Bismuth-based electrocatalysts have shown great promise for the electrochemical reduction of CO2 to formate. However, taming the active crystal facets to realize high selectivity and long-term stability remains a fundamental challenge. Herein, we describe a facile one-step electrodeposition strategy that enables the bismuth nanosheets to dominantly expose the (110) facet via deposition potential modulation. Particularly, the bismuth catalyst structure undergoes in operando reconstruction, in which the highly active (110) facet appears and is well maintained during the electrolysis owing to the reduction from Bi3+ to metallic Bi0. Therefore, the bismuth catalyst with ultrathin nanosheets exhibits high catalytic activity and long-term durability, achieving over 90% Faradaic efficiency for formate over a wide potential range from -0.7 to -1.3 VRHE. When assembled in a Zn-CO2 battery, the bismuth-based cathode catalyst also demonstrates stable cycling, further confirming the robust durability of the (110)-facet-stabilized catalyst under operating conditions. Mechanistic studies reveal that the (110) facet facilitates the CO2 activation process and stabilizes the critical *OCHO intermediate, thereby promoting the reaction pathway selectively toward formate formation while suppressing the competitive hydrogen evolution reaction. This work establishes a facet-engineering strategy via a facial electrochemical synthesis as the accessible route for designing high-performance CO2 reduction reaction catalysts.

Proton batteries are critically limited by corrosion of transition metal oxide electrodes in acidic electrolytes, a challenge further aggravated by activated water generated during the hydrated proton desolvation. Managing interfacial activated water by spatially separating protons and activated water is therefore essential for stable and efficient proton storage. Here, hydrothermal carbon (HTC) is introduced onto MoO3 via a facile hydrothermal carbonization of glucose. The resulting HTC coating effectively shields the electrode from direct exposure to acidic electrolytes, promotes hydrated proton desolvation, and confines activated water at the interface. Simultaneously, the hydrothermal carbonization induces oxygen vacancies in MoO3 (Ov-MoO3@C), modulating the electronic structure and facilitating proton intercalation. Owing to the synergistic effects of activated water confinement and oxygen-vacancy introduction, the HTC coating enables efficient spatial separation of protons and active water. Consequently, the Ov-MoO3@C electrode exhibits a 11% enhancement in capacity and a 55% improvement in cycling stability compared with pristine MoO3. This work highlights hydrothermal carbonization as a dual-functional strategy for regulating proton transfer and modulating electronic structure, offering a promising pathway toward high-performance proton batteries.

The corrosion behavior of zirconium alloys for nuclear applications is closely correlated with second phase particles. This study systematically investigates the dissolution, diffusion, and clustering behavior of hydrogen and oxygen atoms in C15 ZrCr2 and ZrFe2 Laves phases using first-principles calculations. Our findings reveal that H preferentially occupy tetrahedral interstitial sites, whereas O exhibit stronger affinity for hexahedral interstitial positions. Compared to ZrCr2, ZrFe2 inhibits the dissolution of impurity atoms. A comprehensive diffusion network of interstitial impurity atoms in the C15 phase is constructed, where both H and O atoms favor intra-ring diffusion over inter-ring diffusion. Moreover, metal vacancies in the C15 phase substantially increase the binding energy of impurity clusters, serving as preferential nucleation sites for hydride and oxide precipitation.

Solid-state polymer-based lithium metal batteries (LMBs) have emerged as a core development direction for next-generation high-energy-density energy storage devices. However, their practical application is hindered by the fragile solid electrolyte interphase (SEI) and limited oxidation stability of polymer electrolytes (PEs). Herein, a rational "physical-chemical" dual-network design coupled with heteroatom incorporation is proposed to construct high-performance polymer electrolytes. In this dual-network structure, nanofibers of poly(vinyl alcohol) (PVA) and Hexakis (1,2,4-triazol-3-ylamino) cyclotriphosphazene (HATA) form a physical cross-linked network rich in phosphorus (P) and nitrogen (N) elements through hydrogen bonding. This physical network is further integrated with a chemically cross-linked network in situ formed by 2-(((3-(aziridin-1-yl)propionyl)oxy)methyl)-2-ethylpropylene-1,3-diol bis(3-(aziridin-1-yl)propionate) (TTMAP) and 1,3-dioxolane (DOL) monomers, realizing the hydrogen bond interaction between the double networks and the synergistic regulation of multiple heteroatoms. This dual-network synergistic architecture expands the electrochemical stability window to 5.8 V, enabling compatibility with high-voltage cathodes. Benefiting from the protective effect of hydrogen bonds on the cathode material and the improvement of ion conduction, the assembled Li||LiFePO4 battery and Li||LiNi0.8Co0.1Mn0.1O2 battery exhibit capacity retention rates of 87.1% (after 400 cycles at 5C) and 77.9% (after 100 cycles at 0.2C), respectively. Furthermore, heteroatoms facilitate the formation of a robust organic-inorganic hybrid SEI layer rich in N and P elements on the Li anode surface, endowing the symmetric Li||Li battery with stable plating/stripping behavior for over 1000 h at a current density of 0.5 mA cm-2 without discernible dendrite formation. Overall, this meticulously engineered polymer electrolyte presents a viable and promising pathway for the advancement of safe, high-performance LMBs.

Ultrahigh-Ni Co-free LiNixMn1-xO2 (x >= 0.9) polycrystalline oxides have been the very promising cathodes for accommodating Li-ions due to their high energy density and cost advantage. Regrettably, the primary grains with anisotropic nature easily give rise to their compromised rate performance and inadequate cycle durability. In this paper, by adopting the component-induced structure/microstructure optimization strategy, a polycrystalline material LiNi0.9Mn0.1O2 (NM-Nb/Mo) with nearly no internal voids and abundantly external contact points has been successfully designed. Concomitant with the unique close-packed structure, the stress concentration generated at the interface of a single primary particle can be effectively restrained, and the ion shuttle barrier of grain interface can be weakened, remarkably reducing the formation of microcracks and improving the Li+ diffusion coefficient. Meanwhile, the reinforced metal-O resulting by introducing the high-valence ions of Nb5+ and Mo6+ can stabilize the chemical structure, further strengthening the cycling stability of NM-Nb/Mo. Thereof, the capacity retention ratio of modified NM-Nb/Mo materials is up to 86.2% after 150 cycles at 2C. Thus, the designed structure-microstructure co-optimization strategy induced by component regulation delivers the significant effect on preparing high-performance Ni-rich Co-free cathode materials.

Ionic devices, combining high conductivity and intrinsic stretchability, have attracted significant attention for next-generation wearable electronics. However, achieving a balancing among ionic conductivity, mechanical properties, and self-healing ability in ionic conductive elastomers (ICEs) remains a critical challenge. Here, a novel strategy is present to overcome this trade-off by designing a skin-like, non-crosslinked, UV sensitivity polyurethane incorporating two orthogonal dynamic covalent interactions: diselenide bonds and anthracene groups. Diselenide groups facilitate efficient self-healing and enhance mechanical properties through chain shuffling and reinforced hydrogen bonding. Meanwhile, anthracene groups impart photo-responsiveness and fluorescent properties, undergoing dimerization under UV irradiation that alters chain topology. Remarkably, the surface-localized dimerization, forming a protective sheath that improves elasticity and environmental adaptability. While preserving a loosely entangled interior network for ionic transport, analogous to the epidermis, dermis, and subcutaneous tissue. After 60s of UV exposure, the tensile strength increased by 145.6 %, ionic conductivity improved by 24.8 %, and self-healing ability was retained. Furthermore, the materials have solvent recyclability even after UV exposure. This is the first report of a UV-driven topology transformation simultaneously enhancing mechanical and electrical performance in ICEs, offering a promising strategy to resolve the trade-off in ICEs and a versatile platform for multi-functional ionic devices.

In sodium-ion batteries, the insufficient cycling stability of hard carbon anode stems from the physical essence of electrochemical-mechanical coupling failure. Herein, a highly heterogeneous state with extensive weak regions was transformed into a rigid skeleton by adapting a metal-catalyzed carbon structure reconfiguration strategy. Crucially, the introduction of long-range ordered curvature features establishes a pool of atomic-level shock-absorbing spring systems within the carbon network. It not only reversibly accommodates mechanical strain along the z-axis direction but also homogenizes the localized stress of the xy plane. As the balanced enhancement of mechanical properties was achieved across multiple dimensions, electrochemical tests confirmed that the architected rigid framework shows no capacity degradation after 1000 cycles at a current density of 2 A g-1. Thus, our study provides a new design paradigm for developing high-performance anodes via a mechanical homogenization design of hard carbon.

Lithium metal anodes suffer from dendrite growth, unstable solid electrolyte interphase, and "dead Li" owing to high barriers and inhomogeneous Li+ desolvation/diffusion kinetics. Here, we present the suspension electrolyte endowed with atom-level catalytic inorganic particles of single atomic cobalt on defect-rich ZnO1-x nanoparticles (SACo@ZO) in a carbonate-based electrolyte, enhancing desolvation/diffusion kinetics and revitalizing dendritic Li. As systematically investigated by in situ electrochemical sum frequency generation (SFG) spectroscopy together with theoretical simulations, the SACo@ZO-assisted suspension electrolyte decreases the potential threshold down to 20 millivolts for driving interfacial desolvation rapidly, providing uniform solvation-free Li+/Li0 flux and capability in revitalizing dendritic Li. Consequently, we achieve a smooth but dense Li plating behavior under room or low-temperature surroundings, lasting for a long life span of 1600 hours. Meanwhile, the practical Li-LiFePO4 cell with SACo@ZO reserves the capacity retention of ~100% at 0.5 C and survives for 1000 cycles under 0°C, demonstrating the feasibility of atomically catalytic suspension electrolyte for high-performance dendrite-free Li metal batteries.

An advanced solid electrolyte interphase (SEI) is considered an effective strategy to regulate lithium (Li) deposition for promoting high-energy Li metal batteries. However, SEIs still fracture due to uneven Li+ flux and external stress accumulation leading to dendrite growth. Considering that the cracking is difficult to avoid and irreversible, the SEI with a homogeneous microcrack network structure is pre-constructed on Li metal via internal stress release inspired by the crackle glaze effect (cracks are not always bad for Li deposition). Herein, an artificial SEI composed of Li3N and Li-Al alloy is fabricated by magnetron sputtering AlN onto Li metal, which confers high ionic conductivity and lithiophilic compound at the microscale. Whereafter, at the mesoscale, a controllable annealing strategy is introduced to form numerous and homogeneous microcracks, which induces the improved uniformity of Li+ flux and appropriate stress release. Benefiting from this artificial SEI with cross-scale structural design, the corresponding Li||Li symmetric battery can cycle for 2000 h with low polarization at 3 mA cm-2, and the lifespan of full battery also exhibits a fourfold enhancement.

Li batteries are the most commercially established and widely utilized energy storage systems in the world. However, the rapid development of technology has led to stringent demands on Li batteries, necessitating the need for higher energy density, longer cycle life, improved safety, and reduced costs. As a result, the development of next‐generation high‐performance Li batteries faces numerous challenges, which require a comprehensive understanding of the fundamental mechanisms and accelerate material exploration and production to meet industrial requirements. However, the critical behaviors of batteries cannot be fully analyzed at the microscale and macroscale, owing to the random and disordered distribution of materials at the mesoscale. To investigate the effects of particles, pores, interfaces, component distribution, and other mesoscale structures on electrochemical processes, finite element analysis has been extensively applied by solving coupled multi‐physics equations. Hence, this review draws on representative and recent studies to introduce the basic principles and workflow of finite element analysis, followed by a clarification of its applicable scope in comparison with density functional theory and molecular dynamics. Then, the applications of finite element analysis in Li batteries are systematically summarized, with particular emphasis on: 1) Li + transport in electrolytes; 2) charge transfer between electrodes and electrolytes; 3) degradation behaviors and evolution of active materials; 4) accelerating design and selection of electrode parameters. Overall, this review outlines the fundamental principles, workflow, and application scope of finite element analysis, while highlighting its specific calculations in Li batteries. Furthermore, it provides prospects and suggestions for advancement of finite element analysis in the development of next‐generation high‐performance Li batteries.

Abstract Li‒S batteries offer a transformative alternative to present energy storage technologies. However, their practical viability is impeded by polysulfide shuttling and lithium dendrite formation. Electrolyte engineering seeks to solve these thorny issues, yet conventional approaches rely on internal, static or invasive modifications. Here we report an acoustic-induced entropy-driven electrolyte design to steer Li‒S chemistry, realizing enhanced sulfur conversion kinetics and sustained lithium working interface. With the aid of comprehensive instrumental and computational toolbox, it is shown that the entropy-driven state of the electrolyte propels the homogeneous nucleation of both sulfur and lithium species, along with dictating Li-ion desolvation process. The designed electrolyte at a lean dosage of 2.9 µL mg –1 readily enables a 1.1 Ah-level pouch cell with a delivered specific energy of 404.1 Wh kg -1 without packaging. Our electrolyte formulation concept using external field modulation offers an appealing solution to overcome key hurdles in Li–S technology toward high-performance devices.

Low-temperature lithium-metal batteries (LT-LMBs) are increasingly pursued for higher energy density and extended cycle life, yet suffer from severely depressed interfacial Li+ desolvation/diffusion kinetics due to the enlarged solvation structures as well as organic electrolyte solidification, ultimately inducing much higher barriers to overcome. Herein, the interfacial structure of the Li+ solvation shell has been remodeled for fast diffusion kinetics in low-temperature surroundings via an atomic catalyst. Briefly, the interfacial electron-delocalization catalysis engineered by anchoring single-atomic Zn into defect-rich vanadium trioxide (SAZn@DRVO) was developed to expedite the Li+ desolvation/diffusion kinetics under a low-temperature environment, achieving stable operation even at -50 degrees C. As verified by coupled microscopic imaging, chemical valence- and electronic-state analyses, and electrochemical validation, the optimal SAZn@DRVO-Li electrode delivers long-cycling stability up to 1200 h at -10 degrees C. Even when increasing the plating capacity to 5 mAh cm-2, it retains robust dendrite-free cycling stability for 400 h at 2 mA cm-2. Even down to -50 degrees C, a stable ultralow overpotential below 550 mV is achieved without short circuit. The optimal full cell delivers a high-capacity retention of similar to 100% after 120 cycles at 0.2C under -20 degrees C, highlighting the feasibility of atom-level catalysis for the development of durable LT-LMBs. (sic)(sic)(sic)(sic)(sic)(LMBs)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)Li+(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)Li+(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)Li+(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(SAZn@DRVO)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)Li+(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)-50 degrees C(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)SAZn@DRVO-Li(sic)(sic)(sic)-10 degrees C(sic)(sic)(sic)(sic)(sic)(sic)1200(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)5 mAh cm-2(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)2 mA cm-2(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)400(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)-50 degrees C(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)550 mV(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)-20 degrees C,0.2C(sic)(sic)(sic)(sic)(sic)120(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)100%,(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).

Biomimetic optoelectronic synaptic devices have garnered significant attention for their ability to emulate biological behaviors, such as brain-like visual perception, at the device level. However, conventional devices are limited when exposed to solar radiation and rainy weather for outdoor working, including surface contamination, structural damage and reduced electrical performance. Herein, a lightweight, waterproof, and thermally comfortable superhydrophobic elastic silicone-containing polyurethane (SESPU) membrane is developed for optoelectronic synaptic devices. Under UV illumination, the device successfully mimics multiple synaptic functions, including excitatory postsynaptic currents, short-/long-term plasticity, and human brain-like learning behaviors. Notably, the device demonstrates exceptional dual-selective cooling performance, achieving a maximum cooling effect of 10.6 °C under solar radiation, thereby ensuring accurate and stable operation in harsh environments. This work presents an innovative strategy for designing biomimetic optoelectronic synaptic devices with enhanced environmental adaptability and long-term durability.

Self-powered elastomeric fiber-based sensors have been widely applied in the fields of smart wearables and beyond, due to their flexibility and lack of need for an external power source. This review summarizes the recent research progress on wearable self-powered integrated sensors based on elastomeric fiber substrates, providing a detailed description of their fabrication methods, working principles, and applications. Based on their composition and working principles, the self-powered integrated sensing systems include energy harvester devices, energy storage devices, sensors, and integrated systems, respectively. An overview of their applications in the fields of biophysical signal detection, electrophysiological signal detection, and human-machine interaction is also provided. By integrating self-powered technology with sensing, data processing, wireless transmission, and other functions, a self-powered wearable sensing system that can monitor, analyze, and transmit data in real time has been developed, providing a more comprehensive solution for personalized medicine and health management. Additionally, the current challenges and future perspectives of self-powered integrated sensors are also proposed.

All‐solid‐state Li metal batteries (ASSLBs) are coming with sulfide solid‐state electrolytes (S‐SSEs) for superior Li + conductivity, but irregular particles and interfaces lead to disorder Li + flux in S‐SSEs that hinder pure Li as an anode. Specially, its mesoscopic structure cannot be adequately described by average size, making it difficult to analyze Li + flux effectively. Herein, a model is constructed on the molding of Li 5.5 PS 4.5 Cl 1.5 (LPSC) particles and defined size as the number ( N ) and consistency ( σ ) to evaluate their effects on Li + transfer and concentration uniformity. Through machine learning of calculation data (Li + concentration with N and σ ) and experimental results, excessive interfaces can hinder Li + transport and local aggregation of irregular interfaces leads to uneven ion transport. Therefore, a particle size gradient S‐SSEs (induced by different size LPSC particles) is predicted to achieve fast and uniform Li + transport. Subsequently, this designed S‐SSE is applied in ASSLBs, which can complete a 1000 h cycle with capacity retention exceeding 80%. This study elucidates that the long cycle ASSLBs can be achieved by adjusting the molding of LPSC particles. Specifically, it demonstrates that the Li + flux of the whole S‐SSEs can be optimized through gradient size design.

The advancement of all-solid-state lithium batteries (ASSLBs) requires innovative breakthroughs in catholyte design to eliminate the need for external pressure and mitigate the adverse effects of inactive catholytes on energy density. Here, we present a capacity-expanding O/Cl-bridged catholyte (1.2LiOH-FeCl3) featuring an abundant, freely rotating FexOyClz framework, endowing it with polymer-like viscoelasticity and an impressive ionic conductivity (6.1 mS cm-1 at 25°C). The polymer-like viscoelasticity creates a soft interface that alleviates volume changes during cycling, enabling zero-pressure ASSLBs to deliver a high capacity retention of 86.6% after 100 cycles, which is a 35.7% improvement compared to the rigid Li2ZrCl6 catholyte (50.9%). Moreover, the fast Li+ transport capability and variable-valence iron coordination center endow 1.2LiOH-FeCl3 catholyte delivering a capacity of 97.7 mAh g-1. When used as a catholyte alongside an LiFePO4 (LFP) cathode material, it increases capacity by 31.3% (196.4 vs. 149.6 mAh g-1 LFP) and boosts energy density by 21.1% (609.4 vs. 503.4 Wh kg-1 LFP) compared to Li2ZrCl6 catholyte. Beyond these properties, the 1.2LiOH-FeCl3 catholyte offers significant cost advantages, priced at just $2.6 kg-1 (16% of the cost of Li2ZrCl6), and supports scalable production at 60°C, making kilogram- to ton-level manufacturing feasible.

Rechargeable Li batteries provide a high energy density to satisfy our daily life. However, a deep understanding of electrochemical electrode/electrolyte interfaces is of crucial importance for designing electrolytes or electrode materials to achieve high-performance Li batteries. In this work, the advantages of sum frequency generation (SFG) spectroscopy are outlined in studying the solvent adsorption manners, the static electric double layer (EDL) structures, the initialization and evolutions of the solid electrolyte interphase (SEI), and the catalytic regulation of interfacial Li+ desolvation dynamics. The fundamental logic to correlate the interfacial molecular information to the transformation, transfer, and diffusion of the ionic charge carriers, and thus to the battery performance, is also highlighted. The technical challenges and solutions for conducting operando SFG on battery systems are discussed, and the physical models beyond the traditional EDL theory for SFG data interpretation are prospected. Finally, efforts to push in situ SFG techniques forward in high time resolution and real-time fine-spectral feature resolution, as well as the applicability in practical rough interface morphologies and chemical heterogeneity, are further prospected.

Rechargeable sodium-ion batteries (SIBs), leveraging their abundant resources and low cost, are poised to become a highly attractive alternative to lithium-ion batteries (LIBs) for large-scale energy storage, thereby promoting the widespread adoption of renewable energy sources. Despite their potential, challenges such as sluggish reaction kinetics and structural degradation hinder their practical application. Herein, we report the preparation of tin-doped CoSe2 nanocubes ingeniously interlaced with graphene oxide nanosheets (Sn-CoSe2/ rGO) for SIB systems. Notably, the Sn-CoSe2/rGO exhibits a stronger selenium-based bond with graphene, which facilitates rapid ion transport and charge transfer. Consequently, the Sn-CoSe2/rGO demonstrates an impressive stable discharge capacity of 314.1 mAh g- 1 at 0.2 A g- 1, outperforming undoped samples (70.6 mAh g- 1). Furthermore, in-situ X-ray diffraction (XRD) and in-situ electrochemical impedance spectroscopy (EIS) were employed to analyze the related effects, further confirming that the interface design can enhance the high reversibility and rate performance of Na-ion storage.