ACS Applied Materials & Interfaces最新文献

Developing adsorbents that couple high uranium affinity with durability in complex environments remains a pivotal challenge for efficient uranium harvesting. Here, we report a hierarchically engineered magnetic composite, Fe₃O₄@PAO@MPN-Met, that integrates (i) a superparamagnetic Fe₃O₄ core for rapid separation, (ii) an amidoxime-rich polyamidoxime (PAO) shell for uranyl chelation, (iii) a bioinspired metal-polyphenol network (MPN) adhesive layer, and (iv) an in situ mineralized Cu²⁺/d-methionine (d-Met) metal-organic framework (MOF) that imparts long-lasting antibiofouling activity. Stepwise solvothermal synthesis, surface grafting, and self-assembly preserve nanoscale morphology while reducing the saturation magnetization only to 16.4 emu/g─still sufficient for 1 min magnetic separation. Under optimal conditions, the material achieves a maximum uranium uptake of 272 mg/g, fitting the Langmuir model and quasi-second-order kinetics, indicative mainly of monolayer chemisorption controlled. Thermodynamic analysis reveals a spontaneous, endothermic, and entropy-driven process. The composite shows outstanding selectivity, with uranyl distribution coefficients at least 2 orders of magnitude higher than those of competing ions. After five adsorption-desorption cycles using 0.1 M HNO₃, 80% of the initial capacity is retained. Crucially, the Cu-Met nanochannels confer broad-spectrum antibacterial performance, suppressing Pseudomonas aeruginosa formation by 98.54%. In natural Bohai Sea water, after 7 days of adsorption, the uranium adsorption capacity is 0.322 mg/g, highlighting its salt tolerance and antifouling resilience. This multifunctional design, marrying strong amidoxime chelation, magnetic recoverability, and MOF-mediated antibacterial action, offers a viable route toward selective, reusable, and biofouling-resistant adsorbents for large-scale uranium harvesting from seawater.

Ionically bonded interfaces are crucial for achieving selective and stable direct seawater electrolysis, yet their vulnerability under corrosive and high-current conditions limits long-term performance. Here, we report a two-dimensional Fe-MOF@PW₈O₂₆.B₂O₃ heterostructured electrocatalyst, synthesized via a solid-liquid interfacial growth strategy, that integrates robust Fe-O-W and tunable Fe-P-W ionic bonds to strengthen interfacial electronic coupling, redox flexibility, and structural integrity. Subsurface B₂O₃ enhances surface hydroxylation via Lewis acid-base interactions, facilitating catalyst assembly and OH^- affinity, while phosphate polyanions at the interface act as electrostatic shields that repel Cl^- ions and modulate the redox environment of Fe active sites. This interfacial configuration enables chlorine-suppressive oxygen evolution with a Faradaic efficiency of 97.93%, achieving a current density of 1.75 A cm^-2 at 2.0 V and stable operation above 1.5 A cm^-2 for over 500 h in alkaline seawater, with an exceptionally low corrosion rate of 0.016 μm per year. NEXAFS and XPS analyses confirm the presence of dual ionic linkages, while DFT calculations reveal their cooperative role in stabilizing the electronic structure and interfacial charge distribution. Beyond hydrogen production, the spent electrolyte is repurposed for CO₂ mineralization, achieving 88.76% conversion to stable carbonates, with cytotoxicity assays confirming reduced environmental toxicity. Together, this study establishes a multifunctional ionically engineered platform for durable, chlorine-free seawater electrolysis and integrated carbon capture, advancing the prospects of circular hydrogen systems.

A promising method for directing cell behavior and tissue regeneration is the use of smart materials that can transform physical inputs into bioelectrical signals. In this study, the mechanoelectrical control of preosteoblast activity was investigated using a piezoelectric smart biointerface based on positively poled poly(vinylidene fluoride) (PVDF). Distinct mechanical regimes, including vibrational and cyclic stretching, were applied through customized bioreactors, enabling controlled mechanoelectrical inputs ranging from 63 to 227 μVpp mm^-2. The biological response of MC3T3-E1 cells was evaluated in terms of metabolic activity, intracellular calcium signaling, alkaline phosphatase (ALP) activity, matrix mineralization, and gene expression (RUNX2, ALP, OPN, and OCN). The results demonstrated that stretching stimulation combined with higher mechano electric inputs (113-227 μVpp mm^-2) enhanced calcium influx and enhanced osteogenic differentiation, while lower impulses (∼63 μVpp mm^-2) under vibrational circumstances increased cell proliferation. These findings highlight the intensity- and mode-dependent nature of mechanoelectrical signaling in regulating osteogenic commitment. All things considered, this study shows how piezoelectric smart materials can be used as bioresponsive platforms to precisely control cell proliferation and differentiation, creating avenues for bone tissue engineering's next-generation regenerative techniques.

The pursuit of durable and eco-friendly antifouling surfaces has become a critical challenge across engineered systems, ranging from architectural coatings to marine infrastructure. Herein, we propose an innovative stepwise physicochemical antifouling mechanism through the rational integration of hierarchical superamphiphobic architectures with bactericidal copper oxide nanoparticles. The designed coating operates via a sequential defense protocol: physical antiadhesion enabled by a superamphiphobic surface exhibiting ultralow surface energy, coupled with a chemical antibacterial effect through controlled Cu²⁺ ion release from embedded CuO nanoparticles. When the action time reaches 24 h, the coating shows excellent antibacterial effects against Gram-negative Escherichia coli (E. coli), Pseudomonas aeruginosa (P. aeruginosa), and Gram-positive Staphylococcus aureus (S. aureus). A scalable spray-coating technique was developed using 3-aminopropyltriethoxysilane (APTES)-functionalized CuO/SiO₂ nanocomposites with 1H,1H,2H,2H-perfluorodecyltriethoxysilane (PFDTES) modification for the coating fabrication. Systematic characterization combining Cassie-Baxter modeling, X-ray Photoelectron Spectroscopy (XPS) analysis, and bacterial viability assays confirms the mechanistic coupling between topographical liquid repellency and chemical bactericidal activity. The contact angle (CA) value of CuO-SiO₂/APTES@PFDTES calculated by dynamic density functional theory (DDFT) is 165.5°. This work provides a promising strategy for the rational design of advanced superamphiphobic antifouling coatings through physicochemical antibacterial strategies.

Rational design of efficient and robust electrocatalysts for the oxygen evolution reaction (OER) is essential for advancing electrochemical water splitting systems. In this work, we report an Fe-incorporated NiCo layered double hydroxide (NiCoFe-LDH) nanosheet array grown directly on three-dimensional (3D) nickel foam via a facile hydrothermal route. Among the various compositions investigated, optimized NiCoFe-LDH exhibits significantly enhanced OER activity, delivering a low overpotential of 215 mV at 100 mA cm^-2 and maintaining long-term catalytic stability. Structural and compositional analyses reveal that Fe incorporation induces a distinct electronic modulation: Fe doping downshifts the d-band center, which weakens the adsorption of key OER intermediates such as *O and lowers the reaction energy barrier for the rate-determining step, thereby accelerating OER kinetics. Bader charge analysis and the crystal orbital Hamilton population further support weakened metal-oxygen bonding upon Fe substitution. The combined modulation of the local electronic structure and active site configuration provides clear mechanistic insight into the origin of the enhanced OER activity, presenting an effective design strategy for developing transition metal-based electrocatalysts with high OER performance.

Radiative cooling is a passive cooling technology that could potentially address critical sustainability challenges by improving energy efficiency across different applications, including building materials, coatings, electronics, and outdoor devices. Photonic radiative coolers are a discrete category that utilizes photonic structures to optimize the emission properties of the material in the atmospheric transparency window (ATW) regime (8-13 μm). Due to their efficiency and adaptive nature, photonic radiative coolers offer a promising avenue as an adaptable cooling technology. However, a major challenge in transitioning this technology from laboratory to practical use remains. To address this barrier, large area, scalable and low-cost methods and materials need to be implemented. In this study, we demonstrate the fabrication of a transparent microstructured polymer-based radiative cooling (MPRC) film using nanoimprint lithography with a hybrid organic-inorganic UV-curable resist, namely, Ormocomp. We report the optical properties of Ormocomp within the atmospheric transparency window, which had not been previously characterized and utilize them to reveal the underlying mechanisms leading to emissivity enhancement. The MPRC film has over 90% transmission in the visible-NIR wavelengths and provides an─above ambient─cooling effect of -3 °C compared to bare Si reference sample under direct sunlight even though the solar absorptivity of silicon is lower. Our suggested design and fabrication approach is suitable for applications that need optical transparency or can be paired with reflective substrates to further enhance cooling performance, offering a practical and scalable radiative cooling solution.