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Negative enthalpy alloys and local chemical ordering:a concept and route leading to synergy of strength and ductility

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National science Review 2024年第4期11卷 172-184页

作者： Zibing An Tao Yang Caijuan Shi Shengcheng Mao Lihua Wang Ang Li Wei Li Xianmeng Xue Ming Sun Yifan Bai Yapeng He Fuzeng Ren Zhouguang Lu Ming Yan Yang Ren Chain-Tsuan Liu Ze Zhang Xiaodong Han Beijing Key Lab of Microstructure and Property of Advanced materials College of Materials Science &Engineering Beijing University of Technology department of materials science and engineering City University of Hong Kong Key Laboratory of Partial Acceleration Physics& Technology Institute of High Energy PhysicsChinese Academy of Sciences department of materials science &engineering Southern University of Science and Technology department of Physics City University of Hong Kong State Key Laboratory of Silicon materials Department of Materials Science and Engineering Zhejiang University

Solid solutions are ubiquitous in metals and alloys. Local chemical ordering(LCO) is a fundamental sub-nano/nanoscale process that occurs in many solid solutions and can be used as a microstructure to optimize strength and ductility. However, the formation of LCO has not been fully elucidated, let alone how to provide efficient routes for designing LCO to achieve synergistic effects on both superb strength and ductility. Herein, we propose the formation and control of LCO in negative enthalpy alloys. With engineering negative enthalpy in solid solutions, genetic LCO components are formed in negative enthalpy refractory high-entropy alloys(RHEAs). In contrast to conventional ‘trial-and-error' approaches, the control of LCO by using engineering negative enthalpy in RHEAs is instructive and results in superior strength(1160 MPa) and uniform ductility(24.5%) under tension at ambient temperature, which are among the best reported so far. LCO can promote dislocation cross-slip, enhancing the interaction between dislocations and their accumulation at large tensile strains; sustainable strain hardening can thereby be attained to ensure high ductility of the alloy. This work paves the way for new research fields on negative enthalpy solid solutions and alloys for the synergy of strength and ductility as well as new functions.

关键词： negative enthalpy alloys local chemical ordering strength ductility dislocation

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The dynamic surface evolution of halide perovskites induced by external energy stimulation

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National science Review 2024年第4期11卷 185-194页

作者： Feiyu Cheng Pengdong Wang Chenzhe Xu Qingliang Liao Suicai Zhang Haochun Sun Wenqiang Fan Guodong Liu Zhiyun Li Yaping Kong Li Wang Fangsen Li Zhuo Kang Yue Zhang Academy for Advanced Interdisciplinary science and Technology State Key Laboratory for Advanced Metals and Materials University of Science and Technology Beijing Beijing Key Laboratory for Advanced Energy materials and Technologies Key Laboratory of Advanced Materials and Devices for Post-Moore ChipsMinistry of EducationBeijing Advanced Innovation Center for Materials Genome Engineering School of Materials Science and EngineeringUniversity of Science and Technology Beijing Vacuum Interconnected nanotech Workstation(nano-X) Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of Sciences Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences

Tracking the dynamic surface evolution of metal halide perovskite is crucial for understanding the corresponding fundamental principles of photoelectric properties and intrinsic instability. However, due to the volatility elements and soft lattice nature of perovskites, several important dynamic behaviors remain unclear. Here, an ultra-high vacuum（UHV） interconnection system integrated by surface-sensitive probing techniques has been developed to investigate the freshly cleaved surface of CH3NH3PbBr3in situ under given energy stimulation. On this basis, the detailed three-step chemical decomposition pathway of perovskites has been clarified. Meanwhile, the evolution of crystal structure from cubic phase to tetragonal phase on the perovskite surface has been revealed under energy stimulation. Accompanied by chemical composition and crystal structure evolution, electronic structure changes including energy level position,hole effective mass, and Rashba splitting have also been accurately determined. These findings provide a clear perspective on the physical origin of optoelectronic properties and the decomposition mechanism of perovskites.

关键词： metal halide perovskite external energy stimulation surface dynamic evolution surface electronic structure ultra-high vacuum interconnection system

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Weakly Polarized Organic Cation-Modified Hydrated Vanadium Oxides for High-Energy Efficiency Aqueous Zinc-Ion Batteries

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nano-Micro Letters 2024年第7期16卷 169-186页

作者： Xiaoxiao Jia Chaofeng Liu Zhi Wang Di Huang Guozhong Cao department of materials science and engineering University of WashingtonSeattleWA 98195USA School of materials science and engineering Tongji UniversityShanghai 201804People’s Republic of China

Vanadium oxides,par-ticularly hydrated forms like V_(2)O_(5)·nH_(2)O(VOH),stand out as promising cathode candidates for aqueous zinc ion batteries due to their adjustable layered structure,unique electronic characteristics,and high theoretical capacities.However,challenges such as vanadium dissolution,sluggish Zn^(2+)diffusion kinetics,and low operating voltage still hinder their direct application.In this study,we present a novel vanadium oxide([C_(6)H_(6)N(CH_(3))_(3)]_(1.08)V_(8)O_(20)·0.06H_(2)O,TMPA-VOH),developed by pre-inserting trimethylphenylammonium(TMPA+)cations into VOH.The incorporation of weakly polarized organic cations capitalizes on both ionic pre-intercalation and molecular pre-intercalation effects,resulting in a phase and morphology transition,an expansion of the interlayer distance,extrusion of weakly bonded interlayer water,and a substantial increase in V^(4+)content.These modifications synergistically reduce the electrostatic interactions between Zn^(2+)and the V-O lattice,enhancing structural stability and reaction kinetics during cycling.As a result,TMPA-VOH achieves an elevated open circuit voltage and operation voltage,exhibits a large specific capacity(451 mAh g^(-1)at 0.1 A g^(-1))coupled with high energy efficiency(89%),the significantly-reduced battery polarization,and outstanding rate capability and cycling stability.The concept introduced in this study holds great promise for the development of high-performance oxide-based energy storage materials.

关键词： Zinc-ion battery Vanadium oxide V_(2)O_(5)·nH_(2)O Pre-intercalation Interlayer engineering

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nanoparticle Exsolution on Perovskite Oxides:Insights into Mechanism,Characteristics and Novel Strategies

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nano-Micro Letters 2024年第2期16卷 312-346页

作者： Yo Han Kim Hyeongwon Jeong Bo‑Ram Won Hyejin Jeon Chan‑ho Park Dayoung Park Yeeun Kim Somi Lee Jae‑ha Myung department of materials science and engineering Incheon National UniversityIncheon 22012Republic of Korea

Supported nanoparticles have attracted considerable attention as a promising catalyst for achieving unique properties in numerous applications,including fuel cells,chemical conversion,and batteries.nanocatalysts demonstrate high activity by expanding the number of active sites,but they also intensify deactivation issues,such as agglomeration and poisoning,simultaneously.Exsolution for bottomup synthesis of supported nanoparticles has emerged as a breakthrough technique to overcome limitations associated with conventional nanomaterials.nanoparticles are uniformly exsolved from perovskite oxide supports and socketed into the oxide support by a one-step reduction process.Their uniformity and stability,resulting from the socketed structure,play a crucial role in the development of novel nanocatalysts.Recently,tremendous research efforts have been dedicated to further controlling exsolution particles.To effectively address exsolution at a more precise level,understanding the underlying mechanism is essential.This review presents a comprehensive overview of the exsolution mechanism,with a focus on its driving force,processes,properties,and synergetic strategies,as well as new pathways for optimizing nanocatalysts in diverse applications.

关键词： Supported nanoparticle Exsolution In situ growth Mechanism Perovskite oxide Catalyst

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Organic near-infrared optoelectronic materials and devices:an overview

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Advanced Photonics 2024年第1期6卷 17-42页

作者： Zong-Lu Che Chang-Cun Yan Xue-Dong Wang Liang-Sheng Liao Soochow University Institute of Functional Nano and Soft Materials(FUNSOM)Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSuzhouChina Soochow University College of ChemistryChemical Engineering and Materials ScienceJiangsu Engineering Laboratory of Novel Functional Polymeric MaterialsSuzhouChina Macao University of science and Technology Macao Institute of Materials Science and EngineeringMacaoChina

Near-infrared(NIR)light has shown great potential for military and civilian applications owing to its advantages in the composition of sunlight,invisibility to human eyes,deeper penetration into biological tissues,and low optical loss in optical fibers.Therefore,organic optoelectronic materials that can absorb or emit NIR light have aroused great scientific interest in basic science and practical applications.Based on these NIR organic optoelectronic materials,NIR optoelectronic devices have been greatly improved in performance and application.In this review,the representative NIR organic optoelectronic materials used in organic solar cells,organic photodetectors,organic light-emitting diodes,organic lasers,and organic optical waveguide devices are briefly introduced,and the potential applications of each kind of device are briefly summarized.Finally,we summarize and take up the development of NIR organic optoelectronic materials and devices.

关键词： near-infrared organic optoelectronic materials organic solar cells organic light-emitting devices organic optical waveguides

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On-surface synthesis and characterization of polyynic carbon chains

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National science Review 2024年第3期11卷 192-199页

作者： Wenze Gao Wei Zheng Luye Sun Faming Kang Zheng Zhou Wei Xu Interdisciplinary materials Research Center School of Materials Science and Engineering Tongji University

Carbyne, an elusive sp-hybridized linear carbon allotrope, has fascinated chemists and physicists for decades. Due to its high chemical reactivity and extreme instability, carbyne was much less explored in contrast to the sp2-hybridized carbon allotropes such as graphene. Herein, we report the on-surface synthesis of polyynic carbon chains by demetallization of organometallic polyynes on the Au（111） surface;the longest one observed consists of ～60 alkyne units（120 carbon atoms）. The polyynic structure of carbon chains with alternating triple and single bonds was unambiguously revealed by bond-resolved atomic force microscopy. Moreover, an atomically precise polyyne, C14, was successfully produced via tip-induced dehalogenation and ring-opening of the decachloroanthracene molecule(C14Cl10) on a bilayer NaCl/Au（111） surface at 4.7 K, and a band gap of 5.8 eV was measured by scanning tunnelling spectroscopy,in a good agreement with the theoretical HOMO–LUMO gap（5.48 eV）.

关键词： polyyne scanning probe microscopy carbon allotrope on-surface synthesis organometallic polyyne

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3D printed silicon-based micro-lattices with ultrahigh areal/gravimetric capacities and robust structural stability for lithium-ion batteries

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nano Research 2024年第4期17卷 2693-2703页

作者： Jie Fu Dong Wang Yan Li Xianzheng Liu Rui Zhang Zhiyuan Liu Pengdong Liu Lijuan Zhang Xuefei Li Guangwu Wen School of materials science and engineering Shandong University of TechnologyZibo 255000China Shandong Si-nano materials Technology Co. Ltd.Zibo 255000China

nanostructured silicon anodes have shown extraordinary lithium storage properties for lithium-ion batteries(LIBs)but are usually achieved at low areal loadings(<1.5 mg·cm^(-2))with low areal capacity.Sustaining sound... 详细信息

nanostructured silicon anodes have shown extraordinary lithium storage properties for lithium-ion batteries(LIBs)but are usually achieved at low areal loadings(nanotube(3D-Si/G/C)electrode for simultaneously achieving ultrahigh areal/gravimetric capacities at high mass loading.The periodically arranged vertical channels and hierarchically porous filaments facilitate sufficient electrolyte infiltration and rapid ion diffusion,and the carbonaceous network provides excellent electron transport properties and mechanical integrity,thus endowing the printed 3D-Si/G/C electrode with fast electrochemical reaction kinetics and reversibility at high mass loading.Consequently,the 3D-Si/G/C with high areal mass loading of 12.9 mg·cm^(-2) exhibits excellent areal capacity of 12.8 mAh·cm^(-2) and specific capacity of 1007 mAh·g^(-1),respectively.In-situ optical microscope and ex-situ scanning electron microscope(SEM)confirm that the hierarchically porous filaments with interconnected carbon skeletons effectively suppress the volume change of silicon and maintain stable micro-lattice architecture.A 3D printed 3D-Si/G/C-1||3D-LiFePO_(4)/G full cell holds excellent cyclic stability(capacity retention rate of 78%after 50 cycles)with an initial Coulombic efficiency(ICE)of 96%.This work validates the feasibility of 3D printing on constructing high mass loading silicon anode for practical high energy-density LIBs.

关键词： silicon anode areal capacity three-dimensional(3D)printing lithium-ion batteries

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Sequential reactant water management by complementary multisite catalysts for surpassing platinum hydrogen evolution activity

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nano Research 2024年第3期17卷 1232-1241页

作者： Yu Lin Defang Ding Shicheng Zhu Qunlei Wen Huangjingwei Li Zhen Li Youwen Liu Yi Shen China engineering Research Center of nano-Geomaterials of Ministry of Education Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China State Key Laboratory of materials Processing and Die&Mould Technology and School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Alkaline hydrogen evolution reaction(HER)offers a near-zero-emission approach to advance hydrogen energy.However,the activity limited by the multiple reaction steps involving H_(2)O molecules transfer,absorption,and activation still unqualified the thresholds of economic viability.Herein,we proposed a multisite complementary strategy that incorporates hydrophilic Mo and electrophilic V into Ni-based catalysts to divide the distinct steps on atomically dispersive sites and thus realize sequential regulation of the HER process.The Isotopic labeled in situ Raman spectroscopy describes 4-coordinated hydrogen bonded H_(2)O to be free H_(2)O passing the inner Helmholtz plane in the vicinity of the catalysts under the action of hydrophilic Mo sites.Furthermore,potential-dependent electrochemical impedance spectroscopy(EIS)reveals that electrophilic V sites with abundant 3d empty orbitals could activate the lone-pair electrons in the free H_(2)O molecules to produce more protic hydrogen,and dimerize into H_(2) at the Ni sites.By the sequential management of reactive H_(2)O molecules,NiMoV oxides multisite catalysts surpass Pt/C hydrogen evolution activity(49 mV@10 mA∙cm^(-2) over 140 h).Profoundly,this study provides a tangible model to deepen the comprehension of the catalyst–electrolyte interface and create efficient catalysts for diverse reactions.

关键词： hydrogen evolution activity complementary multisite catalysts sequential reactive water management interfacial water molecules

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Graphene from microwave-initiated upcycling of waste polyethylene for electrocatalytic reduction of chloramphenicol

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Chinese Chemical Letters 2024年第4期35卷 187-192页

作者： Qiang Cao Xue-Feng Cheng Jia Wang Chang Zhou Liu-Jun Yang Guan Wang Dong-Yun Chen Jing-Hui He Jian-Mei Lu College of Chemistry Chemical Engineering and Materials ScienceCollaborative Innovation Center of Suzhou Nano Science and TechnologySoochow UniversitySuzhou 215123China

Waste polyolefin plastics, accounting for 50% of all plastic waste, represent a tremendously unexploited carbon source. Efficiently upcycling polyolefin waste into value-added carbon materials for waste water treatment avoiding using noble metals is challenging but economically and environmentally sustainable. In this work, MAX-Ti_(3)AlC_(2) supported Fe selectively catalyzes polyolefin into few-layered graphene in 5 min under microwave treatment. Graphene and MAX supported Fe(Fe@MLC) can completely(99.9%)degrade chloramphenicol(CAP) within 60 min, retain robust after 10 cycles and work efficiently at a wide p H range(3.87–13.03), avoiding the usage of noble metal. Moreover, the electrochemical active surface area(ECSA) of Fe@MLC is 2.7 times higher than that of commercial Pt/C. This work provides a cheap and efficient catalyst that promotes deconstruction of plastic wastes and indirectly degrades antibiotics thereby realizes the treatment of waste water with waste plastic.

关键词： Microwave Ti_(3)AlC_(2) Electrochemistry Dechlorination Chloramphenicol

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Carbon cathode with heteroatom doping and ultrahigh surface area enabling enhanced capacitive behavior for potassium-ion hybrid capacitors

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Rare Metals 2024年第5期43卷 2136-2149页

作者： Yan Xiong Ya-Fei Zhang Chun-Liu Zhu Lei Yang Huan-Yu Liang Jing Shi Jing-Wei Chen Wei-Qian Tian Shuai Liu Zhi Li Jing-Yi Wu Huan-Lei Wang School of materials science and engineering Ocean University of China department of Chemical and materials engineering University of Alberta

Potassium-ion hybrid capacitors （PIHCs） are widely regarded as highly promising energy storage devices,due to their exceptional energy density,impressive power density,and abundant potassium resources.Unfortunately,restricted by the inherent capacitive storage mechanism,the carbon cathodes possess a much lower specific capacity than battery-type anodes.Therefore designing high-performance carbon cathodes is extremely urgent for the development of PIHCs.Herein,N,O codoped porous carbon （NOPC） was fabricated through the NaCl hard template method and combined KOH/melamine chemical activation technique,displaying the characteristics of abundant N/O content （4.7 at%/16.9 at%）,ultrahigh specific surface area (3092 m2·g-1) and hierarchical pore network.The designed NOPC cathode delivers a high specific capacity (164.4 mAh·g-1at 0.05 A·g-1) and superior cyclability (95.1%retention ratio at 2 A·g-1over2500 cycles).Notably,the adjustable ratio of micropores to mesopores facilitates the achievement of the optimal balance between capacity and rate capability.Moreover,the pseudocapacitance can be further augmented through the incorporation of N/O functional groups.As expected,the graphite//NOPC based PIHC possesses a high energy density of 113 Wh·kg-1at 747 W·kg-1and excellen capacity retention of 84.4%after 4000 cycles at 1.0 A·g-1This work introduces a novel strategy for designing carbon cathodes that enhances the electrochemical performance of PIHCs.

关键词： Template method N/O co-doping High specific surface area Carbon cathode Potassium-ion capacitors

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