Recharging primary batteries is of great importance for increasing the energy density of energy storage systems to power electric aircraft and beyond. Carbon fluoride (CF) cathodes are characterized by high specific capacity and energy density (865 mAh g and 2180 Wh kg, respectively). Preventing the crystallization of LiF with an intermediate and lowering the energy barrier from LiF to CF is expected to render the Li/CF battery reversible.
View Article and Find Full Text PDFThe solid electrolyte interphase (SEI) membrane on the Li metal anode tends to breakdown and undergo reconstruction during operation, causing Li metal batteries to experience accelerated decay. Notably, an SEI membrane with self-healing characteristics can help considerably in stabilizing the Li-electrolyte interface; however, uniformly fixing the repairing agent onto the anode remains a challenging task. By leveraging the noteworthy film-forming attributes of bis(fluorosulfonyl)imide (FSI) anions and the photopolymerization property of the vinyl group, the ionic liquid 1-vinyl-3-methylimidazolium bis(fluorosulfonyl)imide (VMI-FSI) was crosslinked with polyethylene oxide (PEO) in this study to form a self-healing film fixing FSI groups as the repairing agent.
View Article and Find Full Text PDFNi-rich cathode materials suffer from rapid capacity fading caused by interface side reactions and bulk structure degradation. Previous studies show that Co is conducive to bulk structure stability and sulfate can react with the residual lithium (LiOH and LiCO) on the surface of Ni-rich cathode materials and form a uniform coating to suppress the side reactions between the cathode and electrolyte. Here, CoSO is utilized as a modifier for LiNiCoMnO (NCM811) cathode materials.
View Article and Find Full Text PDFThe comprehensive performance of the state-of-the-art solid-state electrolytes (SSEs) cannot match the requirements of commercial applications, and constructing an organic-inorganic composite electrolyte on a porous electrode is an effective coping strategy. However, there are few studies focused on the influence of inorganic ceramics on the polymerization of multi-organic components. In this study, it was found that the addition of LiLaZrTaO (LLZO) weakens the interaction between different polymers and makes organic and inorganic components contact directly in the solid electrolyte.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2022
Li- and Mn-rich cathodes (LMRs) with cationic and anionic redox reactions are considered as promising cathode materials for high-energy-density Li-ion batteries. However, the oxygen redox process leads to lattice oxygen loss and structure degradation, which would induce serious voltage fade and capacity loss and thus limit the practical application. High-valent and electrochemical inactive d element doping is an effective method to tune the crystal and electronic structures, which are the main factors for the electrochemical stability.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2021
Surficial residual LiOH and/or LiCO on Ni-rich cathodes arouse troubles for their practical applications, such as slurry gelling and durability degrading. To assure acceptable performance, the strategy of "washing and heat treatment" is generally utilized to remove them in industry, which is unavoidable to generate plenty of wastewater. In this work, we investigated the mechanism of slurry gelling caused by residual lithium on Ni-rich materials and then proposed a simple and efficient method to convert the detrimental residual lithium to the useful surface layer of LiF or LiBOB at 220 °C without water washing.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2021
In this work, a novel multilayer solid electrolyte interphase (SEI) is demonstrated to prolong the durability of a lithium-metal anode. It is generated via reducing lithium bis(oxalate) borate (LiBOB) and fluoroethylene carbonate (FEC) in the electrolyte containing them as additives. The as-obtained SEI could be roughly divided into three layers: the polycarbonates surface membrane, LiF-rich middle layer, and B-containing polymer bottom film corresponding to their sequentially reductive potentials of 0.
View Article and Find Full Text PDFACS 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 PDFA general polymer-assisted spinodal decomposition strategy is used to prepare hierarchically porous sodium super ionic conductor (NASICON)-structured polyanion-type materials (e.g., Na V (PO ) , Li V (PO ) , K V (PO ) , Na MnV(PO ) , and Na TiV(PO ) ) in a tetrahydrofuran/ethanol/H O synthesis system.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2021
Ni-rich layered materials are widely accepted as pivotal cathode materials to realize low-cost high-energy-density batteries. However, they still suffer from the intrinsic mechanically induced degradation due to the large lattice deformation. Here, we fabricate a strengthened shell layer on polycrystalline secondary particles to address the unfavorable influence of particle cracking instead of suppressing their bulky pulverization.
View Article and Find Full Text PDFA polycarboxylic/ether composite polymer electrolyte derived from two-arm monomer and polyethylene oxide (PEO) was synthesized on the cathode. The composite electrolyte exhibits a high ionic conductivity of 3.6 × 10 S cm, high oxidation stability, excellent stability towards Li metal and makes Li/LiFePO present good cyclic and rate performance at 25°C.
View Article and Find Full Text PDFLiLaZrTaO (LLZTO) and polyvinylidene fluoride (PVDF) composite electrolytes (LPCEs) with a high ceramic content up to 80 wt% have been developed. Hot pressing can significantly reduce the porosity of LPCEs and increase the conductivity to 1.08 × 10 S cm at 60 °C, then the LPCEs can sustain Li plating/stripping cycling for over 1500 h, and make LiFePO/LPCE/Li cell display a capacity retention of 86% in 200 cycles.
View Article and Find Full Text PDFACS Appl Mater Interfaces
June 2020
Lithium metal is considered to be the ultimate anode for lithium-ion batteries (LIBs) because of its ultrahigh capacity and lowest electrochemical potential. However, the high reactivity of the lithium metal triggers continuous electrolyte consumption and dendrite growth, resulting in short cycle lifetime and serious safety issues. Massive efforts have been made to stabilize the surface of the lithium metal anode.
View Article and Find Full Text PDFSodium metal anode (SMA) is one of the most favored choices for the next-generation rechargeable battery technologies owing to its low cost and natural abundance. However, the poor reversibility resulted from dendrite growth and formation of unstable solid electrolyte interphase has significantly hindered the practical application of SMAs. Herein, we report that a nucleation buffer layer comprising elaborately designed core-shell C@Sb nanoparticles (NPs) enables the homogeneous electrochemical deposition of sodium metal for long-term cycling.
View Article and Find Full Text PDFFast ion conduction in solid-state matrices constitutes the foundation for a wide spectrum of electrochemical systems that use solid electrolytes (SEs), examples of which include solid-state batteries (SSBs), solid oxide fuel cells (SOFCs), and diversified gas sensors. Mixing different solid conductors to form composite solid electrolytes (CSEs) introduces unique opportunities for SEs to possess exceptional overall performance far superior to their individual parental solids, thanks to the abundant chemistry and physics at the new interfaces thus created. In this review, we provide a comprehensive and in-depth examination of the development and understanding of CSEs for SSBs, with special focus on their physiochemical properties and mechanisms of ion transport therein.
View Article and Find Full Text PDFLayered germanium phosphide (GeP), a recently developed two-dimensional material, promises highly attractive theoretical capacity for use as a lithium-ion battery anode. Here, we comprehensively investigate its electrochemical performance and the modification mechanism. GeP flakes demonstrate large initial discharge/charge capacity and high initial Coulombic efficiency.
View Article and Find Full Text PDFNi-rich cathode materials LiNiCoMnO ( ≥ 0.6) have attracted much attention due to their high capacity and low cost. However, they usually suffer from rapid capacity decay and short cycle life due to their surface/interface instability, accompanied by the high Ni content.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2020
Sodium metal is an ideal anode material for metal rechargeable batteries, owing to its high theoretical capacity (1166 mAh g ), low cost, and earth-abundance. However, the dendritic growth upon Na plating, stemming from unstable solid electrolyte interphase (SEI) film, is a major and most notable problem. Here, a sodium benzenedithiolate (PhS Na )-rich protection layer is synthesized in situ on sodium by a facile method that effectively prevents dendrite growth in the carbonate electrolyte, leading to stabilized sodium metal electrodeposition for 400 cycles (800 h) of repeated plating/stripping at a current density of 1 mA cm .
View Article and Find Full Text PDFManganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries (ZIBs) because of the low price and high security. However, the practical application of MnO in ZIBs is still plagued by the low specific capacity and poor rate capability. Herein, highly crystalline MnO materials with interconnected mesostructures and controllable pore sizes are obtained via a ligand-assisted self-assembly process and used as high-performance electrode materials for reversible aqueous ZIBs.
View Article and Find Full Text PDFHard carbon materials are considered as the most promising anode for sodium-ion batteries (SIBs). However, the high cost and poor rate performance hinder their application in SIBs. Moreover, the controversial mechanism of Na-ion storage restricts the improvement of hard carbon anodes.
View Article and Find Full Text PDFAs one type of bifunctional oxygen electrocatalyst for Zn-air battery, herein, FeNi alloy was successfully embedded into N-doped carbon with tailored architectures by integrating MOF precursor method and polymer coating/encapsulation strategy. The content of Fe in primary precursor has been proven to be able to obviously affect the morphology of the final catalyst. Benefiting from the mature active site (e.
View Article and Find Full Text PDFACS Appl Mater Interfaces
August 2019
The state-of-the-art electrolytes utilized in lithium-ion batteries are based on liquid carbonates combining a number of additives to fulfill the practical requirements including safety and low temperature. The plenty of components result in the quadruple times of probable radical groups involved into the interfacial reactions, rendering it too difficult to control the surface layer. This work tends to simplify the system with the fluorine-substituted ether as the functional cosolvent to expand the functions of basic electrolytes.
View Article and Find Full Text PDFIn this work, mesoporous hard carbon materials were synthesized and modified by compositing a carbon coating and carbon nanotubes (CNTs), reducing the surface area and improving the conductivities without changing the microstructures of the anodes, which enhances the coulombic efficiencies and rate performances of sodium-ion batteries (SIBs).
View Article and Find Full Text PDFA hexagonal FeSe nanoparticle anode with a novel reaction mechanism and mechanical stability may fully facilitate the desirable rate capability and cycling performance in sodium-ion batteries. In situ TEM reveals that hexagonal FeSe nanoparticle transition to the Fe and Na2Se phase during sodiation, while the products transform to the tetragonal FeSe phase after desodiation.
View Article and Find Full Text PDFBattery materials, which store energy by combining mechanisms of intercalation, conversion, and alloying, provide promisingly high energy density but usually suffer from fast capacity decay due to the drastic volume change upon cycling. Particularly, the significant volume shrinkage upon mass (Li, Na, etc.) extraction inevitably leads to the formation of pores in materials and their final pulverization after cycling.
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