ABSTRACT Complex degradation trajectories compromise the lifetime reliability and operational safety of lithium‐ion batteries in advanced energy‐storage systems. Aging pathways induced by temperature, rate, and voltage‐abuse stresses are often entangled in conventional health‐estimation models, limiting transferable degradation representation and future‐trajectory updating under distribution shifts. Here, a generalizable, mechanism‐anchored health‐management framework is developed for lithium‐ion batteries under heterogeneous aging conditions. Using aging‐condition identification as a proxy task, we identify a degradation‐sensitive 3.3–3.4 V charging window in LiFePO 4 /graphite cells, where statistically selected features are linked to incremental‐capacity fingerprints. These electrochemically anchored features are integrated with a condition‐aware soft mixture‐of‐experts model to disentangle heterogeneous feature–state‐of‐health (SOH) relationships with and without condition labels during inference. Cross‐dataset continual learning enables adaptation to an unseen data source while mitigating catastrophic forgetting. Finally, data‐driven SOH observations are assimilated into a physics‐inspired parametric degradation model through an adaptive unscented Kalman filter, converting pointwise health estimates into online‐updatable degradation trajectories. The framework achieves robust SOH estimation across multi‐stress aging conditions and stable 100–300‐step look‐ahead trajectory prediction, establishing an interpretable route from electrochemical fingerprints to trajectory‐level battery prognostics.
ABSTRACT Lithium‐iodine batteries are hindered by the polyiodide shuttle effect, where conventional mitigation strategies face a fundamental trade‐off between active material confinement and redox reversibility. Herein, we report a monolithic host‐separator continuum that address this dilemma through spatially organized compartmentalization. The architecture integrates an oxidized sulfonated lignin‐functionalized graphene aerogel (GA@SOL) core with an encapsulating sulfonated cellulose polymer (SCP) shell via sequential infiltration and freeze‐drying, minimizing the interfacial discontinuities inherent in stacked configurations. Within the conductive scaffold, iodine adsorption spontaneously generates a mixed‐valence iodine species (I − /I 2 /I 3 − ) via balanced Lewis acid‐base interactions, establishing a redox‐active environment that preserves electronic connectivity without compromising reaction kinetics. Concurrently, the sulfonate‐rich SCP shell establishes an electrostatic Donnan barrier that selectively repels polyiodide anions while facilitating Li + transport. The resulting GA@SOL‐I 2 @SCP cathode delivers 252 mAh g −1 at 1 C with 89.6% retention over 1500 cycles, a Li + transference number of 0.63, and mitigated self‐discharge (76.1% capacity retention after 120 h). Operando spectroscopy and in situ impedance monitoring confirm sustained polyiodide accessibility and suppressed anode corrosion. This work demonstrates that structural continuity and mixed‐valence‐enabled charge transport can decouple confinement from kinetic penalty, offering a design framework for conversion‐type energy storage systems plagued by soluble intermediates.
ABSTRACT Rechargeable aqueous zinc‐ion batteries offer a cost‐effective and safe solution for large‐scale energy storage. However, uncontrolled Zn dendrite growth, parasitic hydrogen evolution, and poor Zn plating/stripping reversibility still limit their practical deployment. Herein, a Ga‐In liquid metal‐containing hydrogel electrolyte is designed to stabilize the Zn anode. The controlled release of liquid metal regulates the Zn/electrolyte interfacial environment, promotes preferential Zn deposition along the (103) plane, and alleviates structural embrittlement, thereby improving long‐term interfacial stability. Meanwhile, liquid metal released within the hydrogel facilitates the dissolution of Zn dendrites, reducing the risk of internal short circuits. As a result, Zn symmetric cells using the designed hydrogel electrolyte deliver stable cycling for 6000 h at 1 mA cm −2 and 1 mAh cm −2 . Moreover, Zn || NH 4 + ‐V 2 O 5 full cells operate steadily for over 1750 h at 200 mA g −1 with 85% capacity retention. These results demonstrate that a hydrogel electrolyte with controllable liquid metal release provides an effective strategy for stabilizing Zn anodes in aqueous zinc‐ion batteries.
ABSTRACT Constructing a self‐adaptive solid electrolyte interphase (SEI) for wide‐temperature aqueous zinc ion batteries (AZIBs) remains unexplored yet highly challenging. Herein, a temperature‐responsive electrical double layer (EDL) is designed via screening high donor‐number additive, and the EDL composition exhibits temperature‐responsive behavior where elevated temperatures promote anion accumulation and low‐to‐ambient temperatures favor additive enrichment, thereby driving distinct self‐adaptive interfacial chemistries. Experimental and theoretical analyses reveal that low‐to‐ambient temperatures facilitate organic‐inorganic hybrid SEI formation through preferential additive decomposition, whereas high temperatures yield a robust inorganic‐rich SEI via anion decomposition. The self‐adaptive SEIs can significantly modulate Zn 2+ nucleation kinetics across temperatures, promoting uniform Zn deposition with progressively increasing grain sizes during prolonged cycling. Consequently, Zn||Zn cell showcases highly reversible plating/stripping exceeding 5300 cycles at 50 mA cm −2 , while exhibiting broad thermal tolerance across a wide temperature range of −40°C to 60°C. Zn||I 2 full batteries deliver good cycling life of 1000–30 000 cycles, and Ah‐level pouch cell further validates practicality. This work builds the correlation among the temperature‐responsive EDL, interfacial chemistry, and electrochemical performance, advancing wide‐temperature batteries.
ABSTRACT Aqueous Zn‐Te batteries offer high capacity via a six‐electron TeO 2 /Te/ZnTe reaction, yet suffer from low discharge voltage (∼0.6 V) due to the sluggish conversion kinetics and high overpotential of TeO 2 /Te. Although Cl − enables a lower‐overpotential TeCl 4 /Te conversion, the TeCl 4 hydrolysis leads to an unstable high‐voltage discharge plateau at ∼1.2 V. Besides, the accumulation of poorly conductive tellurium halide along charge hinders electron transport between the reaction zone and current collector, leading to inefficient electrochemical oxidation of Te. Here, based on the hard‐soft acid‐base (HSAB) principle, a borderline base Br − is introduced to reconstruct the coordination of the soft acid Te 4+ to form more stable phases and prevent voltage degradation. Meanwhile, Br 3 − is in situ generated via deep charging, which unlocks a chemical oxidation bypass for Te with facile electron transfer at the solid/electrolyte interface. This improves the oxidation efficiency of Te and increases the proportion of high‐voltage plateau capacity during subsequent discharge. A low‐content polyvinyl pyrrolidone addition further improves the capacity retention through its adsorption effect. Accordingly, the Zn‐Te battery delivers high capacities of 837 mAh g −1 at 0.5 A g −1 and 483 mAh g −1 at 5 A g −1 , with more than half capacity stably contributed by the high‐voltage plateau.
