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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

Thickness and sp3 bond modulation of（Ti/tetrahedral amorphous carbon）_n multilayer coatings

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Tungsten 2025年第1期7卷 152-160页

作者： Zhi-Jun Xie Jia-Lin Li Ling Gong Xiang-Li Zhong Hong-Jia Song Jin-Bin Wang National-Provincial laboratory of Special Function Thin Film materials School of Materials Science and Engineering Xiangtan University

The durability of wear-resistant tetrahedral amorphous carbon（ta-C） coatings is intimately linked to their thickness and the concentration of *** enhance the lifespan of the coatings,we have prepared a multilayer coating consisting of alternating layers of Ti and ta-C,denoted as（Ti/ta-C）_n,using arc ion plating.A multi-layer structure in conjunction with stage cooling is employed to enhance the thickness and promote *** results indicate that the ID/IGvalue,representing the ratio of the intensity of the D peak to that of the G peak in Raman spectroscopy,decreases from 0.85 when no stage cooling is applied to 0.35 when stage cooling is employed,suggesting an enhancement in the fraction of sp3bonds within the *** obtained（Ti/ta-C）_n multilayer coating without peeling off has a maximum thickness of 1.14 μm,which is almost double that of the ta-C coating single layer *** the same time,the coating has a low coefficient of friction,down to 0.069,and maintains excellent friction properties with a wear rate of 3.4×10-6mm3·N-1·*** results conclusively show that the preparation technology can enhance both thickness and sp3bonding in ta-C coatings,significantly expanding their utility across tools,molds,and precision engineering components.

关键词： Arc ion plating Multilayer structure sp3 bond Ta-C coating Wear resistance

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

Highly mass activity electrocatalysts with ultralow Pt loading on carbon black for hydrogen evolution reaction

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International Journal of Minerals,Metallurgy and materials 2025年第1期32卷 182-190页

作者： Shaorou Ke Yajing Zhao Xin Min Yanghong Li Ruiyu Mi Yangai Liu Xiaowen Wu Minghao Fang Zhaohui Huang Engineering research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid WastersNational Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of Geosciences(Beijing)Beijing 100083China

Pt-based nanocatalysts offer excellent prospects for various ***,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable *** this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ ***~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt *** unique structure is beneficial for the hydrogen evolution *** catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C *** activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.

关键词： hydrogen evolution reaction ultralow platinum in-situ synthesis ultrasound

“Zero‑Strain” NiNb_(2)O_(6) Fibers for All‑Climate Lithium Storage

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Nano-Micro Letters 2025年第1期17卷 348-360页

作者： Yan Zhao Qiang Yuan Liting Yang Guisheng Liang Yifeng Cheng Limin Wu Chunfu Lin Renchao Che College of Physics Donghua UniversityShanghai 201620People’s Republic of China School of materials Science and Engineering Institute of Materials for Energy and EnvironmentQingdao UniversityQingdao 266071People’s Republic of China laboratory of advanced materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsAcademy for Engineering&TechnologyFudan UniversityShanghai 200438People’s Republic of China Zhejiang laboratory Hangzhou 311100People’s Republic of China Inner Mongolia University Hohhot 010021People’s Republic of China

Niobates are promising all-climate Li^(+)-storage anode material due to their fast charge transport,large specific capacities,and resistance to electrolyte ***,their moderate unit-cellvolume expansion(generally 5%–10%)during Li^(+)storage causes unsatisfactory long-term ***,“zero-strain”NiNb_(2)O_(6) fibers are explored as a new anode material with comprehensively good electrochemical *** Li^(+)storage,the expansion of electrochemical inactive NiO_(6) octahedra almost fully offsets the shrinkage of active NbO_(6) octahedra through reversible O *** superior volume-accommodation capability of the NiO_(6) layers guarantees the“zero-strain”behavior of NiNb_(2)O_(6) in a broad temperature range(0.53%//0.51%//0.74%at 25//−10//60℃),leading to the excellent cyclability of the NiNb_(2)O_(6) fibers(92.8%//99.2%//91.1%capacity retention after 1000//2000//1000 cycles at 10C and 25//−10//60℃).This NiNb_(2)O_(6) material further exhibits a large reversible capacity(300//184//318 mAh g−1 at 0.1C and 25//−10//60℃)and outstanding rate performance(10 to 0.5C capacity percentage of 64.3%//50.0%//65.4%at 25//−10//60℃).Therefore,the NiNb_(2)O_(6) fibers are especially suitable for large-capacity,fast-charging,long-life,and all-climate lithium-ion batteries.

关键词： NiNb_(2)O_(6)porous fiber “Zero-strain”mechanism Electrochemical property Harsh-temperature operation Operando characterization

Reverse modulation of defect density of Ce-MOF-808 by solventassisted ligand exchange for dicyclopentadiene hydrogenation

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Science China Chemistry 2025年

作者： Danfeng Zhao Fajie Hu Rushuo Li Xinmeng Xu Zhaokun Wang Zuoshuai Xi Jun Tong Xiubing Huang Ge Wang advanced Innovation Center for materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule & Structure Construction School of Materials Science and Engineering University of Science and Technology Beijing

Defect engineering is a pivotal strategy for tailoring the electronic structure and physicochemical properties of catalysts, yet the straightforward manipulation of defect density in porous materials presents a current challenge. In this work, we achieved precise control over the coordination unsaturated site（CUS） content and pore architecture of Ce-MOF-808 by employing 2-fluorobenzoic acid（2-FBA） as a modifier. Leveraging the p Kadisparities among three ligands（1,3,5-tricarboxylic benzoic acid,formic acid, and 2-FBA）, we preserved the spn topology of Ce-MOF within an aqueous system, while realizing partial substitution of the auxiliary ligands and saturation of the CUS. The amount of 2-FBA was negatively correlated with the number of ligand defects, and the consequent decrease in Ce3+content and the increase in the number of ligand linkages also induced crystal structure transformation. The modulation of the defect structure was correlated with the catalytic performance of dicyclopentadiene（DCPD） hydrogenation reaction, in which Ce-MMF0.15, constructed by the modulation of 0.15 mol amount of 2-fluorobenzoic acid, exhibited an optimal ligand defect density and micro-mesoporous structure, enabling almost complete conversion of DCPD at 100 ℃ and 2 MPa. This article also elucidates the correlation between the regulation of defect density and the accessibility of frustrated Lewis pair（FLP） active sites, guiding the application of novel porous intrinsic FLP materials in hydrogenation catalysis.

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Homologous CoS2 interface with directed electron transfer and strong chloridion repulsion for efficient seawater oxidation

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Science China Chemistry 2025年

作者： Yuan Tian Jiang-Bo Chen Jie Ying Ge Tian Yu-Xuan Xiao Yi Lu Si-Ming Wu Wei Geng Ling Shen Xiao-Yu Yang State Key laboratory of advanced Technology for materials Synthesis and Processing and School of Materials Science and Engineering and Shenzhen Research Institute & Laoshan Laboratory Wuhan University of Technology School of Chemical Engineering and Technology Sun Yat-Sen University National Energy Key laboratory for New Hydrogen-Ammonia Energy Technologies Foshan Xianhu laboratory

Seawater electrolysis is a highly promising method to produce high energy density hydrogen,especially in dry areas that have scarce freshwater ***,application of seawater electrolysis is confronted by two major problems associated with catalysts employed for the anodic oxygen evolution reaction （OER） including the competitive hypochlorite evolution reaction（HCER） and strong chloridion （Cl–） triggered *** studies aimed at overcoming these problems,a facile method has been developed to synthesize a homologous CoS2heterojunction as an OER *** to a difference in work functions at the interface and increased electron density,this material has directed electron transfer and strong chloridion repulsion properties,*** have shown that CoS2achieves low overpotentials of 289 and 322 mV at 10 mA cm-2current density in respective alkaline （1 M KOH） and alkaline simulated seawater ***,the outstanding stability of CoS2is reflected in a negligible decline in activity during promotion of the OER for 100 *** of density functional theory calculations reveal that the homologous CoS2heterojunction promotes directed electron transport for optimizing adsorption/desorption of reactive species and heightens the Cl-adsorption energy for strongly repulsing Cl-,phenomena that enhance OER performance in alkaline simulated seawater.

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Recent Strategies and Advances in Hydrogel‑Based Delivery Platforms for Bone Regeneration

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Nano-Micro Letters 2025年第3期17卷 389-439页

作者： Xiao Wang Jia Zeng Donglin Gan Kun Ling Mingfang He Jianshu Li Yongping Lu Scientific and Technological Innovation Center for Biomedical materials and Clinical research Guangyuan Key Laboratory of Multifunctional Medical HydrogelGuangyuan Central HospitalGuangyuan 628000People’s Republic of China Jiangsu Collaborative Innovation Center of Biomedical Functional materials Jiangsu Key Laboratory of Bio‑Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023People’s Republic of China College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065People’s Republic of China

Bioactive molecules have shown great promise for effectively regulating various bone formation processes,rendering them attractive therapeutics for bone ***,the widespread application of bioactive molecules is limited by their low accumulation and short half-lives in *** have emerged as ideal carriers to address these challenges,offering the potential to prolong retention times at lesion sites,extend half-lives in vivo and mitigate side effects,avoid burst release,and promote adsorption under physiological *** review systematically summarizes the recent advances in the development of bioactive molecule-loaded hydrogels for bone regeneration,encompassing applications in cranial defect repair,femoral defect repair,periodontal bone regeneration,and bone regeneration with underlying ***,this review discusses the current strategies aimed at improving the release profiles of bioactive molecules through stimuli-responsive delivery,carrier-assisted delivery,and sequential ***,this review elucidates the existing challenges and future directions of hydrogel encapsulated bioactive molecules in the field of bone regeneration.

关键词： Hydrogel Bone regeneration Bioactive molecules Drug delivery Nano-/microscale carriers

Mechanical properties and microstructures of Mg-6Si alloys fabricated using the tungsten-inert-gas arc additive manufacturing

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China Foundry 2025年

作者： Peng-cheng Zhou Guo-qiang You Jin-yu Feng Lei Wang Xiao Lin Bin Jiang College of materials Science and Engineering Chongqing University National Engineering research Center for Magnesium Alloys Chongqing University National Key laboratory of advanced Casting Technologies Chongqing University

Si-containing Mg alloys solidified at conventional rates often contain coarse and sharp Mg2Si phases,which can result in inferior material *** this study,Mg-6wt.%Si （Mg-6Si） alloy was prepared by wire arc additive manufacturing （WAAM）,employing the gas tungsten arc welding technique with rapid *** microstructures and mechanical properties of the WAAM alloy were investigated and compared with those of the as-cast samples produced using a metal *** results indicate that the WAAM Mg-6Si is harder and stronger than the as-cast *** microhardness of the WAAM Mg-6Si increases by 36.6%in comparison to that of as-cast Mg-6Si ***,the average tensile strengths at room temperature and 150°C increases by 63.4%and 21.3%,*** refines both the Mg2Si phase and the overall grains,resulting in a homogeneous morphology and improved mechanical *** granular Mg2Si phase,characterized by fine particles with a diffused distribution,shows a significant increase in *** acicular Mg2Si phase is distributed along the grain boundaries,and its concentration significantly *** average grain size of the Mg2Si phase is about 9.20μm,about 5 times *** refinement and distribution of the granular Mg2Si phase,as well as the reduction in the amount of needle-like Mg2Si particles,are the key factors for improving the mechanical properties of WAAM Mg-6Si alloy.

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