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Boosting cationic and anionic redox activity of Li-rich layered oxide cathodes via Li/Ni disordered regulation

Journal of Energy Chemistry 2025年第1期100卷 533-543页

作者： Zewen liu Zhen Wu Hao Wang Xudong Zhang Yuanzhen Chen Yongning liu Shengwu Guo Shenghua Chen Yanli Nan Yan liu State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University School of Materials Science and Engineering Xi'an University of Architecture and Technology Hefei Advanced Computing Center Operation Management Corp Ltd Network Information Center Xi'an Jiaotong University

Lithium-rich layered oxides （LLOs） are increasingly recognized as promising cathode materials for nextgeneration high-energy-density lithium-ion batteries （LIBs）.However,they suffer from voltage decay and low initial Coulombic efficiency （ICE） due to severe structural degradation caused by irreversible O ***,we introduce a three-in-one strategy of increasing Ni and Mn content,along with Li/Ni disordering and TM–O covalency regulation to boost cationic and anionic redox activity simultaneously and thus enhance the electrochemical activity of *** target material,Li1.2Ni0.168Mn0.558Co0.074O2（L1）,exhibits an improved ICE of 87.2%and specific capacity of 293.2 mA h g-1and minimal voltage decay of less than 0.53 m V cycle-1over 300 cycles at 1C,compared to Li1.2Ni0.13Mn0.54Co0.13O2（Ls）(274.4 mA h g-1for initial capacity,73.8%for ICE and voltage decay of 0.84 mV/cycle over 300 cycles at 1C).Theoretical calculations reveal that the density of states （DOS） area near the Fermi energy level for L1 is larger than that of Ls,indicating higher anionic and cationic redox reactivity than ***,L1 exhibits increased O-vacancy formation energy due to higher Li/Ni disordering of 4.76%（quantified by X-ray diffraction Rietveld refinement） and enhanced TM–O covalency,making lattice O release more difficult and thus improving electrochemical *** increased Li/Ni disordering also leads to more Ni2+presence in the Li layer,which acts as a pillar during Li+de-embedding,improving structural *** research not only presents a viable approach to designing low-Co LLOs with enhanced capacity and ICE but also contributes significantly to the fundamental understanding of structural regulation in high-performance LIB cathodes.

关键词： Ice

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Mesh-supported V2O5-WO3/TiO2 nanosheet array catalysts for efficient removal of NOx

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Tungsten 2025年第1期7卷 100-111页

作者： Zhi-Qi Zhang liu Yang Wen Luo Vladimir An Jing Li Bao-Dan liu School of Materials Science and Engineering Northeastern University Foshan Graduate School of Innovation Northeastern University Kizhner Research Center School of Advanced Manufacturing Technologies Tomsk Polytechnic University

The design and synthesis of vanadium-based denitration catalysts with low-temperature activity pose significant challenges in the field of toxic gas *** this study,we have developed a novel approach to fabricate highly efficient V2O5-WO3/TiO2monolithic mesh catalysts for NOxreduction at low ***,TiO2nanosheets with strong adhesion and large surface area were grown on Ti mesh using plasma electrolytic oxidation technology and hydrothermal ***,super-small traces of WO3and V2O5active nano-species were subsequently deposited on TiO2nanosheets using the deposition-precipitation *** to traditional ceramic-based V2O5-WO3/TiO2catalysts,our V2O5-WO3/TiO2monolithic mesh catalyst exhibits superior mechanical performance,excellent thermal conductivity,lower pressure drop,higher utilization of active components,and stronger synergistic ***,the V2O5-WO3/TiO2monolithic mesh catalysts exhibited excellent low-temperature catalytic activity with 98% of NOxconversion at 220℃,and remarkable long-term SO2tolerance and water resistance in the selective catalytic reduction（SCR） of NOxwith *** SCR reaction of tiny V2O5and WO3active species supported on TiO2nanosheets directly demonstrated to follow the Eley-Rideal mechanism by in situ infrared spectra.

关键词： Low temperature activity Monolithic mesh catalysts NH3-SCR SO2 tolerance V2O5-WO3/TiO2

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DIGNN-A:Real-Time Network Intrusion Detection with Integrated Neural Networks Based on Dynamic Graph

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Computers, Materials & Continua 2025年第1期82卷 817-842页

作者： Jizhao liu Minghao Guo College of Computer Zhongyuan University of TechnologyZhengzhou450007China

The increasing popularity of the Internet and the widespread use of information technology have led to a rise in the number and sophistication of network attacks and security *** detection systems are crucial to network security,playing a pivotal role in safeguarding networks from potential ***,in the context of an evolving landscape of sophisticated and elusive attacks,existing intrusion detection methodologies often overlook critical aspects such as changes in network topology over time and interactions between *** address these issues,this paper proposes a real-time network intrusion detection method based on graph neural *** proposedmethod leverages the advantages of graph neural networks and employs a straightforward graph construction method to represent network traffic as dynamic graph-structured ***,a graph convolution operation with a multi-head attention mechanism is utilized to enhance the model’s ability to capture the intricate relationships within the graph structure ***,it uses an integrated graph neural network to address dynamic graphs’structural and topological changes at different time points and the challenges of edge embedding in intrusion detection *** edge classification problem is effectively transformed into node classification by employing a line graph data representation,which facilitates fine-grained intrusion detection tasks on dynamic graph node feature *** efficacy of the proposed method is evaluated using two commonly used intrusion detection datasets,UNSW-NB15 and NF-ToN-IoT-v2,and results are compared with previous studies in this *** experimental results demonstrate that our proposed method achieves 99.3%and 99.96%accuracy on the two datasets,respectively,and outperforms the benchmark model in several evaluation metrics.

关键词： Intrusion detection graph neural networks attention mechanisms line graphs dynamic graph neural networks

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NHC-mediated photocatalytic para-selective C–H acylation of aryl alcohols: regioselectivity control via remote radical spiro cyclization

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Science china Chemistry 2025年

作者： Tinglei Zhang Lala Wang Xiaolin Peng Tianhui Liao Dongmei Chen Ting Tu Donghan liu Ziye Cheng Shiqing Huang Shi-Chao Ren Xinglong Zhang Yonggui Robin chi State Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education Guizhou University Qiannan Medical College for Nationalities School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University Department of Chemistry The Chinese University of Hong Kong Institute of High Performance Computing Agency for Science Technology and Research

Friedel-Crafts reaction and transition-metal catalysis represent primary methodologies for arene acylation; however, suffer from certain limitations, such as electronic effect-dependent reactivity, regioselectivity issues, the necessity of directing group, and relatively exceptionally limited exploration in meta-and para-acylations. N-heterocyclic carbene(NHC) catalysis has recently emerged as a promising alternative strategy for arene acylation, offering distinct regioselectivity profiles that are challenging to achieve through known methods. Herein, an NHC-mediated photo-catalytic para-selective C–H acylation of aryl alcohols is disclosed. The reaction employs a remote radical-induced temporary spiro cyclization strategy, proceeding via tandem radical dearomatization, radical acylation, rearomatization processes. Combined experimental and computational mechanistic studies support the proposed reaction pathway and observe an exclusive para-selectivity regardless of the nature of the substituents on the substrates. Despite the less satisfactory yields, the current method exhibits non-electronic nature-based reactivity and regioselectivity, enabling quick access to acylated arenes that are difficult or impossible for reported methods.

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Research progress of catalysts for direct coal liquefaction

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Journal of Energy Chemistry 2025年第1期100卷 481-497页

作者： Wei Song Penggao liu Xinyue Chen Ting Wang Chunrong He Rui Hao Kaiyu liu State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources College of Chemistry Xinjiang University College of Chemistry and Chemical Engineering Henan Polytechnic University Hunan Provincial Key Laboratory of Chemical Power Sources College of Chemistry and Chemical Engineering Central South University

Coal direct liquefaction technology is a crucial contemporary coal chemical technology for efficient and clean use of coal resources. The development of direct coal liquefaction technology and the promotion of alternative energy sources are important measures to guarantee energy security and economic security. However, several challenges need to be addressed, including low conversion rate, inadequate oil yield, significant coking, demanding reaction conditions, and high energy consumption. Extensive research has been conducted on these issues, but further exploration is required in certain aspects such as pyrolysis of macromolecules during the liquefaction process, hydrogen activation, catalysts' performance and stability, solvent hydrogenation, as well as interactions between free radicals to understand their mechanisms better. This paper presents a comprehensive analysis of the design strategy for efficient catalysts in coal liquefaction, encompassing the mechanism of coal liquefaction, catalyst construction,and enhancement of catalytic conversion efficiency. It serves as a comprehensive guide for further research endeavors. Firstly, it systematically summarizes the conversion mechanism of direct coal liquefaction, provides detailed descriptions of various catalyst design strategies, and especially outlines the catalytic mechanism. Furthermore, it addresses the challenges and prospects associated with constructing efficient catalysts for direct coal liquefaction based on an understanding of their action mechanisms.

关键词： Direct coal liquefaction Catalysts Mechanism of action Solvent hydrogenation

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Miyaoka-type inequalities for terminal threefolds with nef anti-canonical divisors

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Science china Mathematics 2025年第1期68卷 1-18页

作者： Masataka Iwai Chen Jiang Haidong liu Department of Mathematics Graduate School of ScienceOsaka University Shanghai Center for Mathematical Sciences & School of Mathematical Sciences Fudan University Department of mathematics Sun Yat-sen University

In this paper,we study Miyaoka-type inequalities on Chern classes of terminal projective 3-folds with nef anti-canonical *** X be a terminal projective 3-fold such that-KXis *** show that if c1（X） · c2（X）≠0,then c1（X） · c2（X） ≥ 1/252;if further X is not rationally connected,then c1（X） · c2（X） ≥ 4/5 and this inequality is *** order to prove this,we give a partial classification of such varieties along with many *** also study the nonvanishing of c1（X）dim X-2· c2（X） for terminal weak Fano varieties and prove a Miyaoka-Kawamata-type inequality.

关键词： terminal threefolds Miyaoka-type inequality boundedness

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Multiphysics simulation and optimization of the in-situ beneficiation process of ilmenite minerals from lunar regolith

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Science china Earth Sciences 2025年第1期68卷 195-207页

作者： Peng ZHANG Xin liu Guanghui liu Wei DAI Hanzhe YANG Haibo ZHENG Zhi WANG Ran NIU Yifan BAI Yang ZHANG Chengbao liu Ge YANG Junwei YANG Guang ZHANG Technology and Engineering Center for Space Utilization Chinese Academy of Sciences Beijing Hegong Simulation Co. Ltd

The exploration and utilization of lunar resources have become the major objectives of future lunar exploration missions. The classified collection and processing of lunar minerals is the basic prerequisite for the in-situ exploration and utilization of lunar resources. In this study, we propose a scheme for in-situ separation of magnetic minerals from lunar soils using the dry magnetic separation method. The scheme can realize the purpose of separating magnetic minerals from lunar regolith by altering the motion trajectory of lunar regolith particles with different magnetic properties. Detailed modeling of the dry magnetic separation device is conducted, and the three-dimensional distribution of magnetic parameters is calculated and analyzed. Based on the characterization and analysis of the Chang E-5's samples, the morphologies and physical parameters of lunar regolith particles are modeled and simulated. A discrete element simulation of the motion process of lunar regolith particles under multi-physical field conditions is performed, and the influences of key parameters on the beneficiation performance of lunar magnetic minerals are investigated. Our results indicate that optimal separation and beneficiation of lunar regolith particles can be achieved under specific conditions of magnetic field strength and drum speed. Additionally, we analyze the effects of lunar weak gravity conditions and the charged nature of lunar particles on the beneficiation process, showing that these factors can obviously enhance the beneficiation process of lunar ilmenites. This study demonstrates the feasibility of using the dry magnetic separation method for the beneficiation of magnetic minerals from lunar regolith, providing a theoretical basis for the scientific tasks of collecting, processing, and utilizing lunar mineral resources.

关键词： Lunar regolith In-situ resource utilization Magnetic separation Classified sampling

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

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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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Observation of topological charge transformations in acoustic vortex using passive periodic systems

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Science china(Physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 140-147页

作者： Di-Chao Chen Xie liu Changqing Xu Da-Jian Wu Ying Cheng Xiao-Jun liu School of Physics and Technology Nanjing Normal University Key Laboratory of Modern Acoustics School of Physics Nanjing University

Vortex transmutation utilizes a periodic system, which not only enables the alteration of the topological charge(TC) of unstable input vortices but also facilitates their transformation into stable structures. This approach is crucial for investigating the characteristics of vortices in various wave systems. Here, we achieve acoustic vortex TC transmutation by employing a welldesigned dual-structured plate external system(DPES). The interactions between the acoustic vortex and the finite-order discrete rotational symmetry lead to the transformation of its topological charge when complete rotational symmetry is broken to Nthorder discrete symmetry. Our results experimentally demonstrate the acoustic vortex TC transmutation based on passive artificial structures, enabling numerous applications in particle manipulation and information multiplexing as well as advancing our understanding and control over free-space acoustic vortices.

关键词： acoustic vortex topological charge transformation artificial structure

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秦艽生物鹼甲的藥理作用 Ⅱ.秦艽生物鹼甲的抗炎作用及与一些临床有效藥物的比較

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生理学报 1959年第2期 151-157页

作者：籍秀娟劉耕陶宋振玉中国医学科学院药物研究所药理室中国医学科学院药物研究所药理室北京

从大鼠后足掌部向踝关节皮下注射蛋清0.1毫升,半小时后踝关节卽呈腫胀且消退很慢。如于注射蛋清前半小时腹腔注射秦艽甲90毫克/千克,則踝关节部腫胀程度较轻,且消退亦快。但在去除两侧腎上腺的大鼠及用戊巴此妥纳麻醉的正常大鼠,则预先... 详细信息

从大鼠后足掌部向踝关节皮下注射蛋清0.1毫升,半小时后踝关节卽呈腫胀且消退很慢。如于注射蛋清前半小时腹腔注射秦艽甲90毫克/千克,則踝关节部腫胀程度较轻,且消退亦快。但在去除两侧腎上腺的大鼠及用戊巴此妥纳麻醉的正常大鼠,则预先注射秦艽甲并不能抑制蛋清性“关节炎”的产生,亦不促进其消退。可见秦艽甲对蛋清性“关节炎”的作用必须在动物两侧腎上腺保持完整时才能发生。但秦艽甲并非直接作用于腎上腺,而是通过神经系统的。秦艽甲对因注射甲醛而产生的“关节炎”的作用也是如此。预先注射氯喹、秦艽中性酒精浸剂、水杨酸鈉或考地松,虽不抑制蛋清性“关节炎”的产生,但都能加速关节部腫胀的消退。对因注射甲醛而产生的“关节炎”的治疗作用,秦艽鹼甲甲与氯喹、考地松及秦艽中性酒精浸剂相似,但较水杨酸钠略强。

关键词：蛋清秦艽祛风湿药大鼠关节炎动物腹腔注射

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