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Maneuvering charge polarization and transport in 2HMoS2 for enhanced electrocatalytic hydrogen evolution reaction

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Nano Research 2016年第9期9卷 2662-2671页

作者： Wei Ye Chenhao Ren Daobin Liu Chengming Wang Ning Zhang wensheng yan Li Song Hefei National Laboratory for Physical Sciences at the Microscale iChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Hefei Science Center(CAS)School of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China

Semiconducting 2H-MoS2with high chemical stability is a promising alternative to the existing electrocatalysts for the hydrogen evolution reaction (HER); however, the HER performance largely suffers from the limited number of active S sites and low mobility for charge transport. In this work, we demonstrate that the limitations of 2H-MoS2for the HER can be overcome by forming hybrid structures with metallic nanowires. Taking the integration with Pd as a proofof- concept, we show with solid experimental evidence that the one-dimensional structure of metallic nanowires facilitates electron transport to active S sites, while the interfacial charge polarization between MoS2and Pd increases the electron density of the S sites for improved activity. As a result, the hybrid structure exhibits a current density of 122 mA·cm-2at -300 mV versus RHE and a Tafel slope of 44 mV·decade-1with excellent durability, well exceeding the performances of bare 2H-MoS2and metallic 1T-MoS2. This work provides insights into electrocatalyst design based on charge transport and polarization, which can be extended to other hybrid structures. [Figure not available: see fulltext.] © 2016, Tsinghua University Press and Springer-Verlag Berlin Heidelberg.

关键词： hydrogen evolution molybdenum disulfide charge transport charge polarization nanowire

Asymmetrically coordinated main group atomic In-S_(1)N_(3)interface sites for promoting electrochemical CO_(2)reduction

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Nano Research 2024年第6期17卷 5011-5021页

作者： yan Gao Jinlong Ge Jingqiao Zhang Ting Cao Zhiyi Sun wensheng yan Yu Wang Jie Lin Wenxing Chen Zheng Liu Anhui Provincial Engineering Laboratory of Silicon-based Materials Bengbu UniversityBengbu 233030China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China SEPA Key Laboratory of Eco-Industry Chinese Research Academy of Environmental SciencesBeijing 100012China Ningbo Institute of Materials Technology and Engineering Chinese Academy of ScienceNingbo 315201China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Shanghai Synchrotron Radiation Facilities Shanghai Institute of Applied PhysicsChinese Academy of ScienceShanghai 201204China

Designing catalysts with highly active,selectivity,and stability for electrocatalytic CO_(2)to formate is currently a severe ***,we developed an electronic structure engineering on carbon nano frameworks embedded with nitrogen and sulfur asymmetrically dual-coordinated indium active sites toward the efficient electrocatalytic CO_(2)reduction *** expected,atomically dispersed In-based catalysts with In-S_(1)N_(3)atomic interface with asymmetrically coordinated exhibited high efficiency for CO_(2)reduction reaction(CO_(2)RR)to *** achieved a maximum Faradaic efficiency(FE)of 94.3%towards formate generation at−0.8 V *** hydrogen electrode(RHE),outperforming that of catalysts with In-S2N2 and In-N4 atomic *** at a potential of−1.10 V ***,In-S_(1)N_(3)achieves an impressive Faradaic efficiency of 93.7%in flow *** catalytic performance of In-S_(1)N_(3)sites was confirmed to be enhanced through in-situ X-ray absorption near-edge structure(XANES)measurements under electrochemical *** discovery provides the guidance for performance regulation of main group metal catalysts toward CO_(2)RR at atomic scale.

关键词： indium single-site catalyst main group metal asymmetrical coordination CO_(2)reduction reaction structure-activity relationship

Ultrahigh-temperature ferromagnetism in MoS_(2) Moirésuperlattice/graphene hybrid heterostructures

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Nano Research 2021年第11期14卷 4182-4187页

作者： Liang Cai Hengli Duan Qinghua Liu Chao Wang Hao Tan Wei Hu Fengchun Hu Zhihu Sun wensheng yan National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei230029China

Realizing high-temperature ferromagnetism in two-dimensional(2D)semiconductor nanosheets is significant for their applications in next-generation magnetic and electronic ***,this goal could be achieved on a MoS_(2) Moirésuperlattice grown on the reduced graphene oxide(RGO)substrate by a hydrothermal *** as-synthesized bilayer MoS_(2) superlattice structure with rotating angle(ϕ=13°±1°)of two hexagonal MoS_(2) lattices,possesses outstanding ferromagnetic property and an ultra-high Curie temperature of 990 *** X-ray absorption near-edge structure and ultraviolet photoelectron spectroscopies combined with density functional theory calculation indicate that the covalent interactions between MoS_(2) Moirésuperlattice and RGO substrate lead to the formation of interfacial Mo-S-C bonds and complete spin polarization of Mo 4d electrons near the Fermi *** design could be generalized and may open up a possibility for tailoring the magnetism of other 2D materials.

关键词： MoS2 moirésuperlattice high-temperature ferromagnetism XAFS hybrid heterostructures 2D nanosheets

Continuous and fast magneto-ionic control of magnetism in Ta/Co/ BiFeO_(3)/SrRuO_(3) multiferroic heterostructure

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Journal of Materiomics 2022年第6期8卷 1141-1148页

作者： Zhiwei Chen Haoyang Sun Xiang Zhou Hengli Duan wensheng yan Yuewei Yin Xiaoguang Li Hefei National Research Center for Physical Sciences at the Microscale Department of Physics and CAS Key Laboratory of Strongly-Coupled Quantum Matter PhysicsUniversity of Science and Technology of ChinaHefei230026China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei230029China Collaborative Innovation Center of Advanced Microstructures Nanjing UniversityNanjing210093China

Room temperature electric field controlled magnetism is extremely promising for the next-generation high-performance spintronic ***,based on the ferroelectric switching driven oxygen ion migration in the Ta/Co/BiFeO_(3)/SrRuO_(3) heterostructures,the magnetic moment,magnetic coercive field,exchange bias field,and junction resistance are reversibly manipulated by tuning the ferroelectric polarization of the BiFeO_(3) *** these phenomena are consistently explained by the oxygen ion migration induced CoOx/Co redox effect,which is evidenced by the synchrotron X-ray absorption spectroscopy ***,owing to the controllable ferroelectric switching dynamics of the BiFeO_(3) thin film,the magnetic coercive field of the Co thin film can be continuously and precisely tuned by controlling the ferroelectric polarization of the BiFeO_(3) thin film,and the manipulating speed of the voltage control of magnetism can be fast to 100 *** nonvolatile,stable,reversible,fast,and reproducible voltage control of magnetism shows great potential for designing low-power and high-speed spintronics.

关键词： Voltage control of magnetism Nonvolatile Magneto-ionic effect Multiferroic heterostructure Ferroelectric switching dynamics

Cobalt single atom site catalysts with ultrahigh metal loading for enhanced aerobic oxidation of ethylbenzene

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Nano Research 2021年第7期14卷 2418-2423页

作者： Yu Xiong Wenming Sun Yunhu Han Pingyu Xin Xusheng Zheng wensheng yan Juncai Dong Jian Zhang Dingsheng Wang Yadong Li Department of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China Department of Chemistry Tsinghua UniversityBeijing 100084China China College of Science China Agricultural UniversityBeijing 100193China Institute of Flexible Electronics Northwestern Polytechnical UniversityXi’an 710072China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100084China

The oxidation of hydrocarbons to produce high value-added compounds(ketones or alcohols)using oxygen in air as the only oxidant is an efficient synthetic strategy from both environmental and economic ***,we successfully synthesized cobalt single atom site catalysts(Co SACs)with high metal loading of 23.58 wt.%supported on carbon nitride(CN),which showed excellent catalytic properties for oxidation of ethylbenzene in ***,Co SACs show a much higher turn-over frequency(19.6 h^(−1))than other reported non-noble catalysts under the same ***,the as-obtained nanosized or homogenous Co catalysts are inert to this *** SACs also exhibit high selectivity(97%)and stability(unchanged after five runs)in this *** calculations reveal that Co SACs show a low energy barrier in the first elementary step and a high resistance to water,which result in the robust catalytic performance for this reaction.

关键词： single atom site high-loading catalysts heterogeneous catalysts ethylbenzene oxidation

Sulfur-vacancy-tunable interlayer magnetic coupling in centimeter-scale M0S2 bilayer

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Nano Research 2022年第2期15卷 881-888页

作者： Hengli Duan Guinan Li Hao Tan Chao Wang Qian Li Chuanchuan Liu Yuewei Yin Xiaoguang Li Zeming Qi wensheng yan National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Hefei National Laboratory for Physical Sciences at the Microscale Department of Physicsand CAS Key Laboratory of Strongly-coupled Quantum Matter PhysicsUniversity of Science and Technology of ChinaHefei 230026China

Endowing bilayer transition-metal dichalcogenides(TMDs)with tunable magnetism is significant to investigate the coupling of multiple electron degrees of freedom(DOFs).However,effectively inducing and tuning the magnetic interaction of bilayer TMDs are still ***,we report a strategy to tune the interlayer exchange interaction of centimeter-scale MoS2 bilayer with substitutional doping of Co ion,by introducing sulfur vacancy(V_(s))to modulate the interlayer electronic *** strategy could transform the interlayer exchange interaction from antiferromagnetism(AFM)to ferromagnetism(FM),as revealed by the magnetic *** characterizations and theoretical calculations indicate that the enhanced magnetization is mainly because the hybridization of Co 3d band and Vs-induced impurity band alters the forms of interlayer orbital hybridizations between the partial Co atoms in upper and lower layers,and also enhances the intralayer *** work paves the way for tuning the interlayer exchange interaction with defects and could be extended to other two-dimensional(2D)magnetic materials.

关键词： interlayer exchange interaction 2D magnetic materials S-vacancy interlayer coupling large-area growth

Metal^(n+)-Metal^(δ+) pair sites steer C-C coupling for selective CO_(2) photoreduction to C_(2) hydrocarbons

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Nano Research 2022年第3期15卷 1882-1891页

作者： Weiwei Shao Xiaodong Li Juncheng Zhu Xiaolong Zu Liang Liang Jun Hu yang Pan Junfa Zhu wensheng yan Yongfu Sun Yi Xie Hefei National Laboratory for Physical Sciences at Microscale CAS Centre for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230026China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China

The major obstacle for selective CO_(2)photoreduction to C_(2)hydrocarbons lies in the difficulty of C–C coupling,which is usually restrained by the repulsive dipole–dipole interaction between adjacent carbonaceous ... 详细信息

关键词： C–C coupling pair sites CO_(2)photoreduction ethylene

Classical spin liquid state in a rhombic lattice metal-organic framework

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Nano Research 2024年第4期17卷 3407-3412页

作者： Sihua Feng Chao Wang Jiyin Zhao Xuguang Liu Chaocheng Liu Zeming Qi Lei Chen Huijuan Wang Minghui Fan Hengli Duan wensheng yan National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230026China Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China School of Materials Science and Engineering Hefei University of TechnologyHefei 230009China Experimental Center of Engineering and Material Science University of Science and Technology of ChinaHefei 230026China

Discovering more and new geometrically frustrated systems remains an active point of inquiry in fundamental physics for the existence of unusual states of ***,we report spin-liquid-like behavior in a two-dimensional(2D)rhombic lattice Fe-metal-organic framework(Fe-MOF)with frustrated *** Fe-MOF exhibits a high frustration factor f=|θCW|/TN≥315,and its long-range magnetic order is suppressed down to 180 *** theoretical calculations demonstrate strong antiferromagnetic coupling between adjacent Fe3+ions,indicating the potential of a classical spin-liquid-like ***,a T-linear heat capacity parameter,γ,originating from electronic contributions and with magnetic field independence up to 8 T,can be observed in the specific heat capacity measurements at low-temperature,providing further proof for the spin-liquid-like *** work highlights the potential of MOF materials in geometrically frustrated systems,and will promote the research of exotic quantum physics phenomena.

关键词： spin-liquid-like state two-dimensional metal-organic framework(2D MOF) rhombic lattice ultralow temperature(ULT)measurements spin-frustrated

Porous γ-Fe_(2)O_(3) nanoparticle decorated with atomically dispersed platinum: Study on atomic site structural change and gas sensor activity evolution

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Nano Research 2021年第5期14卷 1435-1442页

作者： Qiheng Li Zhi Li Qinghua Zhang Lirong Zheng wensheng yan Xiao Liang Lin Gu Chen Chen Dingsheng Wang Qing Peng Yadong Li Department of Chemistry Tsinghua UniversityBeijing100084China School of Physical Sciences University of Chinese Academy of SciencesBeijing100190China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing100049China National Synchrotron Radiation Laboratory(NSRL) University of Science and Technology of ChinaHefei230029China

Decorating semi-conducting metal oxide with noble metal has been recognized as a viable approach to improve the sensitivity of gas sensor. However, conventional method which relys on noble metal nanoparticles is confronted with drawback of significantly increased cost. To maximize the atom efficiency and reduce the cost for practical industrial application, designing sensor material with noble metal isolated single atom sites (ISAS) doping is a desired option. Here, we report an atomically dispersed platinum on one-dimensional arranged porous γ-Fe2O3 nanoparticle composites as highly efficient ethanol gas sensor. The optimized sample (Pt1-Fe2O3-ox) exhibited a high response (Ra/Rg = 102.4) and good selectivity to ethanol gas. It is demonstrated only the Pt single atom sites with high valance can effectively promote the adsorption capacity to ethanol and consequently enhance the sensitivity of sensing process by changing the electrical structure of Fe2O3 support. This work indicates the single atom sites could play a vital role in improving the performance of conventional metal oxides gas sensors and pave way for the exploration of ISAS-enhanced gas sensor for other volatile organic compounds (VOCs).

关键词： isolated single atom sites structure-activity relationship gas sensor nanocomposites