Physics
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Liquid surface curvature profoundly influences physical, chemical, biological, and engineering
processes by modulating surface mechanical and thermodynamic properties. Curved interfaces
are more prevalent than ideal planar ones and exhibit distinct size-dependent behaviors, yet the
molecular-level consequences for interfacial water have not been fully elucidated. Herein we sys-
tematically explore how surface curvature regulates the structure, dynamics, mechanics, and ther-
modynamics of water nanodroplets. We demonstrate that the interfacial width decreases logarith-
mically with decreasing droplet radius R, consistent with curvature-induced suppression of capil-
lary waves. Instantaneous interfacial analysis uncovers enhanced orientational ordering of surface
molecules under higher curvature. Such structural changes give rise to a radius-dependent sur-
face tension: γ(R) is well described by the classical Tolman equation with positive Tolman length
δ. We further demonstrate that short-time fluctuations at the water surface can reliably predict
long-time dynamic propensities, thus providing a practical approach for estimating the long-time
dynamics of interfacial liquids in theoretical and computational investigations. The findings on
curvature-dependent variations in energetics, structure, dynamics, and forces hold significant im-
plications for processes involving micro- and nano-scale water droplets across multiple scientific
and technological fields.
Abstract The influence of water on the molecular dynamics of sequence-defined alternating polymers was investigated using broadband dielectric spectroscopy. Understanding how water couples to polymer dynamics is essential for controlling transport, mechanical properties, and functionality in hydrated soft materials. Two alternating copolymers, P(C 4 EG 4 )3.2k and P(C 8 EG 4 )2.9k, which share identical ethylene glycol segments but differ in aliphatic spacer length, are studied over a wide temperature range and at water contents up to 10 wt%. In the dry state (= 0 wt% water), both polymers exhibit well-defined α- and β-relaxation processes associated with cooperative segmental motion and localized molecular dynamics, respectively. The interpretation of the data consistently shows that, upon hydration, water acts as an efficient plasticizer, leading to a significant increase in free volume, which in turn accelerates α-relaxation and lowers the glass transition temperature. In contrast, the β-relaxation remains much less sensitive to water content. A separate water-related relaxation process emerges, attributed to the reorientational dynamics of confined water molecules. The free volume, estimated from the temperature dependence of the α-relaxation using the Williams–Landel–Ferry (WLF) approach, increases systematically with both temperature and water content. A clear sequence-dependent response is observed: the more polar P(C 4 EG 4 )3.2k shows stronger hydration-induced free volume enhancement and dynamic changes, whereas P(C 8 EG 4 )2.9k exhibits faster intrinsic dynamics but weaker sensitivity to water. These results establish molecular sequence as a key molecular design parameter for controlling hydration-dependent dynamics and transport-relevant properties in polymer systems.

In this work, we investigate the combined effects of Rashba spin-orbit coupling (RSOC) and non-Hermiticity on topological phase transitions in spinful p-wave Kitaev chains. While previous studies have separately examined non-Hermitian (NH) extensions of Kitaev chains and the effects of RSOC in Hermitian systems, the interplay between these two mechanisms remains largely unexplored. We analyze this interplay by considering two distinct types of complex on-site potentials: (i) a uniform gain/loss term and (ii) a complex quasiperiodic one. We demonstrate that the impact of RSOC is highly model-dependent. In particular, RSOC does not affect the topological phase boundary in the Hermitian limit of the uniform gain/loss model (provided the spin-flip hopping is weaker than the pairing strength), but significantly alters the topological landscape in the NH regime. In contrast, for the quasiperiodic model, RSOC modifies the phase boundaries in both the Hermitian and non-Hermitian cases. Notably, we find that the combined interplay of non-Hermiticity and RSOC drives topological transitions at significantly lower potential strengths compared to the Hermitian limit. We derive analytical expressions for the topological phase transitions in both cases and validate our predictions through numerical calculations of energy spectra and real-space winding numbers. This work provides a comprehensive understanding of how non-Hermiticity and RSOC cooperatively reshape topological phase diagrams in one-dimensional superconducting systems.
Efficient and stable noble-metal-free photocatalysts are highly desirable for renewable energy. A three-dimensional polyoxometalate-based metal–organic framework (POMOF), [Cu I 2 Cu II 3 (ptzH) 6 (H 2 O) 2 (OH) 2 ] (SiW 12 O 40 ), was constructed as a photocatalyst through the self-assembly of multivalent copper nodes (Cu + /Cu 2+ ), 5-(2-pyridyl)-1 H -tetrazole organic ligands, and Keggin-type silicotungstate anions. Structural characterization confirmed a stable open framework with ordered nanochannels in Cu 5 -SiW 12 . Relative to pristine SiW 12, a reduced optical band gap (from 3.60 to 3.22 eV) and a negative shift of 0.49 V in the conduction band minimum were observed for Cu 5 -SiW 12 (from 0.14 to −0.35 V). Such property modifications are ascribed to the appreciable electronic coupling between copper centers and SiW 12 moieties, through which synergistic enhancements in light harvesting, charge separation, and charge transport efficiency are achieved. Under optimized reaction conditions, a hydrogen evolution reaction (HER) activity of 5190.89 μmol g –1 h –1 was attained for Cu 5 -SiW 12, representing a 19-fold enhancement over pristine SiW 12 and outperforming numerous reported noble-metal-free photocatalysts. Mechanistic studies attribute the superior performance to synergistic effects: an optimized band structure, framework-enabled charge separation, and in situ generated heteropoly blue (HPB). This study develops a photocatalyst with notable hydrogen evolution activity and provides a viable strategy for the rational design of efficient molecular-based photocatalysts.
loading leads to an enhancement in dye degradation. These results establish a general strategy for integrating catalytic functionality into chemically inert, hydrophobic membranes without compromising distillation performance, providing a pathway toward multifunctional membranes that couple advanced oxidation with membrane separation for water treatment.
doping during the regulation of crystallization kinetics, promoting the formation of a stable alloy phase and effectively passivating halide vacancies. This synergistic regulation strategy significantly improves the film's crystallinity, extends carrier lifetime, and reduces the density of trap states. WBG perovskite solar cells fabricated using this optimized film achieved a power conversion efficiency (PCE) of 23.53%. Notably, after 1500 h of continuous maximum power point tracking (MPPT) testing under 1 sun irradiance, the unencapsulated devices retained 80% of their initial PCE.
Organic bioelectronics relies on materials capable of efficiently transducing signals between ionic biological environments and electronic devices. Conducting polymers are particularly attractive for this purpose due to their mixed ionic-electronic conductivity, mechanical compliance, and chemical tunability. Among them, bis-ethylenedioxythiophene-thiophene (ETE)-based polymers can be synthesized in situ via mild enzymatic reactions, enabling seamless and substrate-free integration with biological systems. Here, we investigate the impact of hydrophilic side-chain engineering on the physicochemical, electrochemical, and biological properties of ETE-based polymers by comparing two polymers which differ only by the presence of a triethylene glycol side chain between the ETE core and the terminal carboxylic group. We show that glycolation leads to increased film hydration and surface roughness without a measurable change in elastic modulus, suggesting competing effects from molecular ordering and ionic cross-linking. In a neuronal cell model, the glycolated polymer exhibits markedly enhanced cytocompatibility and cell adhesion, likely driven by its increased surface roughness and matrix topography. By combining electrochemical quartz crystal microbalance with dissipation monitoring, in-operando UV-vis spectroscopy, and electrochemical atomic force microscopy, we correlate ionic transport, swelling behavior, and nanomechanical responses, revealing enhanced electrochemically induced swelling in the glycolated polymer. Finally, when implemented as active channel materials in organic electrochemical transistors, both polymers display comparable performance, although the glycolated polymer shows slightly reduced cycling stability. These findings highlight the complex trade-offs introduced by side-chain glycolation and provide design guidelines for enzymatically synthesized conducting polymers in bioelectronic interfaces.
Layered oxides for sodium-ion batteries have attracted extensive attention from researchers due to their distinctive advantages. Nevertheless, for O3-type layered oxides with a high initial capacity, critical issues including excessive surface residual sodium, sluggish reaction kinetics, and poor long-term cycling stability remain to be urgently addressed. Herein, a novel wet in situ coating strategy using ammonium phosphomolybdate is proposed. The NFM@NH-Mo material derived from the coating modification of NaNi 1 / 3 Fe 1 / 3 Mn 1 / 3 O 2 (NFM) is endowed with a sodium-ion conductor group (SCG) coating layer. Various kinetic tests demonstrate that the SCG coating layer significantly facilitates the deintercalation and intercalation of Na +, leading to an approximate one-order-of-magnitude enhancement in the Na + diffusion coefficient compared with pristine NFM. In addition, the consumption of surface residual sodium on NFM during the formation of the SCG coating layer effectively reduces the polarization of NFM@NH-Mo. Combined with the electrochemical performance of NFM@NH-Mo at 55 °C, which delivers a capacity retention of 83.10% after 100 cycles against only 70.51% for NFM, the SCG coating layer is proven to suppress the anisotropic stress variation of the NFM material and the side reactions between the active material and electrolyte, thus endowing the modified material with excellent cycling stability at elevated temperatures.
The buried interface of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) PEDOT:PSS/perovskite in inverted perovskite solar cells (PSCs) presents several challenges, such as low work function (WF) causing energy level mismatch, poor conductivity limiting transport, and defect states inducing nonradiative recombination and carrier loss. To address these issues, this work introduced the interfacial modifier sodium acetate (NaOAc) into the PEDOT:PSS precursor solution, enabling molecular-level modulation of the physicochemical properties of the buried interface. Experimental results confirm that sodium ions (Na + ) preferentially coordinate with the sulfonic acid groups at the termini of PEDOT:PSS molecular chains, displacing the nonconductive H + and forming a more ordered molecular packing. This ion-exchange process increases the WF of the PEDOT:PSS film at the buried interface (from 4.27 to 4.38 eV) while enhancing its conductivity by 55%, effectively optimizing interfacial energy level alignment and reducing the hole transport barrier. More importantly, the residual acetate anions exert an in situ passivation effect during the subsequent perovskite crystallization, coordinating with unreacted Pb 2+ at the buried interface, thereby reducing the defect density by 11%. The optimized buried interface exhibits excellent carrier dynamics characteristics, with photoluminescence spectroscopy and electrochemical impedance spectroscopy confirming that the sodium acetate treated PEDOT:PSS buried interface reduces nonradiative recombination and enhances charge extraction. As a result, the device fill factor exceeds 81.7%, and the efficiency improves to 19.38%. When applied to mixed tin lead perovskite (FASnI 3 ) 0.6 (MAPbI 3 ) 0.4, the optimized buried interface further demonstrates universal advantages, achieving an efficiency exceeding 21%. This work reveals the synergistic modulation mechanism of ion coordination engineering at the buried interface on carrier transport and recombination dynamics, providing a new paradigm for the development of high-performance inverted perovskite solar cells.
Electrically tunable soft lenses are essential for emerging applications in soft robotics, adaptive optics, and minimally invasive biomedical imaging. Among various materials, electroactive hydrogels have emerged as ideal candidates for constructing such lenses due to their tissue-like softness and intrinsic electrical actuation capabilities. However, current hydrogel-based actuators often face a fundamental trade-off between high optical transparency and low-voltage responsiveness due to the uncontrolled aggregation of conductive fillers. Herein, we report a transparent, low-voltage-driven electroactive hydrogel lens based on a polyacrylamide (PAM) matrix incorporated with sodium-functionalized multiwalled carbon nanotubes (Na-MWCNTs). By engineering the interfacial chemistry of the nanotubes with surface carboxylate groups (–COONa), uniform dispersion of nanotubes in PAM via electrostatic repulsion at a low loading (≤0.1 mg mL –1 ) was achieved. Consequently, this well-dispersed state preserves high visible-light transmittance, while the incorporation of Na-functionalized MWCNTs modulates the overall charge transport behavior within the hydrogel matrix, facilitating rapid charge redistribution. Under a 30 V stimulus, the focal length of the hydrogel lens can be tuned from 73.6 mm to 53.7 mm, achieving a 27% tunability. Mechanistically, this focal tuning is realized through the asymmetric modulation of surface curvature, driven by an electric-field-induced osmotic pressure gradient. Ultimately, this PAM/Na-MWCNT hydrogel platform offers a versatile solution for next-generation adaptive biomimetic optical devices, endoscopic probes, and soft robotic vision.
High Resolution Image Download MS PowerPoint Slide Quinoidal porphyrinoids represent a promising class of electron accepting materials due to their extended π conjugation, strong electron affinity, and structural rigidity, yet their application in organic solar cells (OSCs) remains unexplored. This work presents the design and synthesis of a nickel based quinoidal porphyrinoid ( NiQP ) and its implementation as an n type acceptor in bulk heterojunction OSCs using PM6 as the donor polymer. NiQP exhibits broad absorption extending into the near-infrared region and a narrow optical bandgap of approximately 1.44 eV, enabling complementary light harvesting with PM6. PM6: NiQP devices deliver a power conversion efficiency (PCE) of 8.47% in as cast films, which increases to 12.51% after solvent vapor annealing (SVA), mainly due to enhanced short circuit current density and fill factor. Photophysical and electrical analyses show that SVA improves nanoscale morphology, exciton diffusion, and dissociation efficiency, while suppressing bimolecular and trap assisted recombination. Energy loss analysis further indicates reduced radiative and non radiative recombination losses in SVA treated devices, accompanied by lower Urbach energy and diminished energetic disorder. These results demonstrate the potential of quinoidal porphyrinoids as efficient electron acceptors and provide guidelines for molecular design and processing strategies in next generation OSCs.
Bone regeneration is an energy-intensive process requiring coordinated regulation of ionic microenvironments and cellular metabolism. Yet, current biomaterials rarely address the dynamic energy requirements of osteogenesis. Inorganic calcium polyphosphates (CPPs), featuring high-energy phosphoanhydride bonds and tunable degradation profiles, offer a promising bioenergetic strategy for metabolically responsive bone repair. Herein, three CPPs with distinct configurations: linear Ca-TPP, cyclic Ca-TMP, and Ca-HMP were synthesized, and their osteogenic effects were systematically investigated by integrating molecular dynamics (MD) simulations with experimental approaches. The results indicate that the configuration-dependent nanoarchitectonic features of CPPs, including phosphate-unit number, charge density, and molecular configuration, govern their stability, solubility, and ion-release behaviors. Specifically, Ca-HMP forms stable assemblies that support sustained phosphate release and long-term energy supply; Ca-TMP displays faster hydrolysis kinetics, preferentially enhancing mitochondrial functional activation and oxidative phosphorylation (OXPHOS); Ca-TPP contributes primarily to extracellular matrix maturation. Importantly, all CPPs exhibit superior pro-osteogenic efficacy compared with crystalline calcium phosphate (Ca–P). CPPs can reprogram cellular metabolism by elevating intracellular ATP levels, increasing mitochondrial membrane potential, and upregulating metabolic and osteogenic genes (including GAPDH, ATP5F1A, ALP, and BMP-2), which is mediated via the activation of AMPK, mTOR, and PI3K-AKT signaling pathways, collectively improving osteogenic differentiation over Ca–P controls. These findings establish CPPs as a class of “smart” metabolic materials that synchronize energy availability with osteogenic demands, providing a promising paradigm for bone regeneration.
Perovskite solar cell (PSCs) modules using cost-effective copper electrodes encounter significant challenges in long-term operational stability, limiting their commercial viability. We systematically investigate the degradation behavior of n-i-p structure PSCs modules under continuous illumination. The P3 interconnection region is identified as the primary site of failure, where localized corrosion initiates and propagates during operation. Using optical microscopy, scanning electron microscopy (SEM), and energy-dispersive X-ray spectroscopy (EDX), we reveal a pronounced redistribution of Cu and iodide species near the P3 region in aged devices. Bias-dependent studies (−2 to +4 V) show that forward bias significantly accelerates degradation, while thermal stress alone does not induce corrosion, indicating a field-driven mechanism. We propose that lateral migration of iodide ions toward the P3 region, followed by electrochemical reactions with Cu, leads to the formation of corrosive products and ultimately electrode failure. A thin bismuth (Bi) interlayer between MoO 3 and Cu effectively suppresses ion migration and interfacial reactions. As a result, the modified modules retain over 90% of their initial performance after 400 h of continuous illumination, compared to rapid failure in control devices. This work provides direct insight into bias-induced degradation in PSC modules and establishes an effective interfacial strategy for enhancing the stability of Cu-based electrodes.
How to make nanomaterials effectively target bacteria and enhance the antibacterial activation of immune cells is crucial for improving antibacterial efficacy. Herein, a magnetic extracellular vesicle that can not only activate macrophages in the infection microenvironment but also effectively kill bacteria is developed for enhancing antibacterial activation in vivo . The modification of d -galactose on the magnetic nanoparticles (GMNPs) and the loading of the GMNPs into macrophage-derived microvesicles (MVs) confer the resulting MVs@GMNPs with cascade-targeting capability, leading to high accumulation at the infection site. In the infectious microenvironment, the chemodynamic effect of the GMNPs triggers their rapid release from MVs. On one hand, the released GMNPs promote the polarization of macrophages toward the M1 phenotype, thereby enhancing antibacterial immune activation. On the other hand, GMNPs selectively bind to Pseudomonas aeruginosa ( P. aeruginosa ), enabling close contact with bacteria and effective chemodynamic therapy against infection. By combining chemical destruction with immune activation, MVs@GMNPs achieve efficient eradication of P. aeruginosa -induced subcutaneous abscesses with a bacterial inhibition rate of 99.8% in vivo .
Developing advanced adsorbents with both high selectivity and low regeneration energy remains a central challenge in realizing energy-efficient CO 2 capture technologies. In this work, we report an ultramicroporous metal–organic framework, PCP-IPAN, designed with CO 2 -philic electrostatic cavities to promote strong yet thermally tunable interactions with CO 2 molecules. Notably, the framework exhibits highly temperature-sensitive adsorption profiles, characterized by a sharp reduction in CO 2 uptake within a narrow temperature range (273–323 K). This significant thermal sensitivity enables a large working capacity and ensures facile desorption at mild temperatures, which is a key requirement for reducing the energy penalty in pressure- and temperature-swing adsorption (P/TSA) processes. Single-component adsorption measurements reveal that PCP-IPAN-Co achieves high CO 2 capacities of 4.60 and 3.32 mmol g –1 at 273 and 298 K (1.0 bar), respectively. Furthermore, it delivers CO 2 /N 2 (15/85) IAST selectivities of 71.6 and 99.3, alongside CO 2 /CH 4 (50/50) IAST selectivities of 39.8 and 19.6 at these temperatures. Dynamic column breakthrough experiments for CO 2 /N 2 and CO 2 /CH 4 binary mixtures confirm the material’s excellent separation selectivity, and vacuum pressure swing adsorption (VPSA) simulations demonstrate its efficient separation energy consumption during cyclic operation. These findings highlight PCP-IPAN as an efficient platform for carbon capture.
High Resolution Image Download MS PowerPoint Slide Cryopreservation depends critically on the suppression of ice formation by cryoprotective agents (CPAs), but limited data are available on the CPA concentration required for vitrification (Cv). Here, we introduce a high-throughput 384-well platform that integrates automated liquid handling, randomized plate layouts, and a binary-search strategy to rapidly determine Cv across hundreds of formulations. Relative to conventional methods, this approach increases throughput by ∼50-fold, compressing a year of measurements into 1 week, while markedly reducing manual labor. Across ∼200 CPA compositions, we demonstrate that environmental boundary conditions strongly influence vitrification behavior: plates sealed with silicone mats exhibited lower Cv than open plates, indicating that sealed configurations promote vitrification. Further, the data reveal a decrease in Cv with increasing CPA molecular weight, consistent with enhanced ice suppression by larger molecules. We also present a simple mixture model that accurately predicts Cv for a broad range of CPA formulations, including mixtures containing up to seven CPAs ( R 2 ≥ 0.93), and we use this model to evaluate published CPA toxicity data to identify formulations that operate near their vitrification threshold while maintaining relatively low toxicity. Together, these results establish a framework for rapid Cv determination, predictive modeling of vitrification behavior, and rational design of CPA formulations.
Earth-abundant tetrahedrite Cu 12 Sb 4 S 13 is a promising p-type thermoelectric (TE) material owing to its intrinsically low lattice thermal conductivity, yet its performance remains limited by insufficient electrical transport and the persistent trade-off between charge and phonon transport. In this study, we present a colloidal route for the scalable synthesis of Ag-substituted Cu 12 Sb 4 S 13 nanocrystals and use these nanocrystal building blocks to construct bulk tetrahedrite TE materials with improved transport balance. Ag incorporation preserves the tetrahedrite framework while inducing lattice expansion, increased microstrain, local bond softening, and enhanced structural disorder, which can be retained to a meaningful extent after densification. These structural perturbations are accompanied by a marked enhancement in electrical conductivity and weighted mobility, together with a substantial suppression of lattice thermal conductivity. The optimally substituted Cu 11.92 Ag 0.08 Sb 4 S 13 sample exhibits the best overall transport performance, reaching a lattice thermal conductivity of 0.30 W m –1 K –1 and a maximum zT max of 1.23 at 690 K, representing an approximately 1.8-fold improvement over pristine Cu 12 Sb 4 S 13, as well as competitive theoretical conversion efficiency and slightly improved hardness. These results highlight Ag-substituted nanocrystals as effective building blocks for improving the TE performance of earth-abundant tetrahedrites through coordinated control of structure and transport.
The dimeric prodrug self-assembly (DPSA) technology, with a simple preparation process, high drug-loading capacity, and excellent safety, could provide an innovative solution to address issues, including the poor stability and low bioavailability of aldehyde-containing plant essential oils (APOs) in agricultural applications. Herein, dimeric prodrugs based on APOs salicylaldehyde (Sal) and citral (Cit) were fabricated by individually conjugating Sal and Cit with oxalyl dihydrazide (Oxa) through a simple Schiff base reaction and subsequently self-assembled into nanoparticles (Sal-Oxa NPs and Cit-Oxa NPs) in aqueous solution for improving the stability and biological activity of APOs. The results showed that a pH of 7 and a temperature of 25 °C were the optimal conditions for the formation of DPSA with superior colloidal stability. The obtained DPSA exhibited excellent physicochemical properties, including low volatility and surface tension, and high photostability, thermal stability, and maximum retention, significantly improving the wettability, adhesion, and deposition of Sal and Cit on different plant leaves. Importantly, DPSA could be decomposed in acidic environments caused by pathogenic fungi to controllably release Sal, Cit, and Oxa to exert multitarget synergistic effects on plant disease. Moreover, DPSA demonstrated better biosafety to tomato and Vicia faba, comparable to that of APOs. Therefore, this study would provide a promising strategy for efficient utilization of APOs in the effective control of plant diseases.
Molecular hybrids consisting of hydrophobic, water-insoluble cobalt phthalocyanine (CoPC) complex and noncatalytic protein bovine serum albumin (BSA) have been developed as a green catalyst for stereoselective oxidations, including C=C epoxidation and C–H hydroxylation. Effective encapsulation of CoPC into the BSA scaffold (CoPC–BSA) was achieved through agitation of BSA and CoPC in an aqueous solution, resulting in a structurally intact, stable protein–cofactor hybrid. Upon activation with H 2 O 2, CoPC–BSA catalyzed epoxidations of styrene and cyclooctene with yields of 87–99%, achieving >99% enantioselectivity for R-styrene oxide. CoPC–BSA also enabled selective C–H oxidation of propanoic acid and methyl phenylacetate under mild conditions. For propanoic acid, L-lactic acid was the sole product of oxidation of propanoic acid, while methyl phenylacetate showed temperature-dependent enantioselectivity. When immobilized on silica beads, R-methyl mandelate with an enantioselectivity >92% at 80 °C was produced at a conversion of ∼99%. These results demonstrate the potential of molecular hybrids for enantioselective oxidations and highlight the critical role of protein flexibility and dynamics in tuning catalytic outcomes.
Quasi-Discrete Channels of Porous Coordination Polymers for Selective Multiscenario CO 2 Recognition
Selective recognition of carbon dioxide (CO 2 ) from mixtures containing many similar species is crucial for industrial energy and environmental applications, yet it remains elusive. Herein, we report an interdigitated coordination polymer (CID-PNA) that leverages quasi-discrete channels for multiscenario CO 2 recognition and separation. CID-PNA features corrugated channels composed of aromatic cavities connected by narrow windows, forming π-rich, nonpolar pockets that preferentially capture CO 2 over C 2 H 2, CH 4, and N 2 . Specifically, CID-PNA achieves excellent CO 2 /C 2 H 2, CO 2 /CH 4, and CO 2 /N 2 selectivity (5.1, 14.8, and 117.7, respectively), a moderate CO 2 adsorption enthalpy of 33.2 kJ mol –1, rapid adsorption–desorption kinetics with cycling completed within minutes at room temperature, and a high CO 2 /H 2 O uptake ratio (3.24) that far exceeds those of benchmark materials (e.g., CALF-20, ALF, and Zeolite-13X). Breakthrough experiments demonstrate that CID-PNA enables one-step purification of high-purity C 2 H 2 (>99.5%), CH 4 (>99.9%), and N 2 (>99.9%) from the corresponding CO 2 -containing mixtures, even under wet-hot flue gas conditions. In situ crystallography, spectroscopy, and theoretical calculations reveal that selective CO 2 binding originates from cooperative C═O···H and π···π interactions within confined aromatic pockets. Overall, the quasi-discrete aromatic channels in CID-PNA integrate strong recognition, rapid transport, and energy-efficient regeneration, offering a general design motif for selective CO 2 separation across diverse gas mixtures.
Two-dimensional titanium carbide (Ti 3 C 2 T x ) MXene nanosheets have a variety of potential applications due to their high electrical conductivity and mechanical strength. However, assembling these nanosheets into multilayer films often results in weak interfacial interactions and low orientation, which severely compromises their electrical and mechanical performance. Here, we achieved highly oriented MXene nanosheets by utilizing shear flow generated during the superspreading process of MXene dispersions. Simultaneously, metal ion-induced gelation is introduced to enhance interlayer interactions and permanently fix the oriented structure. The resulting MXene multilayer films demonstrate excellent electrical conductivity of 17840 ± 905 S·cm –1, which compares favorably with the best values reported for Ti 3 C 2 T x films. These films also exhibit outstanding electromagnetic interference shielding capacity (51.1 dB for a 1.3 μm thick film). Moreover, the tensile strength and Young’s modulus are increased to 2.8 and 2.7 times that of MXene films prepared by conventional solution-casting, reaching 143.0 ± 10.0 MPa and 10.1 ± 0.8 GPa, respectively. This work presents a robust strategy for fabricating high-performance MXene films by synergistically controlling nanosheet orientation and interlayer interaction.
High-quality perovskite films are essential to device efficiency and stability, yet inhomogeneous crystallization and interfacial defects remain major challenges. Here, we introduce a vapor-phase annealing (VPA) strategy to regulate crystallization kinetics and film morphology. By establishing a uniform thermal–humidity field, VPA is proposed to promote a bottom-up crystallization tendency, in contrast to the conventional top-down mode often observed in hot-plate annealing. This shift in growth direction could facilitate homogeneous nucleation, reduce interfacial void formation, and enable more complete precursor conversion with suppressed PbI 2 residue. As a result, the films exhibit improved optoelectronic properties, and additive-free inverted perovskite solar cells achieve a champion power conversion efficiency (PCE) of 22.15% with excellent long-term stability. These results suggest that VPA may provide a scalable route to mitigating crystallization inhomogeneity in perovskite photovoltaics.
The pathological characteristics of Parkinson's Disease (PD) are multifactorial, encompassing the aggregation of α-synuclein, mitochondrial dysfunction, and oxidative stress, necessitating the adoption of multitarget therapeutic strategies. In this study, a borneol-modified carboxymethyl chitosan nanoparticle system (BC/P/HCR NPs) was developed, aiming to codeliver curcumin, rosmarinic acid, and plasmid DNA (pDNA) targeting the SNCA gene for synergistic therapeutic intervention in PD. Borneol is capable of enhancing the permeability of the blood-brain barrier (BBB), while carboxymethyl chitosan contributes to improving the solubility of curcumin and preventing premature drug release. In a C57BL/6 mouse model of PD, BC/P/HCR NPs demonstrated enhanced penetration through the BBB, effectively alleviating motor dysfunction and reducing neuronal damage by downregulating the expression of α-synuclein, restoring mitochondrial function, and mitigating oxidative stress. These findings underscore the potential of BC/P/HCR NPs as a multifunctional nanotherapeutic platform for addressing the complex pathological features of PD.
The skin serves as the primary barrier for human health, yet its integrity is frequently compromised by environmental stressors, leading to wounds where bacterial infection poses a significant clinical obstacle. To address escalating antibiotic resistance and the biocompatibility issues of exogenous antibacterial agents, this project developed an intelligent targeted recognition and efficient antibacterial system (Th A -GH) based on endogenous biocomponents. Leveraging the exceptional spatial addressability and structural programmability of DNA tetrahedra (Th), we integrated bacteria-specific aptamers via edge hybridization and precisely colocalized glucose oxidase (GOx) and horseradish peroxidase (HRP) within the Th nanocavity using extended DNA capture strands. The system mimics natural compartmentalized intracellular environments, significantly enhancing GOx/HRP cascade efficiency through spatial confinement. Th A -GH specifically recognizes and anchors onto bacterial surfaces, where it depletes localized glucose to sever nutrient supply and simultaneously generates highly reactive hydroxyl radicals (·OH) to disrupt bacterial membranes in situ. Experimental data demonstrate that Th A -GH exhibits potent antibacterial activity against both Gram-positive and Gram-negative bacteria in vitro and effectively accelerates the healing of infected wounds in vivo. This study underscores the potential of DNA nanotechnology for precise enzyme regulation, offering a high-efficiency, biocompatible, and targeted non-antibiotic strategy for clinical wound management.
Abstract In this work, we develop a complete and explicit first-class formulation of the massive SU(N ) Yang-Mills model by employing the improved Gauge Unfixing (GU) formalism. Building upon our previous results, where the non-Abelian extension of the improved GU formalism was established, we present here a detailed and self-contained construction of the full first-class structure for this model. We obtain closed-form expressions for all gauge-invariant phase-space variables, constructing them as infinite power series in the discarded second-class constraint. In particular, we show that the spatial gauge field Ãa i acquires an infinite series of corrections governed by the covariant derivative and the structure constants of the Lie algebra, while the spatial momenta πa i transform as a pure colourspace rotation, expressible in compact exponential form. A full first-class Hamiltonian is constructed explicitly, and its mass term reproduces precisely the non-polynomial Stückelberg construction. The equivalence between the Poisson brackets of the GU variables and the Dirac brackets of the original second-class system is verified in full detail for all canonical pairs. A careful counting of physical degrees of freedom confirms the structural consistency of the formalism, yielding 3(N 2 -1) physical degrees of freedom.
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