ACS Applied Materials & Interfaces最新文献

Atherosclerosis is driven by metabolic dysregulation, particularly aberrant cholesterol accumulation and impaired nitric oxide (NO) signaling. However, most therapeutic strategies address these abnormalities separately, while biomaterials capable of translating pathological metabolic dysregulation into localized biochemical regulation remain limited. Herein, we report MMCoac@ChOx/HRP, a macrophage membrane-camouflaged coacervate microreactor formed via liquid–liquid phase separation (LLPS). The microreactor features a macromolecularly crowded core self-assembled from poly(diallyldimethylammonium chloride) and sulfobutylether-β-cyclodextrin, which enables cholesterol recognition and enrichment of cholesterol oxidase (ChOx) and horseradish peroxidase (HRP). These co-encapsulated enzymes achieve high enrichment efficiencies of 87.5 and 92.1%, respectively, to drive cholesterol oxidation and subsequent NO generation. In simulated body fluid, MMCoac@ChOx/HRP depleted cholesterol levels from 5.0 to 2.9 ± 0.4 mM and generated 12.1 ± 0.8 μM NO within 12 h. In vitro, it significantly attenuated macrophage foam cell formation and promoted endothelial repair. Furthermore, following systemic administration in ApoE^–/– mice, MMCoac@ChOx/HRP preferentially accumulated in atherosclerotic aortic plaques, enhanced in situ NO generation, and reduced aortic plaque burden from 27.4 ± 4.5 to 8.2 ± 3.0%. Overall, this study demonstrates a localized metabolic intervention strategy driven by an LLPS-based microreactor. This versatile biomaterial platform effectively modulates the plaque microenvironment, holding great potential for therapeutic interventions against metabolic syndrome.

Insufficient Li⁺ transport kinetics and poor interfacial stability hinder the practical application of polyethylene oxide (PEO)-based solid-state electrolytes (SSEs) in all-solid-state lithium metal batteries. In this work, we propose iodine-induced charge transfer of a covalent organic framework (COF) as an effective strategy to achieve fast ion transport and a stable SSE/Li interface. First, the electron-deficient COF skeleton in the I₂/COF charge-transfer complex anchors TFSI^- anions through enhanced electrostatic interactions, thereby promoting the dissociation of lithium salt to release free Li⁺. Second, the electron deficiency of COF strengthens its dipole–dipole interactions with PEO, leading to suppressed PEO crystallization and enhanced COF/PEO compatibility. Third, the electron-deficient COF tailors the Li⁺ coordination environment via weakening the affinity of PEO and COF toward Li⁺. Consequently, the I₂/COF charge-transfer complex accelerates Li⁺ transport kinetics in PEO-based composite SSEs. Furthermore, the confinement effect of COF toward I₂ via charge transfer effectively inhibits the aggressive lithium anode corrosion by I₂, resulting in the controlled growth of a stable, robust, and conductive solid electrolyte interface (SEI) rich in LiF and LiI. Thus, the I₂/COF charge-transfer complex enables excellent rate capability and cycling stability of the resulting COF/PEO-based composite SSE, maintaining a capacity retention of 88.58% after 1000 cycles at 2 C. This work offers a promising strategy for designing COF/PEO-based composite SSEs for next-generation all-solid-state lithium metal batteries.

Interfacial quality at the SnO₂ electron transport layer (ETL)/perovskite junction critically governs the electron collection and device performance in n-i-p type perovskite solar cells (PSCs). However, the defects within SnO₂ and at the buried interface can impede electron extraction and promote charge recombination. Herein, cesium hexafluorophosphate (CsPF₆) was introduced into the SnO₂ precursor as an interfacial additive. Calculations and experimental measurements indicate that the F atoms of PF₆^– coordinate with undercoordinated Sn sites, whereas Cs participates in the formation of an FA-Cs alloyed layer at the buried perovskite surface. These interactions establish a molecular bridge across the SnO₂/perovskite junction. The resulting bridge suppresses the interfacial defects, improves the energy-level alignment and physical contact, and regulates the perovskite crystallization. The devices incorporating CsPF₆ deliver a champion power conversion efficiency (PCE) of 24.25%. They also show enhanced stability. The unencapsulated devices retain 90.05% of their initial PCE after 1000 h of aging in ambient air. These findings demonstrate that molecular bridging is an effective route to simultaneously improve the efficiency and stability of PSCs.

The chronic recurrence of psoriasis is driven by a self-amplifying inflammatory cascade in which oxidative stress and mitochondrial metabolic dysfunction reinforce each other, and single-target conventional therapies often fail to break this cycle. Here, we present a micro–nano hybrid system, Mito-Ce, constructed by covalently immobilizing ceria nanozymes (CeNPs) onto the surface of isolated functional mitochondria through thiol–maleimide chemistry. This design endows the hybrid with dual functionalities, including mitochondrial bioactivity and durable ROS-scavenging capabilities of CeNPs. In H₂O₂-stimulated macrophages, upon internalization. Mito-Ce markedly reduced intracellular ROS and consequently suppressed the secretion of pro-inflammatory cytokines (IL-6, TNF-α, and IL-1β). Topical application of Mito-Ce to an imiquimod-induced mouse model of psoriasis visibly resolved psoriatic plaques, reduced the PASI score, and reversed epidermal hyperplasia. Beyond local repair, Mito-Ce rebalanced systemic immunity, evidenced by a decline in splenic pathogenic Th17 cells and polarization toward anti-inflammatory M2 macrophages. Transcriptomic profiling further revealed that Mito-Ce broadly reversed the pathological gene expression program, downregulating stress-responsive and phagocytosis-related genes while upregulating genes associated with metabolism, epidermal proliferation, and tissue homeostatic remodeling. These coordinated networks ultimately re-established immune–barrier homeostasis at the molecular level. Collectively, by integrating nanozyme-mediated ROS scavenging with mitochondrial bioactivity, the Mito-Ce hybrid could treat psoriasis through coordinated disruption of the inflammatory cascade, potentially offering a highly effective platform for various chronic inflammatory disorders.

Developing efficient, low-cost, multifunctional additives that require small amounts and can simultaneously protect both the cathode and anode remains a major challenge for the practical application of lithium batteries. Herein, bis(2,4-dimethylpentane-2,4-glycolato)diboron (B₂hmp₂) was introduced to construct a greatly Li⁺-conductive cathode electrolyte interphases (CEIs) at the LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) surface together with robust solid electrolyte interphases (SEIs). Using a common electrolyte with 0.2 wt % B₂hmp₂, the Li||Li cells deliver markedly enhanced long-cycling stability, sustaining stable operation for 500 h at 0.5 mA cm^–2. Furthermore, following 350 cycles at 0.5 C, the capacity retention of 4.5 V Li||NCM811 cells was elevated from 57.2 to 83.6%. Experimental results reveal that the thin, uniform, boron-rich CEI generated by B₂hmp₂ effectively mitigates particle microcracking and restrains the dissolution of transition metal ions. Interface analysis reveals that the modified SEI film enriched with B–O species and LiF facilitates uniform Li plating/stripping without dendrite formation and reduces the continuous parasitic decomposition of electrolyte solvents. This article highlights the value of trace diboron for forming desirable electrolyte interphases to obtain the wonderful long-term cycle performance and rate performance of Li||NCM811 cells.

Solid-state sodium metal batteries are promising candidates for grid-scale energy storage due to their inherent safety and low cost. However, the development of solid electrolytes that support high-rate (>20 C) cycling for fast-charging applications remains a major challenge. Herein, we explore how adding SiO₂ affects the ionic conductivity and dendrite suppression of NaB₃H₈, to develop superior solid electrolytes for high-rate batteries. The composites featuring an amorphous passivating layer with B–O bonds were fabricated via ball milling. Among them, NaB₃H₈-40%SiO₂ exhibits the best conductivity, reaching 0.62 mS cm^–1 at 25 °C, 2 orders of magnitude higher than that of pristine NaB₃H₈. Crucially, by reducing electronic conductivity and enhancing mechanical strength, it possesses a high critical current density of up to 6.5 mA cm^–2, significantly higher than that of other reported hydridoborates. The Na/NaB₃H₈-40%SiO₂/TiS₂ batteries exhibit superior rate capability (216.4 mAh g^–1 at 1 C and 143.1 mAh g^–1 at 20 C) and long-term cycling stability (nearly 100.0% capacity retention after 2000 cycles at 20 C) at 30 °C. This work offers a promising approach for the development of innovative solid electrolytes in fast-charging or high-power-density sodium metal batteries.

Head and neck squamous cell carcinoma (HNSCC) remains difficult to treat, and conventional chemotherapy has limited efficacy and substantial toxicity. We developed a VYQFF peptide-modified brucine liposome (Bru-VYQFF-Lip) and characterized its particle size, zeta potential, polydispersity, encapsulation efficiency, and drug loading. Bru-VYQFF-Lip showed greater uptake in Trop2-high HSC3 cells than in HOK cells and inhibited HNSCC-cell proliferation, migration, and invasion while promoting apoptosis. After intratumoral administration, the VYQFF-modified formulation showed greater local fluorescence retention than the NHS-bearing, non-peptide comparator; this experiment does not establish systemic tumor targeting or direct Trop2-specific recognition. Bru-VYQFF-Lip also suppressed tumor growth in a nude-mouse xenograft model. Terminal serum chemistry and organ histology did not reveal overt hepatorenal or histopathological injury, although the safety assessment was limited by the absence of complete longitudinal and hematological evaluation. Bioinformatic and experimental analyses identified INHBA as a candidate mediator associated with poor prognosis. Mechanistic experiments were consistent with suppression of the INHBA/TGF-β/Smad axis and epithelial-mesenchymal transition. These findings support further evaluation of VYQFF-functionalized brucine liposomes, including physicochemically matched controls, receptor-blocking studies, systemic biodistribution experiments, and comprehensive toxicology.

Dendritic formation and parasitic interfacial reactions occurring on the zinc anode remains a major obstacle to the commercialization of aqueous zinc-ion batteries. Rational electrolyte additive design offers an effective route to move beyond single-function regulation toward synergistic multimechanism control. Compared to multicomponent systems, single-molecule additives with multiple functional groups enable integrated control over solvation structure and interfacial chemistry while reducing complexity and cost. Herein, the natural amino acid hydroxyproline (hyp) is introduced as a multifunctional electrolyte additive for simultaneous regulation of the Zn²⁺ solvation and interfacial chemistry. The −COOH and −OH groups reconstruct the solvation sheath and hydrogen-bond network, while the −NH− group promotes interfacial adsorption and induces a compact, N-rich interphase that homogenizes Zn²⁺ flux and suppresses dendrite growth. Benefiting from this cooperative solvation−interphase regulation, stable Zn plating/stripping is achieved for over 2000 h in Zn//Zn cells, an average coulombic efficiency of 99.79% is maintained over 1500 cycles in Zn//Cu cells, and Zn//LiFePO₄ full cells deliver a capacity of 154 mAh g⁻¹ over 500 cycles at 0.2 A g⁻¹. This work highlights single-molecule, multifunctional electrolyte additive engineering as a rational, scalable strategy for durable, safe aqueous zinc batteries.