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heterointerface engineering of rhombic Rh nanosheets confined on MXene for efficient methanol oxidation

Journal of Energy Chemistry 2024年第6期93卷 419-428,I0011页

作者： Qi Zhang Quanguo Jiang Xiang Yang Chi Zhang Jian Zhang Lu Yang Haiyan He Guobing Ying Huajie Huang College of Materials Science and Engineering Hohai UniversityNanjing 210098JiangsuChina New Energy Technology Engineering Lab of Jiangsu Province College of ScienceNanjing University of Posts&Telecommunications(NUPT)Nanjing 210023JiangsuChina School of Materials Science and Engineering Southeast UniversityNanjing 211100JiangsuChina

Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix largely limits the overall electrocatalytic performance due to their insufficient cooperative effects.Herein,we report a controllable and robust heterointerface engineering strategy for the bottom-up fabrication of rhombic Rh nanosheets in situ confined on Ti_3C_(2)T_x MXene nanolamellas(Rh NS/MXene)via a convenient stereoassembly process.This unique design concept gives the resulting 2D/2D Rh NS/MXene heterostructure intriguing textural features,including large accessible surface areas,strong"face-toface"interfacial interactions,homogeneous Rh nanosheet distribution,ameliorative electronic structure,and high electronic conductivity.As a consequence,the as-prepared Rh NS/MXene nanoarchitectures exhibit exceptional electrocatalytic methanol oxidation properties in terms of a large electrochemically active surface area of 126.2 m~2 g_(Rh)~(-1),a high mass activity of 1056.9 mA mg_(Rh)-~1,and a long service life,which significantly outperform those of conventional particle-shaped Rh catalysts supported by carbon black,carbon nanotubes,reduced graphene oxide,and MXene matrixes as well as the commercial Pt nanoparticle/carbon black and Pd nanoparticle/carbon black catalysts with the same noble metal loading amount.Density functional theory calculations further demonstrate that the direct electronic interaction at the well-contacted 2D/2D heterointerfaces effectively enhances the adsorption energy of Rh nanosheets and induces a left shift of the d-band center,thereby making the Rh NS/MXene configuration suffer less from CO poisoning.This work highlights the importance of rational heterointerface design in the construction of advanced noble metal/MXene electrocatalysts,which may provide new avenues for developing the next-generation DMFC devices.

关键词： Rhodium nanosheet Ti_(3)C_(2)T_(x)MXene heterointerface Electrocatalyst Fuel cell

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In-situ transformed Mott-Schottky heterointerface in silver/manganese oxide nanorods boosting oxygen reduction,oxygen evolution,and hydrogen evolution reactions

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Nano Research 2024年第5期17卷 3622-3632页

作者： Ruiqi Cheng Kaiqi Li Huanxin Li Fengzhan Sun Xiaoqian He Tianshuo Zhao Jiao Zhang Chaopeng Fu Shanghai Key Laboratory of Advanced High-temperature Materials and Precision Forming School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Christopher Ingold Laboratory Department of ChemistryUniversity College LondonLondon WC1H 0AJUK Department of Chemistry Physical&Theoretical Chemistry LaboratoryUniversity of OxfordSouth Parks RoadOxford OX13QZUK Center of Hydrogen Science School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China

The development of non-platinum group metal(non-PGM)and efficient multifunctional electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER)with high activity and stability remains a great challenge.Herein,by in-situ transforming silver manganese composite oxide heterointerface into boosted Mott-Schottky heterointerface through a facile carbon reduction strategy,a nanorod-like silver/manganese oxide with superior multifunctional catalytic activities for ORR,OER and HER and stability was obtained.The nanorod-like silver/manganese oxide with Mott-Schottky heterointerface(designated as Ag/Mn_(3)O_(4))exhibits an ORR half-wave potential of 0.831 V(vs.RHE)in 0.1 M KOH,an OER overpotential of 338 mV and a HER overpotential of 177 mV at the current density of 10 mA·cm^(-2)in 1 M KOH,contributing to its noble-metal benchmarks comparable performance in aqueous aluminum-air(Al-air)battery and laboratorial overall water splitting electrolytic cell.Moreover,in-situ electrochemical Raman and synchrotron radiation spectroscopic measurements were conducted to further illustrate the catalytic mechanism of Ag/Mn_(3)O_(4)Mott-Schottky heterointerface towards various electrocatalytic reactions.At the heterointerface,the Ag phase serves as the electron donor and the active phase for ORR and HER,while the Mn_(3)O_(4)phase serves as the electron acceptor and the active phase for OER,respectively.This work deepens the understanding of the Mott-Schottky effect on electrocatalysis and fills in the gap in fundamental physical principles that are behind measured electrocatalytic activity,which offers substantial implications for the rational design of cost-effective multifunctional electrocatalysts with Mott-Schottky effect.

关键词： heterointerface electron donor-acceptor pair electrocatalyst Al-air battery water splitting

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heterointerface engineering of perovskite defects and energetics for light-emitting diodes

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Nano Research 2023年第4期16卷 5525-5532页

作者： Xiaomeng Zhang Lei Shi Junyang Bai Feijiu Wang Maowei Jiang Key Laboratory of Special Functional Materials of Ministry of Education of China School of Materials ScienceHenan UniversityKaifeng 475004China Henan Key Laboratory of Photovoltaic Materials Henan UniversityKaifeng 475004China

Perovskite light-emitting diodes(PeLEDs)rely on optimized device architecture to realize effective electro-optical converting.Especially,the stacks of dissimilar semiconducting materials form heterointerfaces,at which the defects and energetics of perovskite film greatly affect the device performance.Herein,we focus on the heterointerface engineering of perovskite towards high-quality PeLEDs.The defect engineering at both the bottom-surface(namely buried interface)and top-surface of perovskite film is simultaneously performed by semiconducting passivating molecules,which feature aligned energy levels and superior carrier injection ability regarding to perovskite.Moreover,such defect passivation could influence the heterointerface energetics.The perovskite work function is decreased by our suggested passivator treatment because of interface dipole,which results in band bending at the heterojunction and modulates the carrier dynamics.Hence,the electron injection is greatly enhanced,which boosts the up-conversion electroluminescence in current system.Overall,via the heterointerface engineering of defects and energetics synergistically,efficient PeLEDs with 3-fold enhancement of external quantum efficiency and low driving voltages with respect to pristine ones are achieved based on our proposed PeLED architecture.

关键词： heterointerface defect passivation energetics perovskite light-emitting diodes up-conversion electroluminescence

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High activity and stability in Ni_(2)P/(Co,Ni)OOH heterointerface with a multiple-hierarchy structure for alkaline hydrogen evolution reaction

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Nano Research 2023年第5期16卷 6552-6559页

作者： LiLi Zhang Zongpeng Wang Jitang Zhang Zhiping Lin Qinghua Zhang Wenwu Zhong Guangfeng Wu College of Material Science and Engineering Changchun University of TechnologyChangchun 130051China Zhejiang Provincial Key Laboratory for Cutting Tools Taizhou UniversityJiaojiang 318000China Institution of Physics Chinese Academic of ScienceBeijing 100190China

The fabrication of heterointerface materials with hierarchical morphologies more than two levels is a challenging yet promising approach to achieve optimal electrocatalyst for hydrogen evolution reaction(HER).Here,using a facile two-step method,we are able to prepare the Ni_(2)P/(Co,Ni)OOH heterointerface with a three-level hierarchy morphology.The multiple levels of hierarchy structures not only offer considerable area for active sites loading,but also facilitate the substance transportation,both beneficial for HER.Meanwhile,the strong charge transfer at the Ni_(2)P/(Co,Ni)OOH heterointerface eliminates the spin asymmetry and achieves the thermos-neutral adsorption of active H species.Moreover,the resulted Coulomb attraction stacks the two materials firmly,facilitating the stability.Density functional theory(DFT)and in-situ Raman measurements reveal the sufficient Ni atoms acting as the active sites.With these merits,the Ni_(2)P/(Co,Ni)OOH exhibits much better HER activity than the separate Ni_(2)P or(Co,Ni)OOH,affording a current density of 100 mA/cm^(2)at an overpotential of 169 mV and a Tafel slope of 41 mV/dec,when tested in alkaline electrolyte.This work provides inspiration for optimizing the intrinsic HER activity utilizing multiple-level hierarchy structures.

关键词： hydrogen evolution reaction Ni_(2)P/(Co,Ni)OOH heterointerface hierarchy

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Confinement synergy at the heterointerface for enhanced oxygen evolution

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Nano Research 2023年第7期16卷 8793-8799页

作者： Dongdi Wang Shanshan Ruan Peiyu Ma Ruyang Wang Xilan Ding Ming Zuo Lidong Zhang Zhirong Zhang Jie Zeng Jun Bao National Synchrotron Radiation Laboratory Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)University of Science and Technology of ChinaHefei 230026China Hefei National Laboratory for Physical Sciences at the Microscale Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of SciencesKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesDepartment of Chemical PhysicsUniversity of Science and Technology of ChinaHefei 230026China

Two-dimensional transition metal hydroxides with abundant reserves and low prices have played an indispensable role in energy catalytic applications.Recent reports indicated that the incorporation of Fe species into Co-based catalysts can synergistically enhance oxygen evolution reaction(OER)activity.Constructing a heterointerface on the surface of Co-based catalysts can provide a platform to investigate the role of heterointerface in reaction kinetics.Herein,we constructed a Fe-O-Co heterointerface without electronic effect by depositing FeO_(x)clusters on the oxygen vacancies of CoOOH surface.FeO_(x)/CoOOH exhibited excellent OER intrinsic activity,which can deliver the turnover frequency(TOF)of 4.56 s^(-1)at the overpotentials of 300 mV and the Tafel slope of 33 mV·dec^(-1).In-situ electrochemical impedance spectroscopy(EIS)and density functional theory(DFT)calculations demonstrated that the synergistic effect between Fe sites and Co sites confined at the Fe-O-Co heterointerface accelerated the charge transfer during OER and optimized the adsorption of oxygen intermediates,consequently enhancing OER.

关键词： clusters heterointerface confinement synergy oxygen evolution reaction

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Boosting Sodium Storage of Fe1?xS/MoS2 Composite via heterointerface Engineering

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Nano-Micro Letters 2019年第4期11卷 425-438页

作者： Song Chen Shaozhuan Huang Junping Hu Shuang Fan Yang Shang Mei Er Pam Xiaoxia Li Ye Wang Tingting Xu Yumeng Shi Hui Ying Yang International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education College of Optoelectronic EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China Pillar of Engineering Product Development Singapore University of Technology and Design8 Somapah RoadSingapore 487372Singapore Engineering Technology Research Center for 2D Material Information Function Devices and Systems of Guangdong Province College of Optoelectronic EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China Key Laboratory of Material Physics of Ministry of Education School of Physics and EngineeringZhengzhou UniversityZhengzhou 450052People’s Republic of China

Improving the cycling stability of metal sulfide-based anode materials at high rate is of great significance for advanced sodium ion batteries.However,the sluggish reaction kinetics is a big obstacle for the development of high-performance sodium storage electrodes.Herein,we have rationally engineered the heterointerface by designing the Fe1?xS/MoS2 heterostructure with abundant“ion reservoir”to endow the electrode with excellent cycling stability and rate capability,which is proved by a series of in and ex situ electrochemical investigations.Density functional theory calculations further reveal that the heterointerface greatly decreases sodium ion diffusion barrier and facilitates charge-transfer kinetics.Our present findings not only provide a deep analysis on the correlation between the structure and performance,but also draw inspiration for rational heterointerface engineering toward the next-generation high-performance energy storage devices.

关键词： Heterostructure heterointerface Diffusion barrier Ion reservoir Sodium ion battery

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Band offsets engineering at Cd_xZn_(1-x)S/Cu_2ZnSnS_4 heterointerface

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Chinese Physics B 2016年第12期25卷 390-393页

作者：包乌吉斯古楞萨初荣贵仇方圆 College of New Energy Bohai University College of Engineering Bohai University

Cd1-xZnxS/Cu2ZnSnS4 （CZTS）-based thin film solar cells usually use CdS as a buffer layer, but due to its smaller band gap （2.4 eV）, CdS film has been replaced with higher band gap materials. The cadmium zinc sulfide （CdZnS） ternary compound has a higher band gap than other compounds, which leads to a decrease in window absorption loss. In this paper, the band offsets at Cd1-xZnxS/CuzZnSnS4 （CZTS） heterointerface are calculated by the first-principles, density- functional and pseudopotential method. The band offsets at Cdl xZnxS/CZTS heterointerface are tuned by controlling the composition of Zn in Cd1-xZnxS alloy, the calculated valence band offsets are small, which is consistent with the commonanion rule. The favorable heterointerface of type-I with a moderate barrier height （〈 0.3 eV） can be obtained by controlling the composition of Zn in Cdl-xZnxS alloy between 0.25 and 0.375.

关键词： band offset first-principles calculation Cd1-xZnxS heterointerface

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Constructing heterointerface of Bi/Bi_(2)S_(3)with built-in electric field realizes superior sodium-ion storage capability

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eScience 2023年第4期3卷 99-109页

作者： Rong Liu Lai Yu Xiaoyue He Huanhuan Liu Xinyi Ma Zongzhi Tao Guanglin Wan Nazir Ahmad Bo Peng Liang Shi Genqiang Zhang Hefei National Research Center for Physical Sciences at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefeiAnhui230026China School of Materials Science and Engineering Anhui University of TechnologyMaanshanAnhui243002China

Bismuth sulfide(Bi_(2)S_(3))is a dominant anode material for sodium-ion batteries due to its high theoretical capacity.However,extreme volume fluctuations as well as low electrical conductivity and reaction kinetics still limit its practical applications.Herein,we construct an abundant heterointerface of Bi/Bi_(2)S_(3)by engineering the structure of Bi nanoparticles embedded on Bi_(2)S_(3)nanorods(denoted as Bi-Bi_(2)S_(3)NRs)to effectively solve the above-mentioned obstacles.Theoretical and systematic characterization results reveal that the constructed hetero-interface of Bi/Bi_(2)S_(3)has a built-in electric field,significantly boosts the electrical conductivity,enhances the Na^(+)diffusion kinetics,and buffers the volume variation.With this modification,it can deliver long cycling life,with an ultra-high capacity of 500 mAh g^(-1)over 500 cycles at 1 A g^(-1),and outstanding rate capability,with a capacity of 456 mAh g^(-1)even at 15 A g^(-1).Moreover,a full cell can achieve a high energy density of 180 Wh kg^(-1)at a power density of 40 W kg^(-1).Our research opens up a fresh path for improving the dynamics and structural stability of metal sulfide-based electrode materials for SIBs.

关键词： Sodium-ion battery Anode materials heterointerface Built-in electric field Energy band structure

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Engineering cobalt sulfide/oxide heterostructure with atomically mixed interfaces for synergistic electrocatalytic water splitting

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Nano Research 2022年第2期15卷 1246-1253页

作者： Xiaoyang Wang Yu He Xiaopeng Han Jun Zhao Lanlan Li Jinfeng Zhang Cheng Zhong Yida Deng Wenbin Hu School of Materials Science and Engineering Tianjin Key Laboratory of Composite and Functional MaterialsKey Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China School of Materials Science and Engineering Hebei University of TechnologyTianjin 300130China

It remains challenging to develop economical and bifunctional electrocatalysts toward oxygen/hydrogen evolution reactions(OER/HER).Herein,we construct Co_(9)S_(8) nanoflakes decorated Co_(3)O_(4) nanoarrays with enriched heterogeneous interface zones on Ni foam(Co_(9)S_(8)@CO_(3)O_(4)/NF)via a novel step-wise approach.The Co_(9)S_(8)@Co_(3)O_(4)/NF hybrid manifests excellent performance with low overpotentials of 130 mV for HER(10 mA·cm^(-2))and 331 mV for OER(100 mA·cm^(-2)),delivering a small voltage of 1.52 V for water splitting at 10 mA·cm^(-2) as well as outstanding catalytic durability,which surpasses precious metals and previously reported earth-abundant nanocatalysts.Further experimental and theoretical investigations demonstrate that the excellent performance is attributed to the followings:(i)Highly conductive Ni facilitates the efficient charge transfer;(ii)porous core-shell nanoarchitecture benefits the infiltration and transportation of gases/ions;(iii)heterogeneous interface zones synergistically lower the chemisorption energy of hydrogen/oxygen intermediates.This work will shed light on the controllable synthesis and engineering of heterostructure nanomaterials for clean energy storage and conversion technologies.

关键词： nanocomposite heterointerface electrocatalysis oxygen evolution reaction hydrogen evolution reaction

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Synergistic effects of 1T MoS_(2)and interface engineering on hollow NiCoP nanorods for enhanced hydrogen evolution activity

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Journal of Materials Science & Technology 2023年第14期145卷 165-173页

作者： Qiaomei Luo Lan Sun Yiwei Zhao Chen Wang Hongqiang Xin Danyang Li Fei Ma State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong UniversityXi’an 710049China

Metallic 1T-phase molybdenum disulfide(1T-MoS_(2))shows more excellent electrocatalytic performance for hydrogen evolution reaction(HER)than semiconducting 2H-phase MoS_(2)(2H-MoS_(2)).Therefore,the facile controllable synthesis of hierarchical structure with rich 1T-MoS_(2)is desired for highly efficient electrocatalytic performance.In this work,a simple solvothermal method is proposed to fabricate hol-low NiCoP/MoS_(2)-V heterostructure with 63.2%1T-MoS_(2),in which the abundant catalytic active sites are exposed,the mass transfer properties are improved,and the electronic states are optimized.Moreover,the low energy difference between 2H and 1T phases and near zero free energy of hydrogen adsorption(△G H∗)result in fast kinetics and excellent catalytic performances.Specifically,the NiCoP/MoS_(2)-V com-posite exhibits enhanced HER activity with a low overpotential of 74.6 mV at 10 mA cm^(-2)and superior stability in alkaline electrolytes.This efficient design opens up new vistas for developing high-activity electrocatalysts.

关键词： Hollow hierarchical structure 1T-MoS_(2) heterointerface Optimized electronic states Synergistic effect Superior HER activity

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