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Boosting hydrogen evolution via work-function-accelerated electronic reconfiguration of Mo-based heterojunction

Science China Materials 2025年第1期68卷 189-198页

作者： Xiang Chen Shuai Feng Song Xie Yaping Miao Biao Gao Xuming Zhang Li Huang Yun Li Paul K.Chu Xiang Peng Hubei Key Laboratory of Plasma Chemistry and Advanced Materials Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationSchool of Materials Science and EngineeringWuhan Institute of TechnologyWuhan 430205China Department of Physics Department of Materials Science and Engineeringand Department of Biomedical EngineeringCity University of Hong KongHong Kong 999077China School of Textile Science and Engineering Xi’an Polytechnic UniversityXi’an 710048China The State Key Laboratory of Refractories and Metallurgy Institute of Advanced Materials and NanotechnologyWuhan University of Science and TechnologyWuhan 430081China Guizhou Wujiang Hydropower Development Co. Ltd.Guiyang 550002China

Molybdenum-based catalysts have demonstrated significant potential in the electrocatalytic hydrogen evolution reaction(HER).However,the limited exposure of active sites and strong hydrogen adsorption result in suboptimal ***,a Mo_(2)N±MoSe_(2) heterojunction is prepared on carbon cloth(MNS/CC)to enhance the *** strong electronic interaction between Mo_(2)N and MoSe_(2),combined with the lower work function of Mo_(2)N,creates an intrinsic electric field at the heterojunction interface,which markedly improves charge transfer ***,the optimized electronic structure of Mo sites further enhances charge transfer and intrinsically catalytic activity in *** a result,MNS/CC requires overpotentials of mere 65 and 210 mV to achieve current densities of 20 mA cm^(−2) and 1 A cm^(−2),respectively,with a Tafel slope of only 96 mV dec−***,MNS/CC maintains stable operation at 1 A cm^(−2) for 240 h without significant *** results offer insights into the design of non-precious metal-based electrocatalysts for industrial hydrogen production.

关键词： water splitting hydrogen evolution reaction molybdenum-based catalyst heterojunction electronic interaction

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Improvement of the regenerability and surface electronegativity of rectorite via magnetic modification

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Journal of Molecular Liquids 2025年 427卷

作者： Su, Dan Huang, Jingyi Zhang, Ge Gao, Jing Wen, Zhipan Wang, Yingru School of Chemistry and Environmental Engineering Wuhan Institute of Technology Wuhan430073 China State Key Laboratory of New Textile Materials and Advanced Processing Technology Wuhan Textile University Wuhan430200 China

In this study, the magnetic modification of rectorite was conducted to enhance its regenerability and surface electronegativity. When using the raw rectorite, the removal rate of ciprofloxacin was 78 % and the recovery rate was only 26 % after six regeneration cycles. However, with magnetized modified rectorite (M-REC), the removal rate of ciprofloxacin was 97 % and the recovery rate exceeded 75 %. The magnetic properties, easy magnetic separation and enhanced surface electronegativity of M-REC were confirmed through SEM, TEM, VSM, XRD, BET and XPS characterization. After six regeneration recycles, the basic skeleton structure of M-REC remained largely unchanged, indicating that has excellent stability. Additionally, the adsorption kinetics and thermodynamics of M-REC were investigated, and the Langmuir model accurately described the adsorption isotherm. The adsorption kinetics data fit the pseudo-second order models. The adsorption rate was determined by the number of available adsorption sites on the M-REC surface, and the removal process was primarily driven by chemisorption. Therefore, M-REC is an environmentally friendly adsorption material with potential applications in environmental remediation. © 2025

关键词： Adsorption isotherms

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Design of multifunctional tunable dual-layer metalens based on deep learning

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Optics Express 2025年第10期33卷 21979-21998页

作者： Wang, Yu Wang, Yue Yang, Guohui Zhang, Kuang Yang, Xing Wang, Chunhui Zhang, Yu National Key Laboratory of Laser Spatial Information Harbin Institute of Technology Heilongjiang Harbin150001 China School of Electronic and Information Engineering Harbin Institute of Technology Heilongjiang Harbin150001 China State Key Laboratory of Pulsed Power Laser Technology Advanced Laser Technology Laboratory of Anhui Province Electronic Engineering Institute National University of Defense Technology Hefei230037 China Jianghuai Advance Technology Center Hefei230037 China

To address the challenges of complex control in individually tunable meta-atoms and the limited modulation performance of single-layer holistic tunable metalenses, we propose a dual-layer tunable multifunctional metalens that utilizes holistic modulation based on the tunable BaTiO3 (BTO) material. This design enables rapid switching between different functionalities to be achieved by varying the voltage across the top and bottom layers. To accelerate the device design process, we employ a deep learning algorithm based on the transformer structure and incorporate a band embedding method that aids in predicting the high-frequency response. This approach enables accurate and rapid prediction of the transmittance and phase of meta-atoms in different voltage states, and can generate 100,000 arbitrary geometric meta-atoms in less than 1 s. Detailed simulation results demonstrate that the designed metalens can achieve near-perfect switching between dual-functionality and quadruple-functionality within the visible light range. The switchable functionalities include focal length, focal position, beam deflection angle, beam splitting, and the transitions between these different functionalities. Furthermore, to enhance the manufacturability of the designed metalens, we replace arbitrary geometric meta-atoms with simple geometric meta-atoms to design the structure of the overall metalens, which can also achieve the dual-function switchable effect with minimal performance degradation. © 2025 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreement.

关键词： Geometry

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Intercalation mechanism of surfactants in vanadium pentoxides interlayer framework for improving electrochemical performance of zinc metal batteries

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Journal of Alloys and Compounds 2025年 1031卷

作者： Dou, Peiyao Li, Yuan Zhao, Lei Niu, Shengtao Wang, Yanci Ran, Fen Energy Storage Institute of Lanzhou University of Technology School of Materials Science and Engineering State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals Lanzhou University of Technology Lanzhou730050 China

Zinc metal batteries have aroused great discussion among researchers because of their advantages of abundant resource reserves, environmental protection, and inexpensive. At low current densities, the vanadium-based cathode materials in zinc metal batteries exhibit poor rate performance, slow diffusion of Zn2+, and easy structural collapse severely hinder their industrial practical applications. Hence, there is an urgent need to find a method to stabilize the microstructure and orderly coordinate insertion/extraction of Zn2+ on the vanadium-based cathode. Surfactants have abundant hydrophilic groups and hydrophobic groups, which makes them as additives to maintain the stability of the main system. In this paper, polyethylene glycol, sodium dodecyl benzene sulfonate, and hexadecyl trimethyl ammonium bromide were chosen as non-ionic, anionic, and cationic surfactants, respectively. They were inserted into the interlayer skeleton of vanadium pentoxide using hydrothermal method and heat treatment (in air), and the intercalation mechanisms of different surfactants in vanadium pentoxide cathode material is investigated. Among them, polyethylene glycol is cross inserted in the form of molecules, and compared with the other two surfactants, the cathode has outstanding electrochemical properties and stable structure, while also increasing the transfer rate of Zn2+. In particular, after adding polyethylene glycol, an excellent rate capability of 342.3 mA h g−1 was achieved at a low current density of 0.2 A g−1. Moreover, even when the current density reaches 5.0 A g−1, it is able to sustain an excellent capacity of 173.8 mA h g−1. After 700 cycles, it also maintains a good capacity retention rate. © 2025 Elsevier B.V.

关键词： Cationic surfactants

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Colossal Negative Thermal Expansion via Polar-Nonpolar Transition in Metal-Organic Frameworks

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CCS Chemistry 2025年第2期7卷 564-572页

作者： Liang Chen Rui Ma Qiang Li Xin Chen Yili Cao Chengyi Yu Jinxia Deng Chun-Yu Liu Kenichi Kato Kun Lin Xianran Xing Beijing Advanced Innovation Center for Materials Genome Engineering Institute of Solid State ChemistryUniversity of Science and Technology BeijingBeijing 100083 Key Laboratory of Eco-Textiles Ministry of EducationJiangnan UniversityWuxi 214122 Jiangsu RIKEN SPring-8 Center Sayo-gunHyogo 679-5148

Molecular-based polar structures are among most intriguing candidates for the generation of mechani-cal functions such as the *** struc-tures undergo a symmetry switching upon heating and generally yield anisotropic lattice ***-umetric negative thermal expansion(NTE)remains challenging to observe,most of which exhibits rela-tively small magnitudes as ***,we realize colossal volumetric NTE in metal-organic frame-works(MOFs)via novel polar-nonpolar structure ***,a colossal volumetric NTE(α_(v)=−302.45×10^(−6)K^(−1))was achieved from 320-380 K in CAU-10-CH_(3)due to polar-nonpolar transi-tion(space group from I41md to I41/amd),much larger than most NTE ***-temperature crystallographic analysis reveals that the aluminum-oxygen octahedra turns from low-symmetry to high symmetry upon heating and thus causes a“spring”compression of the octahedral helical chain,thus leading to colossal ***-group modifica-tions further identify the excellent tunability of such *** strongest uniaxial NTE,to date,was simultaneously found in CAU-10-H along the c direction(α_(c)=−577.22×10^(−6)K^(−1)),whereas the CAU-10-NH_(2)contributes to a sluggish phase *** work provides the first example of tailoring a colossal NTE via polar-nonpolar transition in frame-works.

关键词： colossal negative thermal expansion metal-organic frameworks polar structure phase transition aluminum-oxygen octahedra

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边缘电子态调制实现效率超过15%的锡基钙钛矿太阳电池（英文）

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Science China Materials 2025年第5期68卷 1462-1471页

作者：左晨刘庚灵刘聪龚安稳陈凯钟杨徐鑫熊文涛狄大卫胡笑添刘焘谈利承邹炳锁陈义旺 State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures School of ResourcesEnvironment and MaterialsGuangxi University Key Laboratory of Bioinorganic and Synthetic Chemistry (Mo 5 Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen University Institute of Polymers and Energy Chemistry (IPEC)/Film Energy Chemistry for Jiangxi Provincial Key Laboratory (FEC) Nanchang University DGUT-CNAM Institute Dongguan University of Technology State Key Laboratory of Extreme Photonics and Instrumentation College of Optical Science and EngineeringInternational Research Center for Advanced PhotonicsZhejiang University

锡基钙钛矿的严重p型掺杂效应和本征缺陷极大地限制了锡基钙钛矿太阳电池（PSCs）器件性能.本研究提出了一种新型n型有机小分子掺杂剂, NDI2HD-Br2,以缓解锡基钙钛矿的严重p型自掺杂并钝化锡相关缺陷. NDI2HD-Br2中具有高电子密度的羰基... 详细信息

锡基钙钛矿的严重p型掺杂效应和本征缺陷极大地限制了锡基钙钛矿太阳电池（PSCs）器件性能.本研究提出了一种新型n型有机小分子掺杂剂, NDI2HD-Br2,以缓解锡基钙钛矿的严重p型自掺杂并钝化锡相关缺陷. NDI2HD-Br2中具有高电子密度的羰基（C=O）可以向钙钛矿带边提供额外的电子,从而将锡基钙钛矿从p型转化为弱n型半导体（费米能级上移0.15 eV）.通过这种方法,锡基PSCs的功率转换效率（PCE）达到15.01%,开路电压高达0.95 V.此外,掺入NDI2HD-Br2的器件具有出色的长期稳定性,在氮气环境中存储1500小时后仍能保持81%的初始PCE.这项研究为调控锡基钙钛矿的电子结构并钝化其本征缺陷以实现高效稳定的太阳能电池提供了一条新途径.

关键词： perovskite solar cells tin electron transfer defects weak n-type

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Novel and facile fabrication of hydrophobic sponge for the efficient adsorption of marine crude oil by photothermal conversion

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Polymer 2025年 329卷

作者： Zhang, Di Zhao, Jingyuan Zhang, Tong Yue, Kai Zhao, Ruirui Fu, Hiroshi Zhang, Songnan State Key Laboratory of Advanced Separation Membrane Materials/ School of Chemical Engineering and Technology Tiangong University Tianjin300387 China Ministry of Education Key Laboratory for Advanced Textile Composite Materials/ School of Textile Science and Engineering Tiangong University Tianjin300387 China Co. Ltd. Jiangsu Nantong226000 China

With the acceleration of the globalization of world maritime trade, the oil is largely transported. Whereas, the oil spill inevitably occurs during transportation. This not only causes the waste of energy, but also has a huge impact on the ecology. Therefore, it is imperative to develop efficient adsorbent to recover the leaked crude oil. In this study, a new and facile adsorption material was introduced for the treatment of offshore crude oil leakage. This material combined the hydrophobic modification of polydimethylsililane (PDMS) with the loadings of graphene (GR) and ferriferrous oxide (Fe3O4) over melamine sponge (MS), providing it with excellent hydrophobic/oleophilic and photothermal conversion properties. It revealed that the MS/PDMS/GR + Fe3O4 presented the hydrophobic property with the water contact angle of 147° and superior self-cleaning performance, effectively separating the oil and water mixture with the separation efficiency of up to 99 %. In addition, its excellent photothermal conversion ability converted the light energy into heat energy, reducing the crude oil viscosity and improving the adsorption efficiency. Under one sun illumination (1.0 kW m−2), the adsorption capacity of the MS/PDMS/GR + Fe3O4 for the high viscosity crude oil reached to 20.7 gcrude oil/gsorbent, and the surface temperature of sample was more than 60 °C. This material exhibited excellent recycling properties after 10 adsorption and extrusion cycles, and displayed exceptional photothermal stability during light switch cycles (1.0 kW m−2). This MS/PDMS/GR + Fe3O4 offers novel concepts for designing and developing high-performance sorbents for the ocean oil leakage treatment. © 2025 Elsevier Ltd

关键词： Marine pollution

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Fine-grained titanium mediates the biointerfacial and bioenergetic remodeling of macrophage for optimized osseointegration

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材料科学技术（英文版） 2025年第5期208卷 292-306页

作者： Yingjing Fang Hao Gu Wenyue Yang Yintao Zhang Changgong Lan Binghao Wang Min Ruan Liqiang Wang Yuanfei Fu Department of Prosthodontics Shanghai Ninth People's HospitalShanghai Jiao Tong University School of MedicineCollege of StomatologyShanghai Jiao Tong UniversityNational Center for StomatologyNational Clinical Research Center for Oral DiseasesShanghai Key Laboratory of StomatologyShanghai Research Institute of StomatologyShanghai Engineering Research Center of Advanced Dental Technology and MaterialsShanghai 200011China Departments of Oral and Maxillofacial-Head and Neck Oncology Shanghai Ninth People's HospitalShanghai Jiao Tong University School of MedicineCollege of StomatologyShanghai Jiao Tong UniversityNational Center for StomatologyNational Clinical Research Center for Oral DiseasesShanghai Key Laboratory of StomatologyShanghai Research Institute of StomatologyShanghai 200011China Department of Prosthodontics Shanghai Ninth People's HospitalShanghai Jiao Tong University School of MedicineCollege of StomatologyShanghai Jiao Tong UniversityNational Center for StomatologyNational Clinical Research Center for Oral DiseasesShanghai Key Laboratory of StomatologyShanghai Research Institute of StomatologyShanghai Engineering Research Center of Advanced Dental Technology and MaterialsShanghai 200011China State Key Laboratory of Metal Matrix Composites School of Material Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Affiliated Hospital of Youjiang Medical University for Nationalities Youjiang Medical University for NationalitiesGuangxi Key Laboratory of Basic and Translational Research of Bone and Joint Degenerative DiseasesGuangxi Biomedical Materials Engineering Research Center for Bone and Joint Degenerative DiseasesBaise 533000China Departments of Oral and Maxillofacial-Head and Neck Oncology Shanghai Ninth People's HospitalShanghai Jiao Tong University School of MedicineCollege of StomatologyShanghai Jiao Tong UniversityNational Center for StomatologyNational Clinical Research Center for Oral DiseasesShanghai Key Laboratory of StomatologyShang

The remodeling of macrophages mediated by biomaterials is an important step in *** biointerfacial characteristics shaped by implants and the bioenergetic state derived from macrophages are considered the key to macrophage *** this study,the integrated Ti/Zn composites with optimized morphology and bioactive phase were prepared by friction stir processing,which could meet the multi-biofunctional requirements in the application of narrow-diameter *** severe plastic deformation and the hindrance of Zn particles to grain growth promote grain refinement,resulting in enhanced mechanical *** cell interfacial adhesion mediated by the grain boundary collab-orated the energy metabolism reprogramming induced by the released Zn ion,promoting jointly anti-inflammatory cascade in macrophages and favorable osteogenesis in bone marrow mesenchymal stem cells(BMSCs).This study provides a new simultaneous approach of morphology and composition modi-fication for titanium implants,and reveals the important role of grain size and bioactive element in the reversion of macrophage fate as well.

关键词： Grain refinement Zinc Immunomodulation Osseointegration

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Quantitatively regulated and recognized dual-precipitates of Mg-5Sn alloy through an improved twinning-aging-detwinning and strengthening mechanisms

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Journal of Magnesium and Alloys 2025年

作者： Fu, Ruihao Zeng, Ying Wan, Yangjie Qian, Xiaoying Xu, Shiwei Yin, Dongdi Key Laboratory of Advanced Technologies of Materials Ministry of Education School of Material Science and Engineering Southwest Jiaotong University Chengdu610031 China National Engineering Research Center for Magnesium Alloys Chongqing University Chongqing400044 China State Key Laboratory of Advanced Design and Manufacturing Technology for Vehicle Hunan University Changsha410082 China

The orientation of precipitates was regulated by an improved twinning-aging-detwinning (TAD) process in Mg-Sn sheets. A structure with specific proportions of dual-precipitates was regulated, significantly enhancing the material's strength. The formation mechanism of the dual-precipitates was investigated, and the evolution of precipitate orientation was confirmed. A combined SEM, EBSD and TEM method was developed to identify the coupling relationship between complex grain orientation and precipitate orientation. The orientation relationship between precipitates and the matrix could be quantitatively analyzed in the same region. Subsequently, the Orowan model was refined to quantify the strength enhancement effect following the orientation regulation of precipitates. The TAD sample containing dual-precipitates exhibited a 99.1 % increase in TYS, equivalent to an increase of 108 MPa, compared to unregulated samples A. According to Orowan calculations, the theoretical strength increment from the three strengthening mechanisms was 113 MPa, closely matching the experimental increment of 108 MPa. Notably, the materials with a specific proportion of the dual-precipitates showed a substantial increase in strength. © 2025

关键词： Precipitates

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Trace of Atomically Dispersed Pd Enables Unprecedented Butadiene Semihydrogenation Performance Over Copper Catalyst

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ACS Catalysis 2025年第5期15卷 3810-3822页

作者： Zhao Wang Hao Yuan Jian Tao Shu-Lin Liu Ying Hong Zhi-Yi Hu Jian Zhang Bao-Lian Su The State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology Wuhan Hubei 430070 P. R. China State Key Laboratory of Solidification Processing School of Materials Science and Engineering Northwestern Polytechnical University Xi’an Shaanxi 710000 P. R. China The State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology Wuhan Hubei 430070 P. R. China；Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles Namur B-5000 Belgium

Semihydrogenation plays a key role in industrial hydrorefining of light alkenes, with a market above 400 billion by 2027. The high cost of commercial palladium-based catalysts strongly calls for innovation but with great challenges. Herein, copper nanoparticles decorated with a minimized ppm of Pd are developed through a chemical plating process to integrate the catalytic advantages of copper and palladium for achieving maximized catalysis in the semihydrogenation of a fatal impurity of butadiene in alkene feedstocks. The developed Pd–Cu catalyst (i.e., 114 ppm of Pd in Pd0.0033Cu1/TiO2) exhibits an unprecedented catalytic performance superior to commercial Pd/Al2O3, with 100% butene selectivity above 90% of butadiene conversion over 130 h on stream at 90 °C. Further exploration reveals that the atomically dispersed Pd on Cu nanoparticles, obtained at ultralow ppm levels of Pd loading, induces a hidden but critical H2trap, which concentrates H2on the Pd site for further H2dissociation that offers intermediate hydrogen atoms to the tandem butadiene semihydrogenation over the third layer of Cu atoms neighboring Pd through hydrogen spillover. Moreover, a threshold on Pd density was identified at Pd/Cu surficial atomic ratio of 1/138 (i.e., Pd0.0033Cu1/TiO2) for maximizing butadiene semihydrogenation performance, based on an extreme collaboration between Pd for H2dissociation and Cu for butadiene hydrogenation. This work provides important guidance for developing noble metal-saving catalysts in industrial applications.

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