Abstract Solid polymer electrolytes (SPEs) offer an appealing alternative to volatile and flammable organic liquid electrolytes for high‐energy lithium metal batteries (LMBs). Despite their potential, two key challenges, insufficient ionic conductivity and inadequate interfacial performance, continue to hinder practical development. Here, the promising potential of a single‐ion conducting gel polymer electrolyte (SIGPE) derived from a polymerizable deep eutectic monomer (PDEM) is demonstrated. This structure forms dynamic nanophases with a high‐dielectric‐constant dielectricizer through Li + ‐bridged molecular self‐association within a flexible polymer matrix. This design regulates ion pathways to enable rapid Li + conduction, effectively preventing interfacial polarization and promoting ion dissociation, while also exhibiting viscoelastic properties that strengthen interface stability. The resultant SIGPE exhibits a high oxidation voltage of 5.0 V and a near‐unity transference number of 0.86. In the LFP|SIGPE|Li full cell, the formation of an inorganic‐rich SEI layer, driven by hetero species (Li 2 O/LiF), enables a high discharge capacity of 131.9 mAh g −1 at 1 C and stable cycling performance, with 71.9% capacity retention and 99.5% coulombic efficiency after 400 cycles at 1 C and 30 °C. These findings underscore the potential of PDEM‐based SIGPE to enhance performance, safety, and sustainability in LMBs, paving the way for practical use in high‐energy storage systems.

Abstract Solid‐state electrolytes (SSEs) hold significant potential for advancing lithium metal batteries (LMBs) by enhancing safety through the replacement of liquid electrolytes. However, challenges such as low ionic conductivity, limited electrochemical stability, and poor electrolyte/electrode interface compatibility hinder the development of high‐energy‐density LMBs. Herein, a strategy for designing SSEs is proposed using multiple‐bridge engineered composite elastomer electrolytes (CEEs) that incorporate ion‐rotating dipole interactions, ion‐anchoring dipole interactions, and hydrogen bonding, along with a CEE‐based composite elastomer cathode (CEC). This design combines a volume‐adaptive elastomer matrix, a high‐Li + conducting deep eutectic electrolyte, and robust nanowires. The resultant CEE exhibits high ionic conductivity (1.7 × 10 −3 S cm −1 ), a lithium transference number of 0.72, and a wide electrochemical stability window (up to 4.9 V) at 298 K. The engineered uniform Li + flux also promotes stable Li plating/stripping for over 900 h at 0.1 mA cm −2 . Furthermore, the LFP‐based CEC|CEE|Li full cells deliver a reversible capacity of 133 mAh g −1 with 95% retention after 300 cycles in coin cells, and 129 mAh g −1 with 96% retention after 250 cycles in pouch cells at 1 C. This strategy presents a promising approach for designing solid‐state polymer electrolytes to extend the lifespan of high‐energy‐density LMBs.

Abstract Solid polymer electrolytes (SPEs) offer an appealing alternative to volatile and flammable organic liquid electrolytes for high‐energy lithium metal batteries (LMBs). Despite their potential, two key challenges, insufficient ionic conductivity and inadequate interfacial performance, continue to hinder practical development. Here, the promising potential of a single‐ion conducting gel polymer electrolyte (SIGPE) derived from a polymerizable deep eutectic monomer (PDEM) is demonstrated. This structure forms dynamic nanophases with a high‐dielectric‐constant dielectricizer through Li + ‐bridged molecular self‐association within a flexible polymer matrix. This design regulates ion pathways to enable rapid Li + conduction, effectively preventing interfacial polarization and promoting ion dissociation, while also exhibiting viscoelastic properties that strengthen interface stability. The resultant SIGPE exhibits a high oxidation voltage of 5.0 V and a near‐unity transference number of 0.86. In the LFP|SIGPE|Li full cell, the formation of an inorganic‐rich SEI layer, driven by hetero species (Li 2 O/LiF), enables a high discharge capacity of 131.9 mAh g −1 at 1 C and stable cycling performance, with 71.9% capacity retention and 99.5% coulombic efficiency after 400 cycles at 1 C and 30 °C. These findings underscore the potential of PDEM‐based SIGPE to enhance performance, safety, and sustainability in LMBs, paving the way for practical use in high‐energy storage systems.

Abstract Solid‐state electrolytes (SSEs) hold significant potential for advancing lithium metal batteries (LMBs) by enhancing safety through the replacement of liquid electrolytes. However, challenges such as low ionic conductivity, limited electrochemical stability, and poor electrolyte/electrode interface compatibility hinder the development of high‐energy‐density LMBs. Herein, a strategy for designing SSEs is proposed using multiple‐bridge engineered composite elastomer electrolytes (CEEs) that incorporate ion‐rotating dipole interactions, ion‐anchoring dipole interactions, and hydrogen bonding, along with a CEE‐based composite elastomer cathode (CEC). This design combines a volume‐adaptive elastomer matrix, a high‐Li + conducting deep eutectic electrolyte, and robust nanowires. The resultant CEE exhibits high ionic conductivity (1.7 × 10 −3 S cm −1 ), a lithium transference number of 0.72, and a wide electrochemical stability window (up to 4.9 V) at 298 K. The engineered uniform Li + flux also promotes stable Li plating/stripping for over 900 h at 0.1 mA cm −2 . Furthermore, the LFP‐based CEC|CEE|Li full cells deliver a reversible capacity of 133 mAh g −1 with 95% retention after 300 cycles in coin cells, and 129 mAh g −1 with 96% retention after 250 cycles in pouch cells at 1 C. This strategy presents a promising approach for designing solid‐state polymer electrolytes to extend the lifespan of high‐energy‐density LMBs.

Abstract Progress in commercializing solid polymer electrolytes (SPEs) for lithium metal batteries (LMBs) has been impeded by challenges, like concentration polarization, non‐uniform Li + flux, and an unstable solid electrolyte interface (SEI), which contribute to dendrite formation. To address these issues, silica framework (SF)‐based single‐ion conductors are proposed, featuring a unique solvation channel composed of a fluorinated segment, a high‐dipole zwitterion, and a rotation‐motion‐driven ion‐hopping medium. This design promotes low resistance at the cathode/electrode interface, suppresses dendrite growth at the anode/electrolyte interface, and maintains a uniform Li + flux. This results show that continuous ion channels within a robust framework enhance Li‐ion dissociation and transport, achieving high ionic conductivity (σ DC = 8.8 × 10 −4 S cm −1 ), a modulus of 0.9 GPa, a high lithium transference number (≈0.83), and an extended electrochemical stability window (up to 5.2 V) at 25 °C. This design fosters the formation of a hybrid organic/inorganic SEI layer composed of Li 2 CO 3 , LiF, and Li 2 O, enabling ultra‐stable Li plating/stripping for over 4000 h at 0.1 mA cm −2 . Furthermore, the full cells demonstrate excellent rate performance and long‐term cycling stability and capacity retention (81% for Li||LFP and 86% for Li||NCM811 after 400 cycles at 1 C) and high coulombic efficiency, offering a promising strategy to stable LMBs.

Solid polymer electrolytes (SPEs)-based lithium metal batteries (LMBs) are at the forefront of next-generation energy storage, offering remarkable energy density and safety. Despite their high potential, the practical use and commercialization of LMBs encounter two significant challenges: inadequate interfacial stability and low critical current density (CCD). One promising approach to tackle the problems is by designing an advanced SPE that simultaneously ensures uniform and high lithium-ion transport. Achieving uniform ion transport is key to minimizing concentration gradients that lead to dendrite formation, while selective lithium-ion conduction prevents anion accumulation, thereby improving interfacial stability. This review comprehensively examines recent progress in the development of uniform lithium-ion transporting polymer electrolytes (ULPEs) and high lithium-ion conducting polymer electrolytes (HLPEs). By combining the structural uniformity of ULPEs with the enhanced conductivity of HLPEs, uniform-high lithium-ion transporting polymer electrolytes (UHLPEs) have emerged as a promising class of materials capable of simultaneously ensuring high interfacial stability and supporting elevated CCD in practical LMBs. Key molecular design strategies, along with insights into ionic conductivity, electrochemical performance, and interfacial behavior, are systematically reviewed to provide a comprehensive understanding of the way to achieve high CCD, enhanced safety, and extend cycle life.

Ultrathin oxide semiconductors are promising channel materials for next-generation thin-film transistors (TFTs), but their performance is severely limited by bulk and interface defects as the channel thickness approaches a few nanometers. In this study, we show that high-pressure hydrogen annealing (HPHA) effectively mitigates these limitations in 3.6 nm thick ZnO TFTs. HPHA-treated devices exhibit a nearly four-fold increase in on-current, a steeper subthreshold swing, and a negative shift in threshold voltage compared to reference groups. X-ray photoelectron spectroscopy reveals a marked reduction in oxygen vacancies and hydroxyl groups, while capacitance-voltage measurements confirm more than a three-fold decrease in interface trap density. Low-frequency noise analysis further demonstrates noise suppression and a transition in the dominant noise mechanism from carrier number fluctuation to mobility fluctuation. These results establish HPHA as a robust strategy for defect passivation in ultrathin oxide semiconductor channels and provide critical insights for their integration into future low-power, high-density electronic systems.

We designed and synthesized pyrrolidinium-based polyurethane ionenes. These ionenes were synthesized using dihydroxyundecyl pyrrolidinium ionic liquid monomers with various anions (Br–, PF6–, or Tf2N–), along with a poly(ethylene glycol) (1000 or 4000) comonomer and one of three chain extenders: methylene diphenyl 4,4′-diisocyanate (MDI), tolylene-2,4-diisocyanate (TDI), and 4,4′-methylenebis(cyclohexyl isocyanate) (HMDI). To investigate the structure–property relationship, a comprehensive study of the thermal properties and ion conduction of the synthesized ionenes was conducted. The synthesized ionenes mostly exhibit an amorphous morphology; however, only ionenes containing PEG-4000 block show semicrystalline features. The copolymer ionenes containing PF6– anions exhibit higher glass transition temperatures (Tg) compared to those with other anions due to hydrogen bonding with the N–H groups (urethane). Also, the pyrrolidinium/PEG-4000 copolymer ionene with PF6– shows a higher degree of crystallinity. Among the synthesized ionenes, the pyrrolidinium-Tf2N polyurethane copolymer with PEG-1000 exhibits the lowest Tg (−21 °C) and the highest ionic conductivity of 1.04 mS/cm (at 70 °C). These findings suggest that pyrrolidinium-based polyurethane ionenes have potential applications in ion-conductive materials, particularly in energy storage devices such as energy storage (e.g., batteries) and conversion devices (e.g., solar cells).

Abstract Interface control plays a critical role in governing various physical and electronic phenomena, as it significantly influences material properties and device performance. In particular, the interfacial structures and properties of 2D layered crystals in contact with metal or dielectrics have recently attracted considerable attention for nanoelectronic applications owing to their superior scalability and functionality. Nonetheless, a comprehensive understanding of the diverse interfacial phenomena in 2D crystals remains limited, especially for chemically reactive 2D semiconducting systems. Here, the controlled intermixing and compound formation at the metal/elemental 2D semiconductor interface are investigated. Black phosphorus (BP) exhibits intermixing with In, leading to the formation of highly oriented interfacial InP. Comprehensive structural characterizations, including electron diffraction, atomic‐resolution scanning transmission electron microscopy, X‐ray photoelectron spectroscopy, and Raman spectroscopy, confirm the InP interfacial structure. Furthermore, electrical tunability of the BP channel is demonstrated by varying both the initial BP thickness and the amount of In deposited, revealing two competing effects: 1) thinning‐induced bandgap widening of BP, and 2) charge‐transfer‐induced effective bandgap narrowing. The resulting tunable transport characteristics highlight the significance of interfacial compound formation in BP, providing fundamental insights into the tunable properties of diverse 2D heterointerfaces for multifunctional device architectures.

Low-dimensional magnetic materials have garnered significant interest due to their unique physical properties and potential applications. Nevertheless, the synthesis of one-dimensional (1D) magnetic materials presents challenges, and the properties of these 1D materials at the single-chain limit have not been well investigated. We here explore experimentally and theoretically 1D CrX₂ (X= Cl, Br, I) magnetic single chains residing within carbon nanotubes. Single chains of CrX₂ are confirmed by the atomic-resolution scanning transmission electron microscopy (STEM) imaging and spectroscopy analysis. Electron energy loss spectroscopy clearly reveals the high-spin state of the Cr atoms within the chain. Notably, we present the first precise measurement and analysis of Cr spin state at the single-chain level, revealing that these spin states can be controlled by the local atomic bonding configuration (CrX₂ versus CrX₃ phases). Density functional theory (DFT) calculations support the structural stability and provide the magnetic and electronic properties of the 1D CrX₂ chains.