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Sub-2 nm IrO_(2)/Ir nanoclusters with compressive strain and metal vacancies boost water oxidation in acid

Nano Research 2023年第1期16卷 334-342页

作者： Zhijuan Liu Guangjin Wang Jinyu Guo Shuangyin Wang Shuang-Quan Zang Henan key laboratory of Crystalline Molecular functional materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Centerand College of ChemistryZhengzhou UniversityZhengzhou 450001China hunan University State Key Laboratory of Chem/Bio-sensing and ChemometricsCollege of Chemistry and Chemical EngineeringChangsha 410082China School of materials Science and Energy Engineering Foshan UniversityFoshan 528000China

IrO_(2)exhibits good stability but limited electrocatalytic activity for oxygen evolution reaction in acid.Defect engineering is an effective strategy to improve the intrinsic ability of electrocatalysts by tailoring their electronic structure.Herein,we have successfully synthesized IrO_(2)/Ir heterophase with compressive strain and metal vacancies via a simple substitution-etching method.In virtue of the solubility of Cr in strong alkali,metal vacancies could be formed at surface after etching Cr-doped IrO_(2)/Ir in alkali,which leaded to modulated electronic structure.Meanwhile,the substitution of Cr with smaller atom radius would induce the formation of compressive strain and the relocated atoms made the d-band center shifted.With the regulated electronic structure and tuned d-band center,the obtained electrocatalyst only needed 285 mV to reach 10 mA·cm^(−2)in 0.1 M HClO4.Reaction kinetic has been rapidly accelerated as indicated by the smaller Tafel slope and charge transfer resistance.Theoretical calculations revealed that the d-band center and charge density distribution have been regulated with the introduction of defects in IrO_(2)/Ir,which significantly decreased the free energy barrier of rate determining step.This work provides a valuable reference to design effective and defects-rich electrocatalysts.

关键词： IrO_(2)/Ir nanoclusters compressive strain metal vacancies d-band center water oxidation in acid

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Polarization-Dependent Optical Properties and Optoelectronic Devices of 2D materials

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Research 2020年第1期2020卷 848-882页

作者： Ziwei Li Boyi Xu Delang Liang Anlian Pan key laboratory for Micro-Nano Physics and Technology of hunan province College of Materials and EngineeringHunan UniversityChangshaHunan 410082China

The development of optoelectronic devices requires breakthroughs in new material systems and novel device mechanisms,and the demand recently changes from the detection of signal intensity and responsivity to the exploration of sensitivity of polarized state information.Two-dimensional(2D)materials are a rich family exhibiting diverse physical and electronic properties for polarization device applications,including anisotropic materials,valleytronic materials,and other hybrid heterostructures.In this review,we first review the polarized-light-dependent physical mechanism in 2D materials,then present detailed descriptions in optical and optoelectronic properties,involving Raman shift,optical absorption,and light emission and functional optoelectronic devices.Finally,a comment is made on future developments and challenges.The plethora of 2D materials and their heterostructures offers the promise of polarization-dependent scientific discovery and optoelectronic device application.

关键词： optoelectronic polarization polarized

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Interfacial adsorption-insertion mechanism induced by phase boundary toward better aqueous Zn-ion battery

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InfoMat 2021年第9期3卷 1028-1036页

作者： Lutong Shan Yiren Wang Shuquan Liang Boya Tang Yongqiang Yang Ziqing Wang Bingan Lu Jiang Zhou School of materials Science and Engineering Central South UniversityKey Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceChangshaHunanPeople's Republic of China Department of Chemistry University of ManchesterManchesterUK School of Physics and electronics Hunan UniversityChangshaPeople's Republic of China

Biphasic and multiphasic compounds have been well clarified to achieve extraordinary electrochemical properties as advanced energy storage materials.Yet the role of phase boundaries in improving the performance is remained to be illustrated.Herein,we reported the biphasic vanadate,that is,Na_(1.2)V_(3)O_(8)/K_(2)V_(6)O_(16)·1.5H_(2)O(designated as Na0.5K0.5VO),and detected the novel interfacial adsorption-insertion mechanism induced by phase boundaries.Firstprinciples calculations indicated that large amount of Zn^(2+)and H^(+)ions would be absorbed by the phase boundaries and most of them would insert into the host structure,which not only promote the specific capacity,but also effectively reduce diffusion energy barrier toward faster reaction kinetics.Driven by this advanced interfacial adsorption-insertion mechanism,the aqueous Zn/Na_(0.5)K_(0.5)VO is able to perform excellent rate capability as well as long-term cycling performance.A stable capacity of 267 mA h g^(-1)after 800 cycles at 5 A g^(-1)can be achieved.The discovery of this mechanism is beneficial to understand the performance enhancement mechanism of biphasic and multiphasic compounds as well as pave pathway for the strategic design of highperformance energy storage materials.

关键词： aqueous zinc-ion battery cathode energy storage mechanism phase boundary vanadiumbased materials

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Tailoring the electronic acceptor–donor heterointerface between black phosphorus and Co_(3)O_(4) for boosting oxygen bifunctional electrocatalysis

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Chinese Chemical Letters 2023年第2期34卷 284-289页

作者： Jing Zou Yilun Zou Haitao Wang Wei Wang Pingxiu Wu Arramel Jizhou Jiang Xin Li School of Chemistry and Environmental Engineering School of Environmental Ecology and Biological EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Tree Gorges LaboratoryWuhan Institute of TechnologyWuhan 430205China key laboratory of Rare Mineral Ministry of Natural ResourcesGeological Experimental Testing Center of Hubei ProvinceWuhan 430034China key laboratory of hunan province for advanced Carbon-based functional materials Hunan Institute of Science and TechnologyYueyang 414006China Semiconductor electronic Special Gas of Hubei Engineering Research Center Jingzhou 434000China Nano Center Indonesia Jl.PUSPIPTEK Tangerang SelatanBanten 15314Indonesia Institute of Biomass Engineering Key Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642China

Black phosphorus (BP) as an uprising two-dimensional material exhibits attractive potential in the field of electrocatalysis due to the inherent advantages of high carrier mobility and abundant lone pair electrons.However,the exposed active electrons compel BP to be deactivated by oxidative degradation.Herein,the electronic signature of acceptor-donor heterointerfacial interactions between BP and Co_(3)O_(4)is realized via wet ball milling.The preferential migration of active electrons from BP to Co_(3)O_(4)is achieved at the heterointerface since the Fermi level of BP is higher than that of Co_(3)O_(4).Such relative energetic consideration promotes reasonable oxygen electrocatalytic active sites.Moreover,it significantly suppresses the oxidative degradation of BP.Consequently,the resulting Co_(3)O_(4)/BP heterojunction possesses superior oxygen bifunctional electrocatalytic activity than its parent catalysts.Most importantly,this work promotes an efficient route towards BP-based multifunctional catalysts.

关键词： electronic acceptor-donor Black phosphorus Co_(3)O_(4) Charge transfer Oxygen bifunctional electrocatalysis

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Ultrafast probing of plasma ion temperature in proton–boron fusion by nuclear resonance fluorescence emission spectroscopy

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Matter and Radiation at Extremes 2022年第3期7卷 1-9页

作者： T.-T.Qin W.Luo H.-Y.Lan W.-M.Wang School of Nuclear Science and Technology University of South ChinaHengyang 421001China Beijing key laboratory of Opto-electronic functional materials and Micro-nano Devices and Department of Physics Renmin University of ChinaBeijing 100872China

ABSTRACT Aneutronic fusion reactions such as proton-boron fusion could efficiently produce clean energy with quite low neutron doses.However,as a consequence,conventional neutron spectral methods for diagnosing plasma ion temperature would no longer work.Therefore,finding a way to probe the ion temperature in aneutronic fusion plasmas is a crucial task.Here,we present a method to realize ultrafast in situ probing of^(11)B ion temperature for proton-boron fusion by Doppler broadening of the nuclear resonance fluorescence(NRF)emission spectrum.The NRF emission is excited by a collimated,intenseγ-ray beam generated from submicrometer wires irradiated by a recently available petawatt(PW)laser pulse,where theγ-ray beam generation is calculated by three-dimensional particle-in-cell simulation.When the laser power is higher than 1 PW,five NRF signatures of a^(11)B plasma can be clearly identified with high-resolutionγ-ray detectors,as shown by our Geant4 simulations.The correlation between the NRF peak width and^(11)B ion temperature is discussed,and it is found that NRF emission spectroscopy should be sensitive to 11B ion temperatures T_(i)>2.4 keV.This probing method can also be extended to other neutron-free-fusion isotopes,such as^(6)Li and^(15)N.

关键词： spectrum boron spectroscopy

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How to Extend the Bridge Density functional Approximation to the Confined Non-hard Sphere Fluid

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Chinese Journal of Chemical Physics 2006年第4期19卷 319-324页

作者： Shi-qi Zhou key laboratory of Green packaging and Biological Nanotechnolog of hunan province and Institute of Modern Statistical Mechanics Hunan University of Technology Zhuzhou 412008 China

一个理论方法被建议扩大桥密度为到不一致的 Lennard-Jones (LJ ) 液体的不一致的难范围液体的功能的近似(BDFA ) 。为 LJ 液体的 DFT 途径简单，在大量共存阶段精确的份量上和外部地参数。特别， DFT 途径仅仅直接需要第二份订单是的... 详细信息

一个理论方法被建议扩大桥密度为到不一致的 Lennard-Jones (LJ ) 液体的不一致的难范围液体的功能的近似(BDFA ) 。为 LJ 液体的 DFT 途径简单，在大量共存阶段精确的份量上和外部地参数。特别， DFT 途径仅仅直接需要第二份订单是的共存体积液体的关联功能(DCF ) 输入，并且对 subcritical 温度区域因此适用。现在的理论方法能被认为是热力学的不安理论，它不在免费精力的水平，但是在 2000the 秒顺序 DCF 的水平在是的一个不一致的对应物。

关键词：密度泛函理论桥密度泛函近似硬球流体相关函数

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Metal-center effect induced efficient charge transfer of metal-organic framework for strengthening Sb(Ⅴ)capture performance

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Nano Research 2022年第9期15卷 8516-8523页

作者： Deng You Hui Shi Mingming Peng Liming Yang Penghui Shao Kai Yin Haozhi Wang Shenglian Luo Xubiao Luo State key laboratory of Chemo/Biosensing and Chemometrics Hunan UniversityChangsha 410082China key laboratory of Jiangxi province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong UniversityNanchang 330063China National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource utilization Nanchang Hangkong UniversityNanchang 330063China key laboratory of advanced Ceramics and Machining Technology(Ministry of Education) School of Materials Science and EngineeringTianjin UniversityTianjin 300072China

The adsorbents–adsorbates interaction is critical for resourcelization in heavy metal wastewater treatment.Nevertheless,it is still indistinct to depict the impact of metal center effect on heavy metals removal performance in metal-organic frameworks(MOFs)-based adsorbents.Herein,a series of MOFs with different metal centers of Mg(II),La(III),and Zr(IV)are rationally designed,and the effect of electronic structure on the Sb(V)removal performance is systematically investigated.The obtained La-MGs achieve Sb(V)adsorption capacity of 897.6 mg/g,which is about 1.2 and 4.5 times above average than those of Zr-MGs and Mg-MGs,respectively.On account of more edge adsorption sites achieve,the sites utilization efficiency of La-MGs(92.1%)is much better than Zr-MGs(75.0%)and Mg-MGs(20.4%).Furthermore,density functional theory(DFT)calculations reveal that La-MGs are more active than Mg-MGs and Zr-MGs,owing to the lower adsorption energy,higher charge transfer,and stronger bonding interaction,which will promote the Sb(V)removal performance.The experimental results in practical water indicate that La-MGs effectively capture antimony at low concentration,reaching drinking water standard in samples from Ganjiang River.This study opens an avenue for atomic-level insight into high-efficient absorbents design for water treatment from electronic structuremodification of active centers.

关键词： metal-organic frameworks metal center effect electronic structure theoretical calculation Sb(V)removal

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Flexible and free-standing La_(0.33)Ti_(2)(PO_(4))_(3)/C nanofibers film as a novel high-performance anode for sodium-and potassium-ion batteries

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Rare Metals 2023年第10期42卷 3387-3398页

作者： Jing Dai Jian Jing Jian-Ping Yang Wen Zhang Shao-Xiong Liu Qian-Fu Wang Jia-Xing Wen Hai Hu Hui-Fang Li Li Liu National Base for International Science&Technology Cooperation National Local Joint Engineering Laboratory for Key Materials of New Energy Storage BatteryKey Laboratory of Environmentally Friendly Chemistry and Applications of Ministry of EducationHunan Province Key Laboratory of Electrochemical Energy Storage and ConversionSchool of ChemistryXiangtan UniversityXiangtan411105China College of Electromechanical Engineering Shandong Engineering Laboratory for Preparation and Application of High-Performance Carbon-MaterialsQingdao University of Science&TechnologyQingdao266061China

Na superionic conductor(NASICON)-type La_(0.33)Ti_(2)(PO_(4))_(3)(LaTP) is firstly proposed as sodium/potassium storage materials.The density functional theory(DFT) calculations show that LaTP has good electronic character and low Na^(+)/K^(+)migration barriers.The flexible La_(0.33)Ti_(2)(PO_(4))_(3)/C nanofiber film is synthesized via electrostatic spinning and investigated as free-standing electrode applied to sodium-ion batteries(SIBs) and potassiumion batteries(PIBs) in this work.The low band gap and Na^(+)/K^(+) migration barriers of LaTP,unique morphology,and complete conductive carbon net allow the La_(0.33)Ti_(2)(PO_(4))_(3)/C nanofibers film to deliver high capacity(296.3 mAh·g^(-1) for SIBs and 235.8 mAh·g^(-1) for PIBs),excellent rate performance(142.5 mAh·g^(-1) for SIBs and50.5 mAh·g^(-1) for PIBs at 1.00 A·g^(-1)),and superior cyclability above 1000 cycles.The full-cell tests show that the material has a good application prospect,indicating a promising flexible anode material for SIBs and PIBs.

关键词： Potassium-ion batteries(PIBs) Sodium-ion batteries(SIBs) Flexible La_(0.33)Ti_(2)(PO_(4))_(3)/C nanofibers film The first-principles calculations Migration potential energy

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Binuclear Ruthenium Complexes with Benzo[1,2-b;4,5-b＇]- dithiophene Analogues as Bridge Ligands： Syntheses, Characterization and Notable Difference on electronic Coupling

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Chinese Journal of Chemistry 2017年第7期35卷 1170-1178页

作者： Ya-Ping Ou Shunlin Tang Aihui Wang Junhua Li Fuxing Zhang Zhifeng Xu College of Chemistry and Material Science Hengyang Normal University key laboratory of functional Organo-metallic materials of Hengyang Normal University College of Hunan ProvinceHengyangHunan 421008China

Diruthenium ethynyl complexes 1--3 （1： 1,5-dithia-s-indacene-4,8-dione; 2： 4,8-diethoxybenzo[1,2-b：4,5- b＇]dithiophene; 3： 4,8-didodecyloxybenzo[1,2-b：4,5-b＇]dithiophene） have been synthesized by incorporating the re- spective conjugated heterocyclic spacer and characterized by NMR and elemental analysis. The effects of bridge ligands＇ properties on electronic coupling between redox-active ruthenium terminal groups were investigated by electrochemistry, UV/vis/near-IR and IR spectroelectrochemistry combined with density functional theory （DFT） and time-dependent DFT calculations. Electrochemistry results indicated that complexes 1--3 exhibit two fully re- versible oxidation waves, and complexes 2 and 3 with electron-rich and π-conjuagted bridge ligands are character- ized by excellent electrochemical properties. Furthermore, the larger v（C≡C） separation from the IR spectroelec- trochemical results of 2 and 3 and the intense NIR absorption features of singly oxidized species 2＋ and 3＋ re- vealed that their molecular skeletons have superior abilities to delocalize the positive charge. The spin density dis- tribution from DFT calculations proved the conclusions of this study.

关键词： bridge ligands ruthenium terminal groups spectroelectrochemistry electronic coupling

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Self-Exfoliation of Flake Graphite for Bioinspired Compositing with Aramid Nanofiber toward Integration of Mechanical and Thermoconductive Properties

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Nano-Micro Letters 2022年第10期14卷 235-247页

作者： Limei Huang Guang Xiao Yunjing Wang Hao Li Yahong Zhou Lei Jiang Jianfeng Wang College of materials Science and Engineering Hunan UniversityChangsha 410082People’s Republic of China College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082People’s Republic of China CAS key laboratory of Bio-Inspired materials and Interface Sciences Technical Institute of Physics and Chemistry ChineseAcademy of SciencesBeijing 100190People’s Republic of China

Flexible yet highly thermoconductive materials are essential for the development of next-generation flexible electronic devices.Herein,we report a bioinspired nanostructured film with the integration of large ductility and high thermal conductivity based on self-exfoliated pristine graphene and three-dimensional aramid nanofiber network.A self-grinding strategy to directly exfoliate flake graphite into few-layer and few-defect pristine graphene is successfully developed through mutual shear friction between graphite particles,generating largely enhanced yield and productivity in comparison to normal liquid-based exfoliation strategies,such as ultrasonication,high-shear mixing and ball milling.Inspired by nacre,a new bioinspired layered structural design model containing three-dimensional nanofiber network is proposed and implemented with an interconnected aramid nanofiber network and high-loading graphene nanosheets by a developed continuous assembly strategy of sol-gel-film transformation.It is revealed that the bioinspired film not only exhibits nacre-like ductile deformation behavior by releasing the hidden length of curved aramid nanofibers,but also possesses good thermal transport ability by directionally conducting heat along pristine graphene nanosheets.

关键词： Graphene Aramid nanofiber Self-grinding exfoliation Bioinspired structure functional material

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