ACS Applied Materials & Interfaces最新文献

Four lanthanide-oxide-modified Ni-SiO₂ catalysts were prepared via the β-cyclodextrin-assisted impregnation method and were comparatively evaluated for dry reforming of methane (DRM) under the severe conditions of 750 °C, CH₄/CO₂ molar ratio of 1, and GHSV of 84 000 mL g^-1 h^-1. The addition of lanthanide oxide improves the Ni dispersion, the promotional effect of which is related to the type of lanthanide oxide used. The lanthanide oxide enhances the anti-sintering capacity of the modified catalysts, attributable to the confinement effect of the formed Ni-lanthanide oxide interface, which is dependent on the lanthanide oxide dispersion. All of the modified catalysts display a higher CH₄ activity than that of Ni-SiO₂ (145.1-248.7 mmol min^-1 g^-1 of Ni vs 61.6 mmol min^-1 g^-1 of Ni). However, Ni-La-SiO₂ and Ni-Ce-SiO₂ encounter rapid deactivation with k_d values of 0.095 and 0.051 h^-1 compared to Ni-SiO₂ (k_d = 0.058 h^-1), which is assigned to extreme loss of active Ni sites caused by serious sintering and/or an extensive decrease in the surface area. The catalytic stability of Ni-Nd-SiO₂ (k_d = 0.025 h^-1) and Ni-Sm-SiO₂ (k_d = 0.004 h^-1) is significantly improved compared to Ni-La-SiO₂, Ni-Ce-SiO₂, and Ni-SiO₂, and the best stability with a TOS of 70 h is achieved over Ni-Sm-SiO₂, which can be well-explained as the enhanced anti-sintering and anti-coking capacities as well as the stable textural property. The consecutive CH₄/CO₂-TPSR results vigorously prove that the addition of Sm₂O₃ simultaneously enhances the CH₄ decomposition and CO₂ dissociation while reducing the temperature difference of the two reactions, which results in a better balance between carbon generation and total gasification processes, and hence, the high activity and superior anti-coking capacity are achieved over Ni-Sm-SiO₂. The above understanding provides an important guidance for modulating the CH₄ and CO₂ activation to achieve the balance between carbon generation and gasification processes.

Heterotopic ossification (HO), the debilitating abnormal bone formation in soft tissues driven by complex inflammatory and osteogenic pathways, remains a major clinical challenge due to painful recurrence after surgery and the lack of effective, localized treatments circumvent systemic toxicity. Herein, we report a multifunctional electrospun nanofiber scaffold for sustained local delivery of ritonavir, revealing a previously underexplored role for this repurposed protease inhibitor in regulating mesenchymal lineage fate, osteogenesis, osteoclast activity, and immune signaling during HO progression. The scaffold sustainably released ritonavir for 28 days while maintaining high cell viability and mechanical integrity. Local ritonavir delivery suppressed chondrogenic differentiation by downregulating SOX9 and COL2A1 and biased cells toward a fibroblastic phenotype marked by elevated COL1A1 and α-SMA expression, disrupting the chondrogenic template required for ectopic bone formation. In parallel, ritonavir inhibits osteogenic differentiation, enhances osteoclast-mediated resorption, and promotes macrophage polarization toward an anti-inflammatory phenotype with reduced TNF-α and IL-6 secretion. In vivo, the ritonavir-eluting scaffold significantly attenuates ectopic bone formation in a tendon injury-associated HO model and promotes tendon functional recovery by providing mechanical stabilization to the injured tendon. Collectively, this work establishes localized ritonavir delivery as a multifunctional strategy integrating lineage control, bone remodeling regulation, and immunomodulation for HO prevention. This multifunctional therapeutic approach offers a clinically translatable solution for preventing aberrant bone formation and improving outcomes in trauma and orthopedic patients at risk of HO.

Electrochemical nitrogen reduction reaction (eNRR) under ambient conditions offers a promising route for ammonia synthesis, although it currently suffers from slow kinetics and competing hydrogen evolution. Transition metal nitrides (TMNs) enable efficient nitrogen activation via the Mars-van Krevelen mechanism; however, effectively suppressing nitrogen leaching under electrochemical conditions remains challenging. Here, we report a nanostructured ruthenium nitride (RuN) catalyst synthesized via magnetron sputtering, demonstrating its application for eNRR for the first time. Structural characterization confirms a zincblende-like RuN phase, while surface properties (i.e., roughness and wettability) are tuned by the deposition duration. The optimal catalyst achieved an ammonia yield of 3.0 × 10^-10 mol cm^-2 s^-1 at -0.3 V vs RHE and a Faradaic efficiency of 6.1% at -0.1 V vs RHE in a 0.1 mol L^-1 KOH electrolyte, surpassing most reported ambient TMN catalysts. These findings underscore the promise of metal nitride-based electrocatalysts and provide insights into the rational design of next-generation catalysts for sustainable nitrogen fixation.

Proton-conducting solid oxide fuel cells (PCFCs) represent a promising class of energy conversion technologies operating at intermediate to low temperatures. However, the development of efficient oxygen reduction reaction (ORR) catalysts remains a critical challenge for achieving practical performance in PCFCs. In this study, a series of K-doped Sr₂Fe_1.5Mo_0.5O_6-δ (SFM) perovskites with triple-conducting characteristics, synthesized through electrospinning into a nanofiber architecture, are presented as high-performance oxygen electrode materials. The SK30FM electrode demonstrates exceptional electrochemical performance, exhibiting a low polarization resistance of 0.062 Ω cm² under wet air (3% H₂O) at 750 °C, and delivering a peak power density of 645 mW cm^-2 with decent short-term stability during fuel cell operation. These results highlight the significant potential of SFM-based perovskites as advanced oxygen electrodes for PCFCs, while also underscoring the advantages of electrospinning in fabricating nanostructured functional materials.

Bacterial infected wounds pose a serious threat to human health. Developing a novel strategy that integrates real-time infection monitoring with exceptional antibacterial performance is urgent for advancing wound management. Herein, a multifunctional hydrogel (CMCS-PA@Fe/MUG hydrogels) integrating real-time infection diagnosis and therapeutic intervention capabilities has been successfully developed through the formation of Schiff bases between CMCS and PA@Fe solutions with the addition of 4-methylumbelliferyl β-d-glucuronide (MUG). The detection of the bacterial presence is achieved by visually monitoring the blue fluorescence emitted from 4-methylumbelliferyl (4-MU), which is produced through the enzymatic hydrolysis of MUG by pathogen-specific enzymes. In addition, the tissue adhesion and self-healing properties of CMCS-PA@Fe/MUG hydrogels enable them to seamlessly adapt to the mechanical demands of skin movement and stretching. Moreover, the combined photothermal activity of PA@Fe and the intrinsic antibacterial capability of chitosan endow the hydrogel with a superior antibacterial performance. The in vivo experimental results demonstrate that the hydrogel could effectively diagnose the infection status of a wound in real time and promote wound healing. Therefore, this advanced hydrogel sensor provides an innovative solution for infected wound management through real-time infection monitoring and efficient antibacterial strategies.

Rapid wound healing of oral soft tissue may reduce the opportunity for infection and discomfort of patients. Given that recombinant humanized collagen type III (rhCol III) is considered a nonallergenic biomaterial and can help repair skin wound healing and activate tissue remodeling, the potential effect of rhCol III on palate mucosal wound healing was preliminarily evaluated in vitro and in vivo in this study. A mouse model of an oral palate wound was established, and rhCol III solutions were injected periwound, resulting in a significant acceleration in wound healing compared to the control groups. Histological evaluation showed that rhCol III promoted angiogenesis, collagen deposition, and cell proliferation. Furthermore, the results demonstrated that rhCol III could promote human gingival fibroblast (HGF) and human oral keratinocyte (HOK) proliferation, adhesion, and migration. To further explore the mechanism, RNA-sequencing analysis results showed that rhCol III could regulate the focal adhesion signaling pathway of HGFs. The expression of vinculin and phosphorylation of FAK (Tyr397 and Tyr576) in HGFs was upregulated with rhCol III treatment. In addition, inhibition of FAK phosphorylation could inhibit HGF migration. These results suggested that rhCol III promoted HGF migration by upregulating the focal adhesion signaling pathway. These findings suggest that the topical application of rhCol III is a promising treatment for oral soft tissue wounds with the potential for future clinical use.

Ischemic stroke, a predominant cause of global mortality and disability, is characterized by a complex pathological cascade, following cerebral ischemia. Despite some progress in current conventional therapies and light-responsive nanosystems, there remains a lack of precise treatment strategies. Notably, the function of ion channels has attracted considerable attention due to its close association with the pathogenesis of ischemic stroke. Consequently, developing near-infrared (NIR)-responsive nanoplatforms for the targeted modulation of ion channels allows for a more precise treatment of ischemic stroke. Herein, a second NIR window (NIR-II) photothermal responsiveness nanoplatform (MNPs@Mi), camouflaged with a 4T1 cell membrane (CM) for targeted delivery, is designed to synergistically modulate microglial polarization and ion channel activity in the ischemic region. In a mouse model of distal middle cerebral artery occlusion (dMCAO), this integrated nanoplatform significantly shifts microglial polarization from the pro-inflammatory M1 to anti-inflammatory M2 phenotype, enhances neuronal survival, restores blood-brain barrier (BBB) integrity, and improves motor functional recovery. Quantitative analyses reveal a 2.3-fold increase in NeuN-positive cells and a 51.1% reduction in intracerebral IgG extravasation compared to those in the injury model group. Overall, this biomimetic NIR-II-responsive nanoplatform provides a noninvasive, spatiotemporally precise strategy for the treatment of ischemic stroke via the coordinated regulation of ion channels and microglial polarization.

Relaxor ferroelectric (RFE) films are highly desirable for modern electronic devices and power systems due to their ability to store and recycle electrostatic energy. However, achieving both the high energy density U_e and efficiency η simultaneously remains a significant challenge. Herein, lead-free 0.7BaTiO₃-0.3CeO₂ (BT-C) RFE films with a simple chemical composition (containing only four elements of Ba, Ti, O, and Ce) were developed to modulate energy storage performance via tailoring polarization behavior. The (110)-oriented BT-C films show a high energy storage density U_e of 42.7 J/cm³, with an ultrahigh efficiency η of 93.1% at room temperature, which can be attributed to the improved polarization response and suppressed hysteresis. Moreover, these BT-C films exhibit exceptional frequency stability (2 Hz to 5 kHz) and thermal stability (25-120 °C), along with reliable operation endurance (>10⁶ cycles) without performance degradation. The orientation control strategy, combined with polymorphic nanodomains, offers a promising approach for developing high-performance lead-free energy storage materials, indicating their great potential for practical power-storage applications.

The human skin possesses the capability to detect thermal and mechanical stimuli simultaneously. Ingenious flexible sensors have been explored to mimic such functionalities by integrating multiple sensing elements or adopting multimodal sensing principles. However, the widespread application of these sensors has faced obstacles such as complicated manufacturing processes, signal mismatches between different components, and high power consumption. Here, we report a single-mode self-powered flexible sensor capable of simultaneously detecting both temperature and pressure stimuli through the seamless integration of complementary and compatible thermoelectric and triboelectric sensing mechanisms. The resulting hybrid thermoelectric-triboelectric sensor exhibits unique features that are difficult to achieve with existing approaches, including single-mode output (voltage signal only), significantly simplified operation (single-measurement device), ultralow power consumption, adaptive response behavior, and excellent discriminative capability for complex stimuli. Additionally, a deep learning regression model has been implemented to dispose of the single-mode signals, achieving an impressive accuracy of 94.7% in distinguishing contact objects. This work presents an innovative design that substantially simplifies both fabrication and operation while simultaneously enhancing the functionality and energy efficiency of next-generation flexible sensing systems.

As dynamic random-access memory (DRAM) technology continues to scale down to sub-10 nm nodes, achieving high memory density and enhanced operational performance poses increasing challenges. In particular, maintaining sufficient cell capacitance and minimizing the leakage current density have emerged as key issues. To address these issues, the development of novel electrode materials and carefully engineered interfaces between high-k dielectrics and electrodes is crucial. In this study, thermal atomic layer deposition (ALD) of Sn-incorporated MoO_x (TMO) films was performed using (N^tBu)₂(NMe)₂Mo and Sn(dmamp)₂ as the Mo and Sn precursors, respectively. The growth characteristics of the TMO films, particularly the interaction between the MoO_x and SnO_x subcycles, were systematically investigated. Controlled Sn incorporation into MoO_x successively stabilized the formation of the monoclinic MoO₂ phase, resulting in a smooth surface morphology and enhanced thermal and chemical stability. ALD TMO films were employed as an interface control layer (ICL) in a metal-insulator-metal capacitor to improve the interfacial properties between the (Al-doped) TiO₂ and TiN bottom electrodes. ALD TMO films promoted the in situ crystallization of rutile TiO₂ (with a dielectric constant of up to 156) and effectively suppressed the unwanted formation of a low-k TiO_xN_y layer, resulting in significant equivalent oxide thickness (EOT) scaling. Furthermore, the insertion of the TMO ICL significantly reduced the leakage current density of the (Al-doped) TiO₂ films, which was attributed to the higher work function of TMO (4.7-4.8 eV) compared to that of TiN (4.5 eV) and the minimal formation of defective TiO_xN_y. To evaluate the scalability of the ALD TMO ICL, its thickness was varied from 20 to 1 nm. Remarkably, even at the ultrathin thickness of 1-2 nm, TMO ICL maintained high capacitance and low leakage current density, achieving an EOT of 0.58 nm and leakage current density of 2.4 × 10^-7 A/cm². These results highlight the potential of ALD-grown TMO films as ICLs in next-generation DRAM capacitors.