Hydrogels have been widely used in biomedical and environmental applications, yet precise control of mechanical properties (quantified by elastic modulus, G') over a broad range remains essential for expanding their functionality. While pressure treatment typically enhances hydrogel strength through pressure-induced crosslinking, we report a counterintuitive phenomenon in locust bean gum (LBG) hydrogels: High-pressure processing induces softening rather than stiffening. Under repeated compression-decompression cycles up to 1.2 GPa, LBG hydrogels undergo progressive softening, with elastic modulus decreasing to approximately 31% of the initial value. Conversely, repeated freeze-thaw cycles enhance the modulus by approximately 2.3-fold. Scanning electron microscopy reveals a structural transition from a porous network to a flocculent morphology, corresponding to substantial alterations in elastic modulus and viscoelastic behavior. Mechanistic analysis suggests that pressure-induced disruption of hydrogen bonding, water redistribution, and structural rearrangement drive these changes. These findings demonstrate that pressure modulation can serve as a complementary method to conventional freeze-thaw treatment, offering precise control over hydrogel mechanical properties across a wide range.

All-solid-state lithium batteries (ASSLBs) are promising next-generation energy storage systems due to their superior safety. While low-cost Li2ZrCl6 is a candidate halide solid electrolyte, its ionic conductivity remains modest (0.33 mS cm-1). Herein, we report a highly conductive amorphous halide solid electrolyte (1.64 mS cm-1), synthesized using high-energy Li2CO3 as a precursor to replace conventional Li2O. This approach enhances reaction efficiency and reduces cost. The resulting Li2ZrOCl4 (LZOC) structure facilitates Li+ migration, as confirmed by experimental and theoretical results. ASSLBs incorporating the LZOC electrolyte with a Li-In anode and uncoated LiCoO2 (LCO) cathode demonstrate excellent cycling stability (97% capacity retention after 200 cycles at 1 C) and high-rate capability (over 70 mAh g-1 at 2 C). This work establishes the use of low-cost Li2CO3 as a practical strategy for developing high-performance, cost-effective ASSLBs.

The development of highly efficient catalysts for the direct selective oxidation of CH4 to HCHO remains a significant challenge. In this study, a Pd0.6Ru0.6O1.8/10 wt% MgO-Al2O3 catalyst was synthesized and evaluated in a fixed-bed reactor under low-temperature and low-pressure conditions, using molecular oxygen (O2) as the sole oxidant. Research has revealed that the single Al2O3 support facilitates CH4 deep oxidation due to its surface characteristics, resulting in a HCHO selectivity of only 36.8%. The incorporation of MgO to form a composite support effectively optimized the surface properties. At an MgO loading of 10 wt%, the HCHO selectivity significantly increased to 70.1% at 300 and 0.4 MPa (with a CH4 conversion rate of 0.45%). Characterization results indicate that the introduction of MgO formed a MgAl2O4 spinel structure, potentially creating new lattice oxygen active sites. Optimization of reaction conditions revealed that while elevated temperatures enhance conversion rates, they simultaneously reduce selectivity, highlighting the trade-off between conversion and selectivity. This work demonstrates an effective strategy for achieving highly selective oxidation of CH4 to HCHO through catalyst modification.

Halide solid-state electrolytes (SSEs) have emerged as promising candidates owing to their excellent chemical oxidation stability, mechanical deformability, and good compatibility with oxide cathode materials. However, studies on the correlation between ionic conductivity and structural characteristics remain limited. Here, we introduce equivalent state halide anions bromide (Br-) into the Li3YbCl6 matrix through mechanical chemistry and heat treatment, and report the dynamic evolution of the crystal structure of Li3YbCl6-xBrx (0 <= x <= 6). The significant change in the anion sublattice framework leads to the transformation of the initial hexagonal close-packed arrangement of Li3YbCl6 (space group: Pnma) to the cubic close-packed arrangement of Li3YbCl6-xBrx (1 <= x <= 6) (space group: C2/m). Ab initio molecular dynamics (AIMD) and nudged elastic band (NEB) simulations investigate that within the highly symmetric monoclinic crystal system, the ion transport path along the c-axis changes from the octahedron-octahedron configuration to the octahedron-tetrahedron-octahedron configuration. This transformation effectively mitigates c-axis blockage caused by Li/Yb co-occupation and significantly enhances lithium-ion transport within the lattice. The results of this work highlight the complex relationship between structure and ionic transport mechanism and provide valuable insights into the ionic conduction mechanism of this class of halide electrolytes.

Deviatoric stress and microstructural imperfections are considered the main reasons for the promotion of phase transformation (PT) of metals at high pressure. However, structural heterogeneity induced by secondary phases will pose challenges for understanding the high-pressure deformation and PT of metallic composites. For instance, anomalies related to kinetic suppression were observed in the forward (alpha ->omega) and reverse (omega ->alpha) transformation of alpha-Ti confined by TiB upon nonhydrostatic pressure. Here, static/dynamic diamond anvil cells and synchrotron X-ray diffraction were utilized to panoramically resolve the dislocation evolution in plastic flow deformation and strain-induced PT of Ti-TiB microcomposite. Diffraction peak profile analysis reveals a decrease in dislocation density of confined alpha-Ti from plastic flow (1x10(16) m(-2)) to strain-induced PT (6.7x10(15) m(-2)), accompanied with the activation of similar to 60% slip systems and a varying combination of and . Long-range internal stress at Ti/TiB interface increases quasi-linearly to a maximum accounting for similar to 17% of total pressure as the nonhydrostatic pressure increases. It probably indicates the key role of heterogeneous-stress-partition in lowering local stress required for the dislocation-mediated growth of critical omega nucleus. Furthermore, analytical results demonstrate the kinetics of PT of Ti and Ti-TiB could be well unified through the Levitas's strain-induced kinetic equation, though their accumulated plastic strain differs by a factor of similar to 3. This work shed light on the role of heterogeneous phase in high-pressure deformation and PT of metals and display promising applications such as manipulation of pressure-related strength/plasticity and PT kinetics of metals via compatible second-phases.

Abstract High-voltage LiNi0.5Mn1.5O4 (LNMO) cathode is a promising option for transition to sustainable and cost-effective cobalt-free cathodes, and ceramic cathodes can substantially increase energy density by enabling higher active material loading. However, there need to better apprehend fundamental aspects about the sintering modification and degradation mechanism of LNMO ceramic based lithium-ion batteries (LIBs). Here, by modulating sintering atmosphere and temperature, we reveal the influence of densification degree and chemical environment on the conductivity of LNMO ceramics. Meticulous post-mortem analyses illustrate that unusual prolongation of the charging curves and rapid capacity fading stem from the lower electrochemical potential of Au (~4.53 V) than the ultra-high operating voltage (~4.7 V) of LNMO, leading to evident dissolution of the Au collector and interface disruptions between cathode and collector. Furthermore, Au could migrate across the cathode and separator, ultimately reach and deposit on anode surface. We also find that O2-sintered samples could restrain the initial mixed oxidation state of Mn and oxygen vacancies, which alleviates Mn dissolution, oxygen release, irreversible structural evolution of ceramic cathode, and contributes to enhanced conductivity and electrochemical performance. Our findings reveal the collector dissolution and structural degradation mechanisms of LNMO during cycling, and provide a guideline for the design and synthesis of LNMO ceramic cathodes as well as high-voltage LIBs.

Phase transformations of 1-methylpiperidine under static and dynamic compression up to 21 GPa were investigated via in-situ Raman spectroscopy in a diamond anvil cell. Static compression reveals at least three crystalline phases and an amorphous state, which are kinetically sensitive and metastable. Dynamic compression rapidly induces amorphization, and subsequent decompression leads to spontaneous crystallization through Phase III and Phase II. The high-pressure phase behavior of 1-methylpiperidine is kinetically controlled rather than purely thermodynamic, governed by structural evolution, molecular flexibility, and metastable state formation.

In point-of-care testing (POCT) scenarios, electrochemical nucleic acid (ECNA) biosensors usually face limitations in interfacial kinetics and sensitivity. Herein, we present a dual recognition sequences-containing capture probe (DRCP)-based ECNA biosensor in combination with a reverse-transcription asymmetric recombinase polymerase amplification (RT-aRPA) sample pretreatment for fast and ultrasensitive viral RNA detection. The DRCP was self-assembled on electrode surfaces and was designed to consist of two identical ssDNA segments linked by an amide bond, each featuring a recognition sequence with a toehold. The presence of dual toehold domains facilitated the acceleration of target-specific strand displacement by 2.5-fold compared to single recognition sequences-containing capture probe systems, enabling pM-level RNA quantification within 10 min. Contrasting with conventional signal enhancement modes that suffer from sluggish interfacial assembly, the disassembly-induced signal attenuation mechanism effectively minimized the interfacial steric hindrance. Coupled with RT-aRPA, the system achieved 200 copies mL(-1) sensitivity, completing the entire "processed sample-to-result" workflow in 20 min, outperforming PCR-based methods (>2 h) while eliminating bulky instrumentation, and therefore meeting POCT requirements. Furthermore, a field-deployable POCT prototype was validated with the lysed clinical throat swab samples from SARS-CoV-2 patients. This study This study might be useful for the development of advanced ECNA sensors for POCT applications, e.g., electrochemically decentralized POCT diagnosis of early virus infection.

Against the backdrop of global health awareness and personalized medicine, growing demands for health management are driving wearable devices beyond simple motion tracking toward precise, continuous monitoring of physiological indicators. In this context, electrochemical sensors, capable of continuously detecting multiple biochemical markers in sweat and interstitial fluid, have become key enablers of non-invasive or minimally invasive health monitoring. However, traditional wearable sensors often rely on screen-printing techniques, which commonly suffer from low accuracy, poor stability, and inconsistent reproducibility. Micro-electro-mechanical systems (MEMS) offer a promising alternative, leveraging high-precision microfabrication and scalable manufacturing to produce electrochemical sensors with fine structures, stable performance, and high integration. This paper focuses on MEMS-fabricated wearable electrochemical sensors and highlights three representative types: flexible polymer-based sensors adhered to the skin surface for real-time monitoring of multiple metabolites in sweat; integrated sensors combined with microfluidic channels for active collection and guidance of bodily fluids; and microneedle array sensors that penetrate the stratum corneum to directly access biological information in interstitial fluid. We also discuss core challenges including flexibility-process compatibility, 3D structure fabrication, and sensor-circuit integration. These discussions aim to provide technical insights for advancing practical applications of wearable electrochemical sensors in personalized and preventive health monitoring.

Natural small extracellular vesicles (EV) show promise for drug delivery but face two key hurdles to clinical use: low drug-loading efficiency and limited production. Here, we report an innovative lysosome interference strategy based on the pH-responsive degradation of nano-CaCO₃, which achieves a “two birds with one stone” effect. During lysosome-mediated degradation of substances, nano-CaCO₃ dissolves in the acidic lysosome, consuming H+ to raise lysosomal pH and inhibit hydrolytic enzymes. This helps exogenous plasmids escape the endolysosomal pathway, boosting transfection efficiency. Additionally, nano-CaCO₃-induced enhanced lysosome interference suppresses multivesicular body (MVB) fusion with autophagosomes/lysosomes, promoting EV biogenesis and release. In a drug pre-loading experiment, HEK 293T cells pretreated with nano-CaCO₃, when transfected with recombinant IL-10 plasmids, generated IL-10-bioengineered small extracellular vesicles (iEV), with 1.72-fold higher IL-10 expression and 6.4-fold greater EV yield than controls. Both in vitro (cellular) and in vivo (animal model) studies validate that these iEV, delivered via nebulization inhalation, elicit potent anti-inflammatory effects in treating acute lung injury (ALI). This green, non-toxic, and efficient nano-CaCO₃ lysosome interference strategy dual-benefits drug loading and EV yield, offering a novel solution to advance EV-based therapeutics clinically.

The driving force for high-pressure crystallization of polymers is undercooling. According to the pressure-melting point phase diagram of nylon 6(PA6), sufficient pressure (target pressure) can generate adequate undercooling to induce crystallization during pressurization. In this work, a self-designed variable-speed diamond anvil cell (s-dDAC) was employed to subject PA6 to rapid pressurization treatment at a pressurization rate of 1 GPa/s. The effect of target pressure on the crystallization behavior of PA6 was investigated in situ using multiple structural characterization techniques. The results demonstrated that target pressure significantly influenced both the crystal polymorphism and crystallization process of PA6. When the target pressure was <= 2.5 GPa, the melt could not completely solidify during pressurization, exhibiting crystallization lag, and the resulting samples consistof a mixed phase dominated by alpha-phase with minor beta-phase content. When the target pressure was >= 3.0 GPa, the crystallization lag disappears, and the samples comprise a mixed phase dominated by beta-phase with minor alpha-phase content. Regardless of target pressure, the critical pressure at which PA6 melt initiated solidification remains nearly constant at approximately 340 MPa. When the target pressure was >= 3.0 GPa, PA6 melt can continuously solidify within a "pressure window" ranging from 340 MPa to 2.7 GPa. During depressurization, the volume of beta-phase crystals continuously expanded, accompanied by partial crystal destruction. This work represents the first successful preparation of beta-phase-containing PA6 products via rapid pressurization method, with in situ observation of both the pressurization-induced formation process and depressurization-induced destruction process, demonstrating that modulating pressurization conditions can not only control the crystallization kinetics of PA6 but also enable the fabrication of products with distinctive structures.

Manganese oxide has garnered significant attention in the field of supercapacitors. However, it faces several major limitations such as sluggish ionic transport and poor conductivity. This study details the fabrication of a high-performance positive electrode composed of nickel-doped manganese oxide using facile electrodeposition techniques. It was conclusively demonstrated that nickel effectively infiltrated the crystal lattice of birnessite manganese oxide instead of forming a manganese-nickel oxide composite, resulting in an increase in the average valence state of manganese. Nickel-doped manganese oxide exhibited superior specific capacitance (434 F g-1) and cycle stability (93.87 % capacitance retention after 10,000 cycles) compared to manganese oxide, nickel oxide hydroxide, and manganese-nickel oxide composites, underscoring its suitability as a positive electrode material for supercapacitors. Furthermore, the assembled device, featuring nickel-doped manganese oxide as the positive electrode and polypyrrole-coated iron oxide hydroxide as the negative electrode, demonstrated exceptional energy density (65.35 Wh kg-1), positioning it as a promising flexible energy storage solution for wearable electronic devices.

ABSTRACT Accurate discrimination of structurally analogous sulfur‐containing molecules with overlapping photoelectrochemical (PEC) responses remains a major challenge for conventional PEC sensors that rely on one‐dimensional photocurrent readouts. Herein, we develop a dual‐channel PEC fingerprinting platform that pairs Zn‐TCPP with a rationally constructed Cu‐TCPP@Zn‐TCPP MOF‐on‐MOF heterostructure and integrates their paired responses with machine‐learning (ML) algorithms. Unlike traditional single‐signal approaches, Zn‐TCPP and the layered Cu‐TCPP@Zn‐TCPP heterointerface serve as two distinct transduction interfaces that convert molecule‐dependent interfacial interactions into dual‐interface PEC fingerprints. Experimental and theoretical analyses reveal that these discriminative responses arise from coupled molecular and interfacial effects. These effects include molecular‐size‐dependent interfacial accessibility, frontier‐orbital‐influenced hole consumption, and, in the case of glutathione (GSH), Cu–S‐related modulation of the cathodic oxygen‐reduction‐related electron‐consumption pathway. These differences in molecular–interface interactions are used to establish a paired PEC fingerprint dataset. Subsequent ML‐assisted decoding, particularly with an artificial neural network (ANN), resolves the overlapping response patterns. The platform achieves high‐accuracy classification of five representative sulfur‐containing molecules, discrimination among predefined GSH concentration levels, and recognition of binary mixtures and spiked real‐water matrices. This work integrates MOF‐on‐MOF heterointerfacial chemistry with data‐driven fingerprint decoding, providing an interface‐design strategy for intelligent recognition of sulfur‐containing molecules in complex aqueous environments.

Highly ordered ultrathin nanosheets (NSs) of Au(I)-Cys were fabricated through aggregation-induced supramolecular self-assembly triggered by an extended agitation in an alkaline environment. The synthesized Au(I)-Cys NSs exhibited intense luminescence and exceptional chirality. Remarkably, additions of biothiols to Au(I)-Cys NSs have significantly enhanced their luminescence emission, and circular dichroism properties coupled with morphological modulations into nanoflowers, nanodendrites, or closely packed aggregates. These new findings of Aggregation-Induced Luminescence Enhancement (AIEE) and Aggregation-Induced Circular Dichroism Enhancement (AICE) were attributed to multiple interactions involved such as Au-S bonding, stacked H-bonding, and strong aurophilic Au(I)···Au(I), ligand-metal-charge-transfer (LMCT) and ligand-metal-metal-charge-transfer (LMMCT). The AIEE phenomenon of the fabricated Au(I)-Cys NSs was utilized for developing a highly sensitive luminescent platform for determining homocysteine (Hcy), cysteine (Cys), and glutathione (GSH) biothiols in human serum. The developed platform is simple, fast, sensitive, and highly selective for the determination of biothiols through the concentration ranges of (0.25-100.0 μM), (0.625-40.0 μM), and (5.00-600.0 μM), with a lower detection limit (S/N = 3:1) of 0.15, 0.10 and 1.20 μM for Hcy, Cys, and GSH; respectively. Interestingly, irradiation of Au(I)-Cys NSs with a high-energy electron beam during TEM analysis led to an in-situ transformation of the Au(I)-Cys NSs into gold nanoclusters (AuNCs). This phenomenon provided an innovative bottom-up strategy for the synthesis of AuNCs that could be employed in various biological and therapeutic applications. Optimization of the applied voltage and electron beam's exposure time has been found effective in synthesizing precisely designed and size-controlled AuNCs.

Energetic materials have closely correlated safety and high-pressure chemical reaction kinetics. While extensive research has typically focused on structural evolution and reversible phase transitions at high pressures, chemical decomposition pathways remain underexplored. Here, we report a novel pressure-induced chemical reaction in CL-20 during decompression from a peak pressure of 26.2 GPa under nonhydrostatic compression. Infrared spectroscopy confirmed chemical bond cleavage, yielding gaseous decomposition products primarily composed of N2O and CO2. Molecular dynamics simulations revealed that the initial decomposition steps involved H migration, OH transfer, β-scission of the C-C bridge, and cleavage of C-N bonds. Notably, under improved hydrostatic conditions (using KBr as the pressure-transmitting medium), the reaction threshold pressure increased to 30.1 GPa, highlighting the critical roles of shear stress in the diamond anvil cell environment. This study represents the first clear demonstration of decompression-induced chemical reactions in condensed explosives, providing fundamental insights into their intrinsic safety mechanisms as well as their initiation and detonation behaviors.

In this communication, a simple and scalable strategy was proposed to synthesize hollow nanoboxes NiS/NiS2 heterojunction, which involves using Cu2O nanocubes as template, Na2S2O3 as etchant, and combined with sulfurization process. Specifically, the overpotential of ground sample at 20 mA cm- 2 for OER is 284 mV, which are superior to most of the recently reported nickel sulfide-based catalysts. This effective strategy could also be applied to synthesize other hollow and heterogeneous structures materials.

As energy demand continues to rise, electrochemical energy storage has garnered substantial attention. Supercapacitors, renowned for their high power density and long cycle life, have been extensively studied as complementary devices to batteries. Iron-based metal-organic frameworks (Fe-MOFs) and their derivatives have emerged as promising candidates for supercapacitor anode materials due to their abundant pore structures and redox sites. This review offers a comprehensive summary of recent research on Fe-MOFs and their derivatives as supercapacitor electrode. It introduces the synthesis and physical and electrochemical properties of Fe-MOFs, and delves into their energy storage mechanisms, with a focus on their application in supercapacitors. It encompasses Fe-MOFs, Fe-MOF derivatives, iron-based bimetallic MOFs, and composite materials derived from Fe-MOFs. Additionally, it briefly explores the use of other metal MOFs in supercapacitors. The design and utilization of Fe-MOF and its derivatives as electrode materials are discussed, including the impact of carbonization on their performance and their interaction with aqueous electrolytes. This review concludes with a summary and outlook on Fe-MOFs and their derivatives as supercapacitor electrode, aiming to provide valuable insights and guidance for future research in this field.

Cancer immunotherapy is an innovative treatment approach and a crucial element in suppressing tumor recurrence and metastasis. Nevertheless, restricted differentiation and maturation of dendritic cells (DCs) remains a significant obstacle to the efficacy of immunotherapy. Immunoadjuvants have been utilized to modulate the function of immunogenic DCs to enhance cancer immunotherapy efficacy and inhibit tumor recurrence and metastasis. Herein, a biomimetic tumor-targeted nanoadjuvant (M@alpha M) is developed that load an amino acid transport inhibitor (alpha-methyl-L-tryptophan, alpha-MT) in the manganese porphyrin-based metal-organic framework (Mn-MOF, MM) core, and coat with homologous cancer cell membranes on the surface. M@alpha M has a peroxidase-like effect, whereby it generates oxygen to ameliorate the hypoxia while depleting the excess glutathione in the tumor cells. Manganese ions (Mn2+) are released in the acidic tumor microenvironment under ultrasound stimulation, enabling non-invasive and highly penetrating sonodynamic therapy (SDT) to promote immunogenic cell death (ICD). Concurrently the activation of the cyclic GMP-AMP synthase (cGAS)-stimulator of interferon genes (STING) pathway facilitated by the release of Mn2+, combined with the ICD, significantly promotes the maturation of the DCs and enhances the subsequent series of tumor-killing effects. Furthermore, this innovative bionic nanoadjuvant makes the tumor highly sensitive to programmed cell death ligand 1 (PD-L1) checkpoint blockade immunotherapy, effectively suppressing distant tumor growth and inhibiting lung metastasis. The presence of MM makes M@alpha M both a sonosensitiser and an immunoadjuvant, as well as photoacoustic and magnetic resonance imaging agents for integrated nanodiagnostics. These findings offer a potential strategy to overcome the challenge of tumor recurrence and metastasis.

Intelligent sensing means the capability of systems to perceive, learn, analyze, and predict based on external stimuli, mimicking the cognitive functions of the human brain. With the assistance of machine learning algorithms for data processing, soft sensors made from hydrogels and ionogels possess intelligent sensing abilities. Here, the recent advances of hydrogel- and ionogel-based soft sensors are comprehensively investigated and summarized, with a specific focus on machine learning-implemented applications, including handwriting/gesture/object/motion/speech recognition, health monitoring, food detection, and beyond. With current limitations and future perspectives discussed, the fusion of the two is envisioned that can accelerate the development of intelligent sensing in the areas of human-machine interface (HMI), health care, and soft robotics.