High-voltage electrosynthesis of organic-inorganic hybrid with ultrahigh fluorine content toward fast Li-ion transport.

Hybrid materials with a rational organic-inorganic configuration can offer multifunctionality and superior properties. This principle is crucial but challenging to be applied in designing the solid electrolyte interphase (SEI) on lithium metal anodes (LMAs), as it substantially affects Li transport from the electrolyte to the anode. Here, an artificial SEI with an ultrahigh fluorine content (as high as 70.

In Situ Construction of a Multifunctional Interphase Enabling Continuous Capture of Unstable Lattice Oxygen Under Ultrahigh Voltages.

The use of nickel-rich layered materials as cathodes can boost the energy density of lithium batteries. However, developing a safe and long-term stable nickel-rich layered cathode is challenging primarily due to the release of lattice oxygen from the cathode during cycling, especially at high voltages, which will cause a series of adverse effects, leading to battery failure and thermal runaway. Surface coating is often considered effective in capturing active oxygen species; however, its process is rather complicated, and it is difficult to maintain intact on the cathode with large volume changes during cycling.

A locally solvent-tethered polymer electrolyte for long-life lithium metal batteries.

Solid polymer electrolytes exhibit enhanced Li conductivity when plasticized with highly dielectric solvents such as N,N-dimethylformamide (DMF). However, the application of DMF-containing electrolytes in solid-state batteries is hindered by poor cycle life caused by continuous DMF degradation at the anode surface and the resulting unstable solid-electrolyte interphase. Here we report a composite polymer electrolyte with a rationally designed Hofmann-DMF coordination complex to address this issue.

Formation of 2D Amorphous Lithium Sulfide Enabled by MoC Clusters Loaded Carbon Scaffold for High-Performance Lithium Sulfur Batteries.

Lithium-sulfur (Li-S) batteries, operated through the interconversion between sulfur and solid-state lithium sulfide, are regarded as next-generation energy storage systems. However, the sluggish kinetics of lithium sulfide deposition/dissolution, caused by its insoluble and insulated nature, hampers the practical use of Li-S batteries. Herein, leaf-like carbon scaffold (LCS) with the modification of MoC clusters (MoC@LCS) is reported as host material of sulfur powder.

Ultralong Cycling and Safe Lithium-Sulfur Pouch Cells for Sustainable Energy Storage.

While layered metal oxides remain the dominant cathode materials for the state-of-the-art lithium-ion batteries, conversion-type cathodes such as sulfur present unique opportunities in developing cheaper, safer, and more energy-dense next-generation battery technologies. There has been remarkable progress in advancing the laboratory scale lithium-sulfur (Li-S) coin cells to a high level of performance. However, the relevant strategies cannot be readily translated to practical cell formats such as pouch cells and even battery pack.

Achieving Stable Lithium Anodes through Leveraging Inevitable Stress Variations via Adaptive Piezoelectric Effect.

Unleashing the potential of lithium-metal anodes in practical applications is hindered by the inherent stress-related challenges arising from their limitless volume expansion, leading to mechanical failures such as electrode cracking, solid electrolyte interphase damage, and dendritic growth. Despite the various protective strategies to "combat" stress in lithium-metal anodes, they fail to address the intrinsic issue fundamentally. Here, a unique strategy is proposed that leverages the stress generated during the battery cycling via the piezoelectric effect, transforming to the adaptive built-in electric field to accelerate lithium-ion migration, homogenize the lithium deposition, and alleviate the stress concentration.

A corrosion inhibiting layer to tackle the irreversible lithium loss in lithium metal batteries.

Reactive negative electrodes like lithium (Li) suffer serious chemical and electrochemical corrosion by electrolytes during battery storage and operation, resulting in rapidly deteriorated cyclability and short lifespans of batteries. Li corrosion supposedly relates to the features of solid-electrolyte-interphase (SEI). Herein, we quantitatively monitor the Li corrosion and SEI progression (e.

Amorphous Chloride Solid Electrolytes with High Li-Ion Conductivity for Stable Cycling of All-Solid-State High-Nickel Cathodes.

Solid electrolytes (SEs) are central components that enable high-performance, all-solid-state lithium batteries (ASSLBs). Amorphous SEs hold great potential for ASSLBs because their grain-boundary-free characteristics facilitate intact solid-solid contact and uniform Li-ion conduction for high-performance cathodes. However, amorphous oxide SEs with limited ionic conductivities and glassy sulfide SEs with narrow electrochemical windows cannot sustain high-nickel cathodes.

Recycled Tandem Catalysts Promising Ultralow Overpotential Li-CO Batteries.

Lithium-carbon dioxide (Li-CO ) batteries are regarded as a prospective technology to relieve the pressure of greenhouse emissions but are confronted with sluggish CO redox kinetics and low energy efficiency. Developing highly efficient and low-cost catalysts to boost bidirectional activities is craved but remains a huge challenge. Herein, derived from the spent lithium-ion batteries, a tandem catalyst is subtly synthesized and significantly accelerates the CO reduction and evolution reactions (CO RR and CO ER) kinetics with an in-built electric field (BEF).

A Semisolvated Sole-Solvent Electrolyte for High-Voltage Lithium Metal Batteries.

Lithium metal batteries (LMBs) coupled with a high-voltage Ni-rich cathode are promising for meeting the increasing demand for high energy density. However, aggressive electrode chemistry imposes ultimate requirements on the electrolytes used. Among the various optimized electrolytes investigated, localized high-concentration electrolytes (LHCEs) have excellent reversibility against a lithium metal anode.

A LaCl-based lithium superionic conductor compatible with lithium metal.

Inorganic superionic conductors possess high ionic conductivity and excellent thermal stability but their poor interfacial compatibility with lithium metal electrodes precludes application in all-solid-state lithium metal batteries. Here we report a LaCl-based lithium superionic conductor possessing excellent interfacial compatibility with lithium metal electrodes. In contrast to a LiMCl (M = Y, In, Sc and Ho) electrolyte lattice, the UCl-type LaCl lattice has large, one-dimensional channels for rapid Li conduction, interconnected by La vacancies via Ta doping and resulting in a three-dimensional Li migration network.

Surface engineering toward stable lithium metal anodes.

The lithium (Li) metal anode (LMA) is susceptible to failure due to the growth of Li dendrites caused by an unsatisfied solid electrolyte interface (SEI). With this regard, the design of artificial SEIs with improved physicochemical and mechanical properties has been demonstrated to be important to stabilize the LMAs. This review comprehensively summarizes current efficient strategies and key progresses in surface engineering for constructing protective layers to serve as the artificial SEIs, including pretreating the LMAs with the reagents situated in different primary states of matter (solid, liquid, and gas) or using some peculiar pathways (plasma, for example).

Stable Operation of Lithium Metal Batteries with Aggressive Cathode Chemistries at 4.9 V.

High-voltage lithium metal batteries (LMBs) pose severe challenges for the matching of electrolytes with aggressive electrodes, especially at low temperatures. Here, we report a rational modification of the Li solvation structure to extend the voltage and temperature operating ranges of conventional electrolytes. Ion-ion and ion-dipole interactions as well as the electrochemical window of solvents were tailored to improve oxidation stability and de-solvation kinetics of the electrolyte.

In-Situ Electrodeposition of Nanostructured Carbon Strengthened Interface for Stabilizing Lithium Metal Anode.

The lithium metal anode (LMA) is regarded as one of the most promising candidates for high-energy Li-ion batteries. However, the naturally formed solid electrolyte interface (SEI) is unsatisfied, which would cause continuous dendrite growth and thus prevent the practical application of the LMA. Herein, a stable electrolytic carbon-based hybrid (ECH) artificial SEI is constructed on the LMA via the in-situ electrodeposition of an electrolyte sovlent at ultrahigh voltage.

Synthesis of NiSe /Fe O Nanotubes with Heteroepitaxy Configuration as a High-Efficient Oxygen Evolution Electrocatalyst.

The rational design of high-efficient non-noble metal electrocatalysts for oxygen evolution reactions (OER) is of significance in electrochemical energy conversion. However, such low-cost but highly active electrocatalysts remain poorly developed because of the daunting synthetic challenge. Here, the synthesis of NiSe /Fe O nanotubes via a facile self-templating strategy, which manifests unique tetragonal morphology, asymmetric hollow interior, and unusual but adaptable heteroepitaxy structure, is reported.

Stable All-Solid-State Lithium Metal Batteries Enabled by Machine Learning Simulation Designed Halide Electrolytes.

Solid electrolytes (SEs) with superionic conductivity and interfacial stability are highly desirable for stable all-solid-state Li-metal batteries (ASSLMBs). Here, we employ neural network potential to simulate materials composed of Li, Zr/Hf, and Cl using stochastic surface walking method and identify two potential unique layered halide SEs, named LiZrCl and LiHfCl, for stable ASSLMBs. The predicted halide SEs possess high Li conductivity and outstanding compatibility with Li metal anodes.

Self-assembled monolayers direct a LiF-rich interphase toward long-life lithium metal batteries.

High-energy density lithium (Li) metal batteries (LMBs) are promising for energy storage applications but suffer from uncontrollable electrolyte degradation and the consequently formed unstable solid-electrolyte interphase (SEI). In this study, we designed self-assembled monolayers (SAMs) with high-density and long-range-ordered polar carboxyl groups linked to an aluminum oxide-coated separator to provide strong dipole moments, thus offering excess electrons to accelerate the degradation dynamics of carbon-fluorine bond cleavage in Li bis(trifluoromethanesulfonyl)imide. Hence, an SEI with enriched lithium fluoride (LiF) nanocrystals is generated, facilitating rapid Li transfer and suppressing dendritic Li growth.

Artificial Heterogeneous Interphase Layer with Boosted Ion Affinity and Diffusion for Na/K-Metal Batteries.

Metallic Na (K) are considered a promising anode materials for Na-metal and K-metal batteries because of their high theoretical capacity, low electrode potential, and abundant resources. However, the uncontrolled growth of Na (K) dendrites severely damages the stability of the electrode/electrolyte interface, resulting in battery failure. Herein, a heterogeneous interface layer consisting of metal vanadium nanoparticles and sodium sulfide (potassium sulfide) is introduced on the surface of a Na (K) foil (i.

Soybean Protein Fiber Enabled Controllable Li Deposition and a LiF-Nanocrystal-Enriched Interface for Stable Li Metal Batteries.

The proliferation of lithium (Li) dendrites stemming from uncontrollable Li deposition seriously limits the practical application of Li metal batteries. The regulation of uniform Li deposition is thus a prerequisite for promoting a stable Li metal anode. Herein, a commercial lithiophilic skeleton of soybean protein fiber (SPF) is introduced to homogenize the Li-ion flux and induce the biomimetic Li growth behavior.

Construction of Ni(CN) /NiSe Heterostructures by Stepwise Topochemical Pathways for Efficient Electrocatalytic Oxygen Evolution.

Exploiting effective electrocatalysts based on elaborate heterostructures for the oxygen evolution reaction (OER) has been considered as a promising strategy for boosting water splitting efficiency to produce the clean energy-hydrogen. However, constructing catalytically active heterostructures with novel composition and architecture remains poorly developed due to the synthetic challenge. In this work, it is demonstrated that unique Ni(CN) /NiSe heterostructures, composed of single-crystalline Ni(CN) nanoplates surrounded by crystallographically aligned NiSe nanosatellites, can be created from nickel-based Hofmann-type coordination polymers through stepwise topochemical pathways.

Lithium Fluoride in Electrolyte for Stable and Safe Lithium-Metal Batteries.

Electrolyte engineering via fluorinated additives is promising to improve cycling stability and safety of high-energy Li-metal batteries. Here, an electrolyte is reported in a porous lithium fluoride (LiF) strategy to enable efficient carbonate electrolyte engineering for stable and safe Li-metal batteries. Unlike traditionally engineered electrolytes, the prepared electrolyte in the porous LiF nanobox exhibits nonflammability and high electrochemical performance owing to strong interactions between the electrolyte solvent molecules and numerous exposed active LiF (111) crystal planes.

Double-Shelled C@MoS Structures Preloaded with Sulfur: An Additive Reservoir for Stable Lithium Metal Anodes.

The growth of Li dendrites hinders the practical application of lithium metal anodes (LMAs). In this work, a hollow nanostructure, based on hierarchical MoS coated hollow carbon particles preloaded with sulfur (C@MoS /S), was designed to modify the LMA. The C@MoS hollow nanostructures serve as a good scaffold for repeated Li plating/stripping.