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Engineering N3C vacancies in hierarchical porous carbon nitride nanosheets for room temperature ultradeep photocatalytic aerobic oxidative desulfurization

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Science China Chemistry 2025年

作者： Yina Nie Weijie Yang Xin Wang Xiang Li Lele Wei Xiaolin Bai Lin Liu Feng Fu Jun Wan College of Chemistry & chemical Engineering Research Institute of Comprehensive Energy Industrial Technology Shaanxi Key Laboratory of Chemical Reaction Engineering Yan'an University Anhui Engineering Research Center of Carbon Neutrality College of Chemistry and Materials Science Anhui Normal University

The production of ultra-low sulfur clean fuels holds global significance for improving energy efficiency and reducing environmental pollution. Photocatalytic aerobic oxidative desulfurization（PODS） offers an attractive approach to efficiently remove refractory heterocyclic aromatic sulfur compounds under mild conditions. However, the sluggish charge dynamics,insufficient molecule activation, and slow mass transfer within photocatalysts restrict the overall desulfurization efficiency,hindering the widespread application of this technology. Herein, we developed a defective g-C3N4（M1U3CN） photocatalyst with bridged N3Cvacancies and hierarchical porous structures to address these limitations. This catalyst not only demonstrates outstanding dibenzothiophene（DBT） removal efficiency of 99.6% for model oil with high conversion and selectivity but also achieves complete sulfur removal from gasoline as well as 96.7% sulfur removal for distilled diesel at room temperature,successfully achieving ultradeep aerobic oxidative desulfurization. The introduction of rich N3Cvacancies and abundant micromeso-macroporous distribution in M1U3CN enhances kinetic efficiencies by promoting charge carrier separation, mass transfer,and molecular activation simultaneously; resulting in exceptional PODS performance. This work provides a collaborative strategy to overcome kinetic challenges in aerobic oxidative desulfurization via defect and structural engineering of the catalyst.

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Electrode/Electrolyte Optimization‑Induced Double‑Layered Architecture for High‑Performance Aqueous Zinc‑(Dual)Halogen Batteries

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Nano-Micro Letters 2025年第3期17卷 121-137页

作者： Chengwang Zhou Zhezheng Ding Shengzhe Ying Hao Jiang Yan Wang Timing Fang You Zhang Bing Sun Xiao Tang Xiaomin Liu School of Textiles and Clothing School of Chemistry and Chemical EngineeringQingdao UniversityQingdao 266071ShandongPeople’s Republic of China Centre for Clean Energy technology School of Mathematical and Physical SciencesFaculty of ScienceUniversity of Technology SydneyUltimoNSW 2007Australia School of Chemistry and chemical Engineering Henan Normal UniversityXinxiang 453007HenanPeople’s Republic of China

Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources,intrinsic safety,and high theoretical ***,the uncontrollable zinc dendrite growth and spontaneous shuttle effect of active species have prohibited their practical ***,a double-layered protective film based on zinc-ethylenediamine tetramethylene phosphonic acid(ZEA)artificial film and ZnF2-rich solid electrolyte interphase(SEI)layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic *** ZEA-based artificial film shows strong affinity for the ZnF2-rich SEI layer,therefore effectively suppressing the SEI breakage and facilitating the construction of double-layered protective film on the zinc metal *** double-layered architecture not only modulates Zn2+flux and suppresses the zinc dendrite growth,but also blocks the direct contact between the metal anode and electrolyte,thus mitigating the corrosion from the active *** employing optimized metal anodes and electrolytes,the as-developed zinc-(dual)halogen batteries present high areal capacity and satisfactory cycling *** work provides a new avenue for developing aqueous zinc-(dual)halogen batteries.

关键词： Zn metal anodes Double-layered protective film Electrode/electrolyte optimization Aqueous zinc-(dual)halogen batteries

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Dual modulation of homogeneous nanomaterialization and electrochemical activation enhancing zinc ion storage

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Science China Chemistry 2025年第1期68卷 385-393页

作者： Jianwei Wang Huan Wang Kangning Wang Wenhui Wang Wenlin Zhang Yanzhong Zhen School of Chemistry & chemical Engineering Yan'an University

Vanadium-based electrode materials are widely investigated,but the low specific capacity and slow electrochemical kinetics in aqueous zinc-ion batteries still limit their commercial ***,the VS2/Ca V4O9material with the morphology of nanoflower was synthesized by a one-step hydrothermal *** to the blocky structure of pure VS2material,the VS2/Ca V4O9material is composed of thinner homogeneous *** open structures could provide abundant electrochemical active sites and ion transport channels,and then promote the electrochemical reaction *** addition,they can also buffer the bulk strain during the reaction *** improve the utilization of vanadium elements,an in-situ electrochemical activation strategy is used to explore the storage performance of the VS2/Ca V4O9material,the different activation voltage range of 0.4–1.6 and 0.4–1.4 V are selected,*** with the longer activation plateau of activated-VS2,the VS2/Ca V4O9cathode could quickly reach the activation state in the range of 1.4–1.6 V and cause the release of additional Zn storage sites *** VS2/Ca V4O9cathode delivers a higher power density of 37,000 W kg-1and a significant energy density of 423 Wh *** the high current density of 15 A g-1,the VS2/Ca V4O9cathode still has a discharge capacity of 183.9m Ah g-1after 5,000 cycles,and the capacity decay rate per cycle is only 0.0042%.Continuous cyclic voltammetry （CV） curves,electrochemical impedance spectroscopy （EIS） measurements,density functional theory （DFT） calculation and galvanostatic intermittent titration technique （GITT） measurements demonstrate that the VS2/Ca V4O9cathode has a faster ion diffusion/charge transfer ***,the assembled flexible device has an excellent mechanical stability.

关键词： dual modulation homogeneous nanomaterialization electrochemical activation zinc ion storage

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An SPH Framework for Earthquake-Induced Liquefaction Hazard Assessment of Geotechnical Structures

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Computer Modeling in Engineering & Sciences 2025年第1期142卷 251-277页

作者： Sourabh Mhaski G.V.Ramana Department of Civil Engineering Indian Institute of Technology DelhiNew Delhi110016India

Earthquake-induced soil liquefaction poses significant risks to the stability of geotechnical structures *** understanding of the liquefaction triggering,and the post-failure large deformation behaviour is essential for designing resilient *** present study develops a Smoothed Particle Hydrodynamics(SPH)framework for earthquake-induced liquefaction hazard assessment of geotechnical *** coupled flowdeformation behaviour of soils subjected to cyclic loading is described using the PM4Sand model implemented in a three-phase,single-layer SPH framework.A staggered discretisation scheme based on the stress particle SPH approach is adopted to minimise numerical inaccuracies caused by zero-energy modes and tensile ***,non-reflecting boundary conditions for seismic analysis of semi-infinite soil domains using the SPH method are *** numerical framework is employed for the analysis of cyclic direct simple shear test,seismic analysis of a level ground site,and liquefaction-induced failure of the Lower San Fernando *** agreement for liquefaction triggering and post-failure behaviour demonstrates that the SPH framework can be utilised to assess the effect of seismic loading on field-scale geotechnical *** present study also serves as the basis for future advancements of the SPH method for applications related to earthquake geotechnical engineering.

关键词： Earthquake seismic liquefaction stress particle PM4Sand smoothed particle hydrodynamics(SPH)

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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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Observability for the Schr?dinger equation in a uniform magnetic field

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Acta Mathematica Sinica,English Series 2025年

作者： Zhang FANG Department of Mathematics Beijing Institute of Technology

We prove the observability inequalities at two time points for the Schr?dinger equation in a uniform magnetic field in dimensions 2 and 3. The proofs mainly rely on Nazarov’s uncertainty principle. In particular, the observability inequality in three dimensions can also be derived from the approach used to establish the Amerin-Berthier uncertainty principle.

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Unveiling the promotion role of ZnO on Zn-Al spinel oxide for CO2 hydrogenation

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Journal of Energy Chemistry 2025年第1期100卷 18-25页

作者： Tongyao Wang Xinlong Yao Lixin Liang Hongyu Chen Pan Gao Guangjin Hou State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO2hydrogenation. However, the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction intermediates. In this study, we prepared two Zn-Al spinel oxide catalysts via coprecipitation（ZnAl-C）and hydrothermal（ZnAl-H） methods, and conducted a comparative investigation in the CO2hydrogenation reaction. Surprisingly, under similar conditions, ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to ZnAl-H. Comprehensive characterizations using X-ray diffraction（XRD）, Raman spectroscopy and electron paramagnetic resonance（EPR） unveiled that ZnAl-C catalyst had abundant ZnO species on its surface, and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies, which are crucial for CO2adsorption and activation. Additionally, state-of-the-art solid-state nuclear magnetic resonance（NMR） techniques,including ex-situ and in-situ NMR analyses, confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species, which was readily hydrogenated to methanol and DME. These insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO2-to-methanol hydrogenation reaction, which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H catalyst. These molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.

关键词： Reaction intermediates

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Comparative Evaluation and Performance Analysis of Heat Exchangers Featured with Peened Surface

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Journal of Thermal Science 2025年第1期34卷 50-61页

作者： DINESHBABU Chinnadurai SHIVA SANKARAN Nallasamy VENKATESH RAJA Krishnan VENKATESH Rathinavelu Department of Mechanical Engineering Kongunadu College of Engineering and Technology Department of Mechanical Engineering Selvam College of Technology Department of Mechanical Engineering Sona College of Technology Department of Mechanical Engineering Saveetha School of EngineeringSaveetha Institute of Medical and Technical Sciences (SIMATS)Saveetha University

Heat exchangers have the potential for various engineering applications,and their performance is enriched by surface *** proposed system enriches the heat exchanger's performance by adapting a peened stainless steel（SS） surface blasted with copper,grinding,sand,and *** influences peened SS surface modified with a copper blast,grinding,sandblast,and iron blast on the surface morphology of shell and tube heat exchanger surface（STHE） is analyzed via tungsten heated cathode electron gun featured scanning electron microscope and observed coarse grain *** SS surface featured STHE performance is experimentally evaluated by different flow rates（30,60,90,and 120 L/min） underwater fluid medium functioned by the temperature ranges of 25-75℃ and its results are compared with computational fluid dynamic（CFD）/heat transfer research（HTRI） analyzed *** 60 L/min flow rate was spotted as an optimum value for both shell and tube side *** STHE is operated with a 60 L/min flow rate under the different peened surfaces and evaluated its Stanton number,Nusselt number,logarithmic mean temperature difference（LMTD）,overall heat transfer coefficient,number of transfer units（NTU）,effectiveness,and exergy *** iron blasted SS peened surface was observed to have better SHTE performance like Stanton number（0.0012）,Nusselt number（2180）,reduced LMTD of 31℃,improved overall heat transfer co-efficient of 2400 W/（m2·K）,better NTU of 0.5532,good effectiveness value of 0.451 62,and hiked exergy efficiency of 10% respectively.

关键词： penned surface performance analysis shell and tube heat exchanger stainless steel

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Multifunctional Nacre‑Like Nanocomposite Papers for Electromagnetic Interference Shielding via Heterocyclic Aramid/MXene Template‑Assisted In‑Situ Polypyrrole Assembly

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Nano-Micro Letters 2025年第3期17卷 37-54页

作者： Jinhua Xiong Xu Zhao Zonglin Liu He Chen Qian Yan Huanxin Lian Yunxiang Chen Qingyu Peng Xiaodong He National Key Laboratory of Science and technology On Advanced Composites in Special Environments Center for Composite Materials and StructuresHarbin Institute of TechnologyHarbin 150080People’s Republic of China

Robust, ultra-flexible, and multifunctional MXene-basedelectromagnetic interference (EMI) shielding nanocomposite filmsexhibit enormous potential for applications in artificial intelligence,wireless telecommunication, and portable/wearable electronic *** this work, a nacre-inspired multifunctional heterocyclic aramid(HA)/MXene@polypyrrole (PPy) (HMP) nanocomposite paper withlarge-scale, high strength, super toughness, and excellent tolerance tocomplex conditions is fabricated through the strategy of HA/MXenehydrogel template-assisted in-situ assembly of PPy. Benefiting from the"brick-and-mortar" layered structure and the strong hydrogen-bondinginteractions among MXene, HA, and PPy, the paper exhibits remarkable mechanical performances, including high tensile strength (309.7 MPa),outstanding toughness (57.6 MJ m−3), exceptional foldability, and structural stability against ultrasonication. By using the template effect ofHA/MXene to guide the assembly of conductive polymers, the synthesized paper obtains excellent electronic conductivity. More importantly,the highly continuous conductive path enables the nanocomposite paper to achieve a splendid EMI shielding effectiveness (EMI SE) of 54.1 dBat an ultra-thin thickness (25.4 μm) and a high specific EMI SE of 17,204.7 dB cm2g−1. In addition, the papers also have excellent applicationsin electromagnetic protection, electro-/photothermal de-icing, thermal therapy, and fire safety. These findings broaden the ideas for developinghigh-performance and multifunctional MXene-based films with enormous application potential in EMI shielding and thermal management.

关键词： MXene Remarkable mechanical properties Heterocyclic aramid Electromagnetic interference shielding Polypyrrole Multifunctionality

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Domain generalization with semi-supervised learning for people-centric activity recognition

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Science China(Information Sciences) 2025年第1期68卷 171-188页

作者： Jing LIU Wei ZHU Di LI Xing HU Liang SONG Academy for Engineering & technology Fudan University Shanghai East-bund Research institute on Networking Systems of AI School of Optoelectronic Information and Computer Engineering University of Shanghai for Science & Technology

People-centric activity recognition is one of the most critical technologies in a wide range of real-world applications,including intelligent transportation systems, healthcare services, and brain-computer interfaces. Large-scale data collection and annotation make the application of machine learning algorithms prohibitively expensive when adapting to new tasks. One way of circumventing this limitation is to train the model in a semi-supervised learning manner that utilizes a percentage of unlabeled data to reduce the labeling burden in prediction tasks. Despite their appeal, these models often assume that labeled and unlabeled data come from similar distributions, which leads to the domain shift problem caused by the presence of distribution gaps. To address these limitations, we propose herein a novel method for people-centric activity recognition,called domain generalization with semi-supervised learning(DGSSL), that effectively enhances the representation learning and domain alignment capabilities of a model. We first design a new autoregressive discriminator for adversarial training between unlabeled and labeled source domains, extracting domain-specific features to reduce the distribution gaps. Second, we introduce two reconstruction tasks to capture the task-specific features to avoid losing information related to representation learning while maintaining task-specific consistency. Finally, benefiting from the collaborative optimization of these two tasks, the model can accurately predict both the domain and category labels of the source domains for the classification task. We conduct extensive experiments on three real-world sensing datasets. The experimental results show that DGSSL surpasses the three state-of-the-art methods with better performance and generalization.

关键词： activity recognition deep learning domain generalization semi-supervised learning adversarial training

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