Fast-charge high-voltage layered cathodes for sodium-ion batteries
Not provided.
Environmental Sciences & Ecology↗
Engineering topics
Bai, Xuedong
Publications and source records attributed to Bai, Xuedong.
Designing lithium halide solid electrolytes
All-solid-state lithium batteries have attracted widespread attention for next-generation energy storage, potentially providing enhanced safety and cycling stability. The performance of such batteries relies on solid electrolyte materials; hence many structures/phases are being investigated with increasing compositional complexity. Among the various solid electrolytes, lithium halides show promising ionic conductivity and cathode compatibility, however, there are no effective guidelines when moving toward complex compositions that go beyond ab -initio modeling. Here, we show that ionic potential, the ratio of charge number and ion radius, can effectively capture the key interactions within halide materials, making it possible to guide the design of the representative crystal structures. This is demonstrated by the preparation of a family of complex layered halides that combine an enhanced conductivity with a favorable isometric morphology, induced by the high configurational entropy. This work provides insights into the characteristics of complex halide phases and presents a methodology for designing solid materials.
25 ENERGY STORAGE↗
Electric-field control of the nucleation and motion of isolated three-fold polar vertices
Recently various topological polar structures have been discovered in oxide thin films. Despite the increasing evidence of their switchability under electrical and/or mechanical fields, the dynamic property of isolated ones, which is usually required for applications such as data storage, is still absent. Here, we show the controlled nucleation and motion of isolated three-fold vertices under an applied electric field. At the PbTiO 3 /SrRuO 3 interface, a two-unit-cell thick SrTiO 3 layer provides electrical boundary conditions for the formation of three-fold vertices. Utilizing the SrTiO 3 layer and in situ electrical testing system, we find that isolated three-fold vertices can move in a controllable and reversible manner with a velocity up to ~629 nm s -1 . Microstructural evolution of the nucleation and propagation of isolated three-fold vertices is further revealed by phase-field simulations. This work demonstrates the ability to electrically manipulate isolated three-fold vertices, shedding light on the dynamic property of isolated topological polar structures.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Unveiling the Degradation Mechanism of High-Temperature Superconductor Bi 2 Sr 2 CaCu 2 O 8+δ in Water-Bearing Environments
We report the physical properties of copper oxide high-temperature superconductors have been studied extensively, such as its band structure, and doping effects of Bi 2 Sr 2 CaCu 2 O 8+δ (Bi-2212). However, some chemical-related properties of these superconductors are rarely reported, such as their stability in air. Here, we report experiments combined with ab initio calculations that address the effects of water in contact with Bi-2212. The evolution of Bi-2212 flake with exposure to water for different time intervals were tested and characterized by optical microscopy (OM), atomic force microscopy (AFM), Raman spectroscopy, transmission electron microscopy (TEM) and electrical measurements. The thickness of Bi-2212 flakes is gradually decreased in water, and some thin flakes can be completely etched away after a few days. The stability of Bi-2212 in other solvents is also evaluated, including alcohol, acetone, HCl and KOH. The morphology of Bi-2212 flakes is relatively stable in organic solvents. However, the flakes are etched relatively quick in HCl and KOH, especially in acidic environment. Our results imply that hydrogen ion is primarily responsible for the deterioration of their properties. Both TEM and calculation results demonstrate that the atoms in Bi-O plane is relatively stable when compared to the inner atoms in Sr-O, Ca-O and Cu-O planes. This work contributes towards understanding the chemical stability of Bi-2212 superconducting device in environmental medium, which is important for both fundamental studies and practical applications of copper oxide high-temperature superconductors.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Engineering polar vortex from topologically trivial domain architecture
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Tan, Congbing↗
Synthesis of Honeycomb-Structured Beryllium Oxide via Graphene Liquid Cells
Using high-resolution transmission electron microscopy and electron energy-loss spectroscopy, we demonstrate that beryllium oxide crystallizes in the planar hexagonal structure in a graphene liquid cell by a wet-chemistry approach. These liquid cells can feature van-der-Waals pressures up to 1 GPa, producing a miniaturized high-pressure container for the crystallization in solution. The thickness of as-received crystals is beyond the thermodynamic ultra-thin limit above which the wurtzite phase is energetically more favorable according to the theoretical prediction. The crystallization of the planar phase is ascribed to the near-free-standing condition afforded by the graphene surface. Our calculations show that the energy barrier of the phase transition is responsible for the observed thickness beyond the previously predicted limit. These findings open a new door for exploring aqueous-solution approaches of more metal-oxide semiconductors with exotic phase structures and properties in graphene-encapsulated confined cells.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Enabling Stable Cycling of 4.2 V High-Voltage All-Solid-State Batteries with PEO-Based Solid Electrolyte
Poly(ethylene oxide) (PEO)-based solid electrolytes are expected to be exploited in solid-state batteries with high safety. Its narrow electrochemical window, however, limits the potential for high voltage and high energy density applications. In this paper, the electrochemical oxidation behavior of PEO and the failure mechanisms of LiCoO 2 -PEO solid-state batteries are studied. It is found that although for pure PEO it starts to oxidize at a voltage of above 3.9 V versus Li/Li + , the decomposition products have appropriate Li + conductivity that unexpectedly form a relatively stable cathode electrolyte interphase (CEI) layer at the PEO and electrode interface. The performance degradation of the LiCoO 2 -PEO battery originates from the strong oxidizing ability of LiCoO 2 after delithiation at high voltages, which accelerates the decomposition of PEO and drives the self-oxygen-release of LiCoO 2 , leading to the unceasing growth of CEI and the destruction of the LiCoO 2 surface. When LiCoO 2 is well coated or a stable cathode LiMn 0.7 Fe 0.3 PO 4 is used, a substantially improved electrochemical performance can be achieved, with 88.6% capacity retention after 50 cycles for Li 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 coated LiCoO 2 and 90.3% capacity retention after 100 cycles for LiMn 0.7 Fe 0.3 PO 4 . The results suggest that, when paired with stable cathodes, the PEO-based solid polymer electrolytes could be compatible with high voltage operation.
25 ENERGY STORAGE↗
Revealing High Na-Content P2-Type Layered Oxides as Advanced Sodium-Ion Cathodes
Layered Na-based oxides with the general composition of Na x TMO 2 (TM: transition metal) have attracted significant attention for their high compositional diversity that provides tunable electrochemical performance for electrodes in sodium-ion batteries. The various compositions bring forward complex structural chemistry that is decisive for the layered stacking structure, Na-ion conductivity, and the redox activity, potentially promising new avenues in functional material properties. In this work, we have explored the maximum Na content in P2-type layered oxides and discovered that the high-content Na in the host enhances the structural stability; moreover, it promotes the oxidation of low-valent cations to their high oxidation states (in this case Ni 2+ ). This can be rationalized by the increased hybridization of the O(2p)-TM(3d-e g *) states, affecting both the local TM environment as well as the interactions between the NaO 2 and TMO 2 layers. These properties are highly beneficial for the Na storage capabilities as required for cathode materials in sodium-ion batteries. It leads to excellent Na-ion mobility, a large storage capacity (>100 mAh g –1 between 2.0-4.0 V), yet preventing the detrimental sliding of the TMO 2 layers (P2–O2 structural transition), as reflected by the ultralong cycle life (3000 (dis)charge cycles demonstrated). These findings expand the horizons of high Na-content P2-type materials, providing new insights of the electronic and structural chemistry for advanced cathode materials.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Visualizing Anisotropic Oxygen Diffusion in Ceria under Activated Conditions
Oxygen reactivity plays a key role in the performance of ceria-based catalysts. Aberration-corrected transmission electron microscopy and molecular dynamics simulations were used to study the oxygen atom diffusion in ceria under activated conditions. Reactive oxygen atom and its real-time diffusion were visualized. Additionally, the interplay between cerium and oxygen atoms originating from a Coulomb interaction was revealed by the out-of-plane buckling of cerium atoms associated with oxygen transport. Anisotropic oxygen atom diffusion that depends on crystal orientations was discovered, demonstrating a preferential [001] crystallographic diffusion pathway. These findings reveal prospects for applications of anisotropic orientation-relevant fluorite-structured oxides.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Ti Substitution Facilitating Oxygen Oxidation in Na2/3Mg1/3Ti1/6Mn1/2O2 Cathode
Not provided.
Chemistry↗
Diffusion-controlled alloying of single-phase multi-principal transition metal carbides with high toughness and low thermal diffusivity
Multicomponent alloying has displayed extraordinary potential for producing exceptional structural and functional materials. Consequently, the synthesis of single-phase, multi-principal covalent compounds remains a challenge. Here, we present a diffusion-controlled alloying strategy for the realization of covalent multi-principal transition metal carbides (MPTMCs) with a single face-centered cubic phase. The increased interfacial diffusion promoted by the addition of a nonstoichiometric compound leads to rapid formation of the single phase at much lower sintering temperature. Direct atomic-level observations via scanning transmission electron microscopy demonstrate that MPTMCs are composed of a single phase with a random distribution of all cations, which holds the key to the unique combinations of improved fracture toughness, superior Vickers hardness, and extremely lower thermal diffusivity achieved in MPTMCs. Conclusively, the present discovery provides a promising approach toward the design and synthesis of next-generation high-performance materials.
36 MATERIALS SCIENCE↗
Rate mechanism of vanadium oxide coated tin dioxide nanowire electrode for lithium ion battery
Correlating composition and structures with battery performance is key aspect of electrode material design and improvement. Here utilizing in situ open cell transmission electron microscopy, we studied the in situ cycling rate performance of vanadium oxide coated tin dioxide nanowire electrode by tuning the lithiation/delithiation current. In situ results show that the good rate performance of such high capacity compositional material lies in the layered vanadium oxide coating strategy. For cycling at high rate, the layered vanadium oxide also serves as fast ions and electrons transportation route while tin nanoparticles aggregate to the surface with sizes controlled by the coating layer, cycle induced volume change is released to the surface and excellent mechanical tolerance of tin nanoparticle and inner nanowire ensure improved cyclability of the electrode.
25 ENERGY STORAGE↗
In-situ transmission electron microscopy imaging of formation and evolution of Li{sub x}WO{sub 3} during lithiation of WO{sub 3} nanowires
The phase transition from monoclinic WO{sub 3} to cubic Li{sub x}WO{sub 3} during lithiation of WO{sub 3} is one of the key features for tungsten oxide as the most used electrochromic material. Conventionally, the lithium intercalation of WO{sub 3} has been studied by building generic layered electrochromic device combining with structural characterization and electrochemistry measurement at macro scale. In-situ transmission electron microscopy (in-situ TEM) has been proposed as a method for revealing the detailed mechanism of structural, physical, and chemical properties. Here, we use in-situ TEM method to investigate the formation and evolution of Li{sub x}WO{sub 3} in real-time during the electrochemical lithiation of WO{sub 3} nanowires. The dynamic lithiation process is recorded by TEM imaging, diffraction, and electron energy loss spectroscopy. The WO{sub 3}-Li{sub x}WO{sub 3} phase boundary of reaction front has been observed at high resolution. The timeliness of crystallinity of Li{sub x}WO{sub 3} and the intercalation channels for Li ions are also identified. Moreover, the co-existence of both polycrystalline Li-poor area and amorphous Li-rich phases of Li{sub x}WO{sub 3} was found. Our results provide an insight into the basic lithiation process of WO{sub 3}, which is significantly important for understanding the electrochromic mechanism of tungsten oxide.
36 MATERIALS SCIENCE↗
Real-time observation of dynamic process of oxygen vacancy migration in cerium oxides under electric field
The dynamic process of oxygen vacancy migration driven by the external electric field is directly observed at atomic scale in the cerium oxides (CeO{sub 2}) thin film by in-situ transmission electron microscopy method. When a bias voltage of a proper value is applied across the CeO{sub 2} film, the oxygen vacancies are formed near the interface of CeO{sub 2}/anode, followed by their migration along the direction of the external electric field. The structural modulation occurs in the [110] zone axis due to the ordering of oxygen vacancies. The migration of oxygen vacancies results in the reversible structural transformation, i.e., releasing and storing oxygen processes in CeO{sub 2}, which is of great significance for the ionic and electronic applications of the cerium oxides materials, such as oxygen pump, gas sensor, resistive random access memory, etc.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
In-situ optical transmission electron microscope study of exciton phonon replicas in ZnO nanowires by cathodoluminescence
The cathodoluminescence spectrum of single zinc oxide (ZnO) nanowires is measured by in-situ optical Transmission Electron Microscope. The coupling between exciton and longitudinal optical phonon is studied. The band edge emission varies for different excitation spots. This effect is attributed to the exciton propagation along the c axis of the nanowire. Contrary to free exciton emission, the phonon replicas are well confined in ZnO nanowire. They travel along the c axis and emit at the end surface. Bending strain increases the relative intensity of second order phonon replicas when excitons travel along the c-axis.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Ferroelectric Gated Electrcial Transport in CdS Nanotetrapods
Complex nanostructures such as semiconductor nanotetrapods are promising building blocks for next-generation nanoelectronics. Here we construct a field effect transistor (FET) based on single CdS nanotetrapods with a ferroelectric Ba0.7Sr0.3TiO3 (BST) film as high- , switchable gate dielectric. A cryogenic four-probe scanning tunneling microscopy (STM) is used to probe the electrical transport through individual nanotetrapods, which reveals a p-type field effect up to room temperature. The conductance modulation in the FET originates from the channel tuning in the arm-core-arm junctions of nanotetrapods, displaying a single-electron transistor effect at low temperature (8.5 K). The ferroelectric gate dielectric enables not only an enhanced capacitance coupling but the non-volatile memory effect as well. A proof-of-principle of ferroelectric FET operation has thus been demonstrated in a nanoscale three-dimensional object and at the single electron level.
Fu, Wangyang↗