ACS Applied Materials & Interfaces最新文献

Since the development of lithography technology, photoresist has mainly been processed using a solution method. However, with the continuous miniaturization of process nodes, especially in high-NA EUV lithography processes that require photoresist with a thickness of less than 20 nm, the solution method also faces problems such as precise thickness control and pattern collapse due to capillary action during wet development. Therefore, we used tetrakis(dimethylamido)hafnium (TDMAHf) and 2-buten-1,4-diol (BED) to prepare a Hf-based hybrid thin film as a high-resolution dry photoresist using the molecular layer deposition (MLD) method. Based on this hafnium-based photoresist, we developed two development methods, which resulted in positive and negative dual-type photoresists. We employed inductively coupled plasma etching (ICP) for dry development, resulting in a positive photoresist; and 15% tetramethylammonium hydroxide (TMAH) for wet development, resulting in a negative photoresist. We used electron beam exposure for resolution testing. At a voltage of 25 keV, the sensitivity was 2400 μC/cm². At a voltage of 50 keV, the resolution of dry development could reach 20 nm, while that of wet development could reach 7 nm. Our research results indicate that hafnium-based hybrid photoresists have great potential for use and provide reliable support for the development of more advanced dry photoresists.

Solar-driven electricity generation enables autonomous wearables. Enhancing wearable solar thermoelectric generator (STEG) efficiency requires broadband photothermal materials for synergistic optical and thermal energy concentration. To enhance photothermal performance, we developed a strategy to modify the intramolecular charge transfer capacity by adjusting the ligand charge density. Density functional theory calculations show that this manipulation of the ligand charge density reduces the band gap, resulting in narrow band gaps of 0.715, 0.351, and 0.210 eV for the three coordination polymers (CPs), respectively. This improves solar light absorption and photothermal conversion. Under 1-sun irradiation, the maximum temperature of Cu-BTA (BTA = 1,2,4,5-benzenetetraamine tetrahydrochloride) can reach approximately 70.9 °C. Furthermore, after incorporating Cu-BTA into a photothermal film, the film can reach 74.6 °C under irradiation with 1 sun. Importantly, coating the thermoelectric device with the photothermal film enables it to generate a voltage of 98.2 mV under irradiation with 1 sun. Furthermore, the integrated system reflects changes in human body temperature through voltage changes, enabling real-time health monitoring. This work offers a new way for exploring potential applications in wearable devices.

Fabrication of water-dispersible plasmonic gold nanoparticle vesicles (GNVs) by using small-molecule surface ligands for biological applications still remains a significant challenge. In this paper, we demonstrate that a tri(ethylene glycol) terminated octafluoro-4,4'-biphenol ligand (TrOFBL) can self-assemble with 5 or 10 nm gold nanoparticles into hollow-structured GNVs in tetrahydrofuran (THF). After the GNVs are transferred from THF to an aqueous solution, these single-layered plasmonic GNVs remain stable and dispersible. The precise control of the balance between hydrophilic and hydrophobic effects of the small-molecule ligand leads to the stabilization of the GNVs in water. The GNVs can encapsulate a hydrophobic anticancer drug in the interior with a high loading efficiency of 74%. Upon irradiation with a red laser (650 nm), the accumulative release of the drug can reach up to 99% due to the destruction of GNVs induced by local heating. Cellular assays confirm that the GNVs are efficiently internalized by cancer cells and release the drugs upon laser irradiation to induce cytotoxicity. In vivo anticancer result shows that the laser-triggered drug release effectively inhibits tumor growth after irradiation without noticeable systemic toxicity, making them suitable for in vivo tumor therapy.

Pulsed electrolysis is widely regarded as a promising strategy for enhancing the performance of the electrocatalytic nitrate reduction reaction (NO₃^-RR). However, research on the effect of symmetric and asymmetric pulsed electrolysis on the NO₃^-RR remains elusive. Here, the CuMn alloy serves as a model catalyst to systematically investigate the impact of symmetric and asymmetric pulsed electrolysis on the performance of NO₃^-RR. A series of operando measurements and control experiments indicate that a suitable asymmetric pulsed electrolysis can optimize the local microenvironment of the NO₃^-RR, including optimizing the coverage of NO₃^-, enhancing the generation of key N-containing intermediates, and inhibiting the hydrogen evolution reaction, thereby improving the Faradaic efficiency and yield rate of NH₃. Consequently, the Faradaic efficiency and yield rate of NH₃ for the optimal asymmetric pulsed electrolysis between a less negative potential time of 2 s and a more negative potential time of 4 s are 94.03% and 9.13 mg h^-1 cm^-2, respectively, which are 1.42-fold and 2.10-fold higher than those of static electrolysis. Moreover, the Faradaic efficiency of NH₃ for the optimal asymmetric pulsed electrolysis was 66.32% at a lower concentration of NO₃^- (2000 ppm), which is 1.73-fold higher than that of static electrolysis, indicating that the performance of asymmetric pulsed electrolysis is further enhanced in the lower concentration of NO₃^-, further confirming that asymmetric pulsed electrolysis is a feasible strategy to improve the performance of the NO₃^-RR.

Adhesives with excellent adhesion properties are crucial for aquatic activities. However, natural dynamic water can lead to the loss of adhesive molecules and a reduction in adhesion strength. In this work, we propose a unique phase-separated underwater adhesive through the copolymerization of hydrophilic and hydrophobic monomers. The hydrophobic groups repel interfacial water, while the hydrophilic groups form strong bonds with substrates, endowing the adhesive with outstanding adhesion. Moreover, the adhesive exhibits unique self-reinforcing properties in dynamic water. The self-reinforcement is realized through dynamic water-accelerated phase separation kinetics of the adhesive. The dynamic water forms a dense surface of adhesive, reducing adhesive loss and increasing the bonding area. The adhesion strength in dynamic water significantly increases, reaching 1.97-fold of that in static water. In addition, the adhesive demonstrates excellent adaptability and maintains strong adhesion in various water environments. Benefiting from its linear structure and good solubility, the adhesive exhibits recyclability and erasability, which promotes sustainable chemistry and utility. The recycled adhesive retains 95% of its original adhesive strength without obvious damage. The adhesive demonstrates practicality and accessibility in applications such as tube repair and leakage sealing. Overall, this work provides insights into the design and preparation of novel self-reinforcing underwater adhesives.