopy School of Physics and Electronic Science East China Normal University

Double carbohelicenes have attracted considerable attention due to their aesthetic structures, distinct π-conjugation extension, inherent chirality, and intriguing optical and electronic properties. Herein, the concise de novo synthesis of a new double[5]carbohelicene 1 together with its chiroptical properties, isomerization process and lasing application is presented. 1 was synthesized by a simple protocol involving the formation of a 6,6′-bipentacene as the key intermediate. It is worth noting that1 existed as two diastereomers 1-PP/MM and 1-PM, which were successfully isolated and unambiguously confirmed by Xray crystallography. The optical resolution of the racemic 1-PP/MM was successfully achieved by chiral-phase highperformance liquid chromatography（HPLC）, and 1-PP and 1-MM were characterized by circular dichroism. Interestingly, it was found that 1-PP/MM could be completely isomerized to 1-PM upon heating, and the detailed thermodynamics and kinetics of the isomerization process were systematically investigated. 1-PM exhibited deep-red luminescence with emission maximum at 723 nm and fluorescence quantum yield as high as 32.95%. Consequently, we can showcase the lasing application of 1-PM by doping with epoxy resin to assemble a bottle microlaser spontaneously, which the lasing wavelength is 796.6 nm at a threshold of 0.8 m J cm-2. We believe that our studies, including the facile synthesis methodology, detailed isomerization studies, and lasing application, will shed some light on the design and synthesis of novel carbohelical systems with more functions.

关键词： double carbohelicene optical resolution organic laser isomerization X-ray diffraction

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Deciphering Water Oxidation Catalysts:The Dominant Role of Surface Chemistry over Reconstruction Degree in Activity Promotion

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Nano-Micro Letters 2025年第3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi * Zhichuan JXu Chun‑Hua Yan State key laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy Engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China key laboratory of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China State key laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing national laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction

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