ACS Applied Materials & Interfaces最新文献

Pitch-based hard carbon (HC) materials at low cost and high carbon yield represent a promising anode for sodium-ion batteries. However, their limited capacity poses a significant challenge to their practical use. Here, we report a universal strategy to boost sodium storage of pitch-based HC materials via catalytic oxidation with magnesium oxide to produce a high-oxygen pitch. The oxygenic groups suppress pitch softening and molecular rearrangement during carbonization, resulting in a highly disordered structure and substantially closed pores in the obtained HC materials. As a result, the optimized HC materials achieve a specific capacity of 321.7 mAh g^-1 with a significant 80.5% increase over typical pitch-based carbon materials, along with a high initial Coulombic efficiency up to 88.5 and 88.3% capacity retention after 600 cycles. This study provides new insights into the rational design of high-capacity pitch-based HC and holds potential for application in other carbon-based materials.

Exciplex, as one of the important categories of thermally activated delayed fluorescence (TADF), has long been hindered from widespread application due to the lack of stable exciplex-based organic light-emitting diodes (OLEDs). Here, we introduce stable donor molecules to improve exciplex-based OLED stability, utilizing components diindolo[3,2,1-de:3',2',1'-kl]phenazine (DIPz) derivatives, N⁵,N¹³-bis(4-(tert-butyl)phenyl)-2,10-dimesityl-N⁵,N¹³-diphenyldiindolo[3,2,1-de:3',2',1'-kl]phenazine-5,13-diamine (BDDPD) as the donor and triazine derivatives, 3-(9-(3-(4,6-diphenyl-1,3,5-triazin-2-yl)phenyl)dibenzo[b,d]furan-2-yl)-9-phenyl-9H-carbazole (DPTBF-PhCz), 2-(3'-(9,9'-spirobi[fluoren]-2-yl)-[1,1'-biphenyl]-3-yl)-4,6-diphenyl-1,3,5-triazine (Spiro-BDTA), 2,4-diphenyl-6-(3'-(triphenylen-2-yl)-[1,1'-biphenyl]-3-yl)-1,3,5-triazine (DTBTA), as the acceptors. These exciplexes exhibit high photoluminescence quantum yield (PLQY) and reverse intersystem crossing (RISC) rates. As a result, the exciplex-based OLEDs achieve a maximum external quantum efficiency (EQE) of 17.19% while also demonstrating a low efficiency roll-off. Even at a brightness of 1000 cd m^-2, the EQE can still maintain 16.36%. A stable exciplex-based OLED achieves an LT₅₀ of over 1000 h at 1000 cd m^-2, which is one of the best device lifetimes of exciplex-based OLEDs. These exciplexes can not only function as TADF emitters but also act as the host material to sensitize red fluorescent molecules. Red fluorescent OLEDs utilizing developed exciplexes as the host material achieve a high EQE of over 15%, with reduced efficiency roll-off. This research paves the way for a new strategy for the development of efficient and stable exciplex-based OLEDs.

Accurate and early tumor diagnosis is critical for effective cancer treatment, yet current diagnostic modalities often face limitations. Fluorescence imaging (FLI) and magnetic resonance imaging (MRI) both offer substantial potential for cancer diagnosis. However, FLI suffers from poor tissue penetration, while MRI lacks molecular specificity. To address these limitations, we proposed a dual-modal diagnostic strategy by combining FLI and MRI for precise photodynamic therapy (PDT) of tumors. A degradable tumor microenvironment (TME)-responsive nanoplatform, i.e., UCNPs-MB@MnO₂-H1/H2 (UBMD), was developed. Intracellular overexpression of miRNA-21 triggers an in situ hybridization chain reaction between H1-TAMRA and H2-FAM, which significantly amplifies fluorescence resonance energy transfer and enables FLI of miRNA-21 in living cancer cells. On the other hand, UBMD activates MRI in the TME to remarkably amplify tumor MRI signals and to effectively compensate for the shortcoming of weak penetration of FLI in deep tissues. UBMD exhibits an NIR-activated PDT capability to enable tumor-specific in situ diagnostics and imaging. In vivo miRNA-21 FLI and MR imaging in living mice actively guide precise and efficient PDT of tumors.

Herein, the potential use of amine-functionalized cellulose as a low-cost and sustainable sorbent for CO₂ capture is reviewed. This literature analysis specifically highlights various advanced preparation methods used to synthesize functionalized cellulose supports with an enhanced affinity for the sorption of CO₂ molecules. The mechanism of cellulose functionalization with different types of amines is explicitly detailed, considering amine impregnation and grafting to selectively chemisorb CO₂ gas with or without the presence of moisture and at different temperatures and pressures. The final section critically discusses the main limitations to scaling up amine-functionalized cellulose sorbents, particularly issues related to amine oxidation, stability, and degradation.

Passive radiative cooling presents great potential to reduce global energy consumption owing to its sustainable features of zero energy consumption and zero CO₂ emission. Natural silk fibers exhibit a reflective sheen and a triangular cross-sectional morphology, similar to the attributes observed in the Saharan silver ants' hairs that function to protect the ants from overheating under extremely hot conditions. Here, we demonstrate the facile construction of hair-like arrays of short silk fibers (SSFs) through electroflocking, and the efficient passive cooling performance realized by the enhancement in both the reflectance in the visible to near-infrared range and the emittance in the mid-infrared range. The hairy SSFs flocked on a transparent PDMS film can reduce the temperature of a substrate, on which the film is coated, by 7.6 °C relative to a bare PDMS film when exposed to solar radiation. When flocked on common cotton fabric, the SSFs reduced the temperature of the microenvironment between the fabric and simulated skin by 5.6 °C relative to pristine cotton fabric. Remarkably, the SSF-induced temperature reduction surpassed that achieved with pure silk fabric by 3.6 °C. Such a strategy of electroflocking SSFs offers a simple and robust approach for the large-scale production of highly efficient radiative cooling materials.

Aquaporins (AQPs) are transmembrane proteins that transport water, small solutes, and molecules across cell membranes. Studies have reported the role of AQPs in the activation, migration, and proliferation of immune cells, thus modulating the pathogenesis of autoimmune disease. In joints, the enhanced AQP4 expression exaggerates pathological changes like hydrarthrosis, acidosis, and hyperosmotic stress-inducing dysfunction of the articular chondrocytes, leading to articular cartilage destruction in collagen-induced arthritis (CIA). Acetazolamide (AZM), a sulfonamide carbonic anhydrase inhibitor of AQP4, reversibly decreases water permeability through AQP4 and is a potential molecule for targeting AQP4 in the CIA. However, its low solubility and low bioavailability limit its therapeutic effectiveness. Therefore, in this study, we have synthesized a polyphenol drug (gallic acid) (GA) and an amphiphile (glycerol monostearate) (GMS) conjugate to self-assemble into nanoparticles and encapsulated with AZM. Apart from AZM, GA is known for its antioxidant and anti-inflammatory properties. Therefore, intra-articular injection of AZM@GA-GMS NPs efficiently downregulates the expression of AQP4 and associated NLRP3 inflammasome activation. Moreover, the NPs are cytocompatible and showed enzyme-responsive drug release and thus offer a promising therapeutic strategy for RA by inhibiting AQP4-mediated inflammatory pathways. This opens up an avenue for treatment for RA.

The cohybridization of metal-organic frameworks (MOFs), particularly zeolitic imidazolate framework-8 (ZIF-8), with two-dimensional (2D) nanomaterials has emerged as a promising approach to enhance both the barrier properties and active corrosion protection of epoxy (EP)-based coatings. However, the widespread use of these hybrid systems is hindered by environmental concerns associated with toxic methanol used in ZIF-8 synthesis, the limited accessibility of active sites, and the high production costs of 2D nanomaterials. Therefore, there is growing interest in developing alternatives that integrate the beneficial properties of MOFs and 2D materials while offering lower costs, greater environmental compatibility, and increased active site accessibility. Herein, a 2D leaflike zeolitic imidazolate framework (ZIF-L) was utilized as a low-cost, environmentally friendly alternative to ZIF-8 with dual functionality for active and barrier protection properties. The hydrophilicity of ZIF-L was fine-tuned through a facet ligand exchange with benzotriazole (BTA), which acted as both a surface modifier and a corrosion inhibitor. This solvent-assisted ligand exchange was validated by X-ray photoelectron spectroscopy (XPS) analysis. The BTA loading in BTA@ZIF-L was determined to be 14.43 wt %. Incorporating 1 wt % BTA@ZIF-L pigment into the EP matrix resulted in a higher cross-linking density compared to both blank/EP and ZIF-L/EP coatings, yielding ultrahigh impedance values (∼10¹¹ Ω cm²) at the lowest frequency, even after 4.5 months of immersion in a 3.5 wt % NaCl solution. Additionally, the active corrosion inhibition capability of the BTA@ZIF-L/EP coating was demonstrated through electrochemical impedance spectroscopy (EIS) analysis of scratched coatings, showing a 130% increase in the total resistance relative to blank/EP, which was further validated by salt spray testing.

The pursuit of suitable insulating layers and high-quality integration methods is important to further improve the performance of field-effect transistors (FETs). In this study, we employ transferable high-k oxide films as device gate dielectrics to fabricate high-quality optoelectronic devices by optimizing the interface between the dielectric material and the two-dimensional (2D) materials. Through meticulous refinement, a transferred film roughness of 269.27 pm was achieved, resulting in intact, crack-free SrTiO₃ films. The molybdenum disulfide (MoS₂) transistors exhibited remarkable characteristics, including a high on/off ratio (I_ON/I_OFF) of 1 × 10⁸, a subthreshold swing as low as 69.2 mV/dec, and a field-effect mobility reaching 230 cm²/(V·s). Additionally, the SrTiO₃ films were combined with molybdenum telluride (MoTe₂) to fabricate PN junctions capable of functioning as photodetectors at extremely low operating voltages (±2 V). The exceptional performance of both the MoS₂ FETs and the MoTe₂ PN junctions can be attributed to the optimized, high-quality dielectric/semiconductor heterojunction interface. This further demonstrates the versatility of the van der Waals integration method employed in this research.

Metal-enzyme cascade catalysis effectively combines the broad reactivity of chemical catalysis with the high selectivity of biocatalysis, improving reaction efficiency and simplifying the process flow through multiple sequential reactions in the same system. The introduction of exogenous palladium nanoparticles (Pd NPs) into Escherichia coli (E. coli) cells can significantly broaden the range of catalytic reactions facilitated by biological enzymes. Additionally, the targeted cytoplasmic synthesis of Pd NPs enhances their utilization efficiency in intracellular catalytic reactions while also eliminating the need for separating and purifying metals and enzymes. However, current methods largely enable the intracellular synthesis of Pd NPs in the periplasmic space and outer membrane. Moreover, the hydrogen sources commonly used in these methods─such as hydrogen (H₂) and sodium borohydride (NaBH₄)─carry safety risks. In this study, the mechanism of targeted synthesis of Pd NPs on the cytoplasmic side and its process were deeply investigated using a mild hydrogen source, sodium formate, in combination with genetic engineering and preparation conditions. And the constructed functional cell (Pd@E. coli) could catalyze benzaldehyde hydrogenation, with a conversion rate of 41.41% and benzyl alcohol yield of 17.68%, demonstrating considerable catalytic and loading stability. This study provides a reference for constructing catalytic systems for intracellular metal-enzyme cascades. Thus, it could bolster the development opportunities in the areas of non-natural products and drug development and provide ideas for addressing the drawbacks of existing biosynthetic technologies.