Tailoring Solvation Structures via Precise Diluent Engineering for High-Rate 500 Wh kg Lithium-Metal Batteries.

Lithium metal batteries (LMBs), featuring lithium metal anodes (LMAs) paired with high-voltage cathodes, are promising candidates for achieving energy densities exceeding 500 Wh kg. However, their commercialization is hindered by unstable interphases and insufficient Li transport kinetics, especially under high-rate conditions. Here, a hybrid diluent strategy is reported for diluted high-concentration electrolytes (DHCEs) that decouples Li solvation from interfacial stabilization by combining fluorinated aromatics with fluorinated ethers.

Machine learning-assisted Ru-N bond regulation for ammonia synthesis.

Ruthenium-bearing intermetallics (Ru-IMCs) featured with well-defined structures and variable compositions offer new opportunities to develop ammonia synthesis catalysts under mild conditions. However, their complex phase nature and the numerous controlling parameters pose major challenges for catalyst design and exploration. Herein, we demonstrate that a combination of machine learning (ML) and model mining techniques can effectively address these challenges.

Pauling's Rules Guided Design of High-Entropy Sulfide Solid-State Electrolyte with High Ionic Conductivity and Stability.

All-solid-state lithium batteries (ASSLBs) represent a promising next-generation energy storage technology. While sulfide-based solid-state electrolytes (SSEs) offer high ionic conductivity, their practical application is hindered by inherent instability issues. To further enhance the performance, Pauling's rules are considered.

Honeycomb-Like Porous Carbon Framework with Consecutive Conductive Channels for Stable SiO/C Anodes.

Silicon oxide (SiO) materials have been extensively researched. However, slow intrinsic kinetics and significant volume changes hinder the practical deployment of SiO anodes. Herein, an molecular polymerization strategy, in which a loading substrate (PM) is introduced into a mixed solution of silane, is devised to construct SiO/C composites with honeycomb porous frameworks through one-step condensation followed by carbonization at 900 °C without any template or additive.

Liquid-liquid interfacial tension stabilized Li-metal batteries.

A lithium (Li)-metal anode paired with a high-nickel cathode is considered to be a combination that holds promise to surpass the 500 Wh kg threshold. Approaching such high energy density, electrolytes capable of stabilizing both anode and cathode interphases are of importance to secure safe and long-term cycling. Although anion-derived inorganic interphases have shown remarkable success at the Li side, developing intrinsic strategies to concurrently protect both electrodes remains a key challenge.

Biomimetic Sandwich-Structured Tubular Ion Pump Arrays for Lithium Metal Batteries.

Controlling the rapid, uniform deposition and efficient, stable stripping of Li is crucial for achieving durable high-energy-density Li-metal batteries. Herein, unique biomimetic sandwich-structured tubular ion pump arrays achieved by sandwiching ZnSe nanoparticle tubes between ultrathin N-doped graphene-like layers and vertically aligning on N-doped graphene-Ni foam (NG@ZnSe@NG) are reported, working as a highly efficient and robust Li host for homogeneous and stable Li plating/stripping. After complete lithiation, such a biomimetic tubular ion pump featuring symmetric inner and outer layers with high ion-electron transport rates and a key self-accelerating middle layer is generated, accelerating uniform Li deposition into the interior and efficient stripping of Li from the cavity.

Sandwich-Model Cathode Electrolyte Interphase Facilitating All-Climate High-Voltage Nickel-Rich Cathode-Based Lithium Metal Batteries with LiBF-Based Electrolyte.

All-climate lithium metal batteries are highly needed, but remains a huge challenge in cycling life due to the existence of unstable electrode electrolyte interphases, especially with nickel-rich layered oxide cathode at high cut-off voltage. To address this question, a functional and robust sandwich-model cathode electrolyte interphase (CEI) is proposed, derived from a LiBF-based electrolyte modified with para-fluorobenzeneacetonitrile (P-FBCN) additive, to realize the stability of 4.8 V Li||LiNiCoMnO (NCM94) battery operated from -60 to 60 °C.

Electrolyte engineering enables high-energy Li‖CF battery operation at ultralow temperatures.

A lithium metal‖carbon fluoride (Li‖CF) primary battery offers high energy density and long shelf-life but suffers from poor performance at low temperatures. We report a linear ester-based electrolyte comprising ethyl acetate (EA) and ethyl trifluoroacetate (ET) with LiBF salt to address this challenge. EA served as the primary solvent, while ET acted as an anti-solvent, weakening Li coordination due to its strong electron-withdrawing fluorine atoms.

Wide-Temperature, High-Voltage, Flame-Retardant Electrolyte for 4.8 V Li||NCM94 Batteries.

All-climate lithium metal batteries attract great interest, but their poor safety and cycling performance hinder their applications, especially with high cut-off voltage nickel-rich layered oxide cathode. Herein, we develop a high-voltage, wide-temperature, and flame-retardant electrolyte for Li|| LiNiCoMnO (NCM94) batteries with excellent cycling performance through constructing highly Li-conductive, lithophilic gradient cathode electrolyte interphase (CEI). Such CEI exhibits a gradual decrease in C─F and a gradient increase in LiF and LiBO from the outside to the inside, which effectively inhibits structural degradation of the NCM94 cathode.

Construction of self-supporting PDOL electrolyte membranes for stable solid-state lithium metal batteries.

Poly(1,3-dioxolane) (PDOL) solid-state electrolytes (SSEs) have garnered significant attention due to their exceptional interfacial properties and high compatibility with existing battery manufacturing processes. Current research on PDOL-based SSEs primarily focuses on composite structures with supporting frameworks, as standalone 1,3-dioxolane (DOL) cannot effectively isolate the cathode and anode. However, the electrode materials and separators in batteries may inhibit DOL polymerization, resulting in monomer accumulation.

Overcoming the Cathode-Derived LiCO Product by Incorporation of CO Capture to Boost Li-CO Battery Performance.

The development of highly efficient catalysts is critical for the lithium-carbon dioxide (Li-CO) battery. However, the random deposition of lithium carbonate (LiCO) on cathodic active sites leads to catalyst poisoning and severely restricts the discharge capacity. Here, we introduce tetraethylenepentamine (TEPA), an amine-rich redox mediator integrated into the electrolyte, to mediate the CO reduction and evolution reactions (CORR/COER) through a coupled cation-electron transfer mechanism.

Nucleation of biomimetic hydroxyapatite nanoparticles on the surface of human type I collagen using a hybrid all-atom and coarse-grained model.

Inorganic mineral/collagen composite materials are one of the most attractive implant materials for bone repair engineering. Mineralized collagen composites have a similar hierarchical structure and biological activity to natural bone; however, the mechanism of the mineralization process is complex, and the properties of mineralized materials are difficult to control during the preparation process. Currently, this is a significant challenge in coarse-grained organic-inorganic systems.

From Metals to Polymers: Material Evolution and Functional Advancements in Current Collectors.

The rapid advancement of rechargeable batteries is hindered by insufficient energy density, limited design flexibility, and safety concerns, which pose significant challenges to their practical application. This review summarizes the crucial yet often overlooked role of current collectors in addressing these challenges. Recent progress across four types of current collectors, deriving from metal foils, carbonaceous substrates, conductive polymers, and organic-inorganic hybrids is systematically analyzed.

Low-Concentration Electrolyte Engineering for Rechargeable Batteries.

Low-concentration electrolytes (LCEs) present significant potential for actual applications because of their cost-effectiveness, low viscosity, reduced side reactions, and wide-temperature electrochemical stability. However, current electrolyte research predominantly focuses on regulation strategies for conventional 1 m electrolytes, high-concentration electrolytes, and localized high-concentration electrolytes, leaving design principles, optimization methods, and prospects of LCEs inadequately summarized. LCEs face unique challenges that cannot be addressed by the existing theories and approaches applicable to the three common electrolytes mentioned above; thus, tailored strategies to provide development guidance are urgently needed.

Multifunctional electrolyte additive for high power lithium metal batteries at ultra-low temperatures.

Ultra-low-temperature lithium metal batteries face significant challenges, including sluggish ion transport and uncontrolled lithium dendrite formation, particularly at high power. An ideal electrolyte requires high carrier ion concentration, low viscosity, rapid de-solvation, and stable interfaces, but balancing these attributes remains a formidable task. Here, we design and synthesize a multifunctional additive, perfluoroalkylsulfonyl quaternary ammonium nitrate (PQA-NO), which features both cationic (PQA) and anionic (NO) components.

A Fully Flame-Retardant Electrolyte with Laminated SEI for Exceptionally Safe, Long-Life, and High-Voltage Lithium Metal Batteries.

Designing an electrolyte that exhibits intrinsic nonflammability, superior compatibility with lithium metal anodes, and excellent tolerance to high-voltage cathodes is a pivotal, yet highly challenging task for the development of high-energy lithium metal batteries. Herein, these three desirable features are simultaneously achieved by incorporating a fire-retardant diluent, ethoxy(pentafluoro)cyclotriphosphazene, together with a trace additive trioxane into triethylphosphate-based electrolytes. Ethoxy(pentafluoro)cyclotriphosphazene and trioxane both compete against triethylphosphate for the coordination of Li, inducing the formation of a unique laminated solid-electrolyte interphase (SEI) for reversible Li plating/stripping reactions.

Slurry Additive Approach Enables a Mechanically Robust Binder for Silicon-Carbon Anodes in Lithium-Ion Batteries.

Silicon-carbon (Si/C) composites hold great promise as substitutes for conventional graphite anodes in high-specific-energy lithium-ion batteries (LIBs). However, their performance is hindered by silicon's substantial volume expansion during cycling, which can lead to electrode degradation. Traditional poly(acrylic acid) (PAA) binders often struggle to maintain electrode integrity under these conditions.

In Situ Fabricated Non-Flammable Gel Polymer Electrolyte with Stable Interfacial Compatibility for Safer Lithium-ion Batteries.

Gel polymer electrolytes are viewed as one of the highly ideal substitutes for commercial liquid electrolytes due to their excellent properties of non-flowing, non-volatile, high burning point, and compatibility with industrial systems, which collectively contribute to enhanced safety characteristics of batteries. However, the interfacial compatibility issues arising from the unreacted monomers pose significant challenges, leading to poor interfacial compatibility, parasitic reactions, and a subsequent deterioration in battery safety. Herein, a non-flammable gel polymer electrolyte has been designed by in situ polymerization of Poly (ethylene glycol) diacrylate (PEDGA) with the interfacial reinforcement of Ethoxy (pentafluoro) cyclotriphosphazene (PFPN), to improve the interfacial compatibility and further enhance the safety properties.

Quasi-Solid Electrolytes with Flexible Branches and Rigid Skeletons for High-Temperature Li Metal Batteries.

Quasi-solid electrolytes are poised to revolutionize the next generation of high-energy-density lithium metal batteries. However, they face considerable challenges in operating at high temperatures due to severe side reactions, particularly with high-voltage cathodes. Here, we fabricated a nonflammable quasi-solid electrolyte (QSE) using an in situ copolymerization method.

Bioinspired gel polymer electrolyte for wide temperature lithium metal battery.

Stable operation of Li metal batteries with gel polymer electrolytes in a wide temperature range is highly expected. However, insufficient dynamics of ion transport and unstable electrolyte-electrode interfaces at extreme temperatures greatly hinder their practical applications. We report a bioinspired gel polymer electrolyte that enables high-energy-density Li metal batteries to work stably in a wide temperature range from -30 to 80 °C.

Chemical Compatibility of LiAlTi(PO) Solid-State Electrolyte Co-Sintered with LiTiO Anode for Multilayer Ceramic Lithium Batteries.

Multilayer ceramic lithium batteries (MLCBs) are regarded as a new type of oxide-based all-solid-state microbattery for integrated circuits and various wearable devices. The chemical compatibility between the solid electrolyte and electrode active materials during the high-temperature co-sintering process is crucial for determining the structural stability and cycling performance of MLCBs. This study focuses on the typical MLCB composite electrodes composed of the NASICON-type LiAlTi(PO) (LATP) solid electrolyte and the spinel-type LiTiO (LTO) anode material.

In-situ covalently bridged ceramic-polymer electrolyte with fast, durable ions conductive channels for high-safety lithium batteries.

To meet the requirements of high-energy-density lithium batteries, an urgent increasing demand exists for high-safety electrolyte compatibility with high-voltage cathodes. However, the safety issues of widely used ether-based liquid electrolytes and their low oxidation stability have not been effectively resolved. Herein, a covalently bridged electrolyte with ceramics as the crosslinking center is constructed in situ.

Transition Metal-Coordinated Polymer Achieves Stable Seawater Oxidation over NiFe Layered Double Hydroxide.

Seawater electrolysis has emerged as a promising approach for the generation of hydrogen energy, but the production of deleterious chlorine derivatives (e.g., chloride and hypochlorite) presents a significant challenge due to the severe corrosion at the anode.

LiOH Additive Triggering Beneficial Aging Effect of SnO Nanocrystal Colloids for Efficient Wide-Bandgap Perovskite Solar Cells.

Commercial SnO nanocrystals used for producing electron transporting layers (ETLs) of perovskite solar cells (PSC) are prone to aggregation at room temperature and contain many structural defects. Herein, we report that the LiOH additive can simultaneously delay the aggregation and donate the beneficial aging effect to SnO nanocrystals. The resulting SnO ETLs show the desired characteristics, including a broadened absorption range, reduced defects, improved transporting properties, and decreased work function.