Terahertz (THz) signals are crucial for ultrawideband communication and high-resolution radar, demanding miniaturized detectors that can simultaneously measure multiple parameters such as intensity, frequency, polarization, and phase. Traditional detectors fail to meet these needs. To address this, we introduce a plasmon polariton atomic cavity (PPAC) detector based on monolayer graphene, offering a multifunctional, monolithic, and miniaturized solution. With a footprint only one-tenth the size of the incoming wavelength, the PPAC achieves benchmark performance in intensity-, frequency-, and polarization-sensitive detection. Operating at room temperature across 0.22-4.24 THz, it delivers sub-diffraction detection resolution and high-speed operation. Furthermore, we demonstrate its application in free-space THz polarization-coded communication and stealth imaging for physical property analysis. The unique design of PPAC enables strong absorption with weak signal detection, within a structure just 10 times the excitation wavelength in thickness, an accomplishment beyond current technologies. By simultaneously resolving intensity, frequency, and polarization, this detector can replace multiple single-function devices, providing a compact and efficient solution for next-generation ultrawideband communication and high-resolution radar systems.

Co-free high-Ni layered cathode materials LiNiMeO (Me = Mn, Mg, Al, etc.) are a key part of the next-generation high-energy lithium-ion batteries (LIBs) due to their high specific capacity and low cost. However, the hindered Li kinetics and the high reactivity of Ni result in poor rate performance and unsatisfied cycling stability. This work designs a promising strategy for designing a high-performance high-entropy doping Co-free high-Ni layered cathode LiNiMnMgTaMoNaO (HE-Ni90-1.557) by elemental screening and compositional fine-tuning. Compositional fine-tuning optimizes the synergistic relationship between the high-entropy dopant elements, thereby significantly suppresses the kinetic hysteresis induced by Li/Ni mixing. The pillar effect significantly enhances the diffusion kinetics of Li at the high state of charge (SOC). Meanwhile, the high-entropy fine-tuning significantly postpones the H2-H3 phase transition and reduces the dissolution of transition metals and the loss of lattice oxygen in the cathodes. Consequently, the diffusion kinetics of Li at the atomic and electrode particle scales are significantly enhanced. The HE-Ni90-1.557 cathode exhibits an initial capacity of 225.1 mAh g at 0.2 C and a full cell with a high capacity retention of 83.1% after 1500 cycles at 3C. This work provides a promising avenue for commercializing Co-free high-Ni cathodes for next-generation LIBs.

Current challenges in tissue engineering include creation of extracellular environments that support and interact with cells using biochemical, mechanical, and structural cues. Spatial control over these cues is currently limited due to a lack of suitable fabrication techniques. This study introduces Xolography, an emerging dual-color light-sheet volumetric printing technology, to achieve control over structural and mechanical features for hydrogel-based photoresins at micro- to macroscale while printing within minutes. A water-soluble photoswitch photoinitiator system and a library of naturally-derived, synthetic, and thermoresponsive hydrogels for Xolography are proposed. Centimeter-scale, 3D constructs with positive features of 20 µm and negative features of ≈100 µm are fabricated with control over mechanical properties (compressive moduli 0.2 kPa-6.5 MPa). Notably, switching from binary to grayscaled light projection enables spatial control over stiffness (0.2-16 kPa). As a proof of concept, grayscaled Xolography is leveraged with thermoresponsive hydrogels to introduce reversible anisotropic shape changes beyond isometric shrinkage. Xolography of viable cell aggregates is finally demonstrated, laying the foundation for cell-laden printing of dynamic, cell-instructive environments with tunable structural and mechanical cues in a fast one-step process. Overall, these innovations unlock unique possibilities of Xolography across multiple biomedical applications.

Electrochemical oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) provides an environmentally friendly route for producing the sustainable polymer monomer 2,5-furandicarboxylic acid (FDCA). Thus, precisely adjusting the synergistic adsorption among key reactive species, such as HMF and OH, on the carefully designed catalyst surface is essential for achieving satisfactory catalytic performance for HMF oxidation to FDCA as it is closely related to the adsorption strength and configuration of the reaction substrates. This kind of regulation will ultimately facilitate the improvement of HMF oxidation performance. In this work, Pt nanoparticles modified CuO nanowires (denoted as Pt/CuO@CF) are constructed for the selective electrooxidation of HMF to FDCA under alkaline conditions. The well-designed Pt/CuO@CF demonstrates highly impressive catalytic performance across a range of HMF concentrations, ranging from the commonly used concentrations to higher levels typically not explored (10, 25, 50, 75, and 100 mm) with high FE (all above 95%) and outstanding long-term stability (15 cycles). In situ experimental characterizations confirm that the designed heterogeneous interface between Pt and CuO enhances the enrichment of HMF and OH species on the catalyst surface. Theoretical calculations reveal the anchored Pt nanoparticles reduce the adsorption barrier for HMF and OH, thereby promoting the highly selective oxidation of HMF to FDCA.

Formamidinium lead iodide (FAPbI) perovskite films, ensuring optically active phase purity with uniform crystal orientation, are ideal for photovoltaic applications. However, the optically active α-FAPbI phase is easy to degrade into δ-phase due to numerous defects within randomly oriented films. Here, a "quasi-2D" perovskite template is pre-deposited on the film surface within the crystallization process based on the two-step preparation technology, which directly induced pure and highly orientated crystallization of α-FAPbI across the downward growth process. Furthermore, the enlarged interaction between 2D components with colloidal properties and lead iodide delayed the crystallization process effectively, yielding high crystallinity with low trap state density. The resulting perovskite photovoltaic devices exhibited a champion efficiency as high as 25.79% with comprehensively improved device stability. This work provides new insights into the utilization of 2D components and the formation mechanism behind 2D perovskites.

The safety of the P2-type layered transition metal oxides (P2-NaTMO), a promising cathode material for sodium-ion batteries (SIBs), is a prerequisite for grid-scale energy storage systems. However, previous thermal runaway studies mainly focused on morphological changes resulting from gas production detection and thermogravimetric analysis, while the structural transition and chemical reactions underlying these processes are still unclear. Herein, a comprehensive methodology to unveil an interplay mechanism among phase structures, interfacial microcrack, and thermal stability of the charged P2-NaNiMnO (NNMO) and the P2-NaNiLiMnO (NNMO-Li) at elevated temperatures is established. Combining a series of crystallographic and thermodynamic characterization techniques, the specific chemical reactions occurring in the NNMO materials during thermal runaway are clarified first and solidly proved that Li doping effectively hinders the dissolution of transition metal ions, reduces oxygen release, and enhances thermal stability at elevated temperatures. Importantly, based on Arrhenius and nonisothermal kinetic equations, the kinetic triplet model is successfully constructed to in-depth elucidate the thermal decomposition reaction mechanism of P2-NaTMO, demonstrating that such thermodynamic assessment provides a new perspective for building high-safety SIBs.

Efficient magnetization control is a central issue in magnetism and spintronics. Particularly, there are increasing demands for manipulation of magnetic states in van der Waals (vdW) magnets with unconventional functionalities. However, the electrically induced phase transition between ferromagnetic-to-antiferromagnetic states without external magnetic field is yet to be demonstrated. Here, the current-induced magnetic phase transition in a vdW ferromagnet FeGeTe is reported. Based on magneto-transport measurements and theoretical analysis, it is demonstrated that transition in the interlayer magnetic coupling occurs through vertical voltage drop between layers induced by current which is attributed to high anisotropy of the resistivity caused by the vdW gaps. Such magnetic phase transition results in giant modulation of the longitudinal magnetoresistance from 5% to 170%. The electrical tunability of the magnetic phase in FeGeTe with current-in-plane geometry opens a path for electric control of magnetic properties, expanding the ability to use vdW magnets for spintronic applications.

Van der Waals (vdW) dielectrics are extensively employed to enhance the performance of 2D electronic devices. However, current vdW dielectric materials still encounter challenges such as low dielectric constant (κ) and difficulties in synthesizing high-quality single crystals. 2D rare-earth oxyhalides (REOXs) with exceptional electrical properties present an opportunity for the exploration of novel high-κ dielectrics. In this study, for the first time, the synthesis of a series of van der Waals layered gadolinium oxyhalides with thicknesses down to monolayer through a space-confined vdW epitaxy approach and demonstrating their application as a single-crystalline gate dielectric is reported. It exhibits a remarkable relative dielectric constant exceeding 17 and an impressive breakdown field strength of 13.5 MV cm. The 2D transistors directly gated by the REOXs layer exhibit enhanced electron mobility and a low interface trap density. An ultrahigh on/off current ratio of 10 and a near-Boltzmann-limit subthreshold swing is achieved. The superior dielectric properties, combined with the universality and scalability of the production method (e.g., millimeter-scale films are achieved), demonstrate that 2D REOXs can serve as promising gate dielectrics for 2D electronics, thereby expanding the study of high-κ vdW materials and potentially providing new opportunities for the development of low-power electronic devices.

Reducing excess electrolytes offers a promising approach to improve the specific energy of electrochemical energy storage devices. However, using lean electrolytes presents a significant challenge for porous electrode materials due to heterogeneous wetting. The spontaneous wetting of nano- or meso-pores within particles, though seldom discussed, adversely affects wetting under lean electrolyte conditions. Herein, this undesired wetting behavior is mitigated by enlarging the pore-throat ratio, enabling Li-rich layered oxide to function effectively at very low electrolyte/capacity (E/C) ratio of 1.4 g Ah. The resulting pouch cell achieves 606 Wh kg and retains 80% capacity (75% energy) after 70 cycles. Through imaging techniques and molecular dynamics simulations, it is demonstrated that the pore-throat ratio effectively determines the permeability of electrolyte within particles. By elucidating pore-relating mechanisms, this work unveils promising potential of manipulating pore structures in porous electrode materials, an approach that can be applied to improve the specific energy of other devices including semi-solid-state lithium batteries.

Polymer-brush-grafted nanoparticles (PGNPs) that can be covalently crosslinked post-processing enable the fabrication of mechanically robust and chemically stable polymer nanocomposites with high inorganic filler content. Modifying PGNP brushes to append UV-activated crosslinkers along the polymer chains would permit a modular crosslinking strategy applicable to a diverse range of nanocomposite compositions. Further, light-activated crosslinking reactions enable spatial control of crosslink density to program intentionally inhomogeneous mechanical responses. Here, a method of synthesizing composites using UV-crosslinkable brush-coated nanoparticles (referred to as UV-XNPs) is introduced that can be applied to various monomer compositions by incorporating photoinitiators into the polymer brushes. UV crosslinking of processed UV-XNP structures can increase their tensile modulus up to 15-fold without any noticeable alteration to their appearance or shape. By using photomasks to alter UV intensity across a sample, intentionally designed inhomogeneities in crosslink density result in predetermined anisotropic shape changes under strain. This unique capability of UV-XNP materials is applied to stiffness-patterned flexible electronic substrates that prevent the delamination of rigid components under deformation. The potential of UV-XNPs as functional, soft device components is further demonstrated by wearable devices that can be modified post-fabrication to customize their performance, permitting the ability to add functionality to existing device architectures.

Advanced carbon materials are widely utilized in wearable electronics. Nevertheless, the production of carbon materials from fossil-based sources raised concerns regarding their non-renewability, high energy consumption, and the consequent greenhouse gas emissions. Biopolymers, readily available in nature, offer a promising and eco-friendly alternative as a carbon source, enabling the sustainable production of carbon materials for wearable electronics. This review aims to discuss the carbonization mechanisms, carbonization techniques, and processes, as well as the diverse applications of biopolymer-derived carbon materials (BioCMs) in wearable electronics. First, the characteristics of four representative biopolymers, including cellulose, lignin, chitin, and silk fibroin, and their carbonization processes are discussed. Then, typical carbonization techniques, including pyrolysis carbonization, laser-induced carbonization, Joule heating carbonization, hydrothermal transformation, and salt encapsulation carbonization are discussed. The influence of the processes on the morphology and properties of the resultant BioCMs are summarized. Subsequently, applications of BioCMs in wearable devices, including physical sensors, chemical sensors, energy devices, and display devices are discussed. Finally, the challenges currently facing the field and the future opportunities are discussed.

Innovating nanocatalysts with both high intrinsic catalytic activity and high selectivity is crucial for multi-electron reactions, however, their low mass/electron transport at industrial-level currents is often overlooked, which usually leads to low comprehensive performance at the device level. Herein, a Cl/O etching-assisted self-assembly strategy is reported for synthesizing a self-assembled gap-rich PdMn nanofibers with high mass/electron transport highway for greatly enhancing the electrocatalytic reforming of waste plastics at industrial-level currents. The self-assembled PdMn nanofiber shows excellent catalytic activity in upcycling waste plastics into glycolic acid, with a high current density of 223 mA cm@0.75 V (vs RHE), high selectivity (95.6%), and Faraday efficiency (94.3%) to glycolic acid in a flow electrolyzer. Density functional theory calculation, X-ray absorption spectroscopy combined with in situ electrochemical Fourier transform infrared spectroscopy reveals that the introduction of highly oxophilic Mn induces a downshift of the d-band center of Pd, which optimizes the adsorption energy of the reaction intermediates on PdMn surface, thereby facilitating the desorption of glycolic acid as a high-value product. Computational fluid dynamics simulations confirm that the gap-rich nanofiber structure is conducive for mass transfer to deliver an industrial-level current.

Breaking the thermal, mechanical and lightweight performance limit of aerogels has pivotal significance on thermal protection, new energy utilization, high-temperature catalysis, structural engineering, and physics, but is severely limited by the serious discrete characteristics between grain boundary and nano-units interfaces. Herein, a thermodynamically driven surface reaction and confined crystallization process is reported to synthesize a centimeter-scale supercontinuous ZrO nanolayer on ZrO-SiO fiber aerogel surface, which significantly improved its thermal and mechanical properties with density almost unchanged (≈26 mg cm). Systematic structure analysis confirms that the supercontinuous layer achieves a close connection between grains and fibers through Zr─O─Si bonds. The as-prepared aerogel exhibits record-breaking specific strength (≈84615 N m kg, can support up to ≈227 272 times aerogel mass) and dynamic impact resistance (withstanding impacts up to 500 times aerogel mass and up to 200 cycling stability at 80% strain). Besides, its temperature resistance has also been greatly optimized (400 °C enhancement, stability at 1500 °C). This work will provide a new perspective for exploring the limits of lightweight, high strength, and thermal properties of solid materials.

A strong n-type perovskite layer is crucial in achieving high open-circuit voltage (V) and power conversion efficiency (PCE) in the p-i-n solar cells, as the weak n-type perovskites result in a loss of V, and the p-type perovskites contain numerous electron traps that cause the severe carrier recombination. Here, three types of perylene diimide (PDI) based small molecule dopants with different dimensions, including 1D-PDI, 2D-PDI, and 3D-PDI are designed, to produce heavier n-type perovskites. The PDI-based molecules with Selenium atoms have a strong electron-donating ability, effectively enlarging the quasi-Fermi level splitting within the perovskites. Besides, the PDI molecules can coat the surface of the perovskite crystal to form the lattice cage through their conjugate skeletons, which passivates the trap states and improves the n-doping efficiency, as well as the stabilities of perovskites and related devices. With the addition of the 2D-PDI, the small-area solar cells achieved a PCE of 26.06% (25.44% certified) with a high V of 1.18 V and a remarkable fill factor of 87.23%. Furthermore, the rigid and flexible perovskite solar modules yielded high PCEs of 21.48% and 20.71%, respectively. This dimensional regulation strategy provides useful guidance for effective n-type doping and high-performance p-i-n solar cells.

Developing highly efficient catalysts to accelerate sluggish electrode reactions is critical for the deployment of sustainable aqueous electrochemical technologies, yet remains a great challenge. Rationally integrating functional components to tailor surface adsorption behaviors and adsorbate dynamics would divert reaction pathways and alleviate energy barriers, eliminating conventional thermodynamic constraints and ultimately optimizing energy flow within electrochemical systems. This approach has, therefore, garnered significant interest, presenting substantial potential for developing highly efficient catalysts that simultaneously enhance activity, selectivity, and stability. The immense promise and rapid evolution of this design strategy, however, do not overshadow the substantial challenges and ambiguities that persist, impeding the realization of significant breakthroughs in electrocatalyst development. This review explores the latest insights into the principles guiding the design of catalytic surfaces that enable favorable adsorbate dynamics within the contexts of hydrogen and oxygen electrochemistry. Innovative approaches for tailoring adsorbate-surface interactions are discussed, delving into underlying principles that govern these dynamics. Additionally, perspectives on the prevailing challenges are presented and future research directions are proposed. By evaluating the core principles and identifying critical research gaps, this review seeks to inspire rational electrocatalyst design, the discovery of novel reaction mechanisms and concepts, and ultimately, advance the large-scale implementation of electroconversion technologies.

The exchange bias (EB) effect is a fundamental magnetic phenomenon, in which the exchange bias field/coercive field ratio (|H/H|) can improve the stability of spintronic devices. Two-dimensional (2D) magnetic heterostructures have the potential to construct low-power and high-density spintronic devices, while their typically air unstable and |H/H| lesser, limiting the possibility of applications. Here, 2D CrTe nanosheets have been systematically synthesized with an in situ formed ≈2 nm-thick Te doped CrO layer (Te-CrO) on the upper surface by chemical vapor deposition (CVD) method. The strong and air stable EB effect, achieving a |H/H| of up to 80% under an ultralow cooling field of 0.01 T, which is greater than that of the reported 2D magnetic heterostructures. Meanwhile, the uniformity of thickness and chemical composition of the Te-CrO layer can be controlled by the growth conditions which are highly correlated with the EB effect of 2D Te-CrO/CrTe heterostructures. First-principles calculations show that the Te-CrO can provide uncompensated spins in the CrO, thus forming strong spin pinning effect. The systematical investigation of the EB effect in 2D Te-CrO/CrTe heterostructures with high |H/H| will open up exciting opportunities in low-power and high-stability 2D spintronic devices.

Traditional energy-integration X-ray imaging systems rely on total X-ray intensity for image contrast, ignoring energy-specific information. Recently developed multilayer stacked scintillators have enabled multispectral, large-area flat-panel X-ray imaging (FPXI), enhancing material discrimination capabilities. However, increased layering can lead to mutual excitation, which may affect the accurate discrimination of X-ray energy. This issue is tackled by proposing a novel design strategy utilizing rare earth ions doped quantum-cutting scintillators as the top layer. These scintillators create new luminescence centers via energy transfer, resulting in a significantly larger absorption-emission shift, as well as the potential to double the photoluminescence quantum yield (PLQY) and enhance light output. To verify this concept, a three-layer stacked scintillator detector is developed using ytterbium ions (Yb)-doped CsPbCl perovskite nanocrystals (PeNCs) as the top layer, which offers a high PLQY of over 100% and a significant absorption-emission shift of 570 nm. This configuration, CsAgCl and CsCuI as the middle and bottom layers, respectively, ensures non-overlapping optical absorption and radioluminescence (RL) emission spectra. By calculating the optimal thickness for each layer to absorb specific X-ray energies, the detector demonstrates distinct absorption differences across various energy bands, enhancing the identification of materials with similar densities.

Electrochemical oxidation of small molecules shows great promise to substitute oxygen evolution reaction (OER) or hydrogen oxidation reaction (HOR) to enhance reaction kinetics and reduce energy consumption, as well as produce high-valued chemicals or serve as fuels. For these oxidation reactions, high-valence metal sites generated at oxidative potentials are typically considered as active sites to trigger the oxidation process of small molecules. Isolated atom site catalysts (IASCs) have been developed as an ideal system to precisely regulate the oxidation state and coordination environment of single-metal centers, and thus optimize their catalytic property. The isolated metal sites in IASCs inherently possess a positive oxidation state, and can be more readily produce homogeneous high-valence active sites under oxidative potentials than their nanoparticle counterparts. Meanwhile, IASCs merely possess the isolated metal centers but lack ensemble metal sites, which can alter the adsorption configurations of small molecules as compared with nanoparticle counterparts, and thus induce various reaction pathways and mechanisms to change product selectivity. More importantly, the construction of isolated metal centers is discovered to limit metal d-electron back donation to CO 2p orbital and reduce the overly strong adsorption of CO on ensemble metal sites, which resolve the CO poisoning problems in most small molecules electro-oxidation reactions and thus improve catalytic stability. Based on these advantages of IASCs in the fields of electrochemical oxidation of small molecules, this review summarizes recent developments and advancements in IASCs in small molecules electro-oxidation reactions, focusing on anodic HOR in fuel cells and OER in electrolytic cells as well as their alternative reactions, such as formic acid/methanol/ethanol/glycerol/urea/5-hydroxymethylfurfural (HMF) oxidation reactions as key reactions. The catalytic merits of different oxidation reactions and the decoding of structure-activity relationships are specifically discussed to guide the precise design and structural regulation of IASCs from the perspective of a comprehensive reaction mechanism. Finally, future prospects and challenges are put forward, aiming to motivate more application possibilities for diverse functional IASCs.

Assembling natural proteins into large, strong, bone-mimetic scaffolds for repairing bone defects in large-animal load-bearing sites remain elusive. Here this challenge is tackled by assembling pure silk fibroin (SF) into 3D scaffolds with cortical-bone-like lamellae, superior strength, and biodegradability through freeze-casting. The unique lamellae promote the attachment, migration, and proliferation of tissue-regenerative cells (e.g., mesenchymal stem cells [MSCs] and human umbilical vein endothelial cells) around them, and are capable of developing in vitro into cortical-bone organoids with a high number of MSC-derived osteoblasts. High-SF-content lamellar scaffolds, regardless of MSC inoculation, regenerated more bone than non-lamellar or low-SF-content lamellar scaffolds. They accelerated neovascularization by transforming macrophages from M1 to M2 phenotype, promoting bone regeneration to repair large segmental bone defects (LSBD) in minipigs within three months, even without growth factor supplements. The bone regeneration can be further enhanced by controlling the orientation of the lamella to be parallel to the long axis of bone during implantation. This work demonstrates the power of oriented lamellar bone-like protein scaffolds in repairing LSBD in large animal models.

2D Dion-Jacobson (DJ) chiral perovskite materials exhibit significant promise for developing high-performance circularly polarized light (CPL) photodetectors. However, the inherently thick nature of DJ-phase 2D perovskite single crystal limits their ability to differentiate CPL photons with the two opposite polarization states. In addition, the growth of DJ-phase perovskite single crystal thin films (SCTFs) has proven challenging due to the strong interlayer electronic coupling. Here, a nucleation-controlled strategy is employed to grow a novel DJ-phase perovskite [(R/S)-3APr]PbI [(R/S)-3APr = (R/S)-3-Aminopyrrolidine] SCTFs with large area, low thickness and hence high aspect ratios. Structural and photoluminescence analyses reveal that introducing the divalent organic cations into the perovskite framework reduce the interlayer distance, resulting in low exciton binding energy. This facilitates charge separation and transport. The resulting SCTF photodetector showcases excellent detection performance with anisotropy factor for photocurrent as high as 0.65, responsivity of 1.97 A W, detectivity of 5.3 × 10 Jones, and 3-dB frequency of 2940 Hz, demonstrating its potential as a promising candidate for CPL-sensitive photodetectors. This novel approach, therefore, provides a framework for the growth of DJ-phase perovskite SCTFs and advances their applications in sensitive CPL photodetection.

Flexible metal-organic frameworks (MOFs) offer unique opportunities due to their dynamic structural adaptability. This review explores the impact of flexibility on gas adsorption, highlighting key concepts for gas storage and separation. Specific examples demonstrate the principal effectiveness of flexible frameworks in enhancing gas uptake and working capacity. Additionally, mixed gas adsorption and separation of mixtures are reviewed, showcasing their potential in selective gas separation. The review also discusses the critical role of the single gas isotherms analysis and adsorption conditions in designing separation experiments. Advanced combined characterization techniques are crucial for understanding the behavior of flexible MOFs, including monitoring of phase transitions, framework-guest and guest-guest interactions. Key challenges in the practical application of flexible adsorbents are addressed, such as the kinetics of switching, volume change, and potential crystal damage during phase transitions. Furthermore, the effects of additives and shaping on flexibility and the "slipping off effect" are discussed. Finally, the benefits of phase transitions beyond improved working capacity and selectivity are outlined, with a particular focus on the advantages of intrinsic thermal management. This review highlights the potential and challenges of using flexible MOFs in gas storage and separation technologies, offering insights for future research and application.