ACS Appl Mater Interfaces
September 2021
The LiCoO cathode undergoes undesirable electrochemical performance when cycled with a high cut-off voltage (≥4.5 V versus Li/Li). The unstable interface with poor kinetics is one of the main contributors to the performance failure.
View Article and Find Full Text PDFMetallic lithium (Li) has been regarded as an ideal candidate for anode materials in next-generation high-energy-density batteries. However, a ubiquitous spongy Li deposition results in low reversibility, huge interfacial impedance, and even safety issues, hindering its practical application. Herein, we proposed a bifunctional electrolyte (BiFE) to avoid the spongy Li deposition, in which lithium nitrate (LiNO) facilitates a uniform granular Li nucleation via forming a kinetically favorable solid electrolyte interphase and silicon dioxide (SiO) adsorbs anions to stabilize the electric field distribution near the electrode surface.
View Article and Find Full Text PDFLayered LiCoO has drawn tremendous attention as a modeling cathode for Li-ion batteries, while its structural instability, especially in the high delithiation region, remains unsolved. With the aim of revealing the structural fundamentals, LiCoO electrodes are investigated at a long delithiation range using both in situ and ex situ techniques. In the highly delithiated LiCoO electrode, the unique charge compensation process leads to a spatial charge gradient of Co/Co/Co ions from surface to bulk, which can be further manipulated by structural distortion, Li extraction, and surface side reactions.
View Article and Find Full Text PDFAlthough the layered P2-type NaNiMnO materials show high discharge voltage and specific capacity, they suffer from severe structural instabilities and surface reaction upon Na exchange for sodium-ion batteries (SIBs). Therefore, it is quite necessary to reveal the underlying structural evolution mechanism and diffusion kinetics to improve the structural/electrochemical stability for application in SIBs. Here, we synthesize a P2-type NaAlNiMnO material by a small dose of Al replacing the Mn, aiming at enhancing the structural stability without sacrificing the average discharge voltage and theoretical capacity.
View Article and Find Full Text PDFThe electrochemical insertion of Li into graphite initiates a series of thermodynamic and kinetic processes. An in-depth understanding of this phenomenon will deepen the knowledge of electrode material design and optimize rechargeable Li batteries. In this context, the phase transition from dense stage II (LiC) to stage I (LiC) was comprehensively elucidated in a graphite anode via both experimental characterizations and first-principles calculations.
View Article and Find Full Text PDFNanotechnology and carbon coating have been applied to silicon anodes to achieve excellent lithium-ion batteries, but the exclusive influence of carbon coating on solid-electrolyte interphase (SEI) formation is difficult to exhibit distinctly because of the impurity and morphological irregularity of most nanostructured anodes. Here, we design a silicon nanocone-carbon (SNC-C) composite structure as a model anode to demonstrate the significant influences of carbon coating on SEI formation and electrochemical performance, unaffectedly as a result of pure electrode component and distinctly due to regular nanocone morphology. As demonstrated by morphological and elemental analysis, compared to the SNC electrode, the SNC-C electrode maintains a thinner SEI layer (∼10 nm) and more stable structure during cycling as well as longer cycle life (>725 cycles), higher Coulombic efficiency (>99%), and lower electrode polarization.
View Article and Find Full Text PDFThe electronic and ionic conductivity of the LiF-Ti nanocomposite films prepared by the co-sputtering have been investigated by the method of impedance spectrum (IS), current-voltage curves (IV) and isothermal transient ionic current (ITIC) measurements. It is found that the ionic conductivity of the obtained LiF-Ti nanocomposite film is very low. After electrochemical and chemical lithiation, ionic conductivities of the lithiated composite films are increased to be 10-3 and 10-4 S/cm separately.
View Article and Find Full Text PDFThickness, homogeneity and coverage of the surface passivation layer on Si anodes for Li-ion batteries have decisive influences on their cyclic performance and coulombic efficiency, but related information is difficult to obtain, especially during cycling. In this work, a well-defined silicon nanocone (SNC) on silicon wafer sample has been fabricated as a model electrode in lithium ion batteries to investigate the growth of surface species on the SNC electrode during cycling using ex situ scanning electronic microscopy. It is observed that an extra 5 μm thick layer covers the top of the SNCs after 25 cycles at 0.
View Article and Find Full Text PDFRechargeable metallic lithium batteries are the ultimate solution to electrochemical storage due to their high theoretical energy densities. One of the key technological challenges is to control the morphology of metallic lithium electrode during electrochemical dissolution and deposition. Here we have investigated the morphology change of metallic lithium electrode after charging and discharging in nonaqueous batteries by ex situ SEM techniques from a top view.
View Article and Find Full Text PDFThe microstructure and mechanical properties of the solid electrolyte interphase (SEI) in non-aqueous lithium ion batteries are key issues for understanding and optimizing the electrochemical performance of lithium batteries. In this report, the three-dimensional (3D) multi-layered structures and the mechanical properties of the SEI formed on a silicon anode material for next generation lithium ion batteries have been visualized directly for the first time, through a scanning force spectroscopy method. The coverage of the SEI on silicon anodes is also obtained through 2D projection plots.
View Article and Find Full Text PDFElectrochemical behaviors of nano-textured silicon thin film (NTSTF) coated with Al2O3 or Cu layers as anodes for lithium-ion batteries have been investigated. The cyclic performance of NTSTF electrodes is superior to dense Si thin films. The NTSTF with a 5 nm thick Cu coating layer shows superior cyclic performance and rate performance to other NTSTF samples.
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