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Dual-Functional Electrode Promoting Dendrite-Free and CO2 Utilization Enabled High-Reversible Symmetric Na-CO2 Batteries

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Energy & Environmental Materials 2024年第3期7卷 127-136页

作者： Changfan Xu Jiajia Qiu Yulian Dong Yueliang Li Yonglong Shen Huaping Zhao Ute Kaiser Guosheng Shao Yong Lei Fachgebiet Angewandte Nanophysik Institut für Physik & IMN MacroNano Central facility for electron microscopy Electron Microscopy Group of Materials ScienceUlm University School of Materials Science and Engineering Zhengzhou University

Sodium-carbon dioxide （Na-CO2） batteries are regarded as promising energy storage technologies because of their impressive theoretical energy density and CO2reutilization,but their practical applications are restricted by uncontrollable sodium dendrite growth and poor electrochemical kinetics of *** suitable multifunctional electrodes for dendritefree anodes and kinetics-enhanced CO2cathodes is considered one of the most important ways to advance the practical application of ***,RuO2nanoparticles encapsulated in carbon paper （RuCP）are rationally designed and employed as both Na anode host and CO2cathode in *** outstanding sodiophilicity and high catalytic activity of RuCP electrodes can simultaneously contribute to homogenous Na+distribution and dendrite-free sodium structure at the anode,as well as strengthen discharge and charge kinetics at the *** morphological evolution confirmed the uniform deposition of Na on RuCP anode with dense and flat interfaces,delivering enhanced Coulombic efficiency of 99.5%and cycling stability near 1500 ***,Na-CO2batteries with RuCP cathode demonstrated excellent cycling stability（>350 cycles）.Significantly,implementation of a dendrite-free RuCP@Na anode and catalytic-site-rich RuCP cathode allowed for the construction of a symmetric Na-CO2battery with long-duration cyclability,offering inspiration for extensive practical uses of Na-CO2batteries.

关键词： CO2 cathode dendrite free electrocatalysis Na metal anode symmetric CO2 batteries

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The effect of Laves phases and nano-precipitates on the electrochemical corrosion resistance of Mg-Al-Ca alloys under alkaline conditions

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Journal of Magnesium and Alloys 2024年第6期12卷 2447-2461页

作者： Markus Felten Veronika Chaineux Siyuan Zhang Ali Tehranchi Tilmann Hickel Christina Scheu Joshua Spille Marta Lipińska-Chwałek Joachim Mayer Benjamin Berkels Marcus Hans Imke Greving Silja Flenner Sandra Sefa Daniela Zander Chair of Corrosion and Corrosion Protection RWTH Aachen UniversityAachen 52072 Germany Max-Planck-Institut für Eisenforschung GmbH Düsseldorf 40237 Germany Central facility for electron microscopy RWTH Aachen UniversityAachen 52074 Germany Ernst Ruska-Centre for microscopy and Spectroscopy with electrons Forschungszentrum Jülich GmbHJülich 52428Germany Mathematical Image and Signal Processing Aachen Institute for Advanced Study in Computational Engineering ScienceRWTH Aachen UniversityAachen 52062 Germany Materials Chemistry RWTH Aachen UniversityAachen 52074 Germany Institute of Materials Physics Helmholtz-Zentrum HereonGeesthacht 21502 Germany

The electrochemical corrosion mechanisms of Mg alloys were extensively studied in previous investigations of different chemical com-positions,modified surface states and various electrolyte ***,recent research focused on the active state of Mg dissolution,leading to unresolved effects of secondary phases adjacent to a stableα-solid solution passive *** present study investigates the fundamental electrochemical corrosion mechanisms of three different Laves phases with varying phase morphologies and phase fractions in the passive state of Mg-Al-Ca *** microstructure was characterized by(transmission-)electron microscopy and synchrotron-based transmission X-ray *** electrochemical corrosion resistance was determined with a standard three-electrode setup and advanced in-situ flow cell measurements.A new electrochemical activity sequence(C15>C36>α-Mg>C14)was obtained,as a result of a stable passive layer formation on theα-solid ***,nm-scale Mg-rich precipitates were identified within the Laves phases,which tend to inhibit the corrosion kinetics.

关键词： Laves phase STEM Magnesium Corrosion Passive layer

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Ultra-thin robust CNT@GC film integrating effective electromagnetic shielding and flexible Joule heating

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Nano Research 2024年第5期17卷 3462-3471页

作者： Ding Zhang Chunhui Wang Meng Li Weixue Meng Shipeng Zhang Mengdan Yang Xinguang Huang Yingjiu Zhang Yuanyuan Shang Anyuan Cao Key Laboratory of Materials Physics(Ministry of Education) School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou450052China electron microscopy Center Yunnan UniversityKunming650091China School of Materials Science and Engineering Peking UniversityBeijing100871China

The demand for lightweight,thin electromagnetic interference(EMI)shielding film materials with high shielding effectiveness(SE),excellent mechanical properties,and stability in complex environments is particularly pronounced in the realm of flexible and portable electronic ***,we developed an ultra-thin film(CNT@GC)in which the glassy carbon(GC)layer wrapped around and welded carbon nanotubes(CNTs)to form a core-shell network structure,leading to exceptional tensile strength(327.2 MPa)and electrical conductivity(2.87×10^(5) S·m^(−1)).The CNT@GC film achieved EMI SE of 60 dB at a thickness of 2µm after post-acid treatment and high specific SE of 3.49×10^(5) dB·cm^(2)·g^(−1),with comprehensive properties surpassing those of the majority of previous shielding ***,the CNT@GC film exhibited Joule heating capability,reaching a surface temperature of 135℃at 3 V with a fast thermal response of about 0.5 s,enabling anti-icing/de-icing *** work presented a methodology for constructing a robust CNT@GC film with high EMI shielding performance and exceptional Joule heating capability,demonstrating immense potential in wearable devices,defense,and aerospace applications.

关键词： core-shell structure ultra-thin lightweight film robust film electromagnetic shielding Joule heating

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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 306-314,I0007页

作者： Yugang Qi Qing Liang Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science&Engineering Electron Microscopy Centerand International Center of Future ScienceJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsJilin UniversityChangchun 130012JilinChina Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China

Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic *** the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of ***,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery *** introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic *** discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Single atom catalyst Shell coordination optimization

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High-performance terahertz modulators induced by substrate field in Te-based all-2D heterojunctions

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Light(Science & Applications) 2024年第3期13卷 577-586页

作者： Pujing Zhang Qihang Liang Qingli Zhou Jinyu Chen Menglei Li Yuwang Deng Wanlin Liang Liangliang Zhang Qinghua Zhang Lin Gu Chen Ge Kui-juan Jin Cunlin Zhang Guozhen Yang Department of Physics Key Laboratory of Terahertz OptoelectronicsMinistry of Educationand Beijing Advanced Innovation Center for Imaging Theory and TechnologyCapital Normal UniversityBeijing 100048China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China Department of Materials Science and Engineering Beijing National Center for Electron Microscopy and Laboratory of Advanced MaterialsTsinghua UniversityBeijing 100084China

High-performance active terahertz modulators as the indispensable core components are of great importance for the next generation communication ***,they currently suffer from the tradeoff between modulation depth and ***,we introduce two-dimensional(2D)tellurium(Te)nanofilms with the unique structure as a new class of optically controlled terahertz modulators and demonstrate their integrated heterojunctions can successfully improve the device performances to the optimal and applicable levels among the existing all-2D broadband *** photoresponse measurements confirm the significant impact of the stacking *** first clarify the direction of the substrate-induced electric field through first-principles calculations and uncover the unusual interaction mechanism in the photoexcited carrier dynamics associated with the charge transfer and interlayer exciton *** advances the fundamental and applicative research of Te nanomaterials in high-performance terahertz optoelectronics.

关键词： performance field terahertz

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Nickel-iron in the second coordination shell boost single-atomicsite iridium catalysts for high-performance urea electrooxidation

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Nano Research 2024年第5期17卷 3919-3926页

作者： Xiaoyu Chen Jiawei Wan Jing Chai Liang Zhang Fang Zhang Qinghua Zhang Lin Gu Lirong Zheng Ranbo Yu Department of Physical Chemistry School of Metallurgical and Ecological EngineeringUniversity of Science and Technology BeijingBeijing 100083China State Key Laboratory of Biochemical Engineering Key Laboratory of Biopharmaceutical Preparation and DeliveryChinese Academy of SciencesInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center for Combustion Energy School of Vehicle and MobilityState Key Laboratory of Intelligent Green Vehicle and MobilityTsinghua UniversityBeijing 100084China Analysis and Testing Center Beijing Institute of TechnologyBeijing 100081China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China Beijing National Center for electron microscopy and Laboratory of Advanced Materials Department of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Beijing Synchrotron Radiation facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China

Single-atom catalysts(SACs)with high catalytic activity as well as great stability are demonstrating great promotion in electrocatalytic energy conversion,which is also a big challenge to ***,we proposed a facile synthetic strategy to construct nickel-iron bimetallic hydroxide nanoribbon stabilized single-atom iridium catalysts(Ir-NiFe-OH),where the nickel-iron hydroxide nanoribbon not only can serve as good electronic conductor,but also can well stabilize and fully expose single-atom *** as catalyst for urea oxidation reaction(UOR),it exhibited excellent UOR performance that it only needed a low operated potential of 1.38 V to achieve the current density of 100 mA·cm^(-2).In-situ Fourier transform infrared spectroscopy,X-ray absorption spectrum,and density functional theory calculations proved that Ir species are active centers and the existence of both Ni and Fe in the local structure of Ir atom can optimize the d-band center of Ir species,promoting the adsorption of intermediates and desorption of products for *** hydrogen evolution reaction(HER)/UOR electrocatalytic cell demanded voltages of 1.46 and 1.50 V to achieve 50 and 100 mA·cm^(-2),respectively,which demonstrated a higher activity and better stability than those of conventional *** work opens a new avenue to develop catalysts for UORs with boosted activity and stability.

关键词： single-atom iridium coordinate structure nanoribbon urea electrooxidation

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面向碱性析氢反应的原子级优化Fe-Pt金属间化合物催化剂表面终结态探索

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Science Bulletin 2024年第8期69卷 1091-1099页

作者：梁庆孟繁玲李文文邹旭宋可心葛昕姜周刘玉华刘美琦李振宇董韬文陈中军张伟郑伟涛 Key Laboratory of Automobile Materials(Ministry of Education) School of Materials Science and EngineeringElectron Microscopy CenterInternational Center of Future ScienceJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsJilin UniversityChangchun 130012China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China

Controlling the atomic arrangement of elemental atoms in intermetallic catalysts to govern their surface and subsurface properties is a crucial but challenging endeavor in electrocatalytic *** hydrogen evolution reaction(HER),adjusting the d-band center of the conventional noble-metallic Pt by introducing Fe enables the optimization of catalytic ***,a notable gap exists in research on the effective transition from disordered Fe/Pt alloys to highly ordered intermetallic compounds(IMCs)such as FePt_(3)in the alkaline HER,hampering their broader *** this study,a series of catalysts FePt_(3-x)H(x=5,6,7,8 and 9)supported on carbon nanotubes(CNTs)were synthesized via a simple impregnation method,along with a range of heat treatment processes,including annealing in a reductive atmosphere,to regulate the order degree of the arrangement of Fe/Pt atoms within the FePt_(3)*** using advanced microscopy and spectroscopy techniques,we systematically explored the impact of the order degree of FePt_(3)in the *** as-prepared FePt_(3)-8H exhibited notable HER catalytic activity with low overpotentials(η=37 mV in 1.0 mol L^(-1)KOH)at j=10 mA cm^(-2).The surface of the L1_(2)FePt_(3)-8H catalyst was demonstrated to be *** Pt on the surface was not easily oxidized due to the unique Fe/Pt coordination,resulting in significant enhancement of HER performance.

关键词： Intermetallic Hydrogen evolution reaction Surface Catalyst

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Chiral helically grooved gold nanoarrows for concurrently enhancing oxygen and hydrogen evolution from electrochemical water splitting

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Science China Chemistry 2024年

作者： Lufei Huang Tao Wang Ying Li Ping Wang Rui Tian Baowen Zhou Lin Yao China-UK Low Carbon College Shanghai Jiao Tong University electron microscopy Laboratory School of Physics Peking University State Key Laboratory for Mesoscopic Physics and Frontiers Science Center for Nano-optoelectronics School of Physics Peking University Key Laboratory for Power Machinery and Engineering of Ministry of Education Research Center for Renewable Synthetic FuelSchool of Mechanical Engineering Shanghai Jiao Tong University

Electrocatalytic water splitting shows a tremendous promise for storing green and intermittent electricity into storable fuels,paving a sustainable way toward carbon neutrality. The exploration of a bifunctional electrocatalyst for simultaneously enhancing oxygen evolution reaction and hydrogen evolution reaction is at the core yet remains a grand challenge, especially operated in the same electrolyte. In this work, mesoscale gold nanoarrows with special chiral morphology are synthesized for electrocatalytic water splitting. In the same electrolyte of 1 M KOH aqueous solution, the as-designed chiral R-/L-helically grooved gold nanoarrows（R-/L-heliGNAs） demonstrated significantly enhanced performance in both hydrogen evolution reaction and oxygen evolution reaction with overpotentials of 186 and 355 mV at 10 mA cm-2, respectively, compared to the achiral counterpart. For oxygen evolution reaction, the performance is even comparable to commercial notable metal catalysts,i.e., RuO2, of which the overpotential is 310 mV under the same measured conditions. The spin-polarized conductive atomic force microscope（c-AFM）, finite-difference time-domain simulation, in combination with electrochemical investigations, show that the chirality of R-/L-heliGNAs makes a substantial contribution toward the remarkable performance by enhanced electric field distribution for hydrogen evolution reaction and by tuning the spin states of the electrons for oxygen evolution *** study presents an encouraging strategy for simultaneously promoting hydrogen evolution reaction and oxygen evolution reaction that operated in the same electrolyte by imparting chirality toward a mesoscale inorganic electrocatalyst, showing a grand promise for opening up a new way for electrocatalytic water splitting toward green hydrogen.

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Hierarchical Sb-Ni nanoarrays as robust binder-free anodes for high-performance sodium-ion half and full cells

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Nano Research 2017年第9期10卷 3189-3201页

作者： Liying Liang Yang Xu Liaoyong Wen Yueliang Li Min Zhou Chengliang Wang Huaping Zhao Ute Kaiser Yong Lei Institute of Physics & IMN MacroNano (ZIK) Ilmenau University of Technology Professor Schmidt Strasse 26 98693 Ilmenau Germany Central facility for electron microscopy Electron Microscopy Group of Materials Science UIm University Albert~Einstein-Allee 11 89081 UIm Germany

A novel hierarchical electrode material for Na-ion batteries composed of Sb nanoplates on Ni nanorod arrays is developed to tackle the issues of the rapid capacity fading and poor rate capability of Sb-based materials. The three-dimensional (3D) Sb-Ni nanoarrays as anodes exhibit the synergistic effects of the two-dimensional nanoplates and the open and conductive array structure as well as strong structural integrity. Further, their capacitive behavior is confirmed through a kinetics analysis, which shows that their excellent Na-storage performance is attributable to their unique nanostructure. When used as binder-free sodium-ion battery (SIB) anodes, the nanoarrays exhibit a high capacity retention rate (more than 80% over 200 cycles) at a current density of 0.5 A·g–1 and excellent rate capacity (up to 20 A·g–1), with their capacity being 580 mAh·g–1. Moreover, a P2-Na2/3Ni1/3Mn2/3O2//3D Sb-Ni nanoarrays full cell delivers a highly reversible capacity of 579.8 mAh·g–1 over 200 cycles and an energy density as high as 100 Wh·kg–1. This design strategy for ensuring fast and stable Na storage may work with other electrode materials as well.

关键词： hierarchical Sb-Ni nanoarrays binder-free anode capacitive charge storage Na-ion full cell

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Perspective towards atomic-resolution imaging of two-dimensional polymers

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SmartMat 2021年第2期2卷 131-138页

作者： Haoyuan Qi Baokun Liang Ute Kaiser Central facility of electron microscopy Electron Microscopy Group of Materials ScienceUniversität UlmUlmGermany Center for Advancing electronics Dresden(cfaed) Faculty of Chemistry and Food ChemistryTechnische Universität DresdenDresdenGermany

Recent years have witnessed the rise of an emerging class of synthetic twodimensional(2D)materials-2D *** combination of organic chemistry and rational design of polymeric crystals has stimulated tremendous research efforts in the controlled synthesis of 2D ***,despite the advancement in synthetic methodologies,the structural characterization of 2D polymers remains a significant *** aberration-corrected high-resolution transmission electron microscopy(AC-HRTEM)is capable of direct imaging of atomic structures with sub-Ångström resolution,electron radiation damage poses a substantial limit on the achievable image resolution due to instant decomposition of the molecular *** this Perspective,we will briefly discuss radiation damage mitigation strategies,which may eventually result in AC-HRTEM imaging of 2D polymers down to the atomic scale.

关键词： covalent organic frameworks transmission electron microscopy two-dimensional polymers

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