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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

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Effect of Ti Additions on Mechanical and Thermodynamic Properties of W-Ti Alloys: A First-principles Study

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Journal of Wuhan University of Technology(materials Science) 2025年第1期40卷 246-257页

作者： ZHANG Jian NIE Wei HUANG Jin ZHU Ke LIU Ruxia ZHANG Ruizhi LUO Guoqiang SHEN Qiang State Key laboratory of advanced Technology for materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Institute for Carbon Neutrality University of Science and Technology BeijingBeijing 100083China

The mechanical and thermodynamic properties of W-Ti alloys(including W_(15)Ti_(1),W_(14)Ti_(2),W_(12)Ti_(4) and W_(8)Ti_(8) alloys)were investigated by the first-principles approach based on density functional *** results indicate that W-Ti alloys except W_(8)Ti_(8) are thermodynamically *** modulus and hardness of W-Ti alloys are smaller than those of pure tungsten and gradually decrease with increasing Ti ***,their B/G ratios and Poisson's ratios exceed those of pure tungsten,suggesting that the introduction of Ti decreases the mechanical strength while enhancing the ductility of W-Ti *** thermal expansion coefficients for W-Ti alloys all surpass those of pure tungsten,indicating that the introduction of titanium exacerbates the thermal expansion behavior of W-Ti ***,elevated pressure has the capacity to suppress the thermal expansion tendencies in titanium-doped tungsten *** study offers theoretical insights for the design of nuclear materials by exploring the mechanical and thermodynamic properties of W-Ti alloys.

关键词： first-principles mechanical properties thermodynamic properties tungsten-titanium alloys

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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

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Plasmonic tandem heterojunctions enable high-efficiency charge transfer for broad spectrum photocatalytic hydrogen production

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Journal of Energy Chemistry 2025年第1期100卷 710-720页

作者： Wenxuan Chen Xiu-Qing Qiao Guo Hui Bojing Sun Dongfang Hou Meidi Wang Xueqian Wu Tao Wu Dong-Sheng Li College of materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials China Three Gorges University Hubei Three Gorges laboratory College of Chemistry and materials Science and Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University

Rational engineering of semiconductor photocatalysts for efficient hydrogen production is of great significance but still challenging,primarily due to the limitations in charge transfer ***,a fascinating plasmonic tandem heterojunction with the hc-CdS/Mo2C@C heterostructure is aimfully prepared for effectively promoting the charge separation kinetics of the CdS photocatalyst via the synergistic strategy of phase junction,Schottky junction,and photothermal *** difference in atomic configuration between cubic-CdS （c-CdS） and hexagonal-CdS （h-CdS） leads to effective charge separation through a typical Ⅱ charge transfer mechanism,and plasmonic Schottky junction further extracts the electrons in the hc-CdS phase junction to realize gradient charge ***,the photothermal effect of Mo2C@C helps to expand the light absorption,accelerate charge transfer kinetics,and reduce the hydrogen evolution energy *** carbon layer provides a fast channel for charge transfer and protects the photocatalyst from *** a result,the optimized hc-CMC photocatalyst exhibits a significantly high photocatalytic H2production activity of 28.63 mmol/g/h and apparent quantum efficiency of 61.8%,surpassing most of the reported *** study provides a feasible strategy to enhance the charge transfer kinetics and photocatalytic activity of CdS by constructing plasmonic tandem heterogeneous junctions.

关键词： Cadmium sulfide

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Thermally triggered topological polymerization in diacetylene-functionalized covalent organic framework toward enhanced memristive properties

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Science China Chemistry 2025年

作者： Panke Zhou Yuxing Huang Ziyue Yu Cong Zhang Qian Chen Yiping Li Chao Lin Xiong Chen State Key laboratory of Photocatalysis on Energy and Environment Key Laboratory of Advanced Carbon-Based Functional MaterialsCollege of Chemistry Fuzhou University

The development of stimuli-responsive switching memory devices and the elucidation of their switching mechanisms in specific environments are crucial for advancing the field of molecular electronics. Herein, we propose two distinct two-dimensional covalent organic frameworks (COFs), namely Py-EDA and Py-BDA, incorporating acetylene (-C≡C-) or diacetylene(-C≡C-C≡C-) moieties, respectively, targeting fabricate memory devices exhibiting stimuli-responsive switching *** findings demonstrate that the incorporation of acetylene units effectively modulates the electronic band structure and enhances the degree ofπ-conjugation, resulting in devices that exhibit typical bipolar nonvolatile memory performance. Notably,upon thermal treatment, the memory behavior of the ITO/Py-BDA/Ag device transitions to a write-once-read-many-times(WORM) mode, displaying decreased SET voltage, increased ON/OFF current ratio, and remarkable retention reliability and cycle stability. This switching behavior is attributed to the occurrence of interlayer solid-state topological polymerization at 350℃, leading to the transformation of diacetylene columnar arrays into enyne chains within Py-BDA, thereby further promoting interlayer charge transfer and separation.

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“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

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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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Mechanistic insight into the synergy between nickel single atoms and nanoparticles on N-doped carbon for electroreduction of CO2

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Journal of Energy Chemistry 2025年第1期100卷 327-336页

作者： Mingdong Sun Wenwen Guan Cailing Chen Chao Wu Xiaoling Liu Biao Meng Tao Chen Yu Han Jun Wang Shibo Xi Yu Zhou State Key laboratory of materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University advanced Membranes and Porous materials Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology Institute of Sustainability for Chemicals Energy and Environment A*STAR (Agency for Science Technology and Research) College of materials Science and Engineering Sichuan University

The synergy of single atoms （SAs） and nanoparticles （NPs） has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction （CO2RR）;however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst ***,a Ni2+-loaded porous poly（ionic liquids）(PIL) precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing *** catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO2into *** Ni K-edge X-ray absorption near-edge structure （XANES） spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and *** charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active *** the electroreduction of CO2,the coexistence of Ni SAs and NPs strengthened the CO2activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO2→*COOH step,and therefore promoted the catalysis efficiency.

关键词： Activation energy

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Enhanced rate capability and cycle stability of Ti2C MXene for sodium storage through an aniline molecules welding strategy

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Tungsten 2025年第1期7卷 161-171页

作者： Hao Chen Ya-Qin Wang Dong-Ting Zhang Bei Zhao Min-Peng Li Chen-Yang Li Tian-Peng Xu Mao-Cheng Liu State Key laboratory of advanced Processing and Recycling of Non-Ferrous Metals Lanzhou University of Technology School of materials Science and Engineering Lanzhou University of Technology School of Computer and Communication Technology Lanzhou University of Technology

MXenes obtained significant attention in the field of energy storage devices due to their characteristic layered structure,modifiable surface functional groups,large electrochemically active surface,and regulable interlayer ***,the self-restacking and sluggish ions diffusion kinetics performance of MXenes during the alkali metal ions insertion/extraction process severely impedes their cycle stability and rate *** paper proposes an aniline molecule welding strategy for welding p-phenylenediamine（PPDA） into the interlayers of Ti2C through a dehydration condensation *** welded PPDA molecules can contribute pillar effect to the layered structure of *** pillar effect effectively maintains the structural stability during the sodium ions insertion/extraction process and effectively expands the interlayer spacing of Ti2C from 1.16 to 1.38 nm,thereby enhancing ions diffusion kinetics performance and improving the long-term cycle *** Ti2C-PPDA demonstrates outstanding Na+storage capability,exhibiting a specific capacity of 100.2 mAh·g-1at a current density of 0.1 A·g-1over 960 cycles and delivering a remarkable rate capability 81.2 mAh·g-1at a current density of 5 A·*** study demonstrates that expanding interlayer spacing is a promising strategy to enhance the Na+storage capacity and improve long-term cycling stability,which provides significant guidance for the design of two-dimensional Na+storage materials with high-rate capability and cycle stability.

关键词： Diffusion kinetics Expanding interlayer spacing Rate capability Sodium ions storage Ti2C

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Integration of Electrical Properties and Polarization Loss Modulation on Atomic Fe–N‑RGO for Boosting Electromagnetic Wave Absorption

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Nano-Micro Letters 2025年第2期17卷 517-532页

作者： Kaili Zhang Yuefeng Yan Zhen Wang Guansheng Ma Dechang Jia Xiaoxiao Huang Yu Zhou State Key laboratory of Precision Welding&Joining of materials and Structures Harbin Institute of TechnologyHarbin 150001People’s Republic of China School of materials Science and Engineering Harbin Institute of TechnologyHarbin 150001People’s Republic of China MIIT Key laboratory of advanced Structural‑Functional Integration materials&Green Manufacturing Technology Harbin Institute of TechnologyHarbin 150001People’s Republic of China

Developing effective strategies to regulate graphene’s conduction loss and polarization has become a key to expanding its application in the electromagnetic wave absorption(EMWA)*** on the unique energy band structure of graphene,regulating its bandgap and electrical properties by introducing heteroatoms is considered a feasible ***,metal-nitrogen doping reduced graphene oxide(M–N-RGO)was prepared by embedding a series of single metal atoms M–N_(4) sites(M=Mn,Fe,Co,Ni,Cu,Zn,Nb,Cd,and Sn)in RGO using an N-coordination atom-assisted *** composites had adjustable conductivity and polarization to optimize dielectric loss and impedance matching for efficient EMWA *** results showed that the minimum reflection loss(RL_(min))of Fe–N-RGO reaches−74.05 dB(2.0 mm)and the maximum effective absorption bandwidth(EAB_(max))is 7.05 GHz(1.89 mm)even with a low filler loading of only 1 wt%.Combined with X-ray absorption spectra(XAFS),atomic force microscopy,and density functional theory calculation analysis,the Fe–N_(4) can be used as the polarization center to increase dipole polarization,interface polarization and defect-induced polarization due to d-p orbital hybridization and structural ***,electron migration within the Fe further leads to conduction loss,thereby synergistically promoting energy *** study demonstrates the effectiveness of metal-nitrogen doping in regulating the graphene′s dielectric properties,which provides an important basis for further investigation of the loss mechanism.

关键词： Electromagnetic wave absorption Fe-N-RGO Dipole polarization Conduction loss Impedance matching

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