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work-function-induced interfacial electron redistribution of MoO_(2)/WO_(2) heterostructures for high-efficiency electrocatalytic hydrogen evolution reaction

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Rare Metals 2024年第2期43卷 489-499页

作者： Tong-Fei Li Jing Li Lu-Ping Zhang Jia-Wei Ke Meng-Xing Fan Li-Fang Zhang Cheng-Wei Deng Yi Sun Tao Qian Cheng-Lin Yan School of Chemistry and Chemical Engineering Nantong UniversityNantong226019China Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing210023China Aerospace Hydrogen Energy Technology(Shanghai)Co.Ltd. Shanghai201800China Key Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of EnergySoochow UniversitySuzhou215006China Light Industry Institute of Electrochemical Power Sources Suzhou215006China

The engineering of the electronic configurations of active sites,together with the production of more accessible active sites through heterostructure design,has been established as a forceful methodology for boosting water electrolysis performance.Herein,a facile approach is developed to fabricate well-dispersed MoO_(2) and WO_(2) nanoparticles with abundant heterointerfaces entrapped in N,P-doped carbon nanofibers(referred to as MoO_(2)/WO_(2)@N,P-CNFs hereafter)as hydrogen evolution reaction(HER)electrocatalysts in alkaline and acidic electrolytes.Extensive spectroscopic analyses and theoretical findings manifest that the heterointerface formed by the work function modulation of MoO_(2)/WO_(2) triggers the spontaneous electron redistribution from MoO_(2)to WO_(2) and a built-in electric field,which is essential to promote water adsorption,optimize the H-intermediate adsorption energy,result in the enhanced charge transfer efficiency,and ultimately increase the intrinsic HER activity.Simultaneously,the intimate confinement of MoO_(2)/WO_(2) heterostructures in the porous carbon substrate can restrain the active sites from unfavorable coarsening and detachment,thus ensuring facilitated HER kinetics and outstanding structural robustness.As a result,MoO_(2)/WO_(2)@N,P-CNFs exhibit superior catalytic HER performance in acidic and basic solutions,requiring 118 and 95 mV overpotentials to achieve 10 mA·cm^(−2),respectively,surpassing a number of reported non-noble metal-based electrocatalysts.This work provides guidelines for the rational design and construction of special metallic heterocomponents with optimized interfacial electronic structure for various electrochemical technologies.

关键词： Electrospinning MoO_(2)/WO_(2) heterostructure work function Hydrogen evolution reaction

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Correlation of work function and stacking fault energy through Kelvin probe force microscopy and nanohardness in diluteα-magnesium

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Journal of Magnesium and Alloys 2024年第1期12卷 237-250页

作者： Yigit Türe Ali Arslan Kaya Hüseyin Aydin Jiang Peng Servet Turan Eskisehir Technical University Porsuk Vocational SchoolElectronics and Automation DepartmentProgram of MechatronicsEskisehirTurkey Mugla Sitki Kocman University Engineering FacultyMetallurgy and Materials Engineering DepartmentMuglaTurkey Hüseying Aydın TUBITAK MRCTurkey Jiang Peng Chongqing UniversityChina Eskisehir Technical University Engineering FacultyMaterials Science and Engineering DepartmentEskisehirTurkey

Electronic interactions of the Group 2A elements with magnesium have been studied through the dilute solid solutions in binary Mg-Ca,Mg-Sr and Mg-Ba systems.This investigation incorporated the difference in the‘work function'(ΔWF)measured via Kelvin Probe Force Microscopy(KPFM),as a property directly affected by interatomic bond types,i.***.the electronic structure,nanoindentation measurements,and Stacking Fault Energy values reported in the literature.It was shown that the nano-hardness of the solid-solutionα-Mg phase changed in the order of Mg-Ca>Mg-Sr>Mg-Ba.Thus,it was shown,by also considering the nano-hardness levels,that SFE of a solid-solution is closely correlated with its‘work function'level.Nano-hardness measurements on the eutectics andΔWF difference between eutectic phases enabled an assessment of the relative bond strength and the pertinent electronic structures of the eutectics in the three alloys.Correlation withΔWF and at least qualitative verification of those computed SFE values with some experimental measurement techniques were considered important as those computational methods are based on zero Kelvin degree,relatively simple atomic models and a number of assumptions.As asserted by this investigation,if the results of measurement techniques can be qualitatively correlated with those of the computational methods,it can be possible to evaluate the electronic structures in alloys,starting from binary systems,going to ternary and then multi-elemental systems.Our investigation has shown that such a qualitative correlation is possible.After all,the SFE values are not treated as absolute values but rather become essential in comparative investigations when assessing the influences of alloying elements at a fundamental level,that is,free electron density distributions.Our study indicated that the principles of‘electronic metallurgy'in developing multi-elemental alloy systems can be followed via practical experimental methods,i.e.ΔWF measurements using KPFM and nanoindentation.

关键词： Mg alloys Dilute alloys work function Stacking fault energy Kelvin probe force microscopy Short range order Miedema Nanoindentation Eutectics

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Modulating J-V hysteresis of planar perovskite solar cells and mini-modules via work function engineering

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Journal of Energy Chemistry 2023年第10期85卷 19-29,I0003页

作者： Zenghua Wang Bing Cai Deyu Xin Min Zhang Xiaojia Zheng Institute of Chemical Materials China Academy of Engineering PhysicsMianyang 621900SichuanChina

Commercialization of perovskite solar cells(PSCs) requires the development of high-efficiency devices with none current density-voltage(J-V) hysteresis. Here, electron transport layers(ETLs) with gradual change in work function(WF) are successfully fabricated and employed as an ideal model to investigate the energy barriers, charge transfer and recombination kinetics at ETL/perovskite interface. The energy barrier for electron injection existing at ETL/perovskite is directly assessed by surface photovoltage microscopy, and the results demonstrate the tunable barriers have significant impact on the J-V hysteresis and performance of PSCs. By work function engineering of ETL, PSCs exhibit PCEs over 21% with negligible hysteresis. These results provide a critical understanding of the origin reason for hysteresis effect in planar PSCs, and clear reveal that the J-V hysteresis can be effectively suppressed by carefully tuning the interface features in PSCs. By extending this strategy to a modified formamidinium-cesium-rubidium(FA-Cs-Rb) perovskite system, the PCEs are further boosted to 24.18%. Moreover, 5 cm × 5 cm perovskite mini-modules are also fabricated with an impressive efficiency of 20.07%, demonstrating compatibility and effectiveness of our strategy on upscaled devices.

关键词： J-V hysteresis work function Planar perovskite solar cells Energy barriers Charge transfer kinetics Perovskite solar modules

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Efficient optimization of electron transfer pathway by constructing phosphide/ceria interface boosts seawater hydrogen production

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Journal of Energy Chemistry 2024年第8期95卷 490-498页

作者： Yifan Zhao Lingfeng Yang Youyu Long Min Xi Anran Chen Hua Zhang School of Materials and Energy Yunnan University Electron Microscopy Centre of Yunnan University Yunnan University

Developing efficient and durable hydrogen evolution reaction（HER） electrocatalysts is one of the most important issues for the commercialization of seawater electrolysis,but it remains challenging.Here,we report a CeO2-CoP nanoneedle array catalyst loaded on Ti mesh（CeO2-CoP/TM） with workfunction-induced directional charge transport properties.The CeO2-CoP/TM catalyst showed superior HER catalytic activity and stability,with over potentials of 41 and 60 mV to attain 10 mA cm-2,in 1 M KOH and 1 M KOH+seawater electrolyte,respectively.Experimental results and theoretical calculations reveal that the work function drives the charge transfer from CeO2to CoP,which effectively balances the electronic density of CoP and CeO2,optimizes the d-band center,and accelerates the water activation kinetics,thus enhancing the HER activity.The solar-driven water electrolysis device displays a high and stable solar-to-hydrogen conversion efficiency of 19.6%.This study offers a work function-induced directional charge transport strategy to design efficient and durable catalysts for hydrogen production.

关键词： Charge transport Heterostructure Seawater splitting Solar-to-hydrogen work function

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Bilayer borophene:an efficient catalyst for hydrogen evolution reaction

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Frontiers of Chemical Science and Engineering 2024年第3期18卷 13-23页

作者： Na Xing Nan Gao Panbin Ye Xiaowei Yang Haifeng Wang Jijun Zhao College of Sciences/Xinjiang Production&Construction Corps Key Laboratory of Advanced Energy Storage Materials and Technologies Shihezi UniversityShihezi832000China Key Laboratory of Materials Modification by Laser Ion and Electron Beams(Ministry of Education)Dalian University of TechnologyDalian116024China School of Materials Science and Engineering Taizhou UniversityTaizhou318000China

The electrocatalytic hydrogen evolution reaction is a crucial technique for green hydrogen production.However,finding affordable,stable,and efficient catalyst materials to replace noble metal catalysts remains a significant challenge.Recent experimental breakthroughs in the synthesis of two-dimensional bilayer borophene provide a theoretical framework for exploring their physical and chemical properties.In this study,we systematically considered nine types of bilayer borophenes as potential electrocatalysts for the hydrogen evolution reaction.Our first-principles calculations revealed that bilayer borophenes exhibit high stability and excellent conductivity,possessing a relatively large specific surface area with abundant active sites.Both surface boron atoms and the bridge sites between two boron atoms can serve as active sites,displaying high activity for the hydrogen evolution reaction.Notably,the Gibbs free energy change associated with adsorption for these bilayer borophenes can reach as low as−0.002 eV,and the Tafel reaction energy barriers are lower(0.70 eV)than those on Pt.Moreover,the hydrogen evolution reaction activity of these two-dimensional bilayer borophenes can be described by engineering their work function.Additionally,we considered the effect of pH on hydrogen evolution reaction activity,with significant activity observed in an acidic environment.These theoretical results reveal the excellent catalytic performance of two-dimensional bilayer borophenes and provide crucial guidance for the experimental exploration of multilayer boron for various energy applications.

关键词： bilayer borophene hydrogen evolution reaction work function pH effect

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work function Enhancement of Indium Tin Oxide via Oxygen Plasma Immersion Ion Implantation

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Plasma Science and Technology 2013年第8期15卷 791-793页

作者：高欢忠何龙何志江李泽斌吴忠航成卫海艾畦范晓轩区琼荣梁荣庆 Department of Illuminating Engineering and Light Sources Institute for Electric Light SourcesFudan University

Indium tin oxide （ITO） transparent conducting film was treated with oxygen plasma immersion ion implantation （PIII）. X-ray photoelectron spectroscopy （XPS） was employed to characterize the effect. The results suggested that the oxygen content in the surface was increased and maintained for more than 50 h compared with traditional plasma-treated samples. Meanwhile, the work function of ITO estimated by comparing the peak shift in the XPS diagram suggested a corresponding increase by more than 1 eV.

关键词： plasma immersion ion implantation surface treatment work function indium tin oxide

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work function and Electron Affinity of Semiconductors:Doping Effect and Complication due to Fermi Level Pinning

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Energy & Environmental Materials 2021年第3期4卷 273-276页

作者： Guosheng Shao State Center for International Cooperation on Designer Low-carbon and Environmental Materials Zhengzhou UniversityZhengzhou 450001China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China Zhengzhou Materials Genome Institute XingyangZhengzhou 450100China

Semiconductors are a major category of functional materials essential to various applications to sustain the modern society.Most applied materials or devices utilizing semiconductors are enabled by interfaces or junctions,such as solar cells,electronic/photonic devices,environmental sensors,and redox hetero-catalysts.Herein,the author provides a critical commentary on photoemission measurement of the work function and,more importantly,the electron affinity of semiconductors essential for energy band diagram of heterojunctions.Particular effort is made towards addressing complications associated with Fermi level pinning due to surficial states of doped semiconductors.

关键词： band edges electron affinity Fermi pinning ultraviolet photoelectron spectroscopy work function

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Increasing open circuit voltage by adjusting work function of hole-transporting materials in perovskite solar cells

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Nano Research 2016年第6期9卷 1600-1608页

作者： Weibo Yan Yu Li Senyun Ye Yunlong Li Haixia Rao Zhiwei Liu Shufeng Wang Zuqiang Bian Chunhui Huang State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular Engineering Peking University Beijing 100871 China ing 100871 China

A series of conductive polymers, i.e., poly（3-methylthiophene）（PMT）, poly（thiophene）（PT）, poly（3-bromothiophene）（PBT） and poly（3-chlorothiophene）（PCT）, were prepared via the electrochemical polymerization process. Subse- quently, their application as hole-transporting materials （HTMs） in CHBNI-I3Pb｜3 perovskite solar cells was explored. It was found that rationally increasing the work function of HTMs proves beneficial in improving the open circuit voltage （Voc） of the devices with an ITO/conductive-polymer/CHBNHBPbIg/C60/BCP/Ag structure. In addition, the higher-Voc devices with a higher-work-function HTM exhibited higher recombination resistances. The highest open circuit voltage of 1.04 V was obtained from devices with PCT, with a work function of -5.4 eV, as the hole-transporting layer. Its power conversion efficiency attained a value of approximately 16.5%, with a high fill factor of 0.764, an appreciable open voltage of 1.01 V and a short circuit current density of 21.4 mA.cm-2. This simple, controllable and low-cost manner of preparing HTMs will be beneficial to the production of large-area perovskite solar cells with a hole-transportin~ laver.

关键词： perovskite solar cells electrochemical polymerization hole-transporting materials work function recombination resistance

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Increased work function in PEDOT:PSS film under ultraviolet irradiation

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Chinese Physics B 2014年第3期23卷 630-635页

作者：邢英杰钱旻昉郭等柱张耿民 Key Laboratory for the Physics and Chemistry of Nanodevices and Department of Electronics Peking University

An increase of work function （0.3 eV） is achieved by irradiating poly（3,4-ethylenedioxythiophene）：poly（styrene sul- fonate）（PEDOT：PSS） film in vacuum with 254-nm ultraviolet （UV） light. The mechanism for such an improvement is investigated by photoelectron yield spectroscopy, X-ray photo electron energy spectrum, and field emission technique. Sur- face oxidation and composition change are found as the reasons for work function increase. The UV-treated PEDOT：PSS film is used as the hole injection layer in a hole-only device. Hole injection is improved by UV-treated PEDOT：PSS film without baring the enlargement of film resistance. Our result demonstrates that UV treatment is more suitable for modifying the injection barrier than UV ozone exposure.

关键词： poly（3,4-ethylenedioxythiophene）：poly（styrene sulfonate）（PEDOT：PSS） film work function ul- traviolet hole injection layer

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Effect of Gd doping on the magnetism and work function of Fe_(1-x)Gd_x/Fe(001)

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Chinese Physics B 2014年第5期23卷 433-438页

作者：汤可嵚钟克华程燕铭黄志高 College of Physics and Energy Fujian Normal UniversityFujian Provincial Key Laboratory of Quantum Manipulation and New Energy Materials

The magnetism and work function Ф of Fe1-xGdx/Fe （001） films have been investigated using first-principles methods based on the density functional theory. The calculated results reveal that Gd doping on the Fe （001） surface would greatly affect the geometrical structure of the system. The restruction of the surface atoms leads to the transition of magnetic coupling between Gd and Fe atoms from ferromagnetic （FM） for 0.5 ≤x ≤ 0.75 to antiferromagnetic （AFM） for x = 1.0. For Fe1-xGdx/Fe （001）（x = 0.25, 0.5, 0.75, 1.0）, the charge transfer from Gd to Fe leads to a positive dipole formed on the surface, which is responsible for the decrease of the work function. Moreover, it is found that the magnetic moments of Fe and Gd on the surface layer can be strongly influenced by Gd doping. The changes of the work function and magnetism for Fe1-xGdx/Fe （001） can be explained by the electron transfer, the magnetic coupling interaction between Gd and Fe atoms, and the complex surface restruction. Our work strongly suggests that the doping of the metal with a low work function is a promising way for modulating the work function of the magnetic metal gate.

关键词： first-principles method doping magnetism work function

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