Physics
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ABSTRACT Tin dioxide (SnO 2 ) has been demonstrated to convert CO 2 to formate in an electrocatalytic CO 2 reduction reaction (eCO 2 RR). However, suboptimal CO 2 activation and insufficient electrical conductivity pose formidable challenges to achieving desirable eCO 2 RR activity. Herein, a heterostructured CuS@SnO 2 catalyst was designed to realize efficient formate production in eCO 2 RR, which delivers a Faraday efficiency (FE) of 94.9% and partial current density of 243.5 mA cm −2 at −1.1 V versus RHE in alkaline conditions, coupled with excellent electrochemical stability. Systematic investigations reveal that CuS acts as an electron reservoir, and the directional electron transfer channels induce interfacial electron deficiency in SnO 2 , stabilizing Sn active sites during long‐term eCO 2 RR operation. Furthermore, it confers dual effects for promoting formate conversion at the molecular level, which integrates optimized interface electronic structure and enhanced p–p orbital coupling between the key * OCHO intermediate and SnO 2 interface, rendering the enhanced * OCHO adsorption, decreased CO 2 hydrogenation energy barrier, and improved intrinsic formate activity. Beyond catalytic performance, CuS@SnO 2 was further utilized in a Li‐CO 2 battery to enable integrated CO 2 conversion and energy storage functionality. This study provides a strategy to effectively regulate the formate selectivity of eCO 2 RR by heterointerface engineering, and meanwhile bridges rational catalyst design with practical CO 2 conversion technologies.
ABSTRACT Seawater electrocatalysis is essential for energy conversion systems, particularly metal‐air batteries that utilize seawater as the electrolyte. However, developing durable oxygen reduction catalysts for direct seawater operation remains challenging due to severe chloride corrosion and scale deposition. Here, a Pt–Lu 2 O 3 /KB catalyst is rapidly synthesized via a microwave‐assisted method, which constructs an asymmetric Pt–O–Lu interface in which the Lewis‐acidic Lu 2 O 3 regulates the interfacial chemistry by selectively anchoring cathodically generated OH − , thereby suppressing their diffusion and preventing the formation of Ca 2+ and Mg 2+ precipitates. Meanwhile, the local enrichment of OH − at the interface generates electrostatic repulsion with Cl − , effectively inhibiting Cl − adsorption, thereby mitigating site poisoning and enhancing structural stability. As a result, Pt–Lu 2 O 3 /KB exhibits remarkable ORR activity and durability, with a half‐wave potential of 0.88 V (vs. RHE) in alkaline seawater. It demonstrates exceptional ORR performance in zinc–air batteries, with stable operation for 280 h in alkaline seawater and sustained discharge for over 200 h in natural seawater.
Reciprocal Synergistic Evolution of Cu‐Co Sites Boosts Electrocatalytic Nitrate Reduction to Ammonia
ABSTRACT The electrocatalytic nitrate reduction reaction (NO 3 RR) offers a promising route for sustainable ammonia synthesis. Due to the interfacial synergistic effects, Cu–Co catalysts exhibit outstanding activity. However, the underlying evolution of active sites remains poorly understood, which induces the reported advantageous phase‐segregating in situ restructuring. By monitoring Co(OH) 2 /Cu catalysts, our observations revealed that Cu‐ and Co‐related sites undergo dynamic, “seesaw‐like” reciprocal reactivation instead of mutual stabilization. In situ SERS, DMPO‐EPR and DFT calculations show that this process is driven by the competing oxidative/reductive forces under NO 3 RR conditions, which cause site deactivation, and mediated via the transfer of ∙O/∙OH and H* radicals across interfaces. Critically, these radicals trigger the conversion of deactivated CuO x and Co(OH) 2 sites into highly active oxide‐derived Cu 0 and CoOOH, respectively. As the interfacial transfer of radicals constitutes an irreversible process, the observed in situ restructuring is inherently rationalized. This conjugated, seesaw‐like mechanism accelerates a dynamic, self‐regulating redox balance at Cu–Co heterointerface, continuously enhancing the synergy between Cu‐ and Co‐related sites and the overall NO 3 RR performance. Beyond catalyst development, this work offers a mechanistic framework for understanding how competing oxidative and reductive forces are redistributed at heterointerfaces, providing guiding principles for the rational design of next‐generation electrocatalysts.
ABSTRACT O‐type sodium‐based layered oxide cathodes show strong practical applicability due to their high theoretical capacity. However, the narrow ion diffusion channels in the O‐type framework often lead to poor cycling stability, posing a challenge long‐term durability over thousands of cycles. Herein, we establish the Bramfitt lattice mismatch value ( δ interplanar ) as a key quantitative descriptor for intergrowth phase stability and a lattice‐matched O3/O'3 intergrowth structure is proposed, which exhibits superior cycling stability. The ultralow Bramfitt lattice mismatch value ( δ interplanar = 0.71%) in Na + ‐active facets enables tight integration of rigid O3 and flexible O′3 phases, forming a robust rigid‐flexible‐rigid structure. This design effectively mitigates TM slab gliding, resulting in a pure P‐type solid solution region of 86.7% during charge/discharge and a minimal volume expansion of only 2.39%. Moreover, the stable framework suppresses transition metal dissolution and parasitic anion redox, ensuring highly reversible Na + insertion/extraction. The combination of above factors results in an outstanding cycling stability with 79.7% capacity retention after 2000 cycles, significantly outperforming conventional O‐type materials. This work decouples the quantitative role of lattice mismatch in intergrowth phase stability and provides a highly compatible cathode, offering valuable guidance for the construction of high‐performance sodium‐ion batteries geared toward practical large‐scale energy storage.
ABSTRACT Anion exchange membrane water electrolysis (AEMWE) stands as one of the core technologies for the hydrogen economy. In the field of cathodic electrocatalysis, most studies concentrate on optimizing the sluggish water dissociation and hydrogen adsorption kinetics of electrocatalysts yet largely overlook the site‐blocking effect caused by OH intermediate adsorption on active sites during water splitting. In this work, highly dispersed bimetallic Ru and Ni nanoclusters anchored on Tungsten carbide (WC) were synthesized via a microwave‐assisted quasi‐solid‐state route, achieving excellent hydrogen evolution reaction (HER) electrocatalytic activity in 1 m KOH. The Ru‐Ni/WC catalyst delivers a low overpotential of 29 mV at 10 mA cm −2 , with no appreciable activity degradation observed over long‐term continuous operation in alkaline electrolyte. Experimental characterizations and theoretical calculations unambiguously reveal that Ru‐Ni/WC facilitates the formation of an ordered yet flexible interfacial hydrogen bond network. This network not only promotes water dissociation but also enables a bidirectional spillover effect, in which adsorbed H migrates to Ru sites while adsorbed OH shuttles to Ni sites, synergistically accelerating the alkaline HER kinetics. This study offers a fresh insight into tackling the key challenges of AEMWE cathodic catalysis.
The deterministic integration of functional oxide thin films on technologically relevant substrates is a longstanding challenge for oxide electronics. Two-dimensional Ca 2 Nb 3 O 10 nanosheets have emerged as versatile epitaxial templates, enabling high-quality film growth on arbitrary substrates by decoupling the overlying layer from the underlying support. However, the intrinsic gaps inherent in monolayer nanosheet assemblies originate from irregular geometry and stochastic deposition processes. These gaps create exposed substrate regions that introduce a second, distinct growth environment, whose influence on film properties remains poorly understood. Here, we demonstrate that these nanoscale gaps are not merely structural imperfections but rather tunable elements that govern the crystallinity, transport behavior, and magnetic anisotropy of SrRuO 3 thin films. By engineering Ca 2 Nb 3 O 10 nanosheets with controlled lateral size distributions (>20 μm and <2 μm) and systematically varying substrate coverage (≈90% and ≈95%), precise modulation of the crystallographic phase of gap-nucleated SrRuO 3 is achieved. The phase varies from amorphous on SiO 2 to polycrystalline on Si and Al 2 O 3, and coexists with c -axis-oriented epitaxy templated by the nanosheets. This coexistence gives rise to emergent phenomena including nonuniaxial magnetic anisotropy, two-channel anomalous Hall signatures, and stepwise magnetization reversal, all of which are tunable through coverage and substrate selection. Bilayer nanosheet coatings effectively eliminate gap contributions, restoring pristine in-plane easy magnetization axis and confirming complete film–substrate decoupling. Our findings establish a previously unrecognized design paradigm in which the deliberate control of nanosheet gaps enables the engineering of composite magnetic and electronic ground states in oxide thin films, providing a scalable route toward multifunctional spintronic devices on arbitrary substrates.
X-ray detectors play an important role in medical imaging, security inspection, industrial nondestructive testing, and high-energy physics. Oxide single crystals are attractive candidates for direct X-ray detection because of their high chemical stability, good mechanical robustness, and feasibility for large-size crystal growth. However, their ultrahigh intrinsic resistivity often limits photocurrent generation and thus restricts detection sensitivity. Here, Zr doping is proposed as a strategy to regulate carrier transport in LiYMo 2 O 8 (LYMO) single crystals. Pristine LYMO and Zr-doped LYMO crystals were successfully grown by the top-seeded solution growth method. The pristine LYMO crystal exhibits resistivities of 9.96 × 10 13 and 1.44 × 10 14 Ω cm along the a - and c -axes, respectively, with corresponding mobility-lifetime ( μτ ) products of 1.15 × 10 –3 and 1.81 × 10 –3 cm 2 V –1 . After Zr incorporation, the a -axis resistivity decreases to 5.68 × 10 9 Ω cm, while the μτ product increases to 8.97 × 10 –3 cm 2 V –1 . As a result, the a -axis X-ray sensitivity reaches 431 μC Gy –1 cm –2 under 40 keV X-ray irradiation, more than twice that of the pristine LYMO detector. The Zr-doped LYMO detector also maintains low detection limits of 50.1 and 29.8 nGy s –1 along the a - and c -axes, respectively. These results demonstrate that rational Zr 4+ donor doping is an effective approach to balancing resistivity, charge collection efficiency, and baseline stability in high-resistivity oxide crystals for improved X-ray detection.
High Resolution Image Download MS PowerPoint Slide Photoisomerization-based liquid crystal elastomer (LCE) actuators offer precise spatiotemporal control over mechanical deformation, yet their reliance on ultraviolet (UV) irradiation limits biomedical applicability due to phototoxicity and poor tissue penetration. Herein, we report an 808 nm near-infrared (NIR) light-driven photoisomerization actuator based on azobenzene-cross-linked LCEs (Azo-LCEs) integrated with NaYF 4:Yb/Tm@NaYF 4:Yb/Nd@NaYF 4 core–shell–shell upconversion nanoparticles (CSS-UCNPs). The Nd 3+ -sensitized CSS-UCNPs convert 808 nm NIR light into UV/blue upconversion emissions (345–476 nm), driving trans -to- cis isomerization of azobenzene units and inducing macroscopic bending of the LCE films. To evaluate the actuation performance, the UCNPs/Azo-LCE films were tested under continuous-wave 808 nm irradiation for 20 s at power densities of 4–24 W cm –2, reaching a maximum bending angle of 42.8 ± 2.6° at 24 W cm –2 and exhibiting stable cyclic actuation over 50 cycles at 16 W cm –2 . For biologically relevant operation, thermal assessment at lower irradiation intensities revealed only a limited temperature rise in the culture medium under 4–8 W cm –2 irradiation (Δ T = 2.29–4.36 °C), with no obvious cumulative heating during cyclic operation (20 s on/20 s off, 50 cycles). In addition, microgroove-patterned UCNPs/Azo-LCE substrates supported the adhesion and spreading of rat cardiomyoblast cells (H9c2) and guided groove-width-dependent uniaxial alignment. This work establishes a strategy for 808 nm-excited photoisomerization-driven LCE actuation and highlights its potential as an NIR-addressable soft actuator platform for future studies of dynamic cell-guidance, while operating with a modest thermal burden under the tested conditions.
Lactate dehydrogenase (LDH) and interleukin-6 (IL-6) serve as two critical biomarkers for assessing disease progression and cellular model status, providing comprehensive pathological insights from the perspectives of cellular metabolism and immunomodulation, respectively. The most widely used method for LDH detection is a colorimetric assay utilizing nicotinamide adenine dinucleotide (NAD) as a coenzyme and lactate as the substrate, which quantifies LDH activity by measuring formazan dye. Although this method offers high sensitivity, its reliance on sophisticated instrumentation limits its applicability in resource-constrained settings. In this study, we developed a capacitive sensing electrode functionalized with specific antibodies for the simultaneous detection of LDH and IL-6 using electrochemical capacitance spectroscopy (ECS). Unlike label-based methods such as ELISA, this label-free strategy enables direct target recognition without the need for labeling reagents or additional procedural steps. A one-step modification process was employed to construct a protein-passivated graphene bioelectrochemical interface, enabling covalent immobilization of antibodies on the electrode surface. This sensor operates based on a coplanar ITO three-electrode system, exhibiting a significant signal response over a broad concentration range spanning 5 orders of magnitude for the target molecules. These results underscore the potential of ECS for the quantification of LDH and IL-6, supporting its promising application in the development of point-of-care (PoC) biosensors.
Superlattices (SLs) stand out for their unique periodic structure and allow for nuanced tuning of their properties via structural designs and interface feature modification, which have gained broad attention across diverse domains. Particularly, in the thermoelectric field, encouragingly, its existence provides a novel strategy to solve the central issue in the research of thermoelectric materials, namely, the decoupling of thermal transport and electrical transport. The extra phonon scattering at the interface, coupled with charge transfer and energy filtering in the interface, makes it possess extremely low thermal transport properties and excellent electrical transport properties simultaneously. These characteristics position the superlattices as alternatives to traditional thermoelectric materials. Herein, we heavily focus on the intricate relationship between thermal transport tailoring and element selection as well as interface features in the SLs. Then, recent advances in the research of various SL-based thermoelectric material systems and their electric transport modulation mechanisms are reviewed with carefully selected examples, subsequently emphasizing their contributions to energy harvesting and refrigeration. The review culminates in summarizing the challenges and opportunities for the future development of materials, devices, and applications. Overall, this review is expected to contribute to the research and development of high-performance thermoelectric materials and expand their application areas for researchers.
Chimeric antigen receptor macrophages (CAR-Ms) are promising in solid tumor therapy due to their tumor-penetrating property and antigen-specific phagocytosis. However, current CAR-M therapy is limited by the low ex vivo proliferation of macrophages and the complexity of the engineering process. Generating CAR-Ms in vivo can overcome these challenges but still faces an M2-like pro-tumor phenotype polarized by immunosuppressive tumor microenvironment. Herein, we devise macrophage-preferential ionizable cationic lipid-assisted polymeric nanoparticles (iCLANs) to co-deliver mRNAs encoding interferon-γ (IFN-γ) and a CAR molecule, denoted as iCLAN mCAR+mIFN-γ, enabling in vivo engineering of CAR-Ms with a sustained M1-like phenotype. iCLAN mCAR+mIFN-γ can coexpress IFN-γ and CAR in tumor-associated macrophages, thereby producing CAR-Ms capable of maintaining antitumor phenotype to effectively engulf tumor cells in an antigen-specific manner. Intravenous injection of iCLAN mCAR+mIFN-γ in EGFRvIII + breast tumor and CD19 + B-cell lymphoma models directly generates EGFRvIII CAR-Ms or CD19 CAR-Ms within tumors, resulting in significant tumor growth inhibition and remodeling of the immunosuppressive tumor microenvironment. This study provides an efficient strategy for in vivo engineering of M1-like CAR-Ms for cancer therapy.
Soft-lattice nanocrystal photon management hinges on controlling relaxation branching, diverting excitations from interfacial losses into radiative pathways. CsPbCl 3:Yb 3+ quantum cutting benchmarks this, but is still constrained by surface trapping, suboptimal Yb-pair branching energetics, and limited thermal/environmental stability. Here we implement a (2-bromoethyl)trimethylammonium bromide (BETAB)-enabled passivation strategy with annealing-triggered gradient halide reconstruction. BETAB replaces OA/OAm to reduce surface losses, while mild annealing activates ligand-associated Br – as a local reservoir to drive Br – in-diffusion with Cl – counter-migration, writing a continuous radial Cl/Br gradient (Br-rich interior). The graded halide landscape suppresses interfacial quenching and creates a radial band-edge bias that funnels excitations into the QC pathway, accelerating exciton-to-Yb 3+ transfer. Consequently, QC PLQY increases stepwise from 84.7% (pristine) to 125.4% (BETAB-treated) and 155.2% (annealed). Integrated as spectral-conversion films on Si photodetectors, the treated NCs enable 200–1100 nm detection with responsivity up to 0.5 A W –1, EQE of 64.17%, and D * >1.02 × 10 12 Jones (300–1100 nm) and 4.8 × 10 11 Jones (200–300 nm), delivering clear ultrabroadband imaging in 7 × 7 arrays. The reconstructed NCs further show ATQ-like behavior (134% at ∼333 K) and improved aging stability (86.1% retention after 60 days vs 29.2% for pristine). Overall, ligand-enabled gradient writing reroutes relaxation for robust photon management.
The development of efficient and sustainable strategies for imine synthesis remains highly desirable, as conventional approaches often suffer from harsh reaction conditions and limited selectivity. Herein, we report an electrocatalytic strategy that utilizes reproducible electricity to drive the selective oxidative coupling of benzylamine (BA) into imines under mild conditions. A series of disubstituted Keggin polyoxometalates (POMs), M 2 PW 10 O 38 (M = Fe–Zn), were assembled at the gas–liquid interface into well-defined two-dimensional nanosheet superstructures. Structural characterizations reveal a uniform nanosheet morphology, featuring single-cluster assembly and highly ordered arrangements of POM units. Among these, the Fe 2 PW 10 NS exhibits outstanding electrocatalytic performance for BA oxidation, achieving >99% conversion, 99% yield of the target imine, and a Faradaic efficiency of 81.8%, along with excellent cycling stability. Comparative studies highlight the advantages of the cluster-assembled superstructure arising from the high density of accessible active sites and the synergistic effects of the ordered superstructure. Furthermore, substrate scope investigations demonstrate the broad applicability toward diverse amine substrates. This work provides a viable platform for the green and efficient synthesis of value-added imines and offers valuable insights into the design of advanced POM-based electrocatalysts.
Surface plasmon polaritons (SPPs) in metallic nanowires have emerged as powerful candidates for nanoscale optical circuitry, yet their practical application is often limited by significant plasmonic losses and short propagation distances. While prior studies have extensively characterized nanowires under ambient conditions, little is known about how extreme external stimuli modify plasmon transport. To address this knowledge gap, we report measurements of SPP propagation with silver nanowires loaded in a diamond anvil cell (DAC) at hydrostatic pressures up to 6 GPa. By increasing the hydrostatic pressure to 6 GPa, we reveal a doubled propagation distance for the same individual nanowire. The pressure dependence suggests a suppression of dominant damping channels, including suppression of electron–phonon scattering and electron–electron scattering, as supported by density functional theory calculations. These results highlight pressure as a novel tuning knob for plasmonic transport and suggest possible applications in high-pressure optical sensing and adaptive plasmonic wave guides.
Cells generate and respond to mechanical forces across compartments, with the plasma membrane acting as a nanoscale interface for sensing and transmitting tension. How intracellular forces translate into membrane tension during dynamic processes such as neutrophil extracellular trap (NET) formation remains unclear. Here, we combine the mechanosensitive fluorescent probe Flipper-TR with fluorescence lifetime imaging microscopy (FLIM) to map spatiotemporal plasma membrane tension changes in living cells. After validation in HeLa and dHL-60 cells under osmotic perturbation, we apply this approach to primary human neutrophils undergoing NETosis. Membrane tension transiently increases during chromatin decondensation and nuclear swelling within 60 min, followed by a marked decrease after membrane rupture. Prior to rupture, tension is spatially heterogeneous, indicating localized nanoscale mechanical regulation. Cholesterol depletion abolishes the transient increase and reduces heterogeneity without affecting NETosis kinetics. These findings establish the plasma membrane as a dynamic nanoscale reporter of intracellular mechanical stress during NETosis.
Fluid molecular ferroelectrics are a new class of organic materials where ferroelectricity is found in conjunction with 3D fluidity whilst still retaining spontaneous polarization values comparable to their traditional solid-state counterparts. One of the major challenges for soft condensed matter physics is predicting whether a fluid molecular material will form ferroelectric phase with nematic or smectic order. Through the synthesis of 45 systematically varied molecules, and by analogy to solid molecular ferroelectrics, it is shown that subtle hydrogen-fluorine (H/F) substitution(s) allows for tuneable syn-parallel pairing motifs resulting in either specific pairings, leading too geometrically constrained lamellar order, or diversified pairings, stabilising nematic ordering. Large-scale, fully atomistic molecular dynamics simulations reveal that smectic ferroelectricity emerges from discrete lateral pairing modes, whereas nematic phases arise from a multiplicity of equivalent polar configurations. Together, these findings establish experimentally validated design principles for fluid molecular ferroelectrics and provide a predictive framework for engineering functional polar fluids.
ABSTRACT Gel electrolytes, which supply compensating ions for electrochromic reactions and serve as conductive media, are widely used in electrochromic devices (ECDs). However, the complex preparation processes for gel electrolytes often involve the use of large amounts of organic solvents and hazardous or valuable reagents, limiting their widespread adoption in ECDs. This paper presents a straightforward method for fabricating large‐area hydroxypropyl methylcellulose (HPMC) gel electrolytes using a solution casting technique in an aqueous system. The addition of deep eutectic solvents (DES) and the incorporation of SiO 2 nanoparticles significantly improve the conductivity of the gel electrolytes. The resulting HPMC/DES‐SiO 2 gel electrolyte exhibits high transparency (over 92% transmittance), high ionic conductivity (7.55 × 10 −4 S/cm), wide electrochemical window (±3 V), and outstanding thermal stability. The W 18 O 49 /NiO ECD assembled with HPMC/DES‐SiO 2 gel electrolyte shows excellent cycling stability (maintained 94.8% of initial optical modulation after 1000 cycles) and can perform electrochromic response over a wide temperature range from −50°C to 200°C. Furthermore, the entire HPMC and up to 82.7% of LiTFSI and NMA can be recycled and reprocessed into new gel electrolytes, offering a promising solution for the future development of environmentally friendly and efficient ECDs.
ABSTRACT Defect engineering offers a practical route to control interfacial charge states in polymer‐inorganic composites, yet translating this control into optically writable and non‐volatile polarization in soft dielectrics remains difficult. Here, we introduce a Polydimethylsiloxane (PDMS)‐based composite that can be written by light to form an interfacial polarization state. The design relies on FeTiO 3 (FTO) nanoparticles with oxygen‐vacancy associated trap states, whose density is tuned by spark plasma sintering to create a trap‐rich polymer‐oxide interface. Under illumination, photocarriers promote interfacial charge transfer by reducing the effective barrier at the metal‐composite contact, producing a rapid rise in interfacial charge accumulation. After the light is removed, a large fraction of the photoexcited electrons becomes immobilized, leaving a residual polarization that relaxes only slowly. We quantify the write‐relax behavior using a triboelectric nanogenerator configuration as a sensitive probe of interfacial charge transfer, and we directly visualize the photo‐written electrostatic state and its retention by Kelvin probe force microscopy. These results present defect‐mediated charge trapping as a materials‐level mechanism for light‐programmable, long‐retention polarization in soft composites, enabling remotely addressable electrostatic interfaces for soft electronic systems.
ABSTRACT Recently, high‐endurance ferroelectric HfO 2 is highly desirable since the emerging of in‐memory computing requires non‐volatile memories not only to store data but also to execute computation, challenging writing/erasure switching reliability. Understanding and exploitation of the polarization fatigue diagram are crucial for improving endurance performances. Here, we show fatigue‐resistant Sm:HfO 2 thin films by modulating grain boundaries (GBs) in orientation‐controllable orthorhombic phase. On GBs, orientation discontinuity raises energy levels of O 2 p orbitals due to lattice distortion, which promote electron accumulation and yield a high‐symmetry structural transform at the boundary, facilitating 90° switching of out‐of‐plane domains because of lowered switching barrier. Then the domains are frozen in plane by the charged GBs and polarization fatigue takes place. By eliminating GBs associated with phase transform, remarkably‐improved fatigue resistance is achieved in uniform 180° switching, which exhibits the increase of fatigue‐free endurance by 200 times to 2.0 × 10 9 cycles with, more importantly, a large field‐cycling non‐volatile polarization of ∼60 µC/cm 2 , showing the state‐of‐the‐art endurance performances in hafnium oxides. Roadmaps of the fatigue scenarios are given based on key roles of GBs in domain configurations and switching pathways. Our findings open a new perspective for fatigue studying and guide the material design of high‐reliability hafnium oxide memories.
ABSTRACT The development of multilayer ceramic capacitors (MLCCs) with high‐energy storage performance over a wide temperature range is critical for practical applications but remains challenging. Here, we propose a high‐entropy design to disrupt the long‐range ferroelectric order of tetragonal tungsten bronze (TTB) ceramics, inducing a polarization discontinuity composed of coexisting polar nanoregions and non‐polar regions. This unique configuration delays polarization saturation while minimizing hysteresis loss through electrostatic interactions. Consequently, the TTB‐based MLCC achieves a high recoverable energy density ( W rec ) of 15.8 J cm −3 and an ultrahigh energy efficiency ( η ) of 97.5%, yielding a record‐high figure of merit of 632 J cm −3 for TTB‐based ceramic capacitors. Furthermore, the MLCC exhibits outstanding thermal stability from 25°C to 150°C, maintaining W rec ≈ 13.04 ± 0.41 J cm −3 and η ≈ 95.43 ± 2.61%. The high‐entropy‐induced polarization discontinuity offers valuable insights into polarization modulation and provides an effective strategy for designing next‐generation high‐performance dielectrics.
The integration of solution-processed perovskite light-emitting diodes (PeLEDs) with vacuum-deposited organic light-emitting diodes (OLEDs) in tandem architectures offers a promising pathway toward next-generation displays. However, directly stacking electroluminescent units with dissimilar optoelectronic characteristics often results in electroluminescence losses and spectral broadening. To achieve efficient and narrowband tandem emission, we first develop high-performance green PeLEDs as the bottom subunit through rational trap-state management. By precisely optimizing device efficiency-impedance matching, we realize synchronous operation of the PeLED and OLED subunits at their respective maximum efficiencies, producing constructive electroluminescence interference and yielding significant efficiency enhancement. Moreover, delicate regulation of the relative emission contributions ensures optimal spectral overlap and superposition, leading to markedly strengthened narrowband output. Using this strategy, tandem devices integrating PeLEDs with two representative OLEDs deliver record-breaking external quantum efficiencies of 52.3% and 54.8%, with narrow full widths at half maximum of 22 and 24 nm, respectively. This work establishes a fundamental design principle for tandem light-emitting diodes that simultaneously overcome limitations in EL efficiency and color purity in advanced display technologies.
ABSTRACT Enhancing the low‐temperature cycling performance of lithium metal batteries (LMBs) relies on the rational design of solid electrolyte interphases (SEIs). Conventional approaches typically involve tuning electrolyte compositions to indirectly generate SEIs dominated by organic or inorganic components. However, organic‐rich SEI fails to inhibit the growth of Li dendrites, compromising sluggish Li + kinetics, and inorganic‐rich SEI suffers from mechanical brittleness at low temperatures, resulting in inadequate interfacial mechanical stability. Herein, we introduce a siloxane‐based elastomeric coating on the Li anode surface by leveraging its intrinsic solvent phobicity to achieve selective ion conduction, facilitating the formation of a LiF‐rich inner SEI, which synergizes with the elastomer to construct a double‐layer organic‐inorganic SEI. Theoretical calculations and experimental results demonstrate that such a double‐layer SEI combines mechanical flexibility enabled by organic components with promoted Li + transport imparted by inorganic components, synergistically improving the cycling stability of LMBs under low‐temperature conditions. The target LMBs paired with industrial‐standard NCM811 cathodes deliver 99% capacity retention over 300 cycles at –25°C. Unlike indirect electrolyte modification approaches, our method enables direct manipulation of SEI structures and is compatible with various electrolyte systems.
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