solid electrolyte interface

The organization of water molecules and ions between charged mineral surfaces determines the stability of colloidal suspensions and the strength of phase-separated particulate gels. In this article, we assemble a density functional that measures the free energy due to the interaction of water molecules and ions in electric double layers. The model accounts for the finite size of the particles using fundamental measure theory, hydrogen-bonding between water molecules using Wertheim's statistical association theory, long-range dispersion interactions using Barker and Henderson's high-temperature expansion, electrostatic correlations using a functionalized mean-spherical approximation, and Coulomb forces through the Poisson equation...

Stabilizing the Zn anode/electrolyte interface is critical for advancing aqueous zinc ion storage technologies. Addressing this challenge helps minimize parasitic reactions and controls the formation of Zn dendrites, which is fundamental to achieving highly reversible Zn electrochemistry. In this study, 2% by volume of dimethyl sulfoxide (DMSO) is introduced into the baseline zinc sulfate (ZS) electrolyte, which acts as an efficient regulator to form a robust solid-electrolyte interphase (SEI) on the Zn anode...

All-solid-state lithium batteries (ASSLBs) are attracting tremendous attention due to their improved safety and higher energy density. However, the use of a metallic lithium anode poses a major challenge due to its low stability and processability. Instead, the graphite anode exhibits high reversibility for the insertion/deinsertion of lithium ions, giving ASSLBs excellent cyclic stability but a lower energy density. To increase the energy density of ASSLBs with the graphite anode, it is necessary to lower the negative/positive (N/P) capacity ratio and to increase the charging voltage...

Solid-state lithium batteries are promising candidates for the next generation high security and high performance batteries. Here, the lignin derived ultra-thin all-solid composite polymer electrolytes (CPEs) with a thickness of only 13.2 μm, which possessed three dimensional nanofiber ionic bridge networks composed of single-ion lignin based lithium (L-Li) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) as the framework, and poly(ethylene oxide)/lithium bis(trifluoromethanesulfonyl)imide (PEO/LiTFSI) as the filler, was obtained through electrospinning/spraying and hot-pressing process...

Silicon is drawing attention as an emerging anode material for the next generation of lithium-ion batteries due to its higher capacity compared with commercial graphite. However, silicon anions formed during lithiation are highly reactive with binder and electrolyte components, creating an unstable SEI layer and limiting the calendar life of silicon anodes. The reactivity of lithium silicide and the formation of an unstable SEI layer are mitigated by utilizing a mixture of Ca and Mg multivalent cations as an electrolyte additive for Si anodes to improve their calendar life...

Li‒O2 batteries possess the highest theoretical gravimetric energy density among all types of secondary batteries, but they are still far from practical applications. The poor rate performance resulting from the slow mass transfer is one of the primary obstacles in Li‒O2 batteries. To solve this issue, we have designed a rotating cathode with periodic changes of the electrolyte layer thickness, decoupling the maximum transfer rate of Li+ and O2 . During rotating, the thinner electrolyte layer on cathode facilitates the O2 transfer and the thicker electrolyte layer enhances the Li+ transfer...

All-solid-state lithium batteries (ASSLBs) are considered promising energy storage systems due to their high energy density and inherent safety. However, scalable fabrication of ASSLBs based on transition metal sulfide cathodes through the conventional powder cold-pressing method with ultrahigh stacking pressure remains challenging. This article elucidates a dry process methodology for preparing flexible and high-performance FeS2 -based ASSLBs under low stack pressure by utilizing polytetrafluoroethylene (PTFE) binder...

Quasi-solid polymer electrolyte (QPE) lithium (Li)-metal battery holds significant promise in the application of high-energy-density batteries, yet it suffers from low ionic conductivity and poor oxidation stability. Herein, a novel self-built electric field (SBEF) strategy is proposed to enhance Li+ transportation and accelerate the degradation dynamics of carbon-fluorine bond cleavage in LiTFSI by optimizing the termination of MXene. Among them, the SBEF induced by dielectric Nb4C3F2 MXene effectively constructs highly conductive LiF-enriched SEI and CEI stable interfaces, moreover, enhances the electrochemical performance of the QPE...

The practical application of rechargeable aqueous zinc-ion batteries (ZIBs) has been severely hindered by detrimental dendrite growth, uncontrollable hydrogen evolution, and unfavorable side reactions occurring at the Zn metal anode. Here, we applied a Prussian blue analogue (PBA) material K2 Zn3 (Fe(CN)6 )2 as an artificial solid electrolyte interphase (SEI), by which the plentiful -C≡N- ligands at the surface and the large channels in the open framework structure can operate as a highly zincophilic moderator and ion sieve, inducing fast and uniform nucleation and deposition of Zn...

Sodium-metal batteries (SMBs) are ideal for large-scale energy storage due to their stable operation and high capacity. However, they have safety issues caused by severe dendrite growth and side reactions, particularly when using liquid electrolytes. Therefore, it is critically important to develop electrolytes with high ionic conductivity and improved safety that are non-flammable and resistant to dendrites. Here, we developed polymerized polyethylene glycol diacrylate (PEGDA)-modified poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) electrolytes (PPEs) with highly conductive sodium bis(trifluoromethanesulfonyl)imide and corrosion-inhibitive sodium bis(oxalato)borate salts for SMBs...

Polymer polyacrylonitrile (PAN), with exceptional mechanical strength and ionic conductivity, is considered a potential electrolyte. However, the huge interfacial impedance of PAN-derived C≡N polar nitrile groups and Li anode limited its application. In this study, a double-stabilized interface was integrated by in situ polymerization of DOL between electrodes and a three-dimensional (3D) porous PAN polymer matrix containing SN plasticizer and LLZTO ceramic fillers to optimize the challenge of interfacial instability...

The electrochemical interface formed between an electrode and an electrolyte significantly affects the rate and mechanism of the electrode reaction through its structure and properties, which vary across the interface. The scope of the interface has been expanded, along with the development of energy electrochemistry, where a solid-electrolyte interphase may form on the electrode and the active materials change properties near the surface region. Developing a comprehensive understanding of electrochemical interfaces and interphases necessitates three-dimensional spatial resolution characterization...

Inherent dendrite growth and side reactions of zinc anode caused by its unstable interface in aqueous electrolytes severely limit the practical applications of zinc-ion batteries (ZIBs). To overcome these challenges, a protective layer for Zn anode inspired by cytomembrane structure is developed with PVA as framework and silk fibroin gel suspension (SFs) as modifier. This PVA/SFs gel-like layer exerts similar to the solid electrolyte interphase, optimizing the anode-electrolyte interface and Zn2+ solvation structure...

Lithium-ion batteries have found extensive applications due to their high energy density and low self-discharge rates, spanning from compact consumer electronics to large-scale energy storage facilities. Despite their widespread use, challenges such as inherent capacity degradation and the potential for thermal runaway hinder sustainable development. In this study, we introduce a unique approach to synthesize anode materials for lithium-ion batteries, specifically imidazole-intercalated cobalt hydroxide. This innovative material significantly enhances the Li+ desolvation/diffusion reaction and flame-retardant dynamics through complexing and catalytic synergetic effects...

All-solid-state batteries have attracted attention because of their high energy density, safety, and long cycle life. Sulfide active materials exhibit high capacities and enable an enhanced energy density in all-solid-state batteries. In this study, we synthesized electrode-electrolyte bifunctional materials in the system Li2 S-V2 S3 -LiX (X = F, Cl, Br, or I) through a mechanochemical process. In addition, the effects of the addition of lithium halides on the electrochemical properties were investigated. All-solid-state batteries with the Li2 S-V2 S3 -LiI electrode showed the highest capacity of 400 mAh g-1 among all the cells, even though their electronic and ionic conductivities were the same...

High-voltage resistant quasi-solid-state polymer electrolytes (QSPEs) are promising for enhancing the energy density of lithium-metal batteries in practice. However, side reactions occurring at the interfaces between the anodes or cathodes and QSPEs considerably reduce the lifespan of high-voltage LMBs. In this study, a copolymer of vinyl ethylene carbonate (VEC) and poly(ethylene glycol) diacrylate (PEGDA) was used as the framework, with a cellulose membrane (CE) as the supporting layer. Based on density functional theory calculations, 1-butyl-1-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide (Pyr14 TFSI), an ionic liquid, was screened because of its lowest unoccupied molecular orbital energy level as a modifying agent for the in situ P(VEC x -EG y )/Pyr z /LiTFSI@CE QSPEs synthesis...

Constructing an artificial solid electrolyte interphase (SEI) on lithium metal electrodes is a promising approach to address the rampant growth of dangerous lithium morphologies (dendritic and dead Li0 ) and low Coulombic efficiency that plague development of lithium metal batteries, but how Li+ transport behavior in the SEI is coupled with mechanical properties remains unknown. We demonstrate here a facile and scalable solution-processed approach to form a Li3 N-rich SEI with a phase-pure crystalline structure that minimizes the diffusion energy barrier of Li+ across the SEI...

Spin-lattice relaxation measurements are used in 7 Li NMR studies of materials of potential use in solid-state Li-ion batteries as a probe of ion mobility on a fast (nanosecond to picosecond) time scale. The relaxation behavior is often analyzed by assuming exponential behavior or, equivalently, a single T 1 time constant. However, the spin-lattice relaxation of spin I = 3/2 nuclei, such as 7 Li, is in general biexponential; this is a fundamental property of I = 3/2 nuclei and unrelated to any compartmentalization within the solid...

Solid polymer electrolytes (SPEs) have shown great promise in the development of lithium-metal batteries (LMBs), but SPEs' interfacial instability and limited ionic conductivity still prevent their widespread applications. Herein, high-concentration hybrid dual-salt "polymer-in-salt" electrolytes (HDPEs) through formulation optimization were facilely prepared to simultaneously boost ionic conductivity, improve interfacial compatibility, and ensure a wide-temperature-range operation with high safety. An optimized electrolyte (HDPE-0...

Lithium (Li) metal is regarded as the most desirable anode candidates for high-energy-density batteries by virtue of its lowest redox potential and ultrahigh theoretical specific capacity. However, uncontrollable Li dendritic growth, infinite volume variation and unstable solid electrolyte interface (SEI) ineluctably plague its commercialization process. Herein, the three-dimensional (3D) nanofiber functional layers with synergistic soft-rigid feature, consisting of tin oxide (SnO2 )-anchored polyvinylidene fluoride (PVDF) nanofibers, are directly electrospun on copper current collector...