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Interfacial Electronic Modulation of Dual-Monodispersed Pt–Ni_(3)S_(2) as Efficacious Bi-Functional Electrocatalysts for Concurrent H_(2) Evolution and Methanol Selective Oxidation

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Nano-Micro Letters 2024年第4期16卷 415-431页

作者： Qianqian Zhao Bin Zhao Xin Long Renfei Feng Mohsen Shakouri Alisa Paterson Qunfeng Xiao Yu Zhang Xian‑Zhu Fu Jing‑Li Luo Shenzhen Key Laboratory of Energy Electrocatalytic Materials Shenzhen Key Laboratory of Polymer Science and TechnologyGuangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China canadian light source inc. SaskatoonSK S7N 0X4Canada Instrumental Analysis Center of Shenzhen University(Lihu Campus) Shenzhen UniversityShenzhen 518055People’s Republic of China

Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the development of electrochemicallydriven technologies for efficient hydrogen production and avoid CO_(2) emission. Herein, the hetero-nanocrystals between monodispersed Pt(~ 2 nm) and Ni_(3)S_(2)(~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H_(2) generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt–Ni_(3)S_(2) could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH_(3)OH to formate is accomplished at very low potentials(1.45 V) to attain 100 m A cm^(-2) with high electronic utilization rate(~ 98%) and without CO_(2) emission. Meanwhile, the Pt–Ni_(3)S_(2) can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction(HER) at the cathode. Further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction(MOR)//HER reactor by only requiring a cell voltage of 1.60 V to achieve a current density of 50 m A cm^(-2) with good reusability.

关键词： Dual-monodispersed heterostructure Electronic interactive modulation Reaction mechanism Methanol oxidation reaction Hydrogen generation

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Polysulfide regulation by defect-modulated Ta_(3)N_(5-x) electrocatalyst toward superior room-temperature sodium-sulfur batteries

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Science Bulletin 2024年第2期69卷 197-208页

作者： Zhen Zhang Dan Luo Jun Chen Chuyin Ma Matthew Li Haoze Zhang Renfei Feng Rui Gao Haozhen Dou Aiping Yu Xin Wang Zhongwei Chen Department of Chemical Engineering Waterloo Institute for NanotechnologyUniversity of WaterlooWaterloo N2L 3G1Canada Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China South China Academy of Advanced Optoelectronics&International Academy of Optoelectronics at Zhaoqing South China Normal UniversityGuangzhou 510006China Chemical Sciences and Engineering Division Argonne National LaboratoryLemont 60439USA canadian light source Saskatoon S7N 2V3Canada

Resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metalsulfur batteries.Motivated by a theoretical prediction,herein,we strategically propose nitrogenvacancy tantalum nitride(Ta3N5-x)impregnated inside the interconnected nanopores of nitrogendecorated carbon matrix as a new electrocatalyst for regulating sulfur redox reactions in roomtemperature sodium-sulfur batteries.Through a pore-constriction mechanism,the nitrogen vacancies are controllably constructed during the nucleation of Ta3N5-x.The defect manipulation on the local environment enables well-regulated Ta 5d-orbital energy level,not only modulating band structure toward enhanced intrinsic conductivity of Ta-based materials,but also promoting polysulfide stabilization and achieving bifunctional catalytic capability toward completely reversible polysulfide conversion.Moreover,the interconnected continuous Ta3N5-x-in-pore structure facilitates electron and sodium-ion transport and accommodates volume expansion of sulfur species while suppressing their shuttle behavior.Due to these attributes,the as-developed Ta3N5-x-based electrode achieves superior rate capability of 730 mAh g-1 at 3.35 A g-1,long-term cycling stability over 2000 cycles,and high areal capacity over 6 mAh cm-2 under high sulfur loading of 6.2 mg cm-2.This work not only presents a new sulfur electrocatalyst candidate for metal-sulfur batteries,but also sheds light on the controllable material design of defect structure in hopes of inspiring new ideas and directions for future research.

关键词： Tantalum nitride Nitrogen defects Sodium-sulfur batteries Electrocatalysts Polysulfide conversion

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Enriched electrophilic oxygen species facilitate acidic oxygen evolution on Ru-Mo binary oxide catalysts

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Nano Research 2024年第3期17卷 1165-1172页

作者： Yaya Wang Yunzhou Wen Yumeng Cheng Xinhong Chen Mengjiao Zhuansun Tongbao Wang Jun Li Debora Meira Huarui Sun Jun Wei Jia Zhou Yuhang Wang Sisi He Shenzhen Key Laboratory of Flexible Printed Electronics Technology Harbin Institute of Technology(Shenzhen)University TownShenzhen 518055China School of Science Harbin Institute of Technology(Shenzhen)University TownShenzhen 518055China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123China Frontiers Science Center for Transformative Molecules Shanghai Jiao Tong UniversityShanghai 200240China Science Division Canadian Light SourceSaskatoonSKS7N 2V3Canada Photon Science Division Argonne National LaboratoryLemontIL60439USA School of Materials Science and Engineering Harbin Institute of Technology(Shenzhen)University TownShenzhen 518055China

The polymer electrolyte membrane(PEM)electrolyzers are burdened with costly iridium(Ir)-based catalysts and high operation overpotentials for the oxygen evolution reaction(OER).The development of earth-abundant,highly active,and durable electrocatalysts to replace Ir is a critical step in reducing the cost of green hydrogen production.Here we develop a Ru5Mo4Ox binary oxide catalyst that exhibits high activity and stability in acidic OER.The electron-withdrawing property of Mo enriches the electrophilic surface oxygen species,which promotes acidic OER to proceed via the adsorbate evolution pathway.As a result,we achieve a 189 mV overpotential at 10 mA·cm^(-2) and a Tafel slope of 48.8 mV·dec^(-1).Our catalyst demonstrates a substantial 18-fold inc.ease in intrinsic activity,as evaluated by turnover frequency,compared to commercially available RuO_(2) and IrO_(2) catalysts.Moreover,we report a stable OER operation at 10 mA·cm^(-2) for 100 h with a low degradation rate of 2.05 mV·h^(-1).

关键词： electrocatalysis oxygen evolution reaction(OER) ruthenium(Ru)-based oxide molybdenum electrophilic oxygen

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Few-Shot Graph Classification with Structural-Enhanced Contrastive Learning for Graph Data Copyright Protection

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Tsinghua Science and Technology 2024年第2期29卷 605-616页

作者： Kainan Zhang DongMyung Shin Daehee Seo Zhipeng Cai Department of Computer Science Georgia State UniversityAtlantaGA 30303USA LSWare inc. Seoul 08504Republic of Korea College of Intelligence Information Engineering Sangmyung UniversitySeoul 03016Republic of Korea

Open-source licenses can promote the development of machine learning by allowing others to access,modify,and redistribute the training dataset.However,not all open-source licenses may be appropriate for data sharing,as some may not provide adequate protections for sensitive or personal information such as social network data.Additionally,some data may be subject to legal or regulatory restrictions that limit its sharing,regardless of the licensing model used.Hence,obtaining large amounts of labeled data can be difficult,time-consuming,or expensive in many real-world scenarios.Few-shot graph classification,as one application of meta-learning in supervised graph learning,aims to classify unseen graph types by only using a small amount of labeled data.However,the current graph neural network methods lack full usage of graph structures on molecular graphs and social network datasets.Sinc. structural features are known to correlate with molecular properties in chemistry,structure information tends to be ignored with sufficient property information provided.Nevertheless,the common binary classification task of chemical compounds is unsuitable in the few-shot setting requiring novel labels.Hence,this paper focuses on the graph classification tasks of a social network,whose complex topology has an uncertain relationship with its nodes'attributes.With two multi-class graph datasets with large node-attribute dimensions constructed to facilitate the research,we propose a novel learning framework that integrates both meta-learning and contrastive learning to enhance the utilization of graph topological information.Extensive experiments demonstrate the competitive performance of our framework respective to other state-of-the-art methods.

关键词： few-shot learning contrastive learning data copyright protection

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Einstein’s Concept of Clock Synchronization Conflicts with the Second Relativity Postulate

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Journal of Modern Physics 2024年第7期15卷 985-1000页

作者： Steven D. Deines Donatech Corporation Inc. Fairfield Iowa USA

Einstein defined clock synchronization whenever photon pulses with timetags traverse a fixed distance between two clocks with equal time spans ineither direction. Using the second relativity postulate, he found clocksmounted on a rod uniformly moving parallel with the rod’s length cannot besynchronized, but clocks attached to a stationary rod can. He dismissed thisdiscrepancy by claiming simultaneity and clock synchronization were not commonbetween inertial frames, but this paper proves with both Galilean and Lorentztransformations that simultaneity and clock synchronization are preservedbetween inertial frames. His derivation means moving clocks can never besynchronized in a “resting” inertial frame. Ultraprecise atomic clocks intimekeeping labs daily contradict his results. No algebraic error occurred inEinstein’s derivations. The two cases of clocksattached to a rod reveal three major conflicts with the currentsecond postulate. The net velocity between a photon source and detector plusthe “universal” velocity c is mathematically equivalent toEinstein’s clock synchronization method. As the ultraprecise timekeepingcommunity daily synchronizes atomic clocks on the moving Earth withultraprecise time uncertainty well below Einstein’s lowest limit ofsynchronization, the theoretical resolution of the apparent conflict isaccomplished by expanding the second relativity postulate to inc.rporate thenet velocity between the photon source and detector with the emitted velocity c as components of the total velocity c. This means the magnitudeof the total photon velocity can exceed the speed limit (299792458 m/s) set by the standard velocity c. .

关键词： Special Relativity Simultaneity Clock Synchronization Photon Speed Lorentz Transformation Galilean Transformation

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Effective transport network driven by tortuosity gradient enables high-electrochem-active solid-state batteries

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National Science Review 2023年第3期10卷 178-188页

作者： Qing-Song Liu Han-Wen An Xu-Feng Wang Fan-Peng Kong Ye-Cai Sun Yu-Xin Gong Shuai-Feng Lou Yi-Fan Shi Nan Sun Biao Deng Jian Wang Jia-Jun Wang Ministry of Industry and Information Technology(MIIT) Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of Technology(HIT) Chongqing Research Institute of HIT Shanghai Institute of Applied Physics Chinese Academy of Sciences canadian light source inc. University of Saskatchewan

Simultaneously achieving high electro chemical activity and high loading for solid-state batteries has been hindered by slow ion transport within solid electrodes,in particular with an inc.ease in electrode thickness.Ion transport governed by ’point-to-point’ diffusion inside a solid-state electrode is challenging,but still remains elusive.Herein,synchronized electrochemical analysis using X-ray tomography and ptychography reve als new insights into the nature of slow ion transport in solid-state electrodes.’hickness-dependent delithiation kinetics are spatially probed to identify that low-delithiation kinetics originate from the high tortuous and slow longitudinal transport pathways.By fabricating a tortuosity-gradient electrode to create an effective ion-percolation network,the tortuosity-gradient electrode architecture promotes fast charge transport,migrates the heterogeneous solid-state reaction,enhances electrochemical activity and extends cycle life in thick solid-state ele ctrodes.These findings establish effective transport pathways as key design princ.ples for realizing the promise of solid-state high-loading cathodes.

关键词： all-solid-state batteries thick electrodes lithiation/delithiation heterogeneity tortuosity gradient synchrotron techniques

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From Digital Human Modeling to Human Digital Twin: Framework and Perspectives in Human Factors

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Chinese Journal of Mechanical Engineering 2024年第1期37卷 1-14页

作者： Qiqi He Li Li Dai Li Tao Peng Xiangying Zhang Yinc.eng Cai Xujun Zhang Renzhong Tang State Key Laboratory of Fluid Power Components and Mechatronic Systems Zhejiang UniversityHangzhou 310027China ZJU-Sunon Joint Research Center for Smart Furniture Zhejiang UniversityHangzhou 310027China PICO-Lab Bytedance Inc.Shanghai 200233China Sunon Technology Co. Ltd.Hangzhou 311215China

The human digital twin(HDT)emerges as a promising human-centric technology in Industry 5.0,but challenges remain in human modeling and simulation.Digital human modeling(DHM)provides solutions for modeling and simulating human physical and cognitive aspects to support ergonomic analysis.However,it has limitations in real-time data usage,personalized services,and timely interaction.The emerging HDT concept offers new possibilities by integrating multi-source data and artificial intelligence for continuous monitoring and assessment.Hence,this paper reviews the evolution from DHM to HDT and proposes a unified HDT framework from a human factors perspective.The framework comprises the physical twin,the virtual twin,and the linkage between these two.The virtual twin integrates human modeling and AI engines to enable model-data-hybrid-enabled simulation.HDT can potentially upgrade traditional ergonomic methods to intelligent services through real-time analysis,timely feedback,and bidirectional interactions.Finally,the future perspectives of HDT for industrial applications as well as technical and social challenges are discussed.In general,this study outlines a human factors perspective on HDT for the first time,which is useful for cross-disciplinary research and human factors innovation to enhance the development of HDT in industry.

关键词： Human digital twin Digital human modeling Human factors Human-centric technology

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Developing a Clang Libtooling-Based Refactoring Tool for CUDA GPU Programming

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Journal of Software Engineering and Applications 2024年第2期17卷 89-108页

作者： Kian Nejadfard Janche Sang Champ Titles Inc. Cleveland USA Department of Computer Science Cleveland State University Cleveland USA

Refactoring tools, whether fully automated or semi-automated, are essential components of the software development life cycle. As software libraries and frameworks evolve over time, it’s crucial for programs utilizing them to also evolve to remain compatible with modern advancements. Take, for example, NVIDIA CUDA’s platform for general-purpose GPU programming. Embracing the more contemporary unified memory architecture offers several benefits, such as simplifying program source code, reducing bugs stemming from manual memory management between host and device memory, and optimizing memory transfer through automated memory handling. This paper describes our development of a refactoring tool based on Clang’s Libtooling to facilitate this transition automatically, thereby relieving developers from the burden and risks associated with manually refactoring large code bases.

关键词： Refactoring CUDA Unified Memory Clang Libtooling

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Origin of the Dashuigou independent tellurium deposit at Qinghai–Xizang Plateau: constraints from the light stable isotopes C, O, and H

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Acta Geochimica 2024年第2期43卷 385-398页

作者： Jianzhao Yin Yuhong Chao Haoyu Yin Hongyun Shi Shoupu Xiang Wuhan Institute of Technology Wuhan 430074China College of Earth Sciences Jilin UniversityChangchun 130061China Ganzhongnan Institute of Geology and Mineral Exploration Nanchang 330002China Guinea Westfi eld Mining Company-Sarlu Jinzhong 031300China Orient Resources Ltd. RichmondB.C.V7E 1M8Canada Silvercorp Metals inc. Beijing 100027China

By studying the light isotopic compositions of carbon,oxygen,and hydrogen,combined with previous research results on the ore-forming source of the deposit,the authors try to uncover its metallogenic origin.The δ^(18)O and δ^(13)C isotope signatures of dolomite samples vary between 10.2 and 13.0‰,and between−7.2 and−5.2‰,respectively,implying that the carbon derives from the upper mantle.δD and δ^(18) O of quartz,biotite,and muscovite from diff erent ore veins of the deposit vary between−82 and−59‰,and between 11.6 and 12.4‰,respectively,implying that the metallogenic solutions are mainly magmatic.According to the relevant research results of many isotope geologists,the fractionation degree of hydrogen isotopes inc.eases as the depth to the Earth’s core inc.eases,and the more diff erentiated the hydrogen isotopes are,the lower their values will be.In other words,mantle-derived solutions can have extremely low hydrogen isotope values.This means that the δD‰ value−134 of the pyrrhotite sample numbered SD-34 in this article may indicate mantle-derived oreforming fl uid of the deposit.The formation of the Dashuigou tellurium deposit occurred between 91.71 and 80.19 Ma.

关键词： Carbon oxygen and hydrogen isotopes Origin Independent tellurium deposit The Qinghai–Xizang Plateau

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Relating atomic local structures and Curie temperature of NdFeB permanent magnets:an X-ray absorption spectroscopic study

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Rare Metals 2018年第11期37卷 983-988页

作者： Mu-Nan Yang Hang Wang Yong-Feng Hu Liu-Yi-Mei Yang Aimee Maclennan Bin Yang Institute of Engineering Research Jiangxi University of Scienceand Technology canadian light source University of Saskatchewan

Relationship between atomic local structures and Curie temperature of NdFeB permanent magnets was investigated semi-quantitatively using synchrotron radiation technique. Fe K-edge X-ray absorption spectroscopy(XAS) was employed to study the local structure of Fe atoms for samples before and after doping Dy, Tb or Gd. It is found that the bond lengths and coordination numbers are changed. Thus, the exchange interaction between Fe atoms inc.eases with Dy, Tb or Gd doping, resulting in the improvement of Curie temperature of NdFeB permanent magnets. The doping effect is proven by experimental measurement of the magnetic properties. Microstructural characterization using scanning electron microscopy(SEM) was also used to further analyze the effect of different rare earth elements doping on Curie temperature of NdFeB permanent magnets.

关键词： Permanent magnet Synchrotron radiation X-ray absorption fine structure Crystal structure Curie temperature

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