http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

A phononic crystal nanofiber film is fabricated via localized crystallization of polyimide (PI) induced by boron nitride nanosheets. The aligned crystalline domains form efficient phonon transport pathways (6.51 W/(m·K)), while the amorphous PI surrounding the fibers hinders dipole alignment, yielding an ultralow dielectric constant (2.63). This structural engineering resolves the thermal-dielectric trade-off in 3D integrated circuit packaging.

The rapid advancement of 3D heterogeneous integration technology has created stringent requirements for the thermal conductivity of low dielectric materials. However, common low dielectric materials generally have low thermal conductivity, which hinders the ability to simultaneously optimize signal transmission and heat dissipation in integrated systems. Here, a crystallization control strategy is proposed to tackle the challenge of balancing high thermal conductivity with a low dielectric constant. Through precise control of synthesis parameters, a phononic crystal nanofiber (NF) metamaterial film composed of boron nitride nanosheets (BNNS) and crystalline polyimide (PI) bridges has been successfully developed. The crystalline PI bridging structure and BNNS synergistically form a phononic crystal-like metamaterial inside the fiber, enhancing lattice vibration and facilitating heat transfer. Meanwhile, the PI around the fiber maintains a long-range disordered structure, hindering the arrangement of dipoles. The synergistic effect enables the phononic crystal NF film to achieve a high thermal conductivity of up to 6.51 W/(m·k) and a relatively low dielectric constant of 2.63, thereby enhancing the energy efficiency of 3D integrated systems.

Unique oxygen-deficient, hybrid phased titanates are leveraged to achieve nanoconfinement of ammonia borane (AB) via a distinctive one-end-anchored docking (OEAD) mechanism. This approach enables sustained H2 release while mitigating the detrimental reaction between AB and hydrogen peroxide in pathological conditions. The released H2, in synergy with magnesium ions, effectively promotes innervated-vascularized bone regeneration in a diabetic model.

Despite its potential in hydrogen (H2) therapy, ammonia borane (AB) has limited biomedical applications due to its uncontrolled hydrolysis rate and potential to cause cytotoxicity. Existing material-based delivery strategies focus on accelerating AB hydrolysis for H2 production, hence exacerbating these issues. A new nanoconfinement strategy is reported, which loads AB onto oxygen-deficient, hybrid-phased titanate nanocrystals on implant surfaces through a unique one-end-anchored docking (OEAD) mechanism. This nanoconfinement strategy effectively restricts the release of AB molecules, allowing only water molecules to infiltrate the interlayer space for slow hydrolysis and sustained H2 release. This significantly prolongs the duration of H2 release and effectively circumvents the cytotoxicity associated with AB interacting with hydrogen peroxide (H2O2) in the inflammatory microenvironment. In vitro and in vivo have shown that sustained H2 release from the implant surface effectively alleviates diabetes-related oxidative stress, and combined with the release of magnesium ions (Mg2+) synergistically promotes innervated-vascularized bone regeneration.

Pt1-MoL-Mo2C surface single atom alloys (SSAAs) that integrate the advantages of Single atom catalysts (SACs) and Single atom alloys (SAAs) are successfully fabricated via incorporating ultrathin Mo layer on the surface of Mo2C matrix, exhibiting superior catalytic activity toward HER.

Single atom catalysts (SACs) achieve 100% utilization of metal atoms and have versatile support effects, whereas single atom alloys (SAAs) with metallic bonds own the free-atom-like electronic structure. Herein, surface single atom alloys (SSAAs) are developed that integrate the advantages of SACs and SAAs via incorporating an ultrathin metallic layer during the synthetic process of SACs. It is shown that the Pt single atom preferentially coordinates with metallic Mo nanolayer, thereby forming a Pt1-MoL surface atom alloy on Mo2C (marked as Pt1-MoL-Mo2C SSAAs). Comprehensive spectroscopic and theoretical calculations reveal that the Mo nanolayer in SSAAs not only functions as an electron buffer between Pt1 and Mo2C, leading to a free-atom-like d state at Pt1 sites and thereby balancing the adsorption and desorption of H, but also enhances the aggregation, adsorption, and activation of H2O. Consequently, the Pt1-MoL-Mo2C SSAAs exhibit superior alkaline hydrogen evolution reaction (HER) performance compared to Pt1/Mo2C SACs, achieving a low overpotential of 12 mV at 10 mA cm−2 and a low Tafel slope of 17 mV dec−1. This work provides novel insights into the design of advanced single-site catalysts.

A gel polymer electrolyte (GPE) decouples ionic conductivity and mechanical strength via competitive coordination between succinonitrile and polymer, resolving their trade-off. Interpolymer H-bonding compresses GPE, inducing molecular aggregation that channels anions into Li+ solvation shells to stabilize anode interfaces. This enables pouch cells with energy density over 450 Wh kg−1, advancing lithium metal battery electrolyte design.

Gel polymer electrolytes (GPEs) show great potential for lithium-metal batteries, but balancing high ionic conductivity with robust mechanical properties remains challenging. In this study, a competitive coordination strategy is proposed to address this issue by incorporating highly polar succinonitrile (SN) into a poly(methyl methacrylate-co-methacrylamide) (PMAm) matrix. The strong Li+ affinity of SN enables effective displacement of lithium ions from polymer hydrogen-bonding sites, maintaining the polymer's structural integrity while enhancing mechanical strength. Additionally, the hydrogen bonding between polymer chains compresses the polymer matrix, inducing molecular aggregation that creates fast diffusion pathways for Li+ and promotes anion participation in the solvation shell, facilitating the formation of a stable, inorganic-rich solid electrolyte interphase (SEI). As a result, the resulting PMAm-SN GPE exhibits excellent toughness (24.8 MJ m−3), high ionic conductivity (2.8 mS cm−1 at 25 °C) and high Li+ transference number of 0.76. When paired with a LiNi0.6Co0.2Mn0.2O2 cathode, the GPE demonstrates a 90% capacity retention after 500 cycles at 4.3 V. A practical 5 Ah Li/LiNi0.8Co0.1Mn0.1O2 pouch cell delivers 456 Wh kg−1 energy density and demonstrates outstanding safety under thermal and mechanical abuse, showcasing the potential of this GPE for practical applications.

This study combines X-ray magnetic imaging and electrical transport to uncover the anomalous Hall effect in hematite, an insulating oxide exhibiting unconventional altermagnetic properties. Imaging reveals distinct magnetic domains linked to crystal symmetry, and angular-dependent transport measurements highlight unusual symmetry-driven conductivity behaviors. This comprehensive approach establishes hematite as a model altermagnetic material for spintronics research.

Altermagnets are a class of magnetic materials that exhibit unconventional transport properties, such as an anomalous Hall effect (AHE), despite having compensated sublattice magnetic moments. In this study, fundamental experimental evidence of the altermagnetic nature of hematite (α-Fe2O3), is reported combining electrical transport with advanced X-ray photoemission electron microscopy (XPEEM) imaging with linear and circular dichroism contrast. These measurements directly visualize the Néel vector's coupling to the crystal orientation, confirming hematite's altermagnetic order and its symmetry-driven transport behavior. The transport measurements reveal an anisotropic AHE with a pronounced crystal orientation dependence, including a sign inversion for specific Néel vector alignments. Supported by first-principles theoretical calculations, how the interplay between collinear spin and crystal symmetry breaking drives the observed AHE is explained. These findings establish hematite as an altermagnet, paving the way for experimental identification of altermagnetic materials and their integration into spintronic technologies.

This work engineered a bi-heterojunction noise-enhanced negative transconductance (BHN-NTC) transistor using a half-PTCDI-C13 layer, achieving expanded and tunable noise characteristics. This advancement enables efficient multi-bit TRNGs for AI-driven image generation and enhances logic circuit applications.

Reliable true-random number generator (TRNG) hardware demands amplified intrinsic noise and multi-bit entropy output, which are difficult to achieve in conventional single-device TRNG implementation. A bi-heterojunction noise-enhanced negative transconductance (BHN-NTC) transistor is presented, incorporating an asymmetric PTCDI-C13 layer into an NTC transistor. This design enhances electron injection, expanding the NTC region (19 → 27 V) and increasing negative transconductance (−0.036 µS at V GS = −11 V → −0.073 µS at V GS = −15 V) by reducing the electron injection barrier (≈2.13 eV → ≈0.41 eV). The bi-heterojunction configuration introduces a strong correlation between noises, including trapping/detrapping and generation/recombination processes. This property enables a threefold higher entropy throughput in TRNG, achieving a 3-bit output per sampling event. The BHN-NTC-driven TRNG leverages increased noise-induced entropy to generate more diverse latent vectors, mitigating mode collapse and enabling the synthesis of high-quality, realistic images. This significantly enhances StyleGAN2-based image generation, improving performance metrics such as Frechet inception distance (FID) (18.7 → 8.3), kernel inception distance (KID) (0.024 → 0.009), inception score (IS) (6.5 → 9.2), and multi-scale structural similarity (MS-SSIM) (0.43 → 0.21). Consequently, the BHN-NTC transistor establishes a scalable stochastic noise platform, advancing applications in secure electronics and probabilistic stochastic computing.

An in situ mineralized electrolyte with Prussian blue analog electron potential wells revolutionizes aqueous zinc batteries, enabling a 1000 Wh kg−1 cathode and dendrite-free anode. This design mediates rapid iodine-bromine redox reactions, achieves multi-electron transfer, and ensures stable cycling over 6000 cycles. The breakthrough offers a scalable pathway for high-energy, long-lifespan zinc batteries.

The practical applications of aqueous zinc-ion batteries (AZMBs) are hindered by challenges such as low energy density and limited cycle life, which stem from the one-electron transfer at the cathode and dendrite formation at the anode. Herein, inspired by the biomineralization phenomenon in nature, an in situ mineralized electrolyte (IME) containing Prussian blue analogs (PBAs) as an electron potential well is designed. This in situ mineralization strategy promotes uniform, rapid, and reversible charge transfer at the electrode/electrolyte interfaces, enabling the Iodine (I₂) cathode to achieve a specific capacity of 286.4 mAh g⁻¹ at 1 A g⁻¹ and an energy density of 330.8 Wh kg⁻¹. Simultaneously, the potential well facilitates the in situ recovery of Zn dendrites into active Zn2⁺ ions, ensuring stable Zn anode cycling with a practical areal capacity of 5 mAh cm⁻2 for 1500 h. Furthermore, the mediation of iodine-bromine chemistry enables highly reversible Br⁰/Br⁻ and I⁺/I⁰/I⁻ reactions, achieving an energy density of more than 1000 Wh kg−1. Additionally, an enhanced energy density of 503 Wh kg⁻1 and a high energy efficiency of 86.73% over 6000 cycles are achieved. In summary, the in situ mineralization of an electron potential well in electrolyte offers a novel pathway for developing high-energy and long-lifespan AZMBs.

A new silicate electrolyte and synthesized K2.8GdP0.2Si2.8O9 is is developed which exhibits an ionic conductivity of 2.9 × 10−5 S cm−1 via a rational vacancy design strategy. DFT calculations show that potassium ions diffuse on the ac plane. The assembled quasi-solid-state KC/K2.8GdP0.2Si2.8O9/PB cell achieves a remarkable cycling performance at a high current density of 1 C.

Solid-state potassium-ion batteries are promising options for large-scale energy storage due to their high safety and abundance of potassium resources. However, solid-state potassium-ion batteries are still in their infancy and the reported electrolyte materials are very limited, making the exploration of solid electrolytes with high ionic conductivity and physical/electrochemical stability a major challenge. Here novel triclinic K3LnSi3O9 (Ln = Y and Gd) potassium-ion solid electrolyte is reported with low activation energy and high stability. A rational vacancy design strategy is adopted to synthesize K3−xGdPxSi3−xO9 and the result of DFT calculation shows that the diffusion pathways of potassium ions on the ac plane exhibit a fish scale-like network structure. Specifically, the K2.8GdP0.2Si2.8O9 delivers a high ionic conductivity of 2.9 × 10−5 S cm−1 at 25 °C, accompanied by a stable potassium stripping/plating (a long-life cycle over 2000 h). As a result, the assembled quasi-solid-state KC/K2.8GdP0.2Si2.8O9/PB cell achieves a remarkable cycling performance at a high current density of 1 C (500 cycles, 95.9% capacity retention). These results would no doubt boost research for high-safety and high-energy-density solid-state potassium-ion batteries.

LPSBH combines features of argyrodite and glass - ceramic, providing high deformability across the full molding pressure range. This facilitates the formation of high-quality solid–solid interfaces, enabling stable 1000-cycle performance at 25 °C in laminated NCM/Graphite cells under a low stack pressure of 5 MPa.

All-solid-state batteries (ASSBs) are promising next-generation energy storage systems that can replace conventional lithium-ion batteries. Further enhancement in battery performance requires the formation of a stable physical interfacial contact between the active material (AM) in the electrode and the solid electrolyte (SE). However, reducing the resistance at the AM–SE interface remains a key challenge. This study focuses on Li3PS4-xLiBH4 (LPSBH), a sulfide-based SE with an argyrodite structure, synthesized by mechanical milling. Although LPSBH is known for its high ionic conductivity, its mechanical properties are not thoroughly examined. Here, the deformability of LPSBH is evaluated by demonstrating that it can be formed at low pressures to achieve high relative density. A quantitative evaluation of the AM–SE interfacial contact using symmetric cells demonstrates the formation of a good AM–SE interfacial contact within the electrode layer. A 13 mAh-class laminated cell with LPSBH stacked onto the negative electrode achieves 6C charging at 25 °C under a low stacked pressure of 5 MPa, along with significant cycle stability, which retains ≈70% capacity after 1000 cycles under 1C/1C conditions.

Organic thermoluminescent materials are developed using radical pairs for energy storage, controlled by transannular sulfur-oxygen interactions that drive a back electron transfer (BET) process. This results in tunable luminescence, from long afterglows to microsecond flash, depending on temperature. The materials exhibit stability under extreme conditions, such as maintaining luminescence in boiling water, making them ideal for applications like radiation detection and thermoluminescent afterglow imaging.

Precise control over the release of light energy, distinct from conventional thermal energy management, poses significant challenges in luminescent technologies. This study pioneers organic above-room-temperature thermoluminescent materials using radical pairs as energy storage centers (ESCs), enabling controlled light energy release from multi-hour afterglows to microsecond-scale explosive bursts, accelerating the energy release rate by up to 1.8 × 108 times. Notably, the unique transannular interactions between sulfur and oxygen in thianthrene oxides facilitate a thermally driven back electron transfer (BET) process based on radical pairs, central to the energy storage and release mechanism. Due to this BET process, these materials precisely modulate luminescence and exhibit robust stability, maintaining luminescence for 4 h in boiling water and storing energy in air for over six months. These findings advance organic thermoluminescence, highlight the significance of BET processes in various domains, and set new performance benchmarks for luminescent materials under extreme conditions.

A hybrid fluid combining ferrimagnetic nanoplatelets and a ferroelectric nematic displays coexisting magnetization and polarisation at room temperature. This self-assembled multiferroic shows strong magnetoelectric effect and nonlinear optical response, offering a soft, reconfigurable platform for next-generation sensing, actuation, and photonic applications.

Responsiveness to multiple stimuli and adaptivity are paramount for designing smart multifunctional materials. In soft, partially ordered systems, these features can often be achieved via self-assembly, allowing for the combination of diverse components in a complex nanostructured material. Here, an example of a liquid is demonstrated that simultaneously displays both ferroelectric and ferromagnetic types of order. This material is a nanostructured liquid crystalline hybrid comprising ferrimagnetic barium hexaferrite nanoplatelets suspended in a ferroelectric nematic host. Director-mediated interactions drive the self-assembly of nanoplatelets in an intricate network. Due to the coupling between the polar electric and magnetic types of order, this material demonstrates magnetically driven electric and nonlinear optical responses, as well as electrically driven magnetic response. Such multiferroic liquids are highly promising for applications in energy harvesting, nonlinear optics, and sensors.

A high-performance n-type conducting elastomer, engineered via ionic liquid-modulated phase separation of PBFDO/TPU blends, achieves high conductivity (>200 S cm−¹) and stretchability (>200% strain). The first stretchable thermoelectric generator using n-/p-type elastomers demonstrates efficient energy harvesting, with robust performance in wearable applications under mechanical stress.

Stretchable n-type conducting polymers are crucial for advancing high-performance optoelectronic and bioelectronic devices, yet their development lags significantly behind that of p-type counterparts due to the intrinsic challenge of harmonizing electrical conductivity with mechanical compliance. Herein, a novel strategy is reported to engineer a high-performance n-type conductive elastomer by synergistically blending the n-type polymer poly(benzodifurandione) (PBFDO) with thermoplastic polyurethane (TPU) and modulating phase separation via the ionic liquid (IL) 1-butyl-3-methylimidazolium tetrafluoroborate. The resulting PBFDO/TPU/IL composites (PBTI) achieve an unprecedented combination of n-type electrical conductivity exceeding 200 S cm−¹, fracture elongation surpassing 200%, and robust operational stability, outperforming existing stretchable n-type conductive polymers. The controlled phase-segregated morphology ensures efficient charge transport while maintaining elastomeric resilience, addressing the long-standing trade-off between conductivity and stretchability. PBTI is integrated with a p-type PEDOT:PSS-based elastomer to demonstrate its versatility in constructing a stretchable thermoelectric generator (TEG), which exhibits a reliable power output under mechanical deformation. Further applications in fire safety warnings and real-time human physiological monitoring underscore the material's practicality in adaptive wearable and implantable systems. This work breaks new ground in n-type stretchable conductors, paving the way for sophisticated bioelectronics and self-powered devices requiring balanced electronic and mechanical functionalities.

Calcium phosphate oligomers (CPO), polyvinyl alcohol (PVA), and sodium alginate (SA) molecular chains are employed to achieve multiscale crosslinking assembly, progressing from the ionic-molecular level to nanolines, nanorods, nanofibers, microfibers, and ultimately to nanocomposite films and bulk. The resulting organic‒inorganic molecular interactions and highly integrated hierarchical ordered structure endow the nanocomposites with exceptional ultrahigh toughness, significantly outperforming conventional counterparts.

Strength and toughness have traditionally been regarded as mutually exclusive, but simultaneously achieving both high strength and high toughness in organic‒inorganic nanocomposites remains a significant challenge. Inspired by natural nacre and bone, inorganic ionic oligomers and organic molecular chains are employed to achieve multiscale crosslinking assembly, advancing from the ionic-molecular level to nanolines, nanorods, nanofibers, microfibers, and ultimately to nanocomposite films and bulk nanocomposite materials. This process results in a highly integrated organic‒inorganic hierarchical ordered structure, imparting exceptional record-breaking ultrahigh toughness (558.90 ± 34.84 MJ m−3), excellent tensile strength (353.84 ± 18.77 MPa), and fracture energy (2.93 MJ m−2) to the nanocomposite films. The resulting bulk nanocomposite exhibits outstanding bending mechanical properties (a maximum bending stress of 207.17 ± 12.37 MPa, and a bending energy of 37.62 ± 7.33 MJ m−3 without fracture), exceptional fatigue resistance, and remarkable toughness in extreme environments (e.g., −196 and 200 °C). Furthermore, the nanocomposites can undergo hydrothermal-induced recycling and regeneration owing to their noncovalent crosslinking nature. Consequently, these nanocomposites exhibit significant potential for applications in high-performance structural engineering materials. The proposed organic‒inorganic multiscale crosslinking assembly tactic based on inorganic ionic oligomers presents a promising approach for the fabrication of ultrahigh-toughness nanocomposites.

High-entropy effect of mesoporous metal oxide electrocatalysts is demonstrated to lower the energy barrier of the hydrodeoxygenation route and thus facilitate two-step tandem nitrate reduction electrocatalysis for selective ammonia electrosynthesis in a more sustainable manner.

Electrocatalytic nitrate reduction reaction (NO3 −RR) in water offers a sustainable alternative for robust electrosynthesis of value-added ammonia (NH3) in ambient conditions. However, NO3 −RR electrocatalysis generally involves two-step tandem routes and suffers from sluggish hydrodeoxygenation kinetics, which result in a low ammonia selectivity and yield rate. In this work, it is demonstrated that the high-entropy effect of mesoporous metal oxides remarkably decreases the energy barrier of the hydrodeoxygenation route and facilitates two-step tandem electrocatalysis of NO3 −RR, which thus promotes selective NH3 electrosynthesis in an alkaline condition. By comparing a series of high-entropy mesoporous metal oxides and corresponding metal alloys and monometallic counterparts, high-entropy mesoporous (CoMnFeNiCu)3O4 discloses the highest electrocatalytic performance for efficient NH3 electrosynthesis from NO3 −RR, including remarkable NH3 Faradaic efficiency of 96.3%, high NH3 yield rate of 1.83 mmol h−1 mg−1, and excellent recycling stability of 20 cycles, representing one of the best electrocatalysts reported in the past three years. Moreover, cathode NO3 −RR performance for selective NH3 electrosynthesis is enhanced when further coupled with the thermodynamically favorable benzyl alcohol oxidation reaction at the anode. It is expected that the high-entropy effect opens up a new route to design a library of novel tandem mesoporous metal electrocatalysts for the selective electrosynthesis of various valuable chemicals from wastewater.

A multi-element composition modulation strategy is proposed for cathodes of NIBs, exemplified by LFANMT (NaLi0.05Fe0.04Al0.01Ni0.4Mn0.4Ti0.1O2), achieving over 180 mAh g−1 at 4.3 V. A stress-protective layer is constructed to alleviate the internal and external stress differences caused by uneven Na+ extraction during the O3-P3 phase transition. Cathodes exhibiting excellent cycling stability with negligible voltage decay under high voltage is successfully obtained.

Unstable high-capacity cathodes remain a substantial barrier to enhancing the energy density of Na-ion batteries (NIBs). While the high-entropy strategy has demonstrated significant advantages in improving the performance of layered oxide cathodes, the specific capacities of reported high-entropy oxides remain relatively low (<150 mAh g−1). This prompts a reconsideration toward leveraging not just high entropy, but also the synergy among multiple elements to meet the demands for higher energy density. Herein, a multi-element composition modulation strategy is proposed to obtain cathodes without compromising on capacity, exemplified by LFANMT (NaLi0.05Fe0.04Al0.01Ni0.4Mn0.4Ti0.1O2), which achieves a remarkable specific capacity exceeding 180 mAh g−1 at 4.3 V. It is visualized that single-crystal particles with surface compressive stress and bulk tensile stress exhibit superior surface lattice oxygen stability and crack resistance during cycling. Constructing an initial stress-protective layer is beneficial for alleviating the internal and external stress differences caused by uneven Na+ extraction during the O3-P3 phase transition. Through precise elemental modulation, cathodes exhibiting excellent cycling stability with negligible voltage decay under high voltage are successfully obtained. The work provides an effective approach for designing high-capacity O3-type layered oxides for NIBs, emphasizing the importance of synergistic effects among elements.

A synthetic strategy for the formation of Pt islands and their transformation into Pt atomic strings on Ru nanoparticle surfaces is presented. The thermodynamically favored configuration of Pt strings on Ru catalyst is demonstrated to catalyze HER via the faster Volmer–Tafel pathway with a significantly improved intrinsic activity, owing to the well-aligned Pt-Ru sites adjacent to Pt-Pt sites.

The platinum-ruthenium (PtRu) system is highly active for hydrogen evolution reaction (HER) in alkaline media with both Pt and Ru playing active roles in the water dissociation step that generates adsorbed hydrogen atoms. Precise control of the arrangement of Pt atoms on Ru nanoparticles can maximize the Pt-Ru sites for water dissociation and Pt-Pt sites for hydrogen production and can considerably improve HER catalytic performance. By directing the growth and distribution of Pt on Ru hourglass nanoparticles, the arrangement of Pt on Ru is controlled into forming Pt islands, small Pt clusters, and strings of a few Pt atoms. Calculations show that the unique atomic string arrangements of Pt on Ru is the thermodynamically favorable configuration. Additionally, these strings have a favorable combination of Pt-Ru and Pt-Pt sites, making the Pt-string on Ru the most active catalyst with a more than fivefold increase in turnover frequency for alkaline HER compared to the Pt-island on Ru catalyst. The results show how controlling the Pt atomic arrangement on Ru nanoparticle surfaces for the tuning of Pt-Pt and Pt-Ru neighboring sites can direct toward a more efficient HER mechanism and thereby significantly enhancing HER performance.

A rational design strategy stabilizes HE-LLZO by combining thermodynamic assessments and compositional engineering. Through degradation mechanism exploration, lithium-compatible elements are selected, and unstable dopants (e.g., Nb, Mo, W, Cr, Bi) are excluded. A novel HE-LLZO (Li6.6La3Zr0.4Sn0.4Hf0.4Sc0.2Ta0.6O12) exhibits high ionic conductivity (3.69 × 10−4 S cm−1) and stable cycling over 2,500 h.

All-solid-state lithium metal batteries offer enhanced safety and energy density by replacing flammable liquid electrolytes with solid-state electrolytes (SSEs). High-entropy (HE) SSEs, leveraging multi-principal-element compositions, present a vast design space to achieve exceptional ionic conductivity and electrochemical stability. However, the chemical complexity of HE SSEs introduces challenges in interfacial instability with lithium metal anodes due to the unavoidable inclusion of reactive elements. While conventional garnet-type SSEs are considered stable, it is revealed that five HE garnets (HE-LLZOs) undergo corrosion and partial dissolution upon lithium contact. Here, a rational design strategy is introduced to stabilize HE-LLZO by combining thermodynamic assessments of interfacial reactivity with targeted compositional engineering. Through systematic exploration of element-specific degradation mechanisms, selection criteria for lithium-compatible principal elements are established. Guided by computational screening, unstable dopants are excluded (e.g., Nb, Mo, W, Cr, Bi) that drive interfacial degradation and synthesize a novel HE-LLZO (Li6.6La3Zr0.4Sn0.4Hf0.4Sc0.2Ta0.6O12) that exhibits high ionic conductivity (3.69 × 10−4 S cm−1) and stable cycling over 2,500 h. X-ray photoelectron spectroscopy confirms the interfacial stability of Zr, Sn, and Ta while identifying Nb as a destabilizing element. This work provides an integrated computational-experimental framework for understanding element-property relationships in HE oxides, advancing durable SSEs design.

Er3⁺/Mn2⁺ co-doped ZnS/CaZnOS heterostructures are developed for remote temperature and force/sound sensing. The material exhibits UV/NIR photoluminescence, with energy transfer influencing color. Mechanoluminescence intensity is measured against applied power. Temperature-dependent photoluminescence enabled luminescence thermometry. Sound-induced mechanoluminescence, combined with thermometry, facilitated temperature detection during drilling and in heated systems. This demonstrates potential for excitation-light-free temperature probing.

Mechanoluminescence (ML) is a powerful phenomenon that enables light generation induced with mechanical or acoustic waves, and remote temperature sensing via luminescence thermometry techniques. In this work, the multi-functional, ML-active materials based on Er3+ and Mn2+ co-doped ZnS/CaZnOS heterostructure are developed for remote temperature monitoring and visual sensing of force and sound. The material exhibits characteristic photoluminescence (PL) under UV and NIR (up-conversion) excitation, with energy transfer from Er3+ to Mn2+ influencing the emission color. The effects of force-to-light conversion are studied in detail by measuring the ML intensity versus the applied power for Er3+ and Mn2+ emission in the single-doped and co-doped materials. Temperature-dependent PL is utilized to calibrate luminescence thermometry response, with Er3+ thermally-coupled levels and non-thermally-coupled levels of Er3+/Mn2+, providing temperature sensing capabilities. The unique combination of sound-induced ML with luminescence thermometry allowed optical temperature detection, alike during the drilling process, and in the externally heated system, using pulsed sonications. Whereas, applying continuous excitation, the sound-to-heat conversion is studied and visualized using the developed ML-based optical thermometers. This approach demonstrates the excellent application potential of sound-to-light conversion for remote monitoring and, more importantly, for excitation-light-free temperature probing of different systems and working devices.

Herein, an echinoderm-inspired supramolecular ionogel is engineered with extreme robustness and damage tolerance via synergistic integration of hard-soft phase-separated architecture and multi-scale sacrificial bonding. The ionogel achieves advanced tensile strength, toughness, and unprecedented tear resistance, puncture energy, and high-speed impact resistance. Furthermore, a sensing matrix is developed that simultaneously accomplishes real-time limb motion tracking and precise damage localization.

It is a formidable challenge to integrate superior damage tolerance into robust ionogels due to fundamental conflicts between covalent rigidity and dynamic energy dissipation. Herein, an echinoderm-inspired supramolecular ionogel is engineered with extreme robustness and damage tolerance via synergistic integration of hard-soft phase-separated architecture and multi-scale sacrificial bonding. The molecularly programmed hard segments of polyurethane integrate crystalline domains, high-density hydrogen bonds, and π–π stacking, which collectively enhance ionogel robustness, while a judiciously selected ionic liquid (IL) reinforced the hard phase via extensive IL-polymer multiple hydrogen bonds. The crystalline domains synergizing with reversible sacrificial bonds facilitated efficient energy dissipation through dynamic rupture/reformation mechanisms. Consequently, the supramolecular ionogel achieves advanced tensile strength (49.22 MPa), elongation (1721.28%), toughness (424.09 MJ m−3), Young's modulus (48.66 MPa) and unprecedented damage tolerance, manifested as tear resistance (387.02 kJ m−2, 59-fold that of polyurethane), outstanding puncture energy (1326.8 mJ), and exceptional high-speed impact resistance (228.74 MJ m−3 at strain rate of 20 000 s−1). Notably, the ionogel demonstrated autonomous room-temperature self-healing, broad operational temperature adaptability, flame retardancy, and recyclability. Furthermore, a wearable ionogel sensing matrix is developed to simultaneously accomplish real-time limb motion tracking and precise damage localization, targeting next-generation intelligent protective equipment to deliver integrated impact protection and flexible sensing.

A 3D/0D S-scheme heterojunction photocatalyst is constructed by spatially confining ZnSe quantum dots within covalent organic framework (COF) porous cages, enabling coupled CO2 photoreduction and value-added chemical synthesis. COF porous cages serve as nanoreactors, enriching reactant concentrations, and the S-scheme heterojunction facilitates charge separation. This synergistic integration of nanoconfinement and S-scheme charge modulation establishes an efficient and robust bifunctional platform.

Coupling photocatalytic CO2 reduction with the synthesis of value-added chemicals represents a promising strategy to mitigate carbon emissions while maximizing solar energy utilization. Quantum dots (QDs) are attractive photocatalysts for such tandem reactions, owing to their size-tunable band structures, abundant surface-active sites, and strong light-harvesting capabilities. However, their implementation is often hindered by severe aggregation and sluggish mass transfer, which limit their photocatalytic performance. Herein, a spatially confined 3D/0D covalent organic framework (COF)/ZnSe QDs step-scheme (S-scheme) heterojunction photocatalyst is reported, prepared via an in situ encapsulation strategy, for concurrent CO2 photoreduction and organic transformation. The ZnSe QDs are immobilized within the nanoporous cages of the COF, forming a confined microenvironment that suppresses aggregation, enhances photostability, and promotes efficient mass transfer. As a result, the COF/ZnSe heterostructure achieves a CO generation rate of 128.3 µmol g⁻1 h⁻1, while synchronously delivering 95.1% conversion of 1-phenylethanol to 1-phenylethanone under light irradiation. The hierarchical COF matrix acts as a nanoreactor, enriching local CO2 concentration within its porous network, while the rationally designed S-scheme heterojunction facilitates directional charge flow, ensuring robust redox selectivity. This work provides a generalizable strategy for designing advanced heterostructured photocatalysts for efficient bifunctional solar chemical conversions.