ACS Applied Materials & Interfaces最新文献

Immunotherapy shows promise for triple-negative breast cancer (TNBC), yet its effectiveness is restricted by low response rates, poor immune cell infiltration, and systemic side effects. Here, an ultrasound-responsive cerasomal nanoplatform integrating a STING agonist (SR-717@PC-iRGD) is developed for synergistic sonodynamic-immunotherapy. The nanocarrier is self-assembled from cerasome-forming lipids (CFL), porphyrin-conjugated lipids (PL), unsaturated phospholipids (DOPC), DSPC, and DSPE-PEG₂₀₀₀-iRGD, with SR-717 loaded in the lipid bilayer. The resulting assembly yields nanoparticles (NPs) with high SR-717 loading and exceptional stability. The siloxane shell (cerasome) confers high stability and prevents premature drug leakage, while iRGD promotes nanoparticle binding to tumor specific integrin to facilitate accumulation and retention in the tumor. Upon ultrasound irradiation, porphyrin generates reactive oxygen species (ROS) that oxidize the lipid bilayer and disrupt the cerasome, enabling on-demand SR-717 release at tumor site. The released SR-717 activates the STING pathway, driving type-I interferon production, dendritic cell maturation, and CD8⁺ T-cell infiltration. This strategy integrates sonodynamic therapy (SDT) with localized immune activation, addressing challenges of instability and inefficient delivery. The platform thus offers a precise and effective approach to stimulate antitumor immunity and enhance therapeutic outcomes for TNBC where no tumor targeted therapy is currently available.

Supercapacitors, particularly porous carbon-based electric double-layer capacitors (PC-EDLCs), are crucial for next-generation energy storage but face limitations in capacitance enhancement and microstructure manipulation. Conventional carbonization-activation methods suffer from energy inefficiency, poor pore structure regulation, loss of functional groups, and inability to create optimal conducting-adsorption hybrid structures. This study presents a novel, tunable one-step thermal synthesis strategy based on the self-activation reaction of potassium carboxylate precursors. A precarbonization step is induced to enrich the oxygen-containing functional groups at the porous carbon surface, followed by activation at 800 °C. While this pretreatment reduces the specific surface area, it significantly increases the specific capacitance to 279 F g^-1 by introducing substantial pseudocapacitance and optimizing the conductivity of the carbon skeleton. The resulting carbonylated porous carbon exhibits outstanding supercapacitor performance, with a high capacitance retention of 93% after 10,000 cycles and an energy density of 12.8 Wh kg^-1. This work offers an efficient, energy-saving, and structurally tunable pathway for preparing high-performance porous carbon materials.

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.