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Catalytic effect in lithium metal batteries: From heterogeneous catalyst to homogenous catalyst

Journal of Energy Chemistry 2024年第3期90卷 305-326,I0008页

作者： Haining Fan Xuan-Wen Gao Hailong Xu Yichun Ding Shi-Xue dou Wen-Bin Luo School of Fashion and Textiles The Hong Kong Polytechnic UniversityHong Kong 100872China Institute for Energy Electrochemistry and Urban Mines Metallurgy School of MetallurgyNortheastern UniversityShenyang 110819LiaoningChina Institute of Energy Materials Science University of Shanghai for Science and TechnologyShanghai 200000China State Key Laboratory of Solidification Processing School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi'an 710000ShaanxiChina

Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical *** the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic *** order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy *** past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been ***,it is necessary to make a comprehensive review toward key progress in catalyst design and future development *** this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly *** main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as ***,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and *** review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.

关键词： Energy storage and conversion Metal battery Sulfur battery Air battery Catalytic effect Heterogeneous catalyst Homogeneous catalyst

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Co-aromatization of methane and hexane over Pt encapsulated in ZSM-5 zeolite and the electronic effect of K promoters

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Science China Chemistry 2024年第3期67卷 1017-1027页

作者： Bei Liu Fan Wang Xiaomeng dou Pengfei Li Hongwei Xiang Yong Yang Peng He State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China Department of Chemistry Tsinghua UniversityBeijing 100084China National Energy R&D Center for Coal to Liquid Fuels Synfuels China Technology Co.Ltd.Beijing 101407China University of Chinese Academy of Sciences Beijing 101408China Leibniz-Institut für Katalyse e.V.an der Universitat Rostock Rostock 18059Germany

The co-aromatization of methane with higher hydrocarbons represents a promising route to valorize methane, an abundant but underexploited carbon resource. In this study, we elucidate a novel approach to enhance the catalytic co-aromatization of hexane and methane by confining Pt within zeolite catalysts and modulating its electron density. Our findings show that encapsulating Pt within MFI structure is pivotal for activating the feedstock and fostering the formation of aromatic products. Interaction between K atoms and the silanol nest forms siloxy groups which are critical for the stabilization of Pt species. Tuning the K content in PtSn@MFI catalysts adeptly alters the electronic configuration of Pt clusters. This modification is corroborated by infrared and X-ray photoelectron spectroscopy analysis, and density functional theory calculations. Remarkably, the catalyst with 0.8 wt% K exhibits an optimal Pt electron density, driving its superior efficacy in the co-aromatization reaction, converting 0.78 mol of methane for each mole of hexane processed. By employing ~(13)C isotopic labeling and solid-state NMR studies, we demonstrate the participation of methane in the adsorbed species inside the zeolite channel and its incorporation to the benzyl site of the substitute group and phenyl rings in aromatic compounds, underscoring the importance of Pt encapsulation.

关键词： Pt encapsulation MFI zeolite methane activation co-aromatization ^(13)C solid-state NMR

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XRL-SHAP-Cache:an explainable reinforcement learning approach for intelligent edge service caching in content delivery networks

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Science China(Information Sciences) 2024年第7期67卷 46-71页

作者： Xiaolong XU Fan WU Muhammad BILAL Xiaoyu XIA Wanchun dou Lina YAO Weiyi ZHONG School of Software Nanjing University of Information Science and Technology School of Computing and Communications Lancaster University School of Computing Technologies Royal Melbourne Institute of Technology State Key Laboratory for Novel Software Technology Nanjing University School of Computer Science and Engineering University of New South Wales Data 61 Commonwealth Scientific and Industrial Research Organization School of Computer Science Qufu Normal University

Content delivery networks(CDNs) play a pivotal role in the modern internet infrastructure by enabling efficient content delivery across diverse geographical regions. As an essential component of CDNs, the edge caching scheme directly influences the user experience by determining the caching and eviction of content on edge servers. With the emergence of 5G technology, traditional caching schemes have faced challenges in adapting to increasingly complex and dynamic network environments. Consequently, deep reinforcement learning(DRL) offers a promising solution for intelligent zero-touch network governance. However, the blackbox nature of DRL models poses challenges in understanding and making trusting decisions. In this paper,we propose an explainable reinforcement learning(XRL)-based intelligent edge service caching approach,namely XRL-SHAP-Cache, which combines DRL with an explainable artificial intelligence(XAI) technique for cache management in CDNs. Instead of focusing solely on achieving performance gains, this study introduces a novel paradigm for providing interpretable caching strategies, thereby establishing a foundation for future transparent and trustworthy edge caching solutions. Specifically, a multi-level cache scheduling framework for CDNs was formulated theoretically, with the D3QN-based caching scheme serving as the targeted interpretable model. Subsequently, by integrating Deep-SHAP into our framework, the contribution of each state input feature to the agent's Q-value output was calculated, thereby providing valuable insights into the decision-making process. The proposed XRL-SHAP-Cache approach was evaluated through extensive experiments to demonstrate the behavior of the scheduling agent in the face of different environmental *** results demonstrate its strong explainability under various real-life scenarios while maintaining superior performance compared to traditional caching schemes in terms of cache hit ratio, quality of service(QoS),a

关键词： deep reinforcement learning (DRL) explainable artificial intelligence (XAI) multi-level cache content delivery network (CDN) D3QN algorithm Deep-SHAP

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Semiannual oscillation,annual oscillation,quasibiennial oscillation,and solar cycle variation of the OH airglow emission in the mesopause region

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Earth and Planetary Physics 2024年第3期8卷 479-496页

作者： Sheng-Yang Gu Dong Wang YuSong Qin Liang Tang YaFei Wei XianKang dou Electronic Information School Wuhan UniversityWuhan 430072China School of Optoelectronic Engineering Chongqing University of Posts and TelecommunicationsChongqing 400065China

The vertically integrated emission rate,centroid altitude,peak emission rate,and peak height of the hydroxyl(OH)airglow were calculated from Thermosphere Ionosphere Mesosphere Energetics and Dynamics(TIMED)/Sounding of the Atmosphere using Broadband Emission Radiometry(SABER)observations to study the seasonal and interannual variations in the intensity and location of the OH *** emission rate is inversely proportional to the height of the emission,with the semiannual oscillation dominating at low latitudes and the annual oscillation dominating at higher *** OH emission is modulated by the quasibiennial oscillation at the equator,and the quasibiennial oscillation signal is weak at other *** represented the vertical transport of atomic oxygen by using atomic oxygen concentrations obtained from a global atmospheric model,the Specified Dynamics Whole Atmosphere Community Climate Model with thermosphere and ionosphere eXtension *** with the amplitudes of the migrating diurnal tide(DW1)calculated from temperature data observed by TIMED/SABER,we found that both the vertical transport of atomic oxygen and DW1 amplitudes in the equatorial region exhibit semiannual oscillation and quasibiennial oscillation,which have a strong correlation with the variations in the amplitude and phase of semiannual oscillation and quasibiennial oscillation in OH *** is likely that the DW1 affects the vertical transport of atomic oxygen that is involved in the reaction to produce O3,thus affecting the OH *** analyzed the relationship between OH emission and solar activity by using the solar radio flux at 10.7 cm as a proxy for solar *** results showed that the OH emission is well correlated with solar activity,and the modulation of OH emission by solar activity has a significant latitudinal *** small correlation between emission height and solar activity indicates that solar activity modulates OH emission mainly thr

关键词： OH airglow semiannual oscillation quasibiennial oscillation solar activity diurnal tide

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Blade-Coated Porous 3D Carbon Composite Electrodes Coupled with Multiscale Interfaces for Highly Sensitive All-Paper Pressure Sensors

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Nano-Micro Letters 2024年第12期16卷 217-232页

作者： Bowen Zheng Ruisheng Guo Xiaoqiang dou Yueqing Fu Bingjun Yang Xuqing Liu Feng Zhou State Key Laboratory of Solidification Processing Center of Advanced Lubrication and Seal MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China Research Center of Resource Chemistry and Energy Materials State Key Laboratory of Solid LubricationLanzhou Institute of Chemical PhysicsChinese of Academy of SciencesLanzhou 730000People’s Republic of China State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000People’s Republic of China Shandong Laboratory of Advanced Materials and Green Manufacturing at Yantai Yantai 264006People’s Republic of China

Flexible and wearable pressure sensors hold immense promise for health monitoring,covering disease detection and postoperative *** pressure sensors with high sensitivity,wide detection range,and cost-effectiveness is *** leveraging paper for its sustainability,biocompatibility,and inherent porous structure,herein,a solution-processed all-paper resistive pressure sensor is designed with outstanding performance.A ternary composite paste,comprising a compressible 3D carbon skeleton,conductive polymer poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate),and cohesive carbon nanotubes,is blade-coated on paper and naturally dried to form the porous composite electrode with hierachical micro-and nano-structured *** with screen-printed Cu electrodes in submillimeter finger widths on rough paper,this creates a multiscale hierarchical contact interface between electrodes,significantly enhancing sensitivity(1014 kPa-1)and expanding the detection range(up to 300 kPa)of as-resulted all-paper pressure sensor with low detection limit and power *** versatility ranges from subtle wrist pulses,robust finger taps,to large-area spatial force detection,highlighting its intricate submillimetermicrometer-nanometer hierarchical interface and nanometer porosity in the composite ***,this all-paper resistive pressure sensor,with its superior sensing capabilities,large-scale fabrication potential,and cost-effectiveness,paves the way for next-generation wearable electronics,ushering in an era of advanced,sustainable technological solutions.

关键词： Micro-and nano-structures PEDOT:PSS Flexible pressure sensors Health monitoring Multiscale interfaces

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Effects of biodegradation on diamondoid distribution in crude oils from the Bongor Basin,Chad

Energy Geoscience

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Energy Geoscience 2024年第2期5卷 120-128页

作者： Huanxin Song Menghan Chen Lirong dou Dingsheng Cheng Zhigang Wen Cooperative Innovation Center of Unconventional Oil and Gas Yangtze UniversityWuhanHubei430100China College of Resources and Environment Yangtze UniversityWuhanHubei430100China PetroChina Research Institute of Petroleum Exploration&Development Beijing100083China

The sensitivity of biodegradation on diamondoids was investigated using a series of biodegraded oil samples from the Ronier tectonic unit of Bongor Basin,*** results suggest that diamondoids,including adamantanes(As)and diamantanes(Ds),are relatively resistant to biodegradation and obvious biodegradation was observed in oils with a Peters-Moldowan(PM)biodegradation rank of 6 or ***,the sensibility of biodegradation on diamondoids is generally similar to hopanes and regular *** biodegradation evolves,the changes in concentration and components of diamondoids show that the biodegradation process is selective and *** significant increase of MD/MA and DMD/DMA for oils with a PM ranking 6^(+) indicates that diamantanes are generally more resistant to biodegradation than *** similar trends of DMA/MA,EA/MA,MD/D,DMD/MD and other relevant indexes,show that higher alkylation homologs are more resistant to *** commonly used diamondoid ratios,such as MAI,EAI,MDI and DMID-1,are obviously affected by biodegradation at the stage of high-level biodegradation,which may indicate that these ratios should be used with caution in case of severely degraded oils.

关键词： Diamondoids Biodegradation Sensitivity Crude oil Bongor Basin Chad

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Thienothiophene-centered ladder-type π-systems that feature distinct quinoidal π-extension

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Chinese Chemical Letters 2024年第5期35卷 249-253页

作者： Jiaxiang Guo Zeyi Li Tianyu Zhang Xinyu Tian Yue Wang Chuandong dou State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China Jiangsu Engineering Laboratory of Novel Functional Polymeric Materials Soochow UniversitySuzhou 215123China

Quinoidalπ-conjugated structures,a kind of fundamental subunits for organicπ-systems,may produce some intriguing optical,electronic and magnetic properties of polycyclic hydrocarbons(PHs).Herein,we report two thienothiophene-centered ladder-type polycyclic molecules(1 and 2),which possess one quinoidal thienothiophene moiety and two para-quinodimethane(p-QDM)subunits,*** theoretically and experimentally studied,while 1 is a fully closed-shell molecule,2 owns an open-shell structure along with partial contribution of tetraradical state that is induced by the resonance of ***,although 2 has a largerπ-conjugated skeleton and open-shell electronic state,it exhibits larger bandgap and blue-shifted *** the other hand,the reversible oxidation activity of 1 enables the preparation of its dication 1^(2+),and the studies on its single-crystal and aromatic structures demonstrate that its two positive charges are delocalized onto the oxygen atoms,thus achieving fullyπ-extended structure and near-infrared *** study not only gains insight into quinoidalπ-subunits,but also provides an important basis for the development of antiaromatic and open-shellπ-electron materials.

关键词： Thienothiophene Quinoidal conjugation Open-shell structure Aromaticity Photophysical properties

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A systematic understanding of microbial reductive dechlorination towards an improved “one health” soil bioremediation: A review and perspective

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Science China Technological Sciences 2024年第10期67卷 3009-3031页

作者： HE Yan LI ShuYao YUAN Jing CHENG Jie dou JiBo YANG XueLing XU JianMing Zhejiang Provincial Key Laboratory of Agricultural Resources and Environment Institute of Soil and Water Resources and Environmental ScienceCollege of Environmental and Resource SciencesZhejiang University Key Laboratory of Environment Remediation and Ecological Health Ministry of Education Microbiome Network and Department of Agricultural Biology Colorado State University Departments of Chemistry and Chemical & Biomolecular Engineering Institute for Functional Intelligent Materials (I-FIM)National University of Singapore

Chlorinated organic pollutants(COPs), both emerging and traditional, are typical persistent pollutants that harm soil health worldwide. Dechlorinators mediated reductive dechlorination is the optimal way to completely remove COPs from anaerobic soil through a redox reaction driven by electron transfer during microbial anaerobic respiration. Generally, the dechlorinated depletion of COPs in situ often interacts with multiple element biogeochemical activities, e.g., methanogenesis, sulfate reduction, iron reduction, and denitrification. Elucidating the relevance of biogeochemical cycles between COPs and multiple elements and the coupled mechanisms involved, thus, helps to develop effective pollution control strategies with the balance between pollution degradation and element cycles in heterogeneous soil, ultimately contributing to “one health” goal. In this review, we summarized the microbial-chemical coupling redox processes and the driving factors, elucidated the interspecies metabolites exchange and electron transfer mechanisms within COP-dechlorinating communities, and further proposed a detailed design, construction, and analysis framework of engineering COP-dechlorinating microbiomes via “top-down” selfassembly and “bottom-up” synthesis to pave the way from laboratory to practical field application. Especially, we delve into the major challenges and perspectives surrounding the design of state-of-the-art synthetic microbial communities. Our goal is to improve the understanding of the microbial-mediated coupling between reductive dechlorination and element biogeochemical cycling, with a particular focus on the implications for health-integrated soil bioremediation under the “one health” concept.

关键词： reductive dechlorination biogeochemical redox processes interspecies interaction synthetic microbiomes, anaerobic soils

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Comprehensive analysis and mitigation strategies for safety issues of sodium-ion batteries

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Rare Metals 2024年第4期43卷 1343-1349页

作者： Tao Wei Xiao-Ling Xian Shi-Xue dou Wei Chen Shu-Lei Chou Institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou325035China Wenzhou Key Laboratory of Sodium-Ion Batteries Wenzhou University Technology Innovation Institute for Carbon NeutralizationWenzhou325035China Zhejiang Key Laboratory of Carbon Materials College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou325035China Institute for Superconducting and Electronic Materials Australian Institute for Innovative MaterialsUniversity of WollongongInnovation CampusWollongongNSW2522Australia

Sodium-ion batteries show great potential as an alternative energy storage system,but safety concerns remain a major hurdle to their mass *** paper analyzes the key factors and mechanisms leading to safety issues,including thermal runaway,sodium dendrite,internal short circuits,and gas *** promising solutions are proposed,such as high-safety electrode materials in the cathode and anode,high-safety electrolytes,and external battery management *** in also we emphasize the importance of selecting appropriate analysis methods and developing reliable failure models while suggesting advanced machine learning tools for *** a comprehensive approach,this study offers valuable recommendations to optimize materials and solutions for improving the safety of sodium-ion batteries.

关键词： Sodium-ion batteries Safety issues Thermal runaway Sodium dendrites

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Unraveling the mechanism of potassium metal capacitor for highly efficient charge storage

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Science China Chemistry 2024年第5期67卷 1578-1588页

作者： Qianqian Yao Pei Tang Kunyao Peng Zhenyuan Miao Yuecong Chen Qingyun dou Xingbin Yan Department of Materials Science and Engineering Sun Yat-sen UniversityGuangzhou 510275China South China Academy of Advanced Optoelectronics South China Normal UniversityGuangzhou 510006China

Although hybrid metal ion capacitors(MICs) are highly desired to achieve both high power density of supercapacitors and high energy density of rechargeable batteries, the mismatch problem of electrochemical kinetics of negative and positive electrodes in MICs hampers the realization of this goal. Here, a new hybrid capacitor concept-potassium metal capacitor(PMC) is proposed for the first time, where potassium metal and commercial activated carbon(AC) without any modification are applied as negative and positive electrodes, respectively, and the electrolyte is the same as that of non-aqueous potassium ion batteries. The simplest PMC prototype exhibits a good combination of high energy density(184.9 Wh kg^(-1)) and power density(12.4 kW kg^(-1)), which benefits from the synergistic effect of potassium metal and AC electrode. The former experiences fast potassium plating/striping during charging and discharging, and the later possesses complex multiple charge behaviors driven by low potential of potassium metal. Specifically, below open-circuit voltage, transportation of solvated cations in AC pores plays an important role;beyond this voltage, synergy actions of cations and anions, including adsorption/desorption of solvated cations and anions, and ions exchange between them, dominate the capacitance contribution. This work enriches the types of MICs, and deepens the understanding of the energy storage mechanism of non-aqueous hybrid metal capacitors.

关键词： hybrid capacitor potassium metal activated carbon charge storage mechanism

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