Protective buffer layers are a key strategy to facilitate the sputter deposition of transparent front electrodes in semi-transparent perovskite and highly efficient perovskite tandem solar cells. Here, we explore a thin aluminium oxide (AlOx) layer, deposited through atomic layer deposition (ALD), as a buffer layer between the established C60 electron transport layer and sputtered indium tin oxide (ITO) contact in a “p-i-n” (inverted) device architecture. By using multimodal spectroscopic methods, we compare AlOx to the more widely employed SnOx. Although ALD is known as a conformal process, we find that the growth of SnOx (<20 nm) on the C60 layer frequently results in pinholes, whereas ∼ 3–5 nm-thin layers of AlOx allow for a more homogeneous coverage. The presence of in-gap states revealed in the wide-bandgap alumina buffer layer enables efficient charge extraction. Under low-power magnetron sputtering conditions, a 3 nm AlOx buffer layer effectively suppresses sputtering-induced damage, whereas a 1.5 nm AlOx layer does not. Devices with 3 nm AlOx perform similarly to those with 20 nm SnOx, with power conversion efficiencies exceeding 17% for semi-transparent perovskite and 26% for perovskite/silicon tandem devices. Thus, we conclude the suitability of thin AlOx as a sputter-resistant buffer layer offering the advantage of a dense and uniform ALD process, reduced material consumption, and a faster fabrication process for future perovskite tandem and semi-transparent devices.
Wearable ultrasound has emerged as a promising modality for continuous, non-invasive monitoring of deep-tissue physiology, overcoming the limited penetration depth of conventional optical and electrical wearable sensors. However, moving ultrasound from rigid clinical probes to soft, body-conformal wearable systems introduces new challenges. Mechanical deformation, motion, and variable acoustic coupling alter ultrasound signal characteristics over time, while large volumes of high-dimensional data, limited labeled datasets, and constraints on power and computation place additional demands on signal processing and neural network design. This review provides a system-level and problem-oriented overview of wearable ultrasound devices, with a central focus on algorithmic and neural network design. We first analyze how flexible materials, transducer parameters, and structural layouts reshape ultrasound signal statistics under deformation and long-term wear. We then review signal processing, machine learning, and deep learning approaches developed to stabilize waveform tracking, compensate motion- and geometry-induced variability, and enable robust parameter estimation under limited power and data constraints. Building on these algorithmic foundations, we summarize emerging applications in hemodynamics, tissue mechanics, neuromodulation, drug delivery, and multimodal sensing, highlighting how application demands drive device innovation, while altered sensing conditions necessitate new wearable-oriented algorithmic frameworks. By linking physical sensing, adaptive algorithms, and clinical use cases, this review outlines a closed-loop co-design pathway from materials and structures to intelligent inference, aiming to guide development of wearable ultrasound systems for long-term, real-world health monitoring.
Accurate multidimensional radiation dosimetry is crucial for guaranteeing irradiation effects and minimizing negative effects across various fields, while it remains a critical bottleneck for existing dosimetry methods. Here, an approach of using the irradiation dose-dependent photoreduction behavior of Eu3+ to Eu2+ in NaCa1-xEuxPO4 phosphor was presented for two-dimensional radiation dosimetry. Systematic spectroscopy characterization reveals that the photoredox behavior of Eu3+↔Eu2+ can be reasonably interpreted using the local electron transfer model. Upon irradiation, the dose information is encoded into the photoluminescence intensities of Eu in its different valence states, leading to a dose-dependent luminescence color change from red to green. This characteristic enables the determination of spatial dose distribution through the ratio of green to red pixel intensities from the captured digital photographs, eliminating the cumbersome process of point-by-point reading required by traditional luminescence dosimeters. As a proof of concept, NaCa0.999Eu0.001PO4 is utilized for two-dimensional radiation dosimetry. The spatial dose distribution information can be readily obtained by taking photos upon UV illumination and the dose information can be well maintained for over 36 h. This work not only offers an approach for two-dimensional radiation dosimetry but also provides deeper insights into the mechanism underlying photo-induced electron transfer processes in phosphors.
Biological materials achieve exceptional combinations of strength, toughness, and impact resistance by controlling how loads are transmitted, redistributed, and dissipated across hierarchical structures, rather than by relying solely on intrinsic properties of their constituents. Here, we propose that shear is the central organizing variable governing mechanical resilience in these systems. Across diverse biological architectures, localized loading is systematically converted into distributed shear deformation, which is then coupled to multiple dissipation mechanisms, including interfacial sliding, viscoelastic flow, plastic deformation, and sequential bond rupture. We organize these strategies within a unified mechanics framework comprising three fundamental processes: shear generation through geometry, heterogeneity, and architecture; shear distribution across extended volumes via hierarchical load transfer; and shear–dissipation coupling at multiple length scales. This perspective connects previously disparate mechanisms from graded interfaces and sutured geometries at the macroscale, to Bouligand and staggered architectures at the microscale, and coordinated deformation and molecular reconfiguration at the nanoscale. We further show how cross-scale integration enables continuous shear transfer and dissipation, leading to mechanical performance unattainable by individual mechanisms alone. Drawing on these insights, we distill general design principles for engineering materials that mitigate classical strength–toughness trade-offs by programming shear pathways and their associated dissipative mechanisms. Finally, we outline emerging directions, including dynamic control of shear, wave–structure interactions, and adaptive materials, which point toward a new paradigm of mechanics-driven material design.
Polymers with high temperature resistance and high energy density are the optimal dielectric materials for film capacitors in power and electrical applications. However, the key properties of polymer dielectric materials, such as electric polarization and dielectric loss, as well as insulation properties and thermal stability, are mutually contradictory. Combined with the requirements for reliability and long service lifetime, these create great challenges for the intrinsic molecular design of polymer dielectric materials. This review provides an overview of a systematic approach to improve the energy storage performance of high-temperature polymer dielectric materials based on a molecular-scale perspective. Focus on molecular engineering design strategies for enhancing electrical polarization and breakdown resistance is presented. The unique breakdown self-healing behavior of the polymer dielectric materials is thoroughly investigated for the first time. Furthermore, computer-aided computational methods for prospective prediction are presented, allowing for targeted design and development of polymer dielectric materials. Based on a systematic summary of intrinsic polymer dielectric materials for high-temperature energy storage, this review highlights the challenges and future research directions for film capacitors to improve the performance and industrialization of dielectric materials.
Asymmetrically coordinated metal−organic frameworks (MOFs) have emerged as promising pre-catalysts for ethanol oxidation reaction (EOR). However, the dynamic reconstruction of MOFs during electrocatalysis has hindered the acquisition of clear evidence for understanding the regulatory role of ligands in intrinsic activity. Herein, by modelling the sulfur-doped asymmetrically coordinated (Ni−O/Ni−S) MOF (S-Ni-BDC), we established a clear picture of the dynamic reconfiguration of the metal center and sulfur-containing ligands during the EOR process. In-situ spectroscopy characterizations revealed that S-Ni-BDC was rapidly converted into metal oxyhydroxide (NiOOH) containing sulfate anions (SO42−) during the catalytic process. This kind of ligand reconstruction markedly increases the intrinsic EOR activity by strengthening the adsorption of ethanol and reaction intermediates at the Ni centers. Compared with the symmetrically coordinated (Ni−O) MOF (denoted as Ni-BDC), S-Ni-BDC/NF exhibited superior EOR activity, enabling a complete conversion of ethanol to acetic acid. Our work elucidates the intrinsic relationship between ligand structural evolution and catalytic performance, providing a new strategy to boost EOR activity via controlled ligand reconstruction.
Lipid nanoparticles (LNPs) have emerged as the most widely used and clinically validated platform for delivering RNAs, including small interfering RNA (siRNA) and messenger RNA (mRNA), as exemplified by the FDA approvals of Onpattro, Comirnaty, Spikevax, and mRESVIA. LNPs offer various benefits for RNA delivery, such as protecting RNA from enzymatic degradation, increasing cellular uptake and endosomal escape, and improving pharmacokinetics. To further broaden their use across a wide spectrum of diseases, various LNPs have recently been developed with unique biological functions, such as immunomodulation, tissue microenvironmental modulation, endosomal pathway interference, pharmacological activity, and tissue and cell selectivity, giving rise to the emerging concept of bioactive lipid-derived nanoparticles (bioactive LNPs). In this review, we summarize bioactive LNPs incorporating naturally sourced bioactive lipids, bioactive agent-derived lipids, or novel bioactive lipids identified through combinatorial synthesis coupled with high-throughput screening. We also discuss the structure-activity relationship of these bioactive lipids and overview their corresponding LNPs for specific biomedical applications. We further provide perspectives on the challenges and opportunities in translating bioactive lipid-derived LNPs into next-generation RNA nanomedicines.
The transition to sustainable and intelligent construction materials has accelerated the development of Living Building Materials (LBMs), which integrate biological components into synthetic materials for multifunctional performance. Here, we introduce a 3D-printable bacteria-loaded hydrogel composite that not only grows into mechanically reinforced structures via in-situ microbial biomineralization, but also offers low-carbon fabrication, self-strengthening potential, and advanced 3D printability. The dual-network matrix of alginate and gelatin methacrylate (GelMA) is reinforced with laponite nanoclay and glass sand to improve printability, maintain shape fidelity, and improve early mechanical properties. During curing, Sporosarcina pasteurii (S. pasteurii) embedded in the hydrogel germinates and proliferates, inducing uniform calcium carbonate precipitation throughout the matrix. After 14 days of microbial reaction, the resulting bio-composite achieves a compressive strength of 6.9 MPa and a compressive modulus of 855.1 MPa. Moreover, the embedded printing strategy enables the creation of complex, overhanging, and interlaced geometries that would be unattainable by extrusion alone, opening new design possibilities for functional LBMs. To conclude, this platform merges biological self-assembly with advanced manufacturing, offering self-strengthening, low-carbon materials for applications ranging from heritage conservation to artificial reefs and sustainable construction in resource-limited environments.
The functional magnetic properties of nanostructured materials can be distinctly different from their bulk counterparts. Understanding these properties is crucial for basic material science and for applications using nanostructured magnetic materials. However, determining intrinsic magnetic structures, exchange constants and local magnetic anisotropy in nanoparticles poses considerable challenges. Here, polarised neutron powder diffraction (PNPD) data, analysed in the frame of the Local Susceptibility and Model Hamiltonian approaches, is used to gain information on the contribution of the different magnetic sublattices on the magnetisation process in Mn3O4 nanoparticles in unprecedented detail. The magnetic order is found to be a Yafet-Kittel-type canted structure with inter- and intra-sublattice antiferromagnetic couplings, similar to bulk. PNPD corroborates that the c-axis is the hard-axis and the individual contributions of each magnetic site to the easy-plane magnetic anisotropy are determined. Remarkably, the analysis of the PNPD data provides the foremost determination of the microscopic magnetic parameters in nanoparticles, namely, intra- and inter- sub-lattice exchange constants and the local anisotropy parameter. The obtained values are consistent with bulk Mn3O4 experimental and theoretical results. These results open the path for the use of PNPD to gain unique magnetic information in nanostructured materials, particularly in complex, novel, or poorly understood systems.
Sustainable recovery of critical resources demands catalytic platforms that are efficient, scalable, and low-energy. Contact-electro-catalysis (CEC) provides a promising route, yet conventional powder catalysts suffer from poor dispersion and limited recyclability. Here we introduce a prestressing strategy that regulates molecular ordering and interface charge states, yielding prestressed polytetrafluoroethylene (Ps-PTFE) films. Prestressing aligns dipoles, establishes a built-in electric field, and lowers the barrier for interface charge transfer under ultrasound-assisted, thereby amplifying reactive oxygen species generation. Relative to PTFE powders, Ps-PTFE films boost hydroxyl and superoxide radical production by 243.44 % and 152.29 %, respectively, delivering a 9.6-fold enhancement in catalytic efficiency. This enables highly efficient silver leaching from retired photovoltaic cells, with leaching, reduction, and overall recovery efficiencies of 97.37 %, 98.51 %, and 95.94 %, a 19.93 % improvement over conventional approaches. By establishing an all-film-state CEC platform, this work advances a recyclable, low-carbon, and scalable pathway for critical metal recovery, moving towards the United Nations Sustainable Development Goals.
We report an operando, lithium-sensitive investigation of through-thickness lithium redistribution and catholyte degradation in practical-loading Si|Li6PS5Cl (LPSCl)| NMC811 all-solid-state batteries, in which the high voltage NMC811 composite cathode delivers more than 6 mAh cm−2. Unlike recent studies that primarily revealed monotonic lithiation gradients in thick solid-state cathodes, our practical Si-based full-cell configuration exhibits a qualitatively different cathode reaction topology. Neutron radiography shows that the cathode does not react through a simple face-to-face Li-ion gradient. Instead, a persistent interior reaction zone emerges about 37.5–75 µm from the LPSCl interface and exhibits the largest attenuation change throughout the first cycle. During charge, this region becomes the dominant lithium-deficient band within the thick cathode; during discharge, it remains the preferential relithiation pathway. Raising the current density from 0.5 to 1.0 mA cm−2 suppresses utilization of this interior zone and produces a pronounced Li-depleted region at the NMC811|LPSCl interface, indicating a rate-driven transition from interior-dominated utilization to interfacial Li starvation. By combining operando neutron radiography, post-cycling neutron tomography, and cross-sectional Raman mapping, we further show that thiophosphate decomposition localizes preferentially in the same mid-cathode region. These results identify an interior transport–degradation hotspot in thick high-voltage sulfide ASSB cathodes, where localized redox activity accelerates catholyte breakdown, amplifies residual heterogeneity, and increases energy loss. The work shifts the design target for practical high-loading ASSBs from interface engineering alone toward controlling interior cathode utilization and suppressing mid-thickness reaction localization.
Glucose oxidase (GOx)-based enzyme dynamic therapy (EDT) has emerged as a promising anticancer strategy, yet its therapeutic efficacy remains constrained by suboptimal enzyme conformation. Although framework materials have recently been developed to adjust enzyme conformation, GOx conformational optimization remains challenging due to complex subunits. Here, supramolecular chiral nanocarriers successfully immobilize GOx and realize overall conformational optimization of GOx via enhanced stereoselective binding, efficiently improving GOx catalytic activity as well as tumor therapeutic efficiency. Chirality-mediated binding affinity between L-type nanocarriers (LPH) and GOx drives a loose conformation in GOx, facilitating the exposure of enzymatic active sites from the hydrophobic pocket. This optimized configuration enhances active site accessibility, yielding 35% greater enzymatic activity than free GOx. Integration of horseradish peroxidase (HRP) with LPH@GOx nanocarrier (LPH@GH) remarkably promotes production of ·OH and oxidative therapeutic effect. With these cascade reactions, LPH@GH exhibits starvation-oxidative bimodal therapeutic effect, leading to in vivo tumor necrosis (1.6 fold tumor growth inhibition compared with free enzymes). This chiral nanocarrier not only efficiently improves the GOx-based anticancer therapy effects but also presents autofluorescence, allowing real-time tumor detection for integrated tumor diagnosis and therapy.
Conventional ring-opening polymerization (ROP) of lipoic acid (LA) requires photo/thermal assistance, organic solvents, and catalysts, hindering its utility in benign environments, especially in vivo. Herein, we present a new paradigm for room-temperature ROP of LA via a polymerizable deep eutectic solvent (DES)-induced polymerization strategy, achieved by simply blending LA with sodium fatty acids (RONa). This process is driven by synergistic ionic hydrogen-bonding and van der Waals interactions, which disrupts the native crystalline structures of LA and RONa, enabling spontaneous melting and polymerization at ambient conditions while lowering the ring-opening energy barrier of LA by 3.5-fold, without initiators, catalysts, solvents, or external energy. Modulating RONa chain length tailors PolyLA adhesion from 33 kPa to 2 MPa with cryogenic/wet resistance. Harnessing LA’s inherent bioactivity, the optimized PolyLA/RONa is developed tissue adhesive for tissue regeneration. This work innovatively transforms DES from an inert medium to an active platform for green PolyLA-based materials.
Additively manufactured superelastic components that operate across wide temperature ranges are attractive for aerospace, robotics, and reusable energy-absorbing systems. However, achieving sub-room-temperature tensile superelasticity while retaining reliable additive manufacturing processability remains challenging. Here, we address this challenge by decorating pre-alloyed Cu–Al–Mn powder with 2 at.% Ni. During laser powder bed fusion, this feedstock-level Ni addition improves laser absorption and densification, refines the solidification microstructure, and stabilizes the austenite by lowering the phase transformation temperature. The resulting alloy delivers bulk tensile superelasticity from −70 °C to 50 °C, together with a tensile strength of ∼1.3 GPa, an elongation of 9%, and a recoverable strain of ∼4%. This wide-temperature superelasticity is further retained in architected structures, enabling reusable energy absorption and adaptive load bearing across the same thermal window. These findings establish a potentially lower-cost feedstock route to additively manufactured superelastic metamaterials with a wide operating-temperature range for shape-adaptive and reusable load-bearing applications.
Sulfur, based on the positive-valence conversion, is promising for constructing high-voltage and high-energy zinc batteries (ZBs) due to its multi-electron transfer process. However, the redox conversion of multivalent S in ZBs is still limited and suffers from low active materials utilization and large charge/discharge polarization with poor reversibility. This study presents significant progress, for the first time, on the catalytic S0/S4+ redox behavior based on the interchalcogen effect in ZBs using single-atom selenium (SA-Se), which greatly facilitates electronic conductivity and improves ion diffusion behavior. Notably, up to 1.52 V and 1.37 V discharge plateaus with an impressive discharge capacity up to 587 mAh g−1 is achieved in Zn‖S batteries. Furthermore, benefiting from the enhanced absorption of soluble products based on the interchalcogen effect, the high-voltage Zn‖S battery exhibits remarkable conversion dynamics, excellent cycling performance, high energy density, and superior areal capacity. This catalytic strategy of positive-valence conversion of sulfur based on the interchalcogen effect represents a significant advancement in constructing future high-voltage sulfur-based batteries.
While gel polymer electrolytes (GPEs) are safer and more flexible than liquid electrolytes, their inherently disordered polymer networks drastically hinder ion transport and reduce ionic conductivity by two or three orders of magnitude. Thus, achieving liquid-level conductivity in GPEs continues to be a challenge in advancing ionic and energy devices. This study successfully constructs a high conductivity GPE of a liquid-comparable level by ordered network design with selective, efficient photoinitiated thiol–ene click chemistry. The ordered polymer networks suppress crystallization and topological defects, thereby enabling the rapid gelation (< 10 s) at ultra-low content (5 wt%), and they minimize diffusion resistance by reducing ion transport activation energy (5.8 kJ/mol) to the liquid level (6.7 kJ/mol). The optimized GPEs deliver high conductivity across nine widely used electrolytes, achieving a record-high 11.3% efficiency in quasi-solid-state dye-sensitized solar cells utilizing bulky copper complexes, and enabling ultrafast-charging lithium-metal batteries with 83% capacity retention after 1,000 cycles at 5C. This click-enabled GPE design overcomes the long-term conductivity gap between liquid and solid electrolytes, and unlocks the monomer engineering potential for scalable, multifunctional development of electrochemical energy devices.
