Dual functional coordination interactions enable fast polysulfide conversion and robust interphase for high-loading lithium-sulfur batteries.

The stable operation of high-capacity lithium-sulfur batteries (LSBs) has been hampered by slow conversion kinetics of lithium polysulfides (LiPSs) and instability of the lithium metal anodes. Herein, 6-(dibutylamino)-1,3,5-triazine-2,4-thiol (DTD) is introduced as a functional additive for accelerating the kinetics of cathodic conversion and modulating the anode interface. We proposed that a coordination interaction mechanism drives the polysulfide conversion and modulates the Li solvated structure during the binding of the N-active site of DTD to LiPSs and lithium salts.

Breaking Solvation Dominance Effect Enabled by Ion-Dipole Interaction Toward Long-Spanlife Silicon Oxide Anodes in Lithium-Ion Batteries.

Micrometer-sized silicon oxide (SiO) anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process. Herein, an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO anodes. Density functional theory calculations validate a robust ion-dipole interaction between lithium ions (Li) and succinonitrile (SN).

Entropy-Modulated Short-Chain Cathode for Low-Temperature All-Solid-State Li-S Batteries.

All-solid-state Li-S batteries (ASSLSBs) due to high theoretical energy density and exceptional safety are highly desirable for electric aircraft. However, as the flight altitude rises, the low-temperature performance is hampered by inadequate practical capacity. Here, we discover that low-temperature sulfur utilization is constrained by the multi-step endothermic conversion reaction.

Delocalized electronic engineering of TiNbO enables low temperature capability for high-areal-capacity lithium-ion batteries.

High areal capacity and low-temperature ability are critical for lithium-ion batteries (LIBs). However, the practical operation is seriously impeded by the sluggish rates of mass and charge transfer. Herein, the active electronic states of TiNbO material is modulated by dopant and O-vacancies for enhanced low-temperature dynamics.

Light Enables the Cathodic Interface Reaction Reversibility in Solid-State Lithium-Oxygen Batteries.

Limited triple-phase boundaries arising from the accumulation of solid discharge product(s) in solid-state cathodes (SSCs) pose a challenge to high-property solid-state lithium-oxygen batteries (SSLOBs). Light-assisted SSLOBs have been gradually explored as an ingenious system; however, the fundamental mechanisms of the SSCs interface behavior remain unclear. Here, we discovered that light assistance can enhance the fast inner-sphere charge transfer in SSCs and regulate the discharge products with spherical particles generated via the surface growth model.

Enhanced Redox Electrocatalysis in High-Entropy Perovskite Fluorides by Tailoring d-p Hybridization.

High-entropy catalysts featuring exceptional properties are, in no doubt, playing an increasingly significant role in aprotic lithium-oxygen batteries. Despite extensive effort devoted to tracing the origin of their unparalleled performance, the relationships between multiple active sites and reaction intermediates are still obscure. Here, enlightened by theoretical screening, we tailor a high-entropy perovskite fluoride (KCoMnNiMgZnF-HEC) with various active sites to overcome the limitations of conventional catalysts in redox process.

Ion-Dipole-Interaction-Induced Encapsulation of Free Residual Solvent for Long-Cycle Solid-State Lithium Metal Batteries.

Owing to high ionic conductivity and mechanical strength, poly(vinylidene fluoride) (PVDF) electrolytes have attracted increasing attention for solid-state lithium batteries, but highly reactive residual solvents severely plague cycling stability. Herein, we report a free-solvent-capturing strategy triggered by reinforced ion-dipole interactions between Li and residual solvent molecules. Lithium difluoro(oxalato)borate (LiDFOB) salt additive with electron-withdrawing capability serves as a redistributor of the Li electropositive state, which offers more binding sites for residual solvents.

Tailoring the p-Band Center of NS Pair for Accelerating High-Performance Lithium-Oxygen Battery.

The local coordination environment of catalytical moieties directly determines the performance of electrochemical energy storage and conversion devices, such as Li-O batteries (LOBs) cathode. However, understanding how the coordinative structure affects the performance, especially for non-metal system, is still insufficient. Herein, a strategy that introduces S-anion to tailor the electronic structure of nitrogen-carbon catalyst (SNC) is proposed to improve the LOBs performance.

d-p Hybridization-Induced "Trapping-Coupling-Conversion" Enables High-Efficiency Nb Single-Atom Catalysis for Li-S Batteries.

Single-atom catalysts have been paid more attention to improving sluggish reaction kinetics and anchoring polysulfide for lithium-sulfur (Li-S) batteries. It has been demonstrated that -block single-atom elements in the fourth period can chemically interact with the local environment, leading to effective adsorption and catalytic activity toward lithium polysulfides. Enlightened by theoretical screening, for the first time, we design novel single-atom Nb catalysts toward improved sulfur immobilization and catalyzation.

Kirigami-Inspired Flexible Lithium-Ion Batteries via Transformation of Concentrated Stress into Segmented Strain.

Emerging directions in the growing wearable electronics market have spurred the development of flexible energy storage systems that require deformability while maintaining electrochemical performance. However, the traditional fabrication approaches of lithium-ion batteries (LIBs) are challenging to withstand long-cycle bending alternating loads due to the stress concentration caused by the nonuniformity of the actual deformation. Herein, inspired by kirigami, a segmented deformation design of full-cell scale thin-type flexible lithium-ion batteries (FLIBs) with large-scale manufacturing characteristics via the current collector's mechanical blanking process is reported.

DNA Helix Structure Inspired Flexible Lithium-Ion Batteries with High Spiral Deformability and Long-Lived Cyclic Stability.

With the development of flexible devices, it is necessary to design high-performance power supplies with superior flexibility, durability, safety, etc., to ensure that they can be deformed with the device while retaining their electrochemical functions. Herein, we have designed a flexible lithium-ion battery inspired by the DNA helix structure.

Single-Atom Tailored Hierarchical Transition Metal Oxide Nanocages for Efficient Lithium Storage.

Mitigating the mechanical degradation and enhancing the ionic/electronic conductivity are critical but challengeable issues toward improving electrochemical performance of conversion-type anodes in rechargeable batteries. Herein, these challenges are addressed by constructing interconnected 3D hierarchically porous structure synergistic with Nb single atom modulation within a Co O nanocage (3DH-Co O @Nb). Such a hierarchical-structure nanocage affords several fantastic merits such as rapid ion migration and enough inner space for alleviating volume variation induced by intragrain stress and optimized stability of the solid-electrolyte interface.

π-Conjugation Induced Anchoring of Ferrocene on Graphdiyne Enable Shuttle-Free Redox Mediation in Lithium-Oxygen Batteries.

Soluble redox mediators (RMs), an alternative to conventional solid catalysts, have been considered an effective countermeasure to ameliorate sluggish kinetics in the cathode of a lithium-oxygen battery recently. Nevertheless, the high mobility of RMs leads to serious redox shuttling, which induces an undesired lithium-metal degeneration and RM decomposition during trade-off catalysis against the sustainable operation of batteries. Here, a novel carbon family of graphdiyne matrix is first proposed to decouple the charge-carrying redox property of ferrocene and the shuttle effects.

Reversible Silicon Anodes with Long Cycles by Multifunctional Volumetric Buffer Layers.

Establishing a stable, stress-relieving configuration is imperative to achieve a reversible silicon anode for high energy density lithium-ion batteries. Herein, we propose a silicon composite anode (denoted as T-Si@C), which integrates free space and mixed carbon shells doped with rigid TiO/TiSi nanoparticles. In this configuration, the free space accommodates the silicon volume fluctuation during battery operation.

Insights into interfacial effect and local lithium-ion transport in polycrystalline cathodes of solid-state batteries.

Interfacial issues commonly exist in solid-state batteries, and the microstructural complexity combines with the chemical heterogeneity to govern the local interfacial chemistry. The conventional wisdom suggests that "point-to-point" ion diffusion at the interface determines the ion transport kinetics. Here, we show that solid-solid ion transport kinetics are not only impacted by the physical interfacial contact but are also closely associated with the interior local environments within polycrystalline particles.

Interface Issues and Challenges in All-Solid-State Batteries: Lithium, Sodium, and Beyond.

Owing to the promise of high safety and energy density, all-solid-state batteries are attracting incremental interest as one of the most promising next-generation energy storage systems. However, their widespread applications are inhibited by many technical challenges, including low-conductivity electrolytes, dendrite growth, and poor cycle/rate properties. Particularly, the interfacial dynamics between the solid electrolyte and the electrode is considered as a crucial factor in determining solid-state battery performance.

FeOF/TiO Hetero-Nanostructures for High-Areal-Capacity Fluoride Cathodes.

Iron fluoride compounds offer an exciting pathway toward low-cost and high-capacity conversion-type lithium-ion battery (LIB) cathodes. However, due to the sluggishness of the electronic and ionic transport in iron fluorides, mass loadings of active materials in previous studies are typically less than 2.5 mg cm, which is too low for practical applications.

Surface regulation enables high stability of single-crystal lithium-ion cathodes at high voltage.

Single-crystal cathode materials for lithium-ion batteries have attracted increasing interest in providing greater capacity retention than their polycrystalline counterparts. However, after being cycled at high voltages, these single-crystal materials exhibit severe structural instability and capacity fade. Understanding how the surface structural changes determine the performance degradation over cycling is crucial, but remains elusive.

Perovskite LaCoMnO with Tunable Defect and Surface Structures as Cathode Catalysts for Li-O Batteries.

Rechargeable lithium-oxygen batteries have shown great potential as next-generation sustainable and green energy storage systems. The bifunctional catalyst plays an important role in accelerating the cathode kinetics for practical realization of the batteries. Herein, we employ the surface structure and defect engineering to introduce surface-roughened nanolayers and oxygen vacancies on the mesoporous hollow LaCoMnO perovskite catalyst by in situ cation substitution.

Ti-Based Oxide Anode Materials for Advanced Electrochemical Energy Storage: Lithium/Sodium Ion Batteries and Hybrid Pseudocapacitors.

Titanium-based oxides including TiO and M-Ti-O compounds (M = Li, Nb, Na, etc.) family, exhibit advantageous structural dynamics (2D ion diffusion path, open and stable structure for ion accommodations) for practical applications in energy storage systems, such as lithium-ion batteries, sodium-ion batteries, and hybrid pseudocapacitors. Further, Ti-based oxides show high operating voltage relative to the deposition of alkali metal, ensuring full safety by avoiding the formation of lithium and sodium dendrites.

Anisotropically Electrochemical-Mechanical Evolution in Solid-State Batteries and Interfacial Tailored Strategy.

All-solid-state batteries have attracted attention owing to the potential high energy density and safety; however, little success has been made on practical applications of solid-state batteries, which is largely attributed to the solid-solid interface issues. A fundamental elucidation of electrode-electrolyte interface behaviors is of crucial significance but has proven difficult. The interfacial resistance and capacity fading issues in a solid-state battery were probed, revealing a heterogeneous phase transition evolution at solid-solid interfaces.

Scalable submicron/micron silicon particles stabilized in a robust graphite-carbon architecture for enhanced lithium storage.

Silicon-carbon composite is recognized as one of the most promising next-generation anodes for high-energy lithium-ion batteries, especially silicon-graphite composites. Herein, cost-efficient and scalable submicron/micron silicon particles are stabilized in a robust graphite-carbon architecture by solid-phase ball milling and liquid-phase coating methods. The obtained silicon-graphite-carbon composite with a stable encapsulated sandwich-like architecture exhibits impressive lithium storage performance, including high initial Coulombic efficiency of 83.

Unravelling the Interface Layer Formation and Gas Evolution/Suppression on a TiNbO Anode for Lithium-Ion Batteries.

TiNbO (TNO) has been regarded as a promising anode material for high-power lithium-ion batteries because of the high theoretical capacity and rate performance within the operation voltage range of 1.0-3.0 V.