Stability Of Interface Research Articles

Ultrastrong nonflammable in-situ polymer electrolyte with enhanced interface stability boosting high-voltage Li metal batteries under harsh conditions

In-situ polymer electrolytes prepared by Li salt-initiated polymerization are promising electrolytes for solid-state Li metal batteries owing to their enhanced interface contact and facile and green preparation process. However, conventional in-situ polymer electrolytes suffer from poor interface stability, low mechanical strength, low oxidation stability, and certain flammability. Herein, a silsesquioxane (POSS)-nanocage-crosslinked in-situ polymer electrolyte (POSS-DOL@PI-F) regulated by fluorinated plasticizer and enhanced by polyimide skeleton is fabricated by Li salt initiated in-situ polymerization. Polyimide skeleton and POSS-nanocage-crosslinked network significantly enhance the tensile strength (22.8 MPa) and thermal stability (200 °C) of POSS-DOL@PI-F. Fluorinated plasticizer improves ionic conductivity (6.83 × 10−4 S cm−1), flame retardance, and oxidation stability (5.0 V) of POSS-DOL@PI-F. The fluorinated plasticizer of POSS-DOL@PI-F constructs robust LiF-rich solid electrolyte interphases and cathode electrolyte interphases, thereby dramatically enhancing the interface stability of Li metal anodes and LiNi0.8Mn0.1Co0.1O2 (NCM811) cathodes. POSS-DOL@PI-F enables stable, long-term (1200 h), and dendrite-free cycle of Li||Li cells. POSS-DOL@PI-F significantly boosts the performance of Li||NCM811 cells, which display superior cycle stability under harsh conditions of high voltage (4.5 V), high temperature (60 °C), low temperature (−20 °C), and high areal capacity. This work provides a rational design strategy for safe and efficient polymer electrolytes.

Synergetic bifunctional Cu-In alloy interface enables Ah-level Zn metal pouch cells

Rechargeable aqueous zinc-metal batteries, considered as the possible post-lithium-ion battery technology for large-scale energy storage, face severe challenges such as dendrite growth and hydrogen evolution side reaction (HER) on Zn negative electrode. Herein, a three-dimensional Cu-In alloy interface is developed through a facile potential co-replacement route to realize uniform Zn nucleation and HER anticatalytic effect simultaneously. Both theoretical calculations and experimental results demonstrate that this bifunctional Cu-In alloy interface inherits the merits of low Zn-nucleation overpotential and high HER overpotential from individual copper and indium constituents, respectively. Moreover, the dynamical self-reconstruction during cycling leads to an HER-anticatalytic and zincophilic gradient hierarchical structure, enabling highly reversible Zn chemistry with dendrite-free Zn (002) deposition and inhibited HER. Moreover, the improved interface stability featured by negligible pH fluctuations in the diffusion layer and suppressed by-product formation is evidenced by in-situ scanning probe technology, Raman spectroscopy, and electrochemical gas chromatography. Consequently, the lifespan of the CuIn@Zn symmetric cell is extended to more than one year with a voltage hysteresis of 6 mV. Importantly, the CuIn@Zn negative electrode is also successfully coupled with high-loading iodine positive electrode to fabricate Ah-level (1.1 Ah) laminated pouch cell, which exhibits a capacity retention of 67.9% after 1700 cycles.

Boosting the Sodiation Kinetics of Sn Anode Using a Yolk-Shell Nanohybrid Structure for High-Rate and Ultrastable Sodium-Ion Batteries.

Metallic Sn (Tin) is a promising anode material for Na-ion batteries owing to its high theoretical capacity of 870mAhg-1. However, its large volumetric changes, interfacial instability, and sluggish sodiation kinetics limit its practical applications. Herein, a hierarchical yolk-shell nanohybrid composed of an Sn yolk and a Carbon/Silicon oxycarbide (C/SiOC) bilayer shell is prepared via the simple pyrolysis of a silicone oil dispersion containing an Sn precursor. The multifunctional bilayer helps boost sodiation kinetics by providing conductive pathways, enhancing the reversible capacity through surface capacitive reactions, and stabilizing the electrode/electrolyte interface. Abundant void interspaces inside the yolk-shell structure accommodate large volume changes of the Sn yolk. The Sn@C/SiOC nanohybrid demonstrates high specific capacity (≈500mAhg-1 at 1Ag-1), remarkable rate performance up to 10Ag-1, and ultrastable cyclability (91.1% retention after 1500 cycles at 5Ag-1). This yolk-shell nanohybrid structuring can guide the development of various high-capacity anodes for energy storage applications.

Ostwald-Ripening Induced Interfacial Protection Layer Boosts 1,000,000-Cycled Hydronium-Ion Battery.

Collapsing and degradation of active materials caused by the electrode/electrolyte interface instability in aqueous batteries are one of the main obstacles that mitigate the capacity. Herein by reversing the notorious side reactions include the loss and dissolution of electrode materials, as we applied Ostwald ripening (OR) in the electrochemical cycling of a copper hexacyanoferrate electrode in a hydronium-ion batteries, the dissolved Cu and Fe ions undergo a crystallization process that creates a stable interface layer of cross-linked cubes on the electrode surface. The layer exposed the low-index crystal planes (100) and (110) through OR-induced electrode particle growth, supplemented by vacancy-ordered (100) superlattices that facilitated ion migration. Our design stabilized the electrode-electrolyte interface considerably, achieving a cycle life of one million cycles with capacity retention of 91.6 %, and a capacity retention of 91.7 % after 3000 cycles for a full battery.

Ostwald‐Ripening Induced Interfacial Protection Layer Boosts 1,000,000‐Cycled Hydronium‐Ion Battery

AbstractCollapsing and degradation of active materials caused by the electrode/electrolyte interface instability in aqueous batteries are one of the main obstacles that mitigate the capacity. Herein by reversing the notorious side reactions include the loss and dissolution of electrode materials, as we applied Ostwald ripening (OR) in the electrochemical cycling of a copper hexacyanoferrate electrode in a hydronium‐ion batteries, the dissolved Cu and Fe ions undergo a crystallization process that creates a stable interface layer of cross‐linked cubes on the electrode surface. The layer exposed the low‐index crystal planes (100) and (110) through OR‐induced electrode particle growth, supplemented by vacancy–ordered (100) superlattices that facilitated ion migration. Our design stabilized the electrode–electrolyte interface considerably, achieving a cycle life of one million cycles with capacity retention of 91.6 %, and a capacity retention of 91.7 % after 3000 cycles for a full battery.

Ternary Eutectic Electrolyte for Flexible Wide-Temperature Zinc-Ion Batteries from -20 °C to 70 °C.

Aqueous Zn-ion batteries (ZIBs) have attracted attention for grid applications due to their cost-effectiveness and high security. However, their lifespan decreases at high temperatures due to declining interfacial stability and increased side reactions. To address these challenges, a ternary deep eutectic solvent-based flexible electrolyte, comprised of Zn(ClO4)2 ⋅ 6H2O, butanedinitrile (BD), and LiCl in an amphoteric polymer matrix, was developed to enable wide-temperature ZIBs working from -20 °C to 70 °C. The interactions among BD, Li+, and zinc hydrate alongside the amphoteric groups on the polyelectrolyte matrix could effectively suppress the interfacial side reactions and Zn dendrites formation. Consequently, the symmetric Zn cell demonstrates exceptional stability across a wide-temperature range, with the ability to survive up to 2780 hours (1 mA cm-2) at 50 °C. Furthermore, the flexible Zn||PANI battery can operate stably over 1000 cycles at 50 °C, boasting an initial specific capacity of 124.8 mAh g-1 and capacity retention rate of 87.9 % (3 A g-1). This work presents an effective strategy for designing high-stability energy storage devices with excellent security features that can function reliably across diverse temperature conditions.

Ternary Eutectic Electrolyte for Flexible Wide‐Temperature Zinc‐Ion Batteries from −20 °C to 70 °C

AbstractAqueous Zn‐ion batteries (ZIBs) have attracted attention for grid applications due to their cost‐effectiveness and high security. However, their lifespan decreases at high temperatures due to declining interfacial stability and increased side reactions. To address these challenges, a ternary deep eutectic solvent‐based flexible electrolyte, comprised of Zn(ClO4)2 ⋅ 6H2O, butanedinitrile (BD), and LiCl in an amphoteric polymer matrix, was developed to enable wide‐temperature ZIBs working from −20 °C to 70 °C. The interactions among BD, Li+, and zinc hydrate alongside the amphoteric groups on the polyelectrolyte matrix could effectively suppress the interfacial side reactions and Zn dendrites formation. Consequently, the symmetric Zn cell demonstrates exceptional stability across a wide‐temperature range, with the ability to survive up to 2780 hours (1 mA cm−2) at 50 °C. Furthermore, the flexible Zn||PANI battery can operate stably over 1000 cycles at 50 °C, boasting an initial specific capacity of 124.8 mAh g−1 and capacity retention rate of 87.9 % (3 A g−1). This work presents an effective strategy for designing high‐stability energy storage devices with excellent security features that can function reliably across diverse temperature conditions.

Self-Templated 3D Sulfide-Based Solid Composite Electrolyte for Solid-State Sodium Metal Batteries.

Rechargeable solid-state sodium metal batteries (SSMBs) experience growing attention owing to the increased energy density (vs Na-ion batteries) and cost-effective materials. Inorganic sulfide-based Na-ion conductors also possess significant potential as promising solid electrolytes (SEs) in SSMBs. Nevertheless, due to the highly reactive Na metal, poor interface compatibility is the biggest obstacle for inorganic sulfide solid electrolytes such as Na3SbS4 to achieve high performance in SSMBs. To address such electrochemical instability at the interface, new design of sulfide SE nanostructures and interface engineering are highly essential. In this work, a facile and straightforward approach is reported to prepare 3D sulfide-based solid composite electrolytes (SCEs), which utilize porous Na3SbS4 (NSS) as a self-templated framework and fill with a phase transition polymer. The 3D structured SCEs display obviously improved interface stability toward Na metal than pristine sulfide. The assembled SSMBs (with TiS2 or FeS2 as cathodes) deliver outstanding electrochemical cycling performance. Moreover, the cycling of high-voltage oxide cathode Na0.67Ni0.33Mn0.67O2 (NNMO) is also demonstrated in SSMBs using 3D sulfide-based SCEs. This study presents a novel design on the self-templated nanostructure of SCEs, paving the way for the advancement of high-energy sodium metal batteries.

Toward waterproof magnesium metal anodes by uncovering water-induced passivation and drawing water-tolerant interphases.

Magnesium (Mg) metal is a promising anode candidate for high-energy and cost-effective multivalent metal batteries, but suffers from severe surface passivation in conventional electrolytes, especially aqueous solutions. Here, we uncover that MgH2, in addition to the well-known MgO and Mg(OH)2, can be formed during the passivation of Mg by water. The formation mechanism and spatial distribution of MgH2, and its detrimental effect on interfacial dynamics and stability of Mg anode are revealed by comprehensive experimental and theoretical investigations. Furthermore, a graphite-based hydrophobic and Mg2+-permeable water-tolerant interphase is drawn using a pencil on the surface of Mg anodes, allowing them to cycle stably in symmetric (> 900 h) and full cells (> 500 cycles) even after contact with water. The mechanistic understanding of MgH2-involved Mg passivation and the design of pencil-drawn waterproof Mg anodes may inspire the further development of Mg metal batteries with high water resistance.

Zincophilic Sites Enriched Hydrogen-bonded Organic Framework as Multifunctional Regulating Interfacial Layers for Stable Zinc Metal Batteries.

To construct an efficient regulating layer for Zn anodes that can simultaneously address the issues of dendritic growth and side reactions is highly demanded for stable zinc metal batteries (ZMBs). Herein, we fabricate a hydrogen-bonded organic framework (HOF) enriched with zincophilic sites as a multifunctional layer to regulate Zn anodes with controlled spatial ion flux and stable interfacial chemistry (MA-BTA@Zn). The framework with abundant H-bonds helps capture H2O and remove the solvated shells on [Zn(H2O)6]2+, leading to suppressed side reactions. The HOF layer also helps form electrolyte-philic surfaces and expose Zn (002) crystal planes which benefit for rapid conduction and uniform deposition of Zn2+, and weakened sides reactions. Additionally, the electrochemically active zincophilic sites (C=O, -NH2 and triazine groups) favor the targeted guidance and penetration of Zn2+ and provide advantageous sites for uniform Zn deposition. High Young's modulus of the HOF layer further contributes to a high interfacial flexibility and stability against Zn plating-associated stress. The MA-BTA@Zn symmetric cells thereby obtain a substantially extended battery life over 1000 h at 4 mA cm-2. The MA-BTA@Zn||Cu half-cell demonstrates a highly reversible Zn stripping/plating process over 1500 cycles with impressive average Coulombic efficiency (CE) of 99.5% at 10 mA cm-2.

Zincophilic Sites Enriched Hydrogen‐Bonded Organic Framework as Multifunctional Regulating Interfacial Layers for Stable Zinc Metal Batteries

AbstractTo construct an efficient regulating layer for Zn anodes that can simultaneously address the issues of dendritic growth and side reactions is highly demanded for stable zinc metal batteries (ZMBs). Herein, we fabricate a hydrogen‐bonded organic framework (HOF) enriched with zincophilic sites as a multifunctional layer to regulate Zn anodes with controlled spatial ion flux and stable interfacial chemistry (MA‐BTA@Zn). The framework with abundant H‐bonds helps capture H2O and remove the solvated shells on [Zn(H2O)6]2+, leading to suppressed side reactions. The HOF layer also helps form electrolyte‐philic surfaces and expose Zn (002) crystal planes which benefit for rapid conduction and uniform deposition of Zn2+, and weakened sides reactions. Additionally, the electrochemically active zincophilic sites (C=O, −NH2 and triazine groups) favor the targeted guidance and penetration of Zn2+ and provide advantageous sites for uniform Zn deposition. High Young's modulus of the HOF layer further contributes to a high interfacial flexibility and stability against Zn plating‐associated stress. The MA‐BTA@Zn symmetric cells thereby obtain a substantially extended battery life over 1000 h at 4 mA cm−2. The MA‐BTA@Zn||Cu half‐cell demonstrates a highly reversible Zn stripping/plating process over 1500 cycles with impressive average Coulombic efficiency (CE) of 99.5 % at 10 mA cm−2.

Li+ Ion-Dipole Interaction-Enabled a Dynamic Supramolecular Elastomer Interface Layer for Dendrite-Free Lithium Metal Anodes.

The unstable lithium (Li)/electrolyte interface, causing inferior cycling efficiency and unrestrained dendrite growth, has severely hampered the practical deployment of Li metal batteries (LMBs), particularly in carbonate electrolytes. Herein, we present a robust approach capitalizing on a dynamic supramolecular elastomer (DSE) interface layer, which is capable of being reduced with Li metal to spontaneously form strong Li+ ion-dipole interaction, thereby enhancing interfacial stability in carbonate electrolytes. The soft phase in the DSE structure enables fast Li+ transport via loosely coordinated Li+-O interaction, while the hard phase, rich in electronegative lithiophilic sites, drives the generation of fast-ion-conducting solid electrolyte interface components, including Li3N and Li2S. Furthermore, the dynamically resilient DSE network composed of soft and hard phases protects Li anodes from electrolyte corrosion and accommodates volume changes during cycling. All features of the DSE layer synergistically facilitate uniform Li+ deposition and suppress Li dendrite propagation, ensuring a stable and dendrite-free Li anode. Consequently, the symmetric Li||Li cell incorporating the DSE layer achieves cycling stability exceeding 6000 h under 1 mA cm-2 and 1 mA h cm-2 conditions. Furthermore, full cell pairing DSE/Li anode with LiFePO4 (LFP) or high-voltage LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes exhibits high-efficiency Li deposition and cycling stability, even under constrained conditions of limited Li (40 μm) and ultrahigh loading NMC811 cathode (21.5 mg cm-2). This study underscores the effectiveness of the ion-dipole interaction-enabled DSE network in developing stable, high-energy-density LMBs.

Prediction of power conversion efficiency parameter of inverted organic solar cells using artificial intelligence techniques

Organic photovoltaic (OPV) cells are at the forefront of sustainable energy generation due to their lightness, flexibility, and low production costs. These characteristics make OPVs a promising solution for achieving sustainable development goals. However, predicting their lifetime remains challenging task due to complex interactions between internal factors such as material degradation, interface stability, and morphological changes, and external factors like environmental conditions, mechanical stress, and encapsulation quality. In this study, we propose a machine learning-based technique to predict the degradation over time of OPVs. Specifically, we employ multi-layer perceptron (MLP) and long short-term memory (LSTM) neural networks to predict the power conversion efficiency (PCE) of inverted organic solar cells (iOSCs) made from the blend PTB7-Th:PC70BM, with PFN as the electron transport layer (ETL), fabricated under an N2 environment. We evaluate the performance of the proposed technique using several statistical metrics, including mean squared error (MSE), root mean squared error (rMSE), relative squared error (RSE), relative absolute error (RAE), and the correlation coefficient (R). The results demonstrate the high accuracy of our proposed technique, evidenced by the minimal error between predicted and experimentally measured PCE values: 0.0325 for RSE, 0.0729 for RAE, 0.2223 for rMSE, and 0.0541 for MSE using the LSTM model. These findings highlight the potential of proposed models in accurately predicting the performance of OPVs, thus contributing to the advancement of sustainable energy technologies.

MRI and CT compatible asymmetric bilayer hydrogel electrodes for EEG-based brain activity monitoring

The exploration of multi-dimensional brain activity with high temporal and spatial resolution is of great significance in the diagnosis of neurological disease and the study of brain science. Although the integration of electroencephalogram (EEG) with magnetic resonance imaging (MRI) and computed tomography (CT) provides a potential solution to achieve a brain-functional image with high spatiotemporal resolution, the critical issues of interface stability and magnetic compatibility remain challenging. Therefore, in this research, we proposed a conductive hydrogel EEG electrode with an asymmetrical bilayer structure, which shows the potential to overcome the challenges. Benefiting from the bilayer structure with different moduli, the hydrogel electrode exhibits high biological and mechanical compatibility with the heterogeneous brain-electrode interface. As a result, the impedance can be reduced compared with conventional metal electrodes. In addition, the hydrogel-based ionic conductive electrodes, which are free from metal conductors, are compatible with MRI and CT. Therefore, they can obtain high spatiotemporal resolution multi-dimensional brain information in clinical settings. The research outcome provides a new approach for establishing a platform for early diagnosis of brain diseases and the study of brain science.

Rubisco at interfaces I: Conformational flexibility enhances air-water interface and foam stabilization

Rubisco exists in all green leaves and is the most abundant protein species on earth. Extraction methods can affect the molecular conformation of Rubisco, while its influence in the behavior of Rubisco at the air-water interface and foam stabilization is largely unknown. This work focuses on elucidating the role of the Rubisco molecular structure in stabilizing the air-water interface and the multiphase system of foam. Rubisco was extracted from spinach using ultrafiltration (RU) and acid precipitation-alkaline redispersion (RA), respectively. Protein molecular properties were evaluated using SDS-PAGE, DSC, fluorescence spectrometry, and size and zeta-potential measurements. Surface adsorption behavior was measured in the millisecond and longtime regime. Surface mechanical properties were assessed with large amplitude oscillatory dilatation (LAOD) and large amplitude oscillatory shear (LAOS), and LAOD results were analyzed by stress decomposition. Interfacial structures were characterized by imaging Langmuir-Blodgett films with atomic force microscopy. Protein foaming properties were evaluated by whipping. We found that RU was primarily native and more flexible than RA, which was fully denatured and aggregated. Consequently, RU diffused faster to air-water interface (576 ms) than RA (926 ms), and formed stiffer soft solid-like air-water interfaces (Gi’ = 56.7 mN/m; Ed’ = 98.2 mN/m) than RA (Gi’ = 39.6 mN/m; Ed’ = 84.3 mN/m). RU also formed denser and thicker surfaces with higher network connectivity than RA. These advantages endow RU with much higher foam stability (152 min half-life time) than RA (94 min). Our study reveals a clear relationship between the molecular conformation of Rubisco and its air-water interface and foam stabilization properties. It might also guide the development of improved extraction/treatment methods to obtain ideal molecular structures of proteins for foam stabilization.

Exploring the Potential of Halide Electrolytes for Next‐Generation All‐Solid‐State Lithium Batteries

AbstractAll‐solid‐state lithium batteries (ASSLBs) are expected to revolutionize large‐scale energy storage and electric vehicles due to their exceptional safety and high energy density. Central to this technology is the development of solid electrolytes, with halide electrolytes emerging as highly promising candidates, offering high ionic conductivity, robust electrochemical stability and excellent mechanical properties. Since the breakthrough discovery of Li3YCl6 in 2018, research on halide electrolytes has entered a new era. However, despite continuous research efforts, practical challenges persist in their application, including the need to further enhance ionic conductivity, improve moisture resistance, and achieve better compatibility with electrode materials. This review provides a comprehensive overview of recent progress and ongoing challenges in halide electrolytes, examining crystal structures, conduction mechanisms, and scalable synthesis techniques. Various modification strategies are also explored aimed at boosting ionic conductivity and electrochemical stability, with a particular focus on improving interface stability. Finally, future perspectives are outlined for designing high‐performance halide electrolyte materials, offering guidance for ongoing research efforts toward their commercial application in ASSLBs.

Designing Cooperative Ion Transport Pathway in Ultra‐Thin Solid‐State Electrolytes toward Practical Lithium Metal Batteries

AbstractSolid polymer electrolytes (SPEs) are promising for high‐energy‐density solid‐state Li metal batteries due to their decent flexibility, safety, and interfacial stability. However, their development was seriously hindered by the interfacial instability and limited conductivity, leading to inferior electrochemical performance. Herein, we proposed to design ultra‐thin solid‐state electrolyte with long‐range cooperative ion transport pathway to effectively increase the ionic conductivity and stability. The impregnation of PVDF−HFP inside pores of fluorinated covalent organic framework (CF3−COF) can disrupt its symmetry, rendering rapid ion transportation and inhibited anion immigration. The functional groups of CF3−COF can interact with PVDF−HFP to form fast Li+ transport channels, which enables the uniform and confined Li+ conduction within the electrolyte. The introduction of CF3−COF also enhances the mechanical strength and flexibility of SPEs, as well as ensures homogeneous Li deposition and inhibited dendrite growth. Hence, a remarkably high conductivity of 1.21×10−3 S cm−1 can be achieved. Finally, the ultra‐thin SPEs with an extremely long cycle life exceed 9000 h can be obtained while the NCM523/Li pouch cell demonstrates a high capacity of 760 mAh and 96 % capacity retention after cycling, holding great promises to be utilized for practical solid‐state Li metal batteries.

Designing Cooperative Ion Transport Pathway in Ultra-Thin Solid-State Electrolytes toward Practical Lithium Metal Batteries.

Solid polymer electrolytes (SPEs) are promising for high-energy-density solid-state Li metal batteries due to their decent flexibility, safety, and interfacial stability. However, their development was seriously hindered by the interfacial instability and limited conductivity, leading to inferior electrochemical performance. Herein, we proposed to design ultra-thin solid-state electrolyte with long-range cooperative ion transport pathway to effectively increase the ionic conductivity and stability. The impregnation of PVDF-HFP inside pores of fluorinated covalent organic framework (CF3-COF) can disrupt its symmetry, rendering rapid ion transportation and inhibited anion immigration. The functional groups of CF3-COF can interact with PVDF-HFP to form fast Li+ transport channels, which enables the uniform and confined Li+ conduction within the electrolyte. The introduction of CF3-COF also enhances the mechanical strength and flexibility of SPEs, as well as ensures homogeneous Li deposition and inhibited dendrite growth. Hence, a remarkably high conductivity of 1.21×10-3 S cm-1 can be achieved. Finally, the ultra-thin SPEs with an extremely long cycle life exceed 9000 h can be obtained while the NCM523/Li pouch cell demonstrates a high capacity of 760 mAh and 96 % capacity retention after cycling, holding great promises to be utilized for practical solid-state Li metal batteries.

A Rapid Synthesis of Amorphous LiTaOCl4 Solid Electrolytes Through a Two‐Step Reaction Pathway for High‐Rate and Long‐Cycling Lithium Batteries

AbstractA simplified process to prepare solid electrolytes (SEs) that fulfill long cyclability, fast‐charging performance, and wide‐temperature feasibility in all‐solid‐state lithium batteries (ASSLBs) is important. Here, amorphous LiTaOCl4 (aLTOC) SE is synthesized within only four hours via a two‐step reaction by high‐energy ball milling method, which exhibits high ionic conductivity and excellent interfacial compatibility. A bilayer SE based on aLTOC and sulfide along with corresponding ASSLBs, are constructed. Furthermore, slight evolution of the unusual microstructure in the chloride/sulfur interfacial region is observed and analyzed. Density functional theory calculations show that S tends to displace O sites in TaO2Cl4 octahedra instead of Cl sites. As a result of the enhanced interfacial stability and reduced formation of ionically insulating phases, the assembled ASSLBs achieve superior rate performance and cyclability in a wide temperature range. Notably, the ASSLBs show capacity retention of 84.4% and 77.6% after 2000 and 1000 cycles at current density of 10C at 30 and 60 °C, respectively. Importantly, even under −20 °C, the cell works stably over 1600 cycles with capacity retention of 76.3% at 0.5C. The work pave the way for the massive production of high‐performance amorphous chloride electrolytes and the realization of fast‐charging ASSLBs with long cycle life.

A Dynamically Ion-Sieved Electrolyte towards Ultralong-Lifespan Zn-Ion Batteries.

The practical deployment of Zn-ion batteries faces challenges such as dendrite growth, side reactions and cathode dissolution in traditional electrolytes. Here, we develop a highly conductive and dynamically ion-sieved electrolyte to simultaneously enhance the Zn metal reversibility and suppress the cathode dissolution. The dynamic ion screen at the electrode/electrolyte interface is achieved by numerous pyrane rings with a radius of 3.69 Å, which can selectively facilitate the plating/stripping and insertion/extraction process of [Zn(H2O)6]2+ and Zn2+ on the anode and cathode surfaces. As a proof of concept, Zn//Zn symmetric cells deliver exceptional cyclic stability for over 6,800 h and ultrahigh cumulative plated capacity of 1.95 Ah cm-2. Zn//Na2Mn3O7 cells exhibit satisfactory cycling performance with capacity retention of 82.7 % after 4,000 cycles, and the assembled pouch cells achieve excellent stability and durability. This work provides valuable insights into the development of electrolytes aimed at enhancing the interface stability of aqueous batteries.