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Morphology-controlled synthesis of multi-metal-based spinel oxide nanocatalysts and their performance for oxygen reduction

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Electron 2024年第3期2卷 13-19页

作者： Can Li Jinfong Pan Xiaobo Chen Lihua Zhang Anna Dennett Prabhu Bharathan Douglas Lee Guangwen Zhou Jiye Fang Department of Chemistry State University of New York at BinghamtonBinghamtonNew YorkUSA Materials Science and Engineering Program State University of New York at BinghamtonBinghamtonNew YorkUSA Center for Functional Nanomaterials Brookhaven National LaboratoryUptonNew YorkUSA Department of Mechanical Engineering State University of New York at BinghamtonBinghamtonNew YorkUSA

We present a one-pot colloidal synthesis method for producing monodisperse multi-metal(Co,Mn,and Fe)spinel nanocrystals(NCs),including nanocubes,nano-octahedra,and concave *** study explores the mechanism of morphology control,showcasing the pivotal roles of metal precursors and capping ligands in determining the exposed crystal planes on the NC *** cubic spinel NCs,terminated with exclusive{100}-facets,demonstrate superior electrocatalytic activity for the oxygen reduction reaction(ORR)in alkaline media compared to their octahedral and concave cubic ***,at 0.85 V,(CoMn)Fe_(2)O_(4) spinel oxide nanocubes achieve a high mass activity of 23.9 A/g and exhibit excellent stability,highlighting the promising ORR performance associated with{100}-facets of multi-metal spinel oxides over other low-index and high-index *** by exploring the correlation between ORR performance and surface atom arrangement(active sites),surface element composition,as well as other factors,this study introduces a prospective approach for shapecontrolled synthesis of advanced spinel oxide *** underscores the significance of catalyst shape control and suggests potential applications as nonprecious metal ORR electrocatalysts.

关键词： alkaline media morphology control multi-metal spinel catalyst nanocrystals oxygen reduction

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Modulating contact properties by molecular layers in organic thin-film transistors

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Electron 2023年第2期1卷 82-89页

作者： Li Sun Yating Li Jiacheng Xie Liqi Zhou Peng Wang Jian-Bin Xu Yi Shi Xinran Wang Daowei He National Laboratory of Solid State Microstructures Key Lab of Optoelectronic Devices and Systems with Extreme PerformancesSchool of Electronic Science and Engineeringand Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjingChina National Laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional MaterialsCollege of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjingChina Department of Physics University of WarwickCoventryUK Department of Electronic Engineering and Materials Science and Technology Research Center The Chinese University of Hong KongHong Kong SARChina School of Integrated Circuits Nanjing UniversitySuzhouChina

Advanced organic devices and circuits demand both ultrahigh charge carrier mobilities and ultralow-resistance ***,due to a larger access resistance in staggered organic thin-film transistors(OTFTs),the achievement of ultralow contact resistance(Rc)is still a *** modulation of contact resistance by molecular layers near the interface has been rarely ***,we demonstrate that fewlayer organic single crystals are grown on hafnium oxide(HfO_(2))by solution-shearing *** utilize these organic crystals to fabricate bottom-gate staggered OTFTs with different contact *** results show that the contact properties of OTFTs are obviously modulated by crystal *** tri-layer(3L)evaporated-Au C10-DNTT OTFTs exhibit optimal electrical performance,including ultralow Rc of 5.6Ω⋅cm,recorded transfer length of 0.4μm,field-effect mobility over 14 cm^(2)V^(−1)s^(−1),threshold voltage lower than 0.3 V,and long-term air stability over 8 *** main cause is that the metal atoms can penetrate into the charge transport layer,with damage-free,in 3L evaporated-Au OTFTs;nevertheless,it cannot be realized in other *** to layer stacking of conjugated molecules and polymers,our strategy can efficiently modulate the contact resistance to aid the development of highperformance organic devices and circuits.

关键词： contact resistance mobility organic thin-film transistor single crystal

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Porous Microreactor Chip for Photocatalytic Seawater Splitting over 300 Hours at Atmospheric Pressure

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Nano-Micro Letters 2025年第8期17卷 251-263页

作者： Desheng Zhu Zhipeng Dong Chengmei Zhong Junhong Zhang Qi Chen Ni Yin Wencheng Jia Xiong Zheng Fengzai Lv Zhong Chen Zhenchao Dong Wencai Huang Department of Electronic Engineering School of Electronic Science and TechnologyXiamen UniversityXiamen 361005People’s Republic of China Fuzhou Fuzhi Photocatalysis Research Center Fuzhou 350007People’s Republic of China i-Lab CAS Key Laboratory of Nanophotonic Materials and DevicesSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123People’s Republic of China Hefei National Research Center for Physical Sciences at the Microscale and CAS Center for Excellence in Quantum Information and Quantum Physics University of Science and Technology of ChinaHefei 230026People’s Republic of China State Key Laboratory of Physical Chemistry of Solid Surfaces Xiamen UniversityXiamen 361005People’s Republic of China

Photocatalytic seawater splitting is an attractive way for producing green *** progresses have been made recently in catalytic efficiencies,but the activity of catalysts can only maintain stable for about 10 ***,we develop a vacancy-engineered Ag_(3)PO_(4)/CdS porous microreactor chip photocatalyst,operating in seawater with a performance stability exceeding 300 *** is achieved by the establishment of both catalytic selectivity for impurity ions and tailored interactions between vacancies and sulfur *** transport of carriers with strong redox ability is ensured by forming a heterojunction within a space charge region,where the visualization of potential distribution confirms the key design concept of our ***,the separation of oxidation and reduction reactions in space inhibits the reverse recombination,making the chip capable of working at atmospheric ***,in the presence of Pt co-catalysts,a high solar-to-hydrogen efficiency of 0.81%can be achieved in the whole durability *** using a fully solar-driven 256 cm2 hydrogen production prototype,a H_(2) evolution rate of 68.01 mmol h−1 m−2 can be achieved under outdoor *** findings provide a novel approach to achieve high selectivity,and demonstrate an efficient and scalable prototype suitable for practical solar H_(2) production.

关键词： Solar energy Hydrogen energy Photocatalytic seawater splitting Silver phosphate/Cadmium sulfide heterojunction

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General strategy for evaluating the d-band center shift and ethanol oxidation reaction pathway towards Pt-based electrocatalysts

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science China Chemistry 2023年第1期66卷 279-288页

作者： Jin-Hong Zheng Guang Li Jun-Ming Zhang Ningyan Cheng Li-Fei Ji Jian Yang Jialin Zhang Bin-Wei Zhang Yan-Xia Jiang Shi-Gang Sun State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China School of Chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China Center of Advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing 400044China Key Laboratory of Magnetic Molecules&Magnetic Information Materials Ministry of Education School of Chemical and Material ScienceShanxi Normal UniversityTaiyuan 030031China Information Materials and Intelligent Sensing Laboratory of Anhui Province Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationInstitutes of Physical Science and Information TechnologyAnhui UniversityHefei 230039China

The catalytic performance of Pt-based catalysts depends sensitively on their d-band ***,there are still huge challenges to evaluate their d-band centers from experimental technologies,and modulate them to analyze their selectivity in ethanol oxidation reaction(EOR).Here,Pt1Au1alloy supported on the commercial carbon material(Pt_(1)Au_(1)/C)is employed as a typical example to investigate its d-band center shift of surface Pt,and as electrocatalysts to study its selectivity towards ***,a highly reliable in situ Fourier-transform infrared spectroscopy CO-probe strategy is developed to characterize the d-band center shift of surface *** modified electronic effect and site effect of Pt_(1)Au_(1)/C dictated the adsorption configuration of intermediate species and the OH species coverage,thereby influencing its *** importantly,we developed a universal cyclic voltammetry peak differentiation fitting method as an electrochemical analysis technique to investigate CO_(2)selectivity,which is potentially extendable to other Pt-based electrocatalysts.

关键词： PtAu in situ FTIRS d-band center ethanol oxidation reaction CV peak differentiation fitting method

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Halide vapor phase epitaxy of monolayer molybdenum diselenide single crystals

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National science Open 2023年第4期2卷 55-64页

作者： Taotao Li Yang Yang Liqi Zhou Wenjie Sun Weiyi Lin Lei Liu Xilu Zou Si Gao Yuefeng Nie Yi Shi Xinran Wang National Laboratory of Solid State Microstructures School of Electronic Science and Engineering and Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093China National Laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional MaterialsCollege of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093China School of Electronic Science and Engineering Xiamen UniversityXiamen 361005China College of Material Science and Engineering Nanjing Tech UniversityNanjing 201110China School of Integrated Circuits Nanjing UniversitySuzhou 215163China Suzhou Laboratory Suzhou 215000China

Single-crystalline transition metal dichalcogenides(TMD)films are of potential application in future electronics and *** this work,a halide vapor phase epitaxy(HVPE)strategy was proposed and demonstrated for the epitaxy of molybdenum diselenide(MoSe_(2))single crystals,in which metal halide vapors were in-situ produced by the chlorination of molybdenum as sources for the TMD *** with the epitaxial sapphire substrate,unidirectional domain alignment was successfully achieved and monolayer single-crystal MoSe_(2) films have been demonstrated on a 2-inch wafer for the first time.A series of characterizations ranging from centimeter to nanometer scales have been implemented to demonstrate the high quality and uniformity of the MoSe_(2).This work provides a universal strategy for the growth of TMD single-crystal films.

关键词： halide vapor phase epitaxy single-crystal molybdenum diselenide 2D semiconductor wafer-scale

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First-principles study and characterization of high strength and toughness (TiCrZrVNb)C ceramic films

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Ceramics International 2025年第17期51卷 23255-23266页

作者： Xu, Wenju Jia, Bingsen Li, Xianke Li, Jingfeng Li, Hongxuan Liu, Xiaohong Ji, Li Wang, Shunbo Ju, Pengfei Zhou, Huidi Chen, Jianmin State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Lanzhou730000 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing100049 China Key Laboratory of CNC Equipment Reliability Ministry of Education Jilin University Changchun130025 China Shanghai Aerospace Equipment Manufacturer Co. Ltd. Shanghai200245 China

Guided by the first-principles calculations, a fine combination of high strength and toughness was obtained in (TiCrZrVNb)C films. The calculated negative formation energy of −39.98 kJ/mol and negative mixing Gibbs free energy above 1257 K indicated chemical and mono-phase stability, respectively. Moreover, the calculated B/G and Poisson's ratio of 1.49 and 0.23, respectively, are below but close to the toughness critical, indicating possible toughness. Subsequently, (TiCrZrVNb)C films were successfully deposited via multi-arc ion plating under varying negative bias voltages (Vn). The films under different Vn possess the FCC structure and present ranging hardness from 25.93 ± 1.17 GPa at −100 V to the peak value of 32.57 ± 0.98 GPa at −400 V. Importantly, the micropillar compressing tests were conducted to determine the stress-strain curve of this films. The curves show the films under −400 V present both outstanding yield strength of 9.5 GPa and high toughness. This mainly results from two levels of chemical fluctuations (CFs) from the nanoscale to the atomic level. This not only significantly restricts the movement of dislocations, thereby enhancing the strength, but also promotes the uniform distribution of plastic deformation among grains, causing high toughness. © 2025 Elsevier Ltd and Techna Group S.r.l.

关键词： Poisson ratio

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Ultrahigh thermoelectric performance in RbGeI3/CsSnI3 superlattices

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Physical Review B 2024年第8期109卷 085305-085305页

作者： Yaorong Luo Xu Li Hao Cheng Bingxuan An Lan Chen Jian Zhou Di Wu Yurong Yang Department of Materials Science and Engineering National Laboratory of Solid State Microstructures and Collaborative Innovation Center of Advanced Microstructures Jiangsu Key Laboratory of Artificial Functional Materials Nanjing University Nanjing 210093 China School of Science Nanjing University of Posts and Telecommunications Nanjing 210023 China

By first-principles methods combined with Boltzmann transport theory, we perform a systematic investigation of the thermoelectric properties of RbGeI3/CsSnI3 superlattices. RbGeI3/CsSnI3 superlattices construct a quantum well with valence and conduction states near the Fermi level located in CsSnI3 layers, which yields a periodic repetition of two-dimensional transport channels. The quantum-confinement effects and the ultralow lattice thermal conductivity of the superlattices greatly enhance the in-plane thermoelectric power factor and figure of merit (ZT), which further increase when decreasing the thickness of CsSnI3 layers in the superlattices. In (RbGeI3)5/(CsSnI3)1 superlattice, the power factor increases by two times, and ZT is enhanced by nine times, compared to the parent CsSnI3. The ZT of this superlattice is 1.34 at 300 K and 3.78 at 550 K, providing a potential candidate for room-temperature thermoelectric applications. These results also confirm a way to improve the thermoelectric performance of CsSnI3.

关键词： Lattice thermal conductivity Thermoelectric effects Quantum wells Superlattices Density functional calculations

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Electronic structure and spin–orbit coupling in ternary transition metal chalcogenides Cu_(2)TlX_(2)(X = Se, Te)

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Chinese Physics B 2022年第3期31卷 122-127页

作者： Na Qin Xian Du Yangyang Lv Lu Kang Zhongxu Yin Jingsong Zhou Xu Gu Qinqin Zhang Runzhe Xu Wenxuan Zhao Yidian Li Shuhua Yao Yanfeng Chen Zhongkai Liu Lexian Yang Yulin Chen State Key Laboratory of Low Dimensional Quantum Physics Department of PhysicsTsinghua UniversityBeijing 100084China National Laboratory of Solid State Microstructures Department of Materials Science and EngineeringNanjing UniversityNanjing 210093China School of Physical Science and Technology ShanghaiTech University and CAS-Shanghai Science Research CenterShanghai 201210China ShanghaiTech Laboratory for Topological Physics Shanghai 200031China Frontier Science Center for Quantum Information Beijing 100084China Department of Physics Clarendon LaboratoryUniversity of OxfordParks RoadOxford 0XI 3PUUK

Ternary transition metal chalcogenides provide a rich platform to search and study intriguing electronic properties. Using angle-resolved photoemission spectroscopy and ab initio calculation, we investigate the electronic structure of Cu_(2)TlX_(2)(X = Se, Te), ternary transition metal chalcogenides with quasi-two-dimensional crystal structure. The band dispersions near the Fermi level are mainly contributed by the Te/Se p orbitals. According to our ab-initio calculation, the electronic structure changes from a semiconductor with indirect band gap in Cu_(2)TlSe_(2) to a semimetal in Cu_(2)TlTe_(2), suggesting a band-gap tunability with the composition of Se and Te. By comparing ARPES experimental data with the calculated results, we identify strong modulation of the band structure by spin–orbit coupling in the compounds. Our results provide a ternary platform to study and engineer the electronic properties of transition metal chalcogenides related to large spin–orbit coupling.

关键词： transition metal chalcogenides spin–orbit coupling electronic structure angle-resolved photoemission spectroscopy(ARPES)

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Ultra-thick,dense dual-encapsulated Sb anode architecture with conductively elastic networks promises potassium-ion batteries with high areal and volumetric capacities

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escience 2023年第6期3卷 58-68页

作者： Zhonggang Liu Xi Liu Bingchun Wang Xinying Wang Dongzhen Lu Dijun Shen Zhefei Sun Yongchang Liu Wenli Zhang Qiaobao Zhang Yunyong Li School of Materials and Energy Guangdong University of TechnologyNo.100 Waihuan Xi RoadGuangzhou Higher Education Mega CenterGuangzhou 510006China State Key Laboratory of Physical Chemistry of Solid Surfaces College of MaterialsXiamen UniversityXiamenFujian 361005China Beijing Advanced Innovation Center for Materials Genome Engineering Institute for Advanced Materials and TechnologyState Key Laboratory for Advanced Metals and MaterialsUniversity of Science and Technology BeijingBeijing 100083China Guangdong Provincial Key Laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light IndustryGuangdong University of TechnologyNo.100 Waihuan Xi RoadGuangzhou Higher Education Mega CenterGuangzhou 510006China

Ultra-thick,dense alloy-type anodes are promising for achieving large areal and volumetric performance in potassium-ion batteries(PIBs),but severe volume expansion as well as sluggish ion and electron diffusion kinetics heavily impede their widespread ***,we design highly dense(3.1 g cm^(-3))Ti_(3)C_(2)T_(x) MXene and graphene dual-encapsulated nano-Sb monolith architectures(HD-Sb@Ti_(3)C_(2)T_(x)-G)with high-conductivity elastic networks(1560 S m^(-1))and compact dually encapsulated structures,which exhibit a large volumetric capacity of 1780.2 mAh cm^(-3)(gravimetric capacity:565.0 mAh g^(-1)),a long-term stable lifespan of 500 cycles with 82%retention,and a large areal capacity of 8.6 mAh cm^(-2)(loading:31 mg cm^(-2))in *** ex-situ SEM,in-situ TEM,kinetic investigations,and theoretical calculations,we reveal that the excellent areal and volumetric performance mechanism stems from the three dimensional(3D)high-conductivity elastic networks and the dualencapsulated Sb architecture of Ti_(3)C_(2)T_(x) and graphene;these effectively mitigate against volume expansion and the pulverization of Sb,offering good electrolyte penetration and rapid ionic/electronic ***_(3)C_(2)T_(x) also decreases the Kþdiffusion energy barrier,and the ultra-thick compact electrode ensures volumetric and areal *** findings provide a feasible strategy for fabricating ultra-thick,dense alloy-type electrodes to achieve high areal and volumetric capacity energy storage via highly-dense,dual-encapsulated architectures with conductive elastic networks.

关键词： Antimony Dually encapsulated structure Compact monolith Areal capacity Volumetric capacity Potassium-ion batteries

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Origin of the near-room temperature resistance transition in lutetium with H2/N2 gas mixture under high pressure

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National science Review 2024年第7期11卷 26-32页

作者： Di Peng Qiaoshi Zeng Fujun Lan Zhenfang Xing Zhidan Zeng Xiaoxing Ke Yang Ding Ho-kwang Mao Key Laboratory of Materials Physics Institute of Solid State Physics Hefei Institutes of Physical Science(HFIPS)Chinese Academy of Sciences Science Island Branch Graduate School of University of Science and Technology of China Center for High Pressure Science and Technology Advanced Research Shanghai Key Laboratory of Material Frontiers Research in Extreme Environments(MFree) Shanghai Advanced Research in Physical Sciences(SHARPS) State Key Laboratory of Superhard Materials Institute of PhysicsJilin University College of Materials Science&Engineering Beijing University of Technology

The recent report of room-temperature superconductivity at near-ambient pressure in nitrogen-doped lutetium hydride（Lu-H-N） by Dasenbrock-Gammon et al. [Nature 615, 244–250（2023）] has attracted tremendous attention due to its anticipated great impact on technology. However, the results could not be independently reproduced by other groups worldwide in follow-up studies, which elicited intense controversy. Here, we develop a reliable experimental protocol to minimize the extensively concerned extrinsic influences on the sample by starting the reaction from pure lutetium loaded with an H2/N2gas mixture in a diamond anvil cell under different pressures and temperatures and simultaneously monitoring the entire chemical reaction process using in situ four-probe resistance measurements. Therefore, we could repeatedly reproduce the near-room temperature upsurge of electrical resistance at a relatively early stage of the chemical reaction. However, the mechanism is suggested to be a metal-to-semiconductor/insulator transition associated with the structural modulation in the non-stoichiometric Lu-H-N, rather than superconductivity.

关键词： superconductivity high pressure lutetium hydride resistance transition metal-to-semiconductor/insulator transition

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