Physics

ABSTRACT Acidic CO 2 reduction reaction (CO 2 RR) enhances carbon efficiency and electrolyzer stability. Although nickel single‐atom catalysts (Ni‐SACs) effectively convert CO 2 into CO in neutral/alkaline conditions, their performance in acid is hindered by the competing hydrogen evolution reaction (HER). Here we show that tailoring the local strain of Ni‐SACs can enhance HER suppression across a broad potential range. Density functional theory calculations indicate that Ni‐SACs with steeper local curvature reduce *COOH adsorption by 0.23 eV while increasing *H adsorption by 0.55 eV. To validate our predictions, we leveraged carbon nanotubes (CNTs) with different diameters to impose controlled local strain on Ni‐SACs. In Ar‐saturated 0.05 M H 2 SO 4 , Ni‐SACs on 5‐nm CNTs (Ni‐CNT5) demonstrate the lowest hydronium and water reduction current density among all types of CNT support. In a flow cell with pH 1 catholyte, Ni‐CNT5 maintains >95% CO Faradaic efficiency (FE) from −1.0 to −2.4 V, in contrast to Ni‐CNT50 with ∼70% FE(H 2 ) at −2.4 V. Owing to its effective HER inhibition, Ni‐CNT5 achieves 80% single‐pass CO 2 conversion efficiency and operates stably in acidic electrolyte with negligible loss in current or selectivity. Our findings expand the toolbox for SACs engineering, highlighting the critical role of local stress for controlled activity.

ABSTRACT Moisture‐driven energy generators (MEGs) offer a sustainable route for low‐grade energy harvesting, yet their integration into high‐power electronics is limited by internal Joule heating and external thermal loads. Conventional MEGs also lack integrated thermal management and waste heat recovery. Guided by Density Functional Theory and Molecular Dynamics simulations of selective sulfidation, Grotthuss proton hopping, and thermal transport, we develop a sulfidation‐carbonization strategy for a multifunctional hydrogel MEG. Gradient organosulfate groups provide proton‐transport pathways, while highly dispersed in situ carbon dots enhance heat dissipation, structural robustness, and waste heat capture. Theoretical predictions agree with experimental observations. The optimized Al‐based MEG delivers 89 µW cm −2 (0.8 V, 0.35 mA cm −2 ) and operates from −24.9°C to 90.4°C. Importantly, an inert Pt/carbon‐cloth device also retains favorable electrical performance, reaching 29.2 µW cm −2 (0.56 V, 133 µA cm −2 ) at 70% RH. The system achieves a thermal dissipation efficiency of 38.9%, reduces LED temperature by 40.3°C, and enables closed‐loop energy utilization. This work establishes a coupled energy‐harvesting and thermal‐management platform for high‐temperature electronics.

ABSTRACT Construction of a strong metal‐oxide heterointerface via perovskite in situ exsolution synchronously generates oxygen vacancies (Vö) and B‐site cation defects. However, their individual contributions are often conflated and overshadowed by the overall high performance toward CO 2 electrolysis in solid‐state electrolyzers, obscuring their specific roles in modulating perovskite properties. Here we designed a series of Sr 2 Fe 1.35 Mo 0.45 Ni 0.2 O 6−δ (SFMN) with different levels of B‐site Fe/Ni defects and Vö. Cross‐scale experimental and theoretical results revealed that increased B‐site Fe/Ni defects and Vö strengthened Fe 3d−O 2p orbital hybridization, thereby enhancing electrical conductivity, but this trend reversed beyond a certain threshold. Then, in situ topotactic exsolution was performed for SFMN to refill B‐site cation defects while maintaining Vö concentration intact. The resulting sample without B‐site cation defects exhibited a faster oxygen‐ion transport capability than conventionally exsolved SFMN with rich B‐site defects, achieving a high current density of 2.40 A cm −2 at 1.5 V and 850°C, while avoiding SrCO 3 formation. Theoretical calculations demonstrated that refilling B‐site cation defects in exsolved SFMN thermodynamically accelerated CO 2 adsorption and activation, as well as suppressed Sr segregation. This study unravels the crucial impact of B‐site defects on perovskite properties and provides insights for the future development of robust perovskite electrocatalysts.

ABSTRACT To promote industrial uptake of clean hydrogen production technologies such as polymer electrolyte membrane (PEM) water electrolyzers, advancements in catalyst layer (CL) morphology are required. We demonstrate how improved electrochemical performance can be achieved when using an ionomer free porous transport electrode (PTE) coupled with a traditional catalyst coated membrane (CCM) assembly in PEM water electrolyzers. Notably, we reveal that the superior performance achieved when utilizing a hybrid PTE and CCM assembly is due to enhanced ohmic performance caused by optimal contact with both the porous transport layer (PTL) and PEM interfaces. Using operando neutron radiography, we demonstrate that configurations utilizing a CCM resulted in more rapid water replenishment to reaction sites, indicating enhanced membrane hydration beneficial for performance. This enhanced membrane hydration coupled with improved contact area at the PEM‐catalyst layer (CL) and PTL‐CL interfaces was revealed through the reduced ohmic overpotentials of the hybrid PTE‐CCM design, which achieved the lowest ohmic overpotential of 431 mV at 2000 mA cm −2 . While the average in‐plane water distributions are generally similar between cell configurations, we reveal that utilizing a PTE configuration promotes a more homogenous water distribution near the CL‐membrane interface due to enhanced catalyst utilization.

ABSTRACT Regulating the spin state of transition metal compounds is crucial for lithium polysulfide conversion in Li–S batteries, yet challenging. Herein, a sea‐urchin‐like Co 4 N/Co 2 P composite is constructed via the in situ introduction of a second phase, where the induced interfacial strain and electronic modulation lead to the formation of high‐spin Co sites, and the composite is further applied as a modified separator. Due to the differences in crystal structure and electronic properties between Co 4 N and Co 2 P, their interfacial contact induces charge redistribution and lattice mismatch, which subsequently generate localized tensile and compressive strains, along with an asymmetric N─Co─P coordination environment, thereby modulating the local electronic structure of Co active sites. Theoretical calculation and in situ characterization confirmed that the synergistic effect of interfacial strain and electronic effects induces d‐orbital spin splitting and energy level rearrangement, increasing unpaired electrons and elevating the spin state of Co. The enhanced spin state strengthens d–p orbital hybridization with sulfur intermediates, accelerating charge transfer and optimizing adsorption behavior. Accordingly, the Co 4 N/Co 2 P‐modified separator battery delivers 1389.4 mAh g −1 at 0.2 C and retains 905.9 mAh g −1 after 100 cycles (0.35% decay per cycle). This work highlights lattice‐strain‐induced spin‐state modulation as an effective strategy for designing high‐performance electrocatalysts.

ABSTRACT Aqueous magnesium‐ion batteries (AMIBs) have emerged as promising energy storage systems owing to their intrinsic safety, high energy density, and cost‐effectiveness. However, the intercalation of high‐charge‐density Mg 2+ usually leads to irreversible structural degradation toward conventional electrodes with low practical capacity and inferior stability. To overcome the inherent lattice stress caused by Mg‐ion, we investigated a series of flexible organic molecules (FOMs), and for the first time proposed a novel ion‐adaptive strategy, achieving a high‐performance FOM with modulated molecular steric hindrance, high practical capacity, and robust stability in AMIBs. In contrast with ever‐increasing lattice stress with successive Mg‐ion intercalation in conventional electrode, the subsequent ion intercalation reduced the stress by facilitated ion‐storage in the optimized ion‐adaptive FOM, such as tribenzoquinoxaline‐5,10‐dione (3BQ), with ultimately improved practical capacity (332.1 mAh g −1 at 1.0 A g −1 ), ranking among the highest capacity in AMIBs to date. Furthermore, the expanded planar architecture confers enhanced cycling stability on the ion‐adaptive 3BQ, maintaining a high specific capacity of 196.7 mAh g −1 even after 7,000 cycles at 10.0 A g −1 . The novel ion‐adaptive strategy provides a new pathway to design high‐capacity electrode materials in AMIBs and other multivalent‐ion batteries.

ABSTRACT Smart windows based on all‐thin‐film electrochromic devices (ECDs) with coordinated visible (VIS) and infrared (IR) modulation offer promising solutions for energy‐efficient buildings. However, conventional single‐layer ECDs often suffer from limited IR modulation, sluggish kinetics, poor durability, and restricted spectral control. Here, we develop a separated‐function electrochromic device (SF‐ECD) that decouples VIS and IR regulation into independent functional layers. ENZ‐ITO enables electrically driven IR modulation through carrier‐mediated localized surface plasmon resonance (LSPR), while NiO x provides VIS modulation via polaron‐based electrochromism. This architecture achieves synergistic multi‐band optical control, delivering average emissivity modulations of 0.76, 0.68, 0.75, and 0.68 across the 3–5, 8–14, 16–25, and 2.5–25 µm bands, respectively, with a maximum visible transmittance modulation of 52.1% and emissivity modulation of 0.83. The SF‐ECD exhibits rapid IR switching (<5.0 s), excellent cycling stability (>5 × 10 4 cycles), and sustained performance after 1‐year storage. Outdoor tests demonstrate a temperature reduction of 5°C–6°C under solar irradiation, highlighting its potential for advanced thermal management in intelligent buildings.

ABSTRACT Optimization of electrochemical energy storage and conversion devices often depends on the electrode microstructure properties, of which its 3D representation provides the most complete link between manufacturing process and device performance. Deep generative models can address slow experimental throughput and high computational costs of traditional microstructure resolution methods, yet most literature focuses on Generative Adversarial Networks, prone to mode collapse issues. This work applies a generative diffusion model to synthesize 3D‐resolved multiphase microstructures of lithium ion battery and proton exchange membrane fuel cell electrodes, sourced from experimental imaging and computer‐based simulations. Generated volumes are validated against training data based on microstructural descriptors, including volume fraction, specific surface area, and tortuosity factor. Moreover, the standard cubic sub‐volume augmentation strategy used forgenerative model training fails to capture depth‐dependent features in thick and heavily processed microstructures, such as calendered electrodes. A depth‐aware augmentation pipeline is proposed to incorporate full electrode thickness into training samples, improving through‐thickness tortuosity factor accuracy in the generated electrodes. Furthermore, 3D‐resolved multiphysics simulation on the generated microstructures reproduce the performance behavior of their training counterparts with high accuracy. These results establish a diffusion model‐based framework as a viable means to generate commercially relevant electrode data, intended for computational optimization and design of next‐generation energy devices.

ABSTRACT The search for single‐ion magnetism (SIM) has been largely focused on hybrid metal–organic systems. Here, the spin‐relaxation mechanism of SIM is demonstrated in a pure inorganic transition‐metal oxide, , an Ising‐chain magnet, employing neutron diffraction and inelastic neutron scattering (INS), complemented by SpinW simulation and a machine‐learning framework. Interestingly, the SIM mechanism persists even in the presence of long‐range magnetic ordering, a phenomenon rarely observed. This pioneering investigation shows that bistability between the two quantum states is maintained at zero magnetic field, driven by a dominant Orbach spin‐relaxation mechanism with an effective energy barrier meV. This behavior arises from strong spin–phonon coupling in the presence of negative axial anisotropy ( meV) and the high‐spin () Co(II) ion. Furthermore, it is observed that magnon excitations persist up to room temperature, reflecting low‐dimensional magnetic interactions and extended magnetic correlations within the oxide lattice. The interplay between single‐ion magnetism and room‐temperature spin excitations underscores the tunability of magnetic anisotropy in oxide lattices. This work presents a new magnetic domain where anisotropy‐protected single‐ion memory coexists with room‐temperature magnons, allowing materials to combine information storage with collective spin transport.

ABSTRACT The integration of bioactive matrix components and precise spatial architectures represents a promising strategy for regenerating complex tissues like articular cartilage. While decellularized cartilage matrix (DCM) preserves essential regenerative cues, the optimal engineering fabrication strategy to translate its biochemical potential remains to be defined. In this study, we conducted a systematic technological screening by fabricating three distinct DCM‐based topological prototypes: randomized porous scaffolds (RPS) via traditional lyophilization, oriented porous scaffolds (OPS) via ice‐templating, and hierarchical porous scaffolds (HPS) via low‐temperature 3D printing. Our findings reveal that the HPS configuration, characterized by its multi‐scale hierarchical porosity, functions as a biophysical instructor that activates the FAK‐PI3K/AKT mechanotransduction axis. Unlike RPS and OPS, HPS uniquely reprograms the BMSC secretome into a robust paracrine factory, effectively balancing pathological homeostasis and shielding chondrogenesis from inflammatory degradation. This study establishes the hierarchical architecture as the superior engineering fabrication solution for DCM‐based regeneration, offering a new paradigm for instructive cartilage defect repair.

ABSTRACT High‐performance optoelectronic co‐modulated synaptic devices hold pivotal significance in advancing the practicalization of neuromorphic computing, yet challenges remain regarding their capacity to perform high‐level tasks in hardware neural networks. Herein, an optoelectronic synaptic memristor based on a kesterite heterostructure is innovatively proposed. The device enables precise regulation of carrier transport and resistive switching behaviors under dual light and electrical stimuli, achieving a high switching ratio of up to 10 4 , and allowing dynamic modulation of the switching window (2 × 10 2 ∼3 × 10 4 ) and switching voltage (0.16 ∼0.91 V) in a non‐contact manner. Furthermore, it faithfully emulates diverse bio‐synaptic functions, including excitatory postsynaptic current (EPSC), spike‐rate‐dependent plasticity (SRDP), multiparametric modulation of long‐term potentiation/depression (LTP/LTD), and brain‐like neuromorphic learning behaviors, manifesting superior bionic performance. Notably, this device supports two high‐level hardware applications: (1) a multi‐level authorized encryption computing framework relying on light/electrically induced physical unclonable functions (PUF) in memristors, suitable for secure cloud communications; (2) serving as neural network activation units for high‐performance complex pattern classification, outperforming its traditional software‐implemented counterparts. The results clarify the core potential of heterostructures in developing advanced multimodal synaptic memristors and provide a viable strategy toward next‐generation optoelectronic‐integrated neuromorphic systems.

ABSTRACT Herein, a spin‐state regulation strategy is introduced as an electronic structure modulation approach to enhance the electron occupancy of the metal d z 2 orbital and is applied for the first time to capacitive deionization. Specifically, Co‐doped Fe 3 C@Fe 3 O 4 nanocubes assembled on porous carbon are synthesized via a multi‐step calcination‐impregnation‐calcination procedure, in which the increased d z 2 orbital electron occupancy accounts for the enhanced sodium ion adsorption capacity. Cobalt doping withdraws electrons from the low‐energy d x 2 ‐y 2 orbitals of iron, which reduces electron‐pair repulsion, lowers crystal field splitting, and thus promotes orbital degeneracy and stabilizes the high‐spin state. This, in turn, populates the higher‐energy d z 2 orbital, whose electron‐rich lobe electrostatically attracts Na + , and rationally enhances sodium adsorption capacity. Consequently, the electrode delivers a NaCl adsorption capacity of 307.9 mg g −1 at 1.4 V in a 2000 mg L −1 saline solution, with a corresponding deionization rate of 51.9 mg g −1 min −1 . Notably, the prepared electrode delivers an ultrahigh energy efficiency of nearly 98% in 2000 mg L −1 NaCl solution, outperforming most state‐of‐the‐art electrodes. Overall, this work establishes a fundamental design principle by linking spin state modulation to increased d z 2 orbital occupancy and ultimately to enhanced salt adsorption capacity and energy utilization efficiency for advanced desalination materials.

ABSTRACT Selective adsorption removal of perfluoroalkyl carboxylic acids (PFCAs) in multicomponent system remains a critical challenge, as current studies largely focus on fluorinated adsorbent design or single‐component capacity enhancement, lacking systematic strategy. Here, we report three functionalized Zr‐based metal‐organic frameworks, i.e., acetic acid modified MOF‐808 (MOF‐808‐AA), trifluoroacetic acid modified MOF‐808 (MOF‐808‐TFA), and 5‐fluoroisophthalic acid doped MOF‐808‐AA (F‐MOF‐808‐AA) for targeted capture of C4‐C12 PFCAs. In single‐component system, MOF‐808‐TFA exhibits more efficient adsorption for short‐chain PFCAs (C4‐C7: 605–1141 mg g −1 ), whereas F‐MOF‐808‐AA demonstrates higher adsorption capacity for long‐chain PFCAs (C8‐C12: 1576–2062 mg g −1 ). Remarkably, in mixed‐PFCA system, the cumulative adsorption capacity far exceeds the sum of single‐component saturation capacity, demonstrating synergistic enhancement and robust anti‐competition performance. Mechanistic study reveals that long‐chain PFCA preferentially binds Zr 6 cluster via carboxylate exchange. Subsequent chain‐length‐driven displacement creates a dynamically regulated adsorption interface, and short‐chain PFCA can embed into the hydrophobic pore network through non‐coordinative fluorine–fluorine interaction. A packed bed reactor filled with granular absorbent demonstrates a super stable removal performance for C4‐C12 PFCAs in field application. This work reports a new entrainment adsorption mechanism, where pre‐adsorbed long‐chain PFCA entrains short‐chain PFCA, surpassing conventional adsorption limit and offering a highly efficient strategy for PFCA‐contaminated water remediation.

ABSTRACT Photocatalytic O 2 reduction to H 2 O 2 offers a sustainable route for green H 2 O 2 production. However, the rapid and scalable preparation of efficient organic polymer photocatalysts remains challenging. Herein, we report a sonochemical strategy for the gram‐scale synthesis of two novel benzodifuran‐based conjugated polymers, BDF‐CP1 and BDF‐CP2, in aqueous solution without the use of any additional organic solvent. This methodology allows rapid assembly of conjugated architectures within drastically curtailed reaction periods, whose optical absorption profiles and morphological characteristics are comparable to those derived from conventional solvothermal protocols. More importantly, benefiting from its donor–acceptor skeleton, triazine‐linked BDF‐CP1 displays efficient charge transfer, reduced exciton binding energy, and enhanced proton conductivity. Consequently, it delivers an exceptional photocatalytic H 2 O 2 evolution rate of 10984 µmol h − 1 g − 1 in the presence of benzyl alcohol. Experimental and theoretical investigations demonstrate that incorporated triazine moieties as electron acceptors to tailor the electronic configuration of BDF‐CP1, thereby facilitating the formation and stabilization of the vital * OOH intermediate. This work presents a scalable synthetic strategy for constructing conjugated polymer‐based semiconductors and offers new insights into the rational design of high‐performance photocatalysts toward practical solar‐driven H 2 O 2 production.

ABSTRACT Precise control over reversible intercluster conversion and chiroptical inversion in gold nanoclusters (AuNCs) is notoriously difficult. This work presents four chiral AuNCs capable of reversible intercluster transformations accompanied by dynamic circularly polarized luminescence (CPL) inversion and tunable emission colors. These nanoclusters exhibit a large luminescence dissymmetry factor ( g lum = −7.28 × 10 −3 ) and an absolute photoluminescence quantum yield (PLQY) reaching 90.95%, with their responsive chiroptical properties governed by hydrogen‐bonding interactions between solvent molecules and surface ligands. Comprehensive characterizations including single‐crystal x‐ray diffraction (SCXRD), variable‐temperature circular dichroism, time‐resolved FTIR and NMR spectroscopy confirm that O─H···O═S hydrogen bonds between dimethyl sulfoxide and ligand hydroxyl groups disturb intrinsic intra‐cluster structural equilibrium and trigger helicity inversion in crystalline cluster assemblies. Time‐resolved ESI‐MS and kinetic analysis further reveal that structural evolution originates from supramolecular rearrangement, enabling reversible interconversion between high‐ and low‐nuclearity AuNCs. Utilizing time‐dependent fluorochromism and switchable CPL signals, these chiral clusters are applicable to three‐dimensional data encryption and decryption. This study offers a universal hydrogen‐bonding modulation strategy to manipulate AuNC structural transitions and chiroptical responses, facilitating rational fabrication of chiral nanomaterials for optoelectronics and information encryption.

ABSTRACT Abnormal membrane proteins often play a crucial role in the development and progression of cancer, making them ideal targets for cancer treatment. However, traditional membrane protein inhibitor‐based therapies only benefit a small part of patients and suffer from notorious drug resistance due to their occupation‐driven pharmacology. Recently, membrane protein‐instructed peptide self‐assembly has emerged as a powerful tool in precision cancer treatment. Due to its unique merits such as high tumor targeting specificity, long‐term membrane retention, and excellent functional scalability, this strategy is expected to effectively overcome key limitations of traditional membrane protein‐targeting anticancer strategies. This review summarizes research advances in membrane protein‐instructed peptide self‐assembly for cancer therapy over the past five years. First, we introduce the design principles and representative self‐assembly strategies. Subsequently, we highlight the applications and underlying mechanisms of this approach in various cancer treatment modalities, including chemotherapy, molecular targeted therapy, phototherapy, radiotherapy, immunotherapy, and image‐guided surgery. Finally, we briefly outline current challenges and future directions in this field.

ABSTRACT The intrinsic trade‐off between optical transparency and mechanical robustness represents a fundamental challenge in glass‐ceramic materials design. Herein, we demonstrate that engineering microporous collapse pathways in FAU zeolite precursors enables the fabrication of mullite glass‐ceramics with exceptional concurrent optical and mechanical performance through low‐temperature spark plasma sintering (SPS). By implementing two orthogonal controls—precursor collapse pathway (pre‐collapse versus in situ evolution) and framework chemistry (FAU‐Y versus FAU‐X)—we systematically elucidate how these parameters govern defect evolution, crystallization kinetics, and microstructure development. The optimized samples achieve an in‐line transmittance of ∼85% at 550 nm, coupled with a Vickers hardness of ∼8.6 GPa and indentation fracture toughness of ∼1.6 MPa·m 1/2 . Our findings reveal that pre‐collapse shifts degassing and structural reorganization upstream, enabling more controllable pore evolution and significantly enhanced transparency. Furthermore, composition‐regulated nucleation‐growth behavior and aluminum partitioning dictate grain coarsening and mechanical differentiation. This work establishes a comprehensive process‐structure framework for designing transparent, mechanically robust glass‐ceramics through rational engineering of microporous collapse mechanisms under rapid, low‐temperature densification conditions.

ABSTRACT Dynamic structural evolution in catalytic processes, such as atomic reconstruction of catalysts, molecular rearrangement at solid‐liquid interfaces, and quantum‐scale fluctuations, is key to determining their intrinsic activity and selectivity. However, these non‐steady‐state processes often occur on ultrafast timescales ranging from femtoseconds to nanoseconds, far beyond the detection limits of conventional in situ characterization techniques, and have long been regarded as a “black box.” The emergence of femtosecond ultrafast characterization techniques has provided revolutionary tools to address this challenge. This review pioneers a systematic exploration of the non‐steady‐state structural evolutions in catalysis and their structure‐activity relationships with catalytic performance from an ultrafast timescale perspective under femtosecond characterization. It elaborates on the underlying principles of these cutting‐edge techniques and unparalleled capabilities in capturing structural reconstruction, interfacial evolution, and quantum fluctuations. It highlights cross‐disciplinary applications in three major categories of key catalytic reactions (electrocatalysis, photocatalysis, and thermal catalysis), as well as in advanced battery research. Finally, this review outlines the challenges and future directions in the field, aiming to deliver pioneering dynamic‐level insights and strategies for the rational design of next‐generation high‐performance energy conversion and storage systems.

ABSTRACT Zero thermal expansion (ZTE) alloys hold great promise for applications in precision instruments, yet are severely limited by intrinsic brittleness and low thermal conductivity. Herein, enabled by optimizing mixing enthalpy, we report on a dual‐phase metallic composite that shows ZTE (α l = +0.6 × 10 −6 K −1 ) over a wide temperature range of 200–320 K together with high compressive strength (922 MPa) and thermal conductivity (23.2 W·m −1 ·K −1 ). Strong negative mixing enthalpies stabilize the Fe‐based Laves phase with giant room‐temperature negative thermal expansion (NTE, α V = −48 × 10 −6 K −1 , 280–330 K) in Hf 0.875 Ta 0.075 Nb 0.05 Fe 2 (HTNF), and positive mixing enthalpy drives phase separation between Cu and HTNF. Neutron powder diffraction reveals that the NTE of the ferromagnetic HTNF originates from the magnetovolume effect driven by substantial variations in local magnetic moments. The ZTE of the composite is achieved by mutual compensation of lattice expansions between the two phases. Coexistence of hard and soft natural dual phases thus yields such high compressive strength. This work gives an effective strategy for achieving ZTE alloys together with good mechanical properties and thermal conductivity.

ABSTRACT Intracerebral hemorrhage (ICH) triggers excessive reactive oxygen species (ROS) accumulation and persistent neuroinflammation, which synergistically drive progressive neuronal damage and poor neurological functional recovery, severely restricting patient prognosis. Artificial enzymes are hailed for their robustness and economy, yet their catalytic ceiling is often set by an inability to finely sculpt the electronic landscape of active centers. Here, we present V AC ‐V SA /NC, a single‐atom nanozyme (SAN) in which vanadium (V) atomic clusters (AC) orchestrate proximal V single atoms (SA), thereby regulating the local charge distribution and igniting a potent ROS for detoxification. Density functional theory calculations revealed that electrons flowing from V AC to V SA active sites drain electron density around the V SA center, reshape the local charge distribution, and promote a rapid ROS detoxification cascade. To realize targeted blood–brain barrier (BBB) penetration for ICH treatment, we fabricated V AC ‐V SA /NC@M by coating with M1 microglial membranes. In vivo fluorescence imaging confirms that the V AC ‐V SA /NC@M efficiently crosses the BBB and precisely accumulates at hemorrhagic inflammatory lesions. In vitro and in vivo experimental results combined with single‐cell sequencing analysis demonstrate that V AC ‐V SA /NC@M effectively converts proinflammatory M1 microglia into an anti‐inflammatory M2 phenotype, terminates the self‐amplifying neuroinflammatory cascade, and inhibits progressive neuronal death.

ABSTRACT Radiative decay invariably competes with nonradiative decay during the deexcitation process of materials, organic small molecules with highly efficient solar‐thermal and electroluminescence properties simultaneously remain a great challenge. Herein, we propose a novel strategy to achieve simultaneously efficient solar‐thermal and electroluminescence systems based on one molecule by manipulating molecular motion (MM) in aggregates. The proof‐of‐concept organic‐small‐molecule t ‐GDPA‐QCN was developed, where the donor group with a relatively large steric hindrance, the planar acceptor quinoxaline‐6,7‐dicarbonitrile (QCN), was conjugated with the dendritic triphenylamine ( t ‐GDPA) through a phenyl spacer, forming an umbrella‐like donor‐acceptor (D‐A) motif. Because a loose packing mode in pure solid state facilitates MM and consequently elevates nonradiative decay, t ‐GDPA‐QCN shows a solar absorptivity of 37.56%, which leads to superior water evaporation and electricity generation performances. Furthermore, when t ‐GDPA‐QCN is doped into a host material with a suitable size, the MM is effectively restricted, resulting in low nonradiative transitions. Consequently, deep‐red organic light‐emitting diodes (OLEDs) with excellent performance were realized, achieving a maximum external quantum efficiency (EQE) of 3.2% at an emission peak of 664 nm. This work represents the first example of organic‐small‐molecules featuring efficient photothermal and electroluminescence conversion systems simultaneously.

ABSTRACT Critical‐sized bone defects remain a major clinical challenge in orthopedics and regenerative medicine. Bone organoid provided therapy potentials; however, current engineering strategies generally neglect the bioenergetic foundation and intrinsic mechano‐electrical coupling microenvironment of native bone tissue. Herein, we prepared a three‐dimensional native bone electromechanical niche‐mimicking mechano‐electrical coupling scaffold based on piezoelectric potassium sodium niobate and methacrylated gelatin. Experiments demonstrate that this scaffold establishes an enabling physiologically relevant mechanical–electrical microenvironment throughout organoid construction under dynamic mechanical stimulation, which markedly enhances osteogenic differentiation of bone marrow mesenchymal stem cells (BMSCs)and simultaneously endows the engineered organoids with robust pro‐angiogenic and pro‐lymphangiogenic paracrine functions, achieving efficient coordinated regeneration in a rat critical‐sized calvarial defect. RNA‐sequencing together with fluorescent staining proved that mechano‐electrical coupling signals activate the PIEZO1 channel to promote Ca 2+ influx into the cytoplasm and simultaneously upregulate mitochondrial calcium uniporter (MCU) expression, thereby enhancing mitochondrial Ca 2+ . The increased mitochondrial Ca 2 + enrichment promoted tricarboxylic acid cycle enzyme activities and elevated cellular ATP production, which efficiently supports the functional maturation of bone organoids. Overall, this work establishes a bioenergetic engineering construction strategy for bone organoids with enhanced vascular/lymphatic system regeneration, providing both a conceptual framework and an engineering approach for organoid functional optimization and critical‐sized bone defect regenerative treatment.