The development of potassium-ion batteries (PIBs) faces significant challenges due to the lack of suitable electrolytes to achieve satisfactory energy density and long-term stability. This work reports an innovative compact-solvation electrolyte (CSE) strategy leveraging ionic liquid-induced manipulation of solvation structures under low concentration for high-performance PIBs. The CSE, formulated with a low-salt concentration of 0.
View Article and Find Full Text PDFThe stability of the electrode-electrolyte interface is a critical factor influencing the electrochemical performance of Li-metal batteries. However, on the delithiated Ni-rich cathode surface, the strong catalytic effects of transition metals with coordination deficiency significantly aggravate the parasitic reactions with Li-metal-compatible ether-based electrolytes, thereby reducing the cycling stability of high-voltage Ni-rich batteries. Here, we propose an -induction mechanism to address coordination deficiency through the coupling of interfacial orbitals between molecules and the cathode surface.
View Article and Find Full Text PDFHydrogen fluoride (HF)-induced degradation of electrode materials and interphases presents a significant challenge for high-voltage Li-ion batteries. However, progress in developing advanced HF-scavenging additives is hindered by a limited understanding of HF-elimination reactions and the absence of a robust design principle. Herein, it is proposed to analyze the energy decomposition analysis of 24 additives to elucidate the underlying HF-scavenging mechanism and identify key factors influencing HF-additives reactions.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2025
All-solid-state Li-metal battery (ASSLB) chemistry with thin solid-state electrolyte (SSE) membranes features high energy density and intrinsic safety but suffers from severe dendrite formation and poor interface contact during cycling, which hampers the practical application of rechargeable ASSLB. Here, we propose a universal design of thin Li-metal anode (LMA) via a dynamic stability strategy to address these issues. The ultra-thin LMA (20 μm) is in situ constructed with uniform highly Li-ion conductive solid-electrolyte interphase and composite-polymer interphase (CPI) via electroplating process.
View Article and Find Full Text PDFMachine learning (ML) has emerged as a pioneering tool in advancing the research application of high-performance solid-state hydrogen storage materials (HSMs). This review summarizes the state-of-the-art research of ML in resolving crucial issues such as low hydrogen storage capacity and unfavorable de-/hydrogenation cycling conditions. First, the datasets, feature descriptors, and prevalent ML models tailored for HSMs are described.
View Article and Find Full Text PDFAll-polymer aqueous batteries, featuring electrodes and electrolytes made entirely from polymers, advance wearable electronics through their processing ease, inherent safety, and sustainability. Challenges persist with the instability of polymer electrode redox products in aqueous environments, which fail to achieve high performance in all-polymer aqueous batteries. Here, we report a polymer-aqueous electrolyte designed to stabilize polymer electrode redox products by modulating the solvation layers and forming a solid-electrolyte interphase.
View Article and Find Full Text PDFDeveloping rechargeable batteries with high power delivery at low temperatures (LT) below 0 °C is significant for cold-climate applications. Initial anode-free sodium metal batteries (AFSMBs) promise high LT performances because of the low de-solvation energy and smaller Stokes radius of Na, nondiffusion-limited plating/stripping electrochemistry, and maximized energy density. However, the severe reduction in electrolyte ionic conductivity and formation of unstable solid electrolyte interphase (SEI) hinder their practical applications at LT.
View Article and Find Full Text PDFLiMnO (LMO) is an attractive positive electrode material for aqueous lithium-ion batteries (ALIBs), but its inferior cycle performance limits the practical application. The degradation mechanism of LMO in ALIBs is still unclear, resulting in inability to predictably improve its structural stability. The electrode/electrolyte interface is believed to play an important role in electrode degradation.
View Article and Find Full Text PDFIdeal rechargeable lithium battery electrolytes should promote the Faradaic reaction near the electrode surface while mitigating undesired side reactions. Yet, conventional electrolytes usually show sluggish kinetics and severe degradation due to their high desolvation energy and poor compatibility. Here we propose an electrolyte design strategy that overcomes the limitations associated with Li salt dissociation in non-coordinating solvents to enable fast, stable Li chemistries.
View Article and Find Full Text PDFDeveloping advanced electrolytes has been regarded as a pivotal strategy for enhancing the electrochemical performance of batteries; however, the criteria for electrolyte design remain elusive. In this study, we present an electrolyte design chart reframed through intermolecular interactions. By combining systematic nuclear magnetic resonance, Fourier transform infrared measurements, molecular dynamics (MD) simulations, and machine-learning-assisted classifications, we establish semiquantitative correlations between electrolyte components and the electrochemical reversibility of electrolytes.
View Article and Find Full Text PDFLithium metal batteries face problems from sluggish charge transfer at interfaces, as well as parasitic reactions between lithium metal anodes and electrolytes, due to the strong electronegativity of oxygen donor solvents. These factors constrain the reversibility and kinetics of lithium metal batteries at low temperatures. Here, a nonsolvating cosolvent is applied to weaken the electronegativity of donor oxygen in ether solvents, enabling the participation of anionic donors in the solvation structure of Li.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2024
Rational design of advanced electrolytes to improve the high-voltage capability has been attracting wide attention as one critical solution to enable next-generation high-energy-density batteries. However, the limited understanding of electrolyte antioxidant chemistry as well as the lack of valid quantization approaches have resulted in knowledge gap, which hinders the formulation of new electrolytes. Herein, we construct a standard curve based on representative solvation structures to quantify the oxidation stability of ether-based electrolytes, which reveals the linear correlation between the oxidation potential and the atomic charge of the least oxidation-resistant solvent.
View Article and Find Full Text PDFRechargeable all-solid-state lithium metal batteries (ASSLMBs) utilizing inorganic solid-state electrolytes (SSEs) are promising for electric vehicles and large-scale grid energy storage. However, the Li dendrite growth in SSEs still constrains the practical utility of ASSLMBs. To achieve a high dendrite-suppression capability, SSEs must be chemically stable with Li, possess fast Li transfer kinetics, and exhibit high interface energy.
View Article and Find Full Text PDFTailorable lithium (Li) nucleation and uniform early-stage plating is essential for long-lifespan Li metal batteries. Among factors influencing the early plating of Li anode, the substrate is critical, but a fine control of the substrate structure on a scale of ≈10 nm has been rarely achieved. Herein, a carbon consisting of ordered grids is prepared, as a model to investigate the effect of substrate structure on the Li nucleation.
View Article and Find Full Text PDFRechargeable lithium-ion batteries (LIBs) have prospered a rechargeable world, predominantly relying on various metal oxide cathode materials for their abilities to reversibly de-/intercalate lithium-ion, while also serving as lithium sources for batteries. Despite the success of metal oxide, issues including low energy density have raised doubts about their suitability for next-generation lithium batteries. This has sparked interest in metal chlorides, a neglected cathode material family.
View Article and Find Full Text PDFProtection of lithium (Li) metal electrode is a core challenge for all-solid-state Li metal batteries (ASSLMBs). Carbon materials with variant structures have shown great effect of Li protection in liquid electrolytes, however, can accelerate the solid-state electrolyte (SE) decomposition owing to the high electronic conductivity, seriously limiting their application in ASSLMBs. Here, a novel strategy is proposed to tailor the carbon materials for efficient Li protection in ASSLMBs, by in situ forming a rational niobium-based Li-rich disordered rock salt (DRS) shell on the carbon materials, providing a favorable percolating Li diffusion network for speeding the carbon lithiation, and enabling simultaneously improved lithiophilicity and reduced electronic conductivity of the carbon structure at deep lithiation state.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
May 2024
Lithium batteries employing Li or silicon (Si) anodes hold promise for the next-generation energy storage systems. However, their cycling behavior encounters rapid capacity degradation due to the vulnerability of solid electrolyte interphases (SEIs). Though anion-derived SEIs mitigate this degradation, the unavoidable reduction of solvents introduces heterogeneity to SEIs, leading to fractures during cycling.
View Article and Find Full Text PDFLi-ion batteries (LIBs) for electric vehicles and aviation demand high energy density, fast charging and a wide operating temperature range, which are virtually impossible because they require electrolytes to simultaneously have high ionic conductivity, low solvation energy and low melting point and form an anion-derived inorganic interphase. Here we report guidelines for designing such electrolytes by using small-sized solvents with low solvation energy. The tiny solvent in the secondary solvation sheath pulls out the Li in the primary solvation sheath to form a fast ion-conduction ligand channel to enhance Li transport, while the small-sized solvent with low solvation energy also allows the anion to enter the first Li solvation shell to form an inorganic-rich interphase.
View Article and Find Full Text PDFThe growth of disorganized lithium dendrites and weak solid electrolyte interphase greatly impede the practical application of lithium metal batteries. Herein, we designed and synthesized a new kind of stable polyimide covalent organic frameworks (COFs), which have a high density of well-aligned lithiophilic quinoxaline and phthalimide units anchored within the uniform one-dimensional channels. The COFs can serve as an artificial solid electrolyte interphase on lithium metal anode, effectively guiding the uniform deposition of lithium ions and inhibiting the growth of lithium dendrites.
View Article and Find Full Text PDFLow temperatures severely impair the performance of lithium-ion batteries, which demand powerful electrolytes with wide liquidity ranges, facilitated ion diffusion, and lower desolvation energy. The keys lie in establishing mild interactions between Li and solvent molecules internally, which are hard to achieve in commercial ethylene-carbonate based electrolytes. Herein, we tailor the solvation structure with low-ε solvent-dominated coordination, and unlock ethylene-carbonate via electronegativity regulation of carbonyl oxygen.
View Article and Find Full Text PDFThe utilization of layered oxides as cathode materials has significantly contributed to the advancement of the lithium-ion batteries (LIBs) with high energy density and reliability. However, the structural and interfacial instability triggered by side reactions when charged to high voltage has plagued their practical applications. Here, this work reports a novel multifunctional additive, id est, 7-Anilino-3-diethylamino-6-methyl fluoran (ADMF), which exhibits unique characteristics such as preferential adsorption, oxygen scavenging, and electropolymerization protection for high-voltage cathodes.
View Article and Find Full Text PDFHigh-performance Li-ion/metal batteries working at a low temperature (i.e., <-20 °C) are desired but hindered by the sluggish kinetics associated with Li transport and charge transfer.
View Article and Find Full Text PDFBioprocess Biosyst Eng
August 2023
Acidified oil is obtained from by-product of crops oil refining industry, which is considered as a low-cost material for fatty acid production. Hydrolysis of acidified oil by lipase catalysis for producing fatty acid is a sustainable and efficient bioprocess that is an alternative of continuous countercurrent hydrolysis. In this study, lipase from Candida rugosa (CRL) was immobilized on magnetic FeO@SiO via covalent binding strategy for highly efficient hydrolysis of acidified soybean oil.
View Article and Find Full Text PDFElectrolyte optimization by solvent molecule design is recognized as an effective approach for stabilizing lithium (Li) metal batteries. However, the coordination pattern of Li ions (Li ) with solvent molecules is sparsely considered. Here, an electrolyte design strategy is reported based on bi/tridentate chelation of Li and solvent to tune the solvation structure.
View Article and Find Full Text PDF