Nanoscale Horizons最新文献

Utilizing the advanced crystal structure prediction algorithm CBD-GM, this study reports the first prediction of a novel 2D MoS₃ configuration. The results demonstrate that the monolayer MoS₃ exhibits excellent structural and thermal stability, narrow-bandgap semiconductor behavior, high carrier mobility, and pronounced mechanical anisotropy, highlighting its potential for applications in flexible electronics. Building upon this foundation, we designed a series of single-atom catalysts by anchoring transition metal atoms at distinct sulfur coordination sites (S₁, S₂, S₃) of the MoS₃ support. This work reveals that both the dopant element and its coordination site precisely regulate the catalytic activity and selectivity for the CO₂ reduction reaction (CO₂RR). Theoretical screening identified three highly promising candidates: Sc_S2@MoS₃, Sc_S3@MoS₃, and Ni_S3@MoS₃. Sc_S2@MoS₃ favors the formate pathway to HCOOH with a low limiting potential of -0.18 V. Sc_S3@MoS₃ exclusively produces CH₃OH with a rate-determining step of *CHO → *OCHH (U_L = -0.58 V). Ni_S3@MoS₃ can generate both HCOOH (U_L = -0.55 V) and CH₃OH (U_L = -0.72 V) under different potentials. Notably, Sc_S3@MoS₃ exhibits the lowest reaction energy for methanol formation. This study provides crucial theoretical guidance for developing efficient and tunable CO₂ electrocatalysts and expands the Mo-S material family by introducing a metastable but accessible 2D MoS₃ platform with unique coordination environments for single-atom catalysis, thereby broadening the application potential of 2D materials in energy conversion and environmental remediation.

Early and reliable detection of pancreatic cancer (PC) remains a formidable clinical challenge, largely owing to the limited sensitivity, operational unreliability, and enzyme dependence of existing carbohydrate antigen 19-9 (CA19-9) immunoassays. In this work, we determine for the first time that ZnO-Pd nanobolts show intrinsic oxidase-like activity. Furthermore, this attribute was used to fabricate a colorimetric immunoanalytical sensor based on nanozymes for the sensitive and specific detection of CA19-9, a biomarker for PC. In this research, immunoreagent optimization, smartphone-assisted signal analysis, and kinetic analysis of nanozyme catalytic activity were employed to enable highly sensitive detection of CA19-9. Enzyme-kinetic studies showed low Michaelis-Menten constants (K_M) of 0.99 mM, as well as high turnover numbers (k_cat) and catalytic efficiencies (k_cat/K_M) of 4.48 × 10^-4 s^-1 and 0.453 M^-1 s^-1, respectively, indicating high substrate affinity. The optimized nanozyme was functionalized with Goat anti-mouse IgG (GAM IgG), thereby facilitating antigen recognition and signal transduction. The proposed immunoassay demonstrated high analytical sensitivity (LOD of 0.000159 U mL^-1 and LOQ of 0.000482 U mL^-1) and exceptional selectivity even in complex biological matrices. Software-assisted signal processing enabled precise assessment of the limit of detection (LOD) of 0.000359 U mL^-1 and the limit of quantification (LOQ) of 0.00108 U mL^-1. The practical utility of the fabricated immunoassay was further examined using human serum, with recovery rates ranging from 100.6% to 102%, indicating high accuracy and reproducibility. Furthermore, the successful digitalization of assay results into software-based readable data demonstrates the sensing approach's potential for portable, cost-effective, and point-of-care PC diagnostics.

Hybrid electrolytes combining ionic liquids with nanoscale fillers offer a transformative route toward safe, high-performance energy storage; however, the lack of understanding of their charge transport over a broad range of temperature and pressure conditions limits their application. Herein, we address this issue by examining the structural, conducting, viscoelastic and thermodynamic properties of a model quasi-solid electrolyte composed of an ammonium ionic liquid and charged polyhedral oligomeric silsesquioxane (POSS) nanoparticles over an extended temperature (173-393 K) and pressure (0.1-600 MPa) range. We demonstrate that the rigid POSS scaffold creates excess free volume, reduces compressibility and thermal expansion, and introduces reversible shear-thinning viscoelasticity while maintaining efficient ion conduction. Furthermore, our high-pressure experiments reveal that ion dynamics is mostly thermally activated in this nano-hybrid electrolyte and satisfies the density-scaling concept, enabling accurate prediction of ionic conductivity over 12 decades across a wide T-P landscape. This work establishes a fundamental and predictive framework for designing next-generation nano-hybrid electrolytes for operation in extreme environments.

Understanding the transconductance (g_m) at cryogenic temperature remains a major challenge in the physics-based modeling of nanoscale field-effect transistors. Although short-channel drain current (I_D)-gate voltage characteristics can often be described accurately within transport-based formalisms, the corresponding g_m commonly exhibits pronounced low-temperature anomalies that remain unexplained. Here, we investigate a 65 nm Si n-channel transistor measured from 250 K down to 12 K and show that a Landauer-consistent model provides an accurate quasi-ballistic transport baseline for the I_D across the full temperature range, but fails to reproduce the shoulder-like g_m feature that emerges at deep cryogenic temperature. We show that this residual discrepancy originates not from transport nonidealities but from quantum capacitance (C_q)-induced electrostatic renormalization of gate-induced charge modulation. By decomposing the g_m into transport and charge-response contributions, and introducing a gate-control factor governed primarily by the C_q, we derive a compact framework in which the corrected g_m consists of renormalized baseline and differential electrostatic terms. A two-crossover parameterization of C_q in the effective gate-overdrive domain enables simultaneous and self-consistent reproduction of both the I_D and g_m, including the cryogenic shoulder. These results identify anomalous cryogenic g_m as a C_q-induced signature of rapidly varying gate-to-charge coupling in quasi-ballistic transistors.

Our Emerging Investigator Series features exceptional work by early-career nanoscience and nanotechnology researchers. Read Jake McClements's Emerging Investigator Series article 'Unlocking interstitial fluid for acute coronary syndrome diagnosis: ultrasensitive troponin I detection using imprinted polymer nanoparticles' (https://doi.org/10.1039/D5NH00441A) and read more about him in the interview below.

Enhancing electrical conductivity and structural stability of Si-based anodes is crucial to attaining efficient and stable capacity output, promoting their practical applications. Here, we developed a polymer-derived bifunctional coating of nano-Si, which simultaneously provides conductive networks and elastic encapsulation to facilitate electron/ion transport and accommodate Si volume expansion during repeated lithiation/delithiation. A covalent bonding SiOC coating was firstly build onto nano-Si by ball-milling micro-Si with polyvinyl alcohol (PVA), then a cyclized-polyacrylonitrile (cPAN) coating was wrapped onto the above composite through low-temperature pyrolysis of PAN, forming polymer-derived anchoring coatings of nano-Si. The covalent SiOC anchoring layer serves as a bridge for fast electrical conduction and efficient stress buffer, and the cyclized-PAN conformal coating further improves electrical conductivity and mechanical resilience of the whole nanostructure. The as-prepared nanocomposite exhibits excellent electrical and mechanical properties, enabling outstanding electrochemical performance in Li-ion batteries. It exhibits a high initial capacity of 3477 mAh g^-1 and retains 1660 mAh g^-1 after 300 cycles at 1 A g^-1. The graphite-Si/SiOC@cPAN//NCM811 full-cell exhibited a high initial capacity of 180.6 mAh g^-1 and 89% capacity retention after 300 cycles at 1C. This work provides a facile and scalable way to fabricate high-performance Si-based anode materials for high-energy-density Li-ion batteries.

Macrophages are central effectors of innate immunity whose plasticity supports both inflammation and resolution. However, their dysregulated activation underlies many inflammatory, infectious, and degenerative diseases. Here, we show that three two-dimensional MXene nanomaterials, Nb₄C₃, Mo₂Ti₂C₃, and Ta₄C₃, are efficiently internalized by monocytes without compromising viability while reprogramming their activation and differentiation toward an anti-inflammatory macrophage state. Bulk RNA sequencing of murine monocytes treated with each MXene reveals a convergent transcriptional signature characterized by downregulation of proinflammatory genes (e.g., Cxcl9, Cxcl10, Ccl24, Il1b, and Il18), downregulation of Ccr2, and consistent upregulation of genes like Cd28 and Bhlhe41 across MXene treatments. At the protein level, secretion of CXCL10 and CCL24 is significantly reduced. Following early exposure of bone marrow precursors, differentiated macrophage cultures contained a larger CD86^-CD206^- fraction, fewer CD86⁺ and CD206⁺ cells, and reduced basal and LPS-induced activation, consistent with a less polarized, low-activation phenotype. Single-cell mass cytometry (CyTOF) enabled simultaneous immune profiling and label-free detection of MXene-associated elemental signals in peritoneal macrophage populations. In a thioglycolate-induced peritonitis model, MXene co-administration partially attenuated inflammation-associated changes in macrophage subset distribution. These findings establish MXenes as traceable immunoregulatory nanomaterials, enabling simultaneous control and tracking of macrophage responses in vivo. This work introduces a new nanoscale concept of compositionally encoded intrinsically traceable immunomodulatory nanomaterials that couple immune regulation and single-cell tracking even without surface labelling or drug loading.

Sectors that require precise separation between solutes of comparable size often rely on ultrafiltration (UF) and loose nanofiltration (LNF) for a low-cost, scalable, selective separation. However, solute separations in this regime have stubbornly exhibited broad rejection curves where solutes with dimensions substantially smaller than the nominal pore size are rejected. The widened profile of these curves results from three distinct mechanisms. Pore-size heterogeneity convolves the single-pore response with a broad size distribution, and because Hagen-Poiseuille flow scales as the fourth power of radius, the largest pores dominate the permeate and disproportionately leak oversized solutes. Confined (hindered) transport leads to intrapore hydrodynamics, slowing a solute relative to the background solvent velocity and effectively rejecting solutes that would intuitively pass through based on size exclusion alone. Finally, the pore array presents only a limited open area to an approaching solute; under single-pass operation, a solute that does not encounter a pore mouth is recorded as rejected regardless of its size. Despite these challenges in achieving sharp separations, no fundamental phenomena preclude much narrower rejection curves in principle. Advancing toward an ideal "step function" rejection profile requires a systematic dissection of each broadening mechanism and a scaffolded approach where geometric, intrapore, and process architecture might collectively enable unprecedented precision in practical size-selective separations.

Micron-scale hexagonal Cs₄PbBr₆ perovskite microdisks (MDs), comprising a zero-dimensional phase, act as efficient energy donors when interfaced with the organic dye 1,1'-dioctadecyl-3,3,3',3'-tetramethylindocarbocyanine-perchlorate (DiIC₁₈). Upon dye binding and selective excitation of the MDs, efficient singlet energy transfer (ET) occurs, as evidenced by the quenching of MD photoluminescence (PL), enhanced dye emission, and the emergence of an ET-induced rise component in the dye lifetime profile. Single-particle measurements under donor-selective excitation show strong ET-induced donor-acceptor PL anticorrelation, marked by a pronounced zero-delay dip [g²(0)] in the antibunching cross-correlation. Additional evidence for ET comes from single-particle PL trajectory analysis showing strong temporal correlation between donor and acceptor signals, and from simultaneous donor/acceptor-channel imaging under donor-only excitation, where spatially colocalized MD images confirm ET-mediated excitation of dye molecules distributed all over the MDs. Solution-phase ensemble measurements demonstrate relatively high ET efficiency (>50%) even at low bulk dye concentrations (∼1 µM). Spatially-resolved analysis further reveals ∼55% higher ET efficiency at the MD core compared to the edges, indicating preferential dye accumulation within the cavities located mostly in the core region. These results demonstrate that Cs₄PbBr₆ MDs serve as efficient ET platforms with tunable ET efficiency, providing promising potential for applications in photocatalysis, sensing, and light-harvesting technologies.

Solar-driven interfacial evaporation has been widely studied for seawater desalination and wastewater treatment. However, it is still difficult to achieve efficient heat localization and continuous water transport in a single evaporator. In this work, a PAN-PS-PAN sandwich-structured photothermal evaporator was fabricated by sequential electrospinning using a dual-channel needle assembly. The evaporator consisted of polyacrylonitrile-polystyrene-polyacrylonitrile (PAN-PS-PAN, PPPS) layers. Carbon nanoparticles (C NPs) were incorporated into both PAN and PS precursor solutions, with a higher nominal C NP fraction in the PAN-based precursor. The PAN-rich outer layers remained strongly hydrophilic and supported water redistribution toward the evaporation interface, whereas the PS-rich middle layer remained hydrophobic and served as the principal internal thermal barrier. Therefore, the PAN-PS-PAN structure enabled continuous water supply while retaining most heat near the evaporation interface. Owing to this structural design, the PPPS evaporator showed improved water supply and heat utilization. Under one-sun irradiation, the evaporation rate reached 1.33 kg m^-2 h^-1, and the solar-to-vapor conversion efficiency was 90.5%. The evaporator also showed good purification ability for organic dye solutions, acidic and alkaline water, Tween 80/kerosene emulsion, and PEG aqueous solutions with different concentrations. These results demonstrate the potential of the PPPS evaporator for solar-driven seawater desalination and complex wastewater purification.