Aggregate (Hoboken, N.J.)最新文献

Supercapacitors (SCs) are studied and used in various fields due to their high power density, fast charging/discharging rate, as well as long cycle life. Compared to other traditional electrode and electrolyte materials, supramolecular hydrogels have great advantages in the application of SCs due to their excellent properties. Unlike covalent bonds, supramolecular systems are assembled through dynamic reversible bonds, including host–guest interactions, ion interactions, electrostatic interactions, hydrogen bonding, coordination interactions, etc. The resulting supramolecular hydrogels show some special functions, such as stretching, compression, adhesion, self-healing, stimulus responsiveness, etc., making them strong candidates for the next generation of energy storage devices. This paper reviews the representative progress of electrodes, electrolytes, and SCs based on supramolecular hydrogels. Besides, the properties of supramolecular hydrogels, such as conductivity, extensibility, compressibility and elasticity, self-healing, frost resistance, adhesion, and flexibility, are also reviewed to highlight the key role of excellent properties of hydrogel materials in SCs. In addition, this article also discusses the challenges faced by current technologies, hoping to continue promoting future research in this field.

Photoisomerization and photoluminescence are two distinct energy dissipation pathways in light-driven molecular motors. The photoisomerization properties of discrete molecular motors have been well established in solution, but their photoluminescent properties have been rarely reported—especially in aggregates. Here, it is shown that an overcrowded alkene-based molecular motor exhibits distinct dynamic properties in solution and aggregate states, for example, gel and solid states. Despite the poor emissive properties of molecular motors in solution, a bright emission is observed in the aggregate states, including in gel and the crystalline solid. The emission wavelength is highly dependent on the nature of the supramolecular packing and order in the aggregates. As a result, the fluorescent color can be readily tuned reversibly via mechanical grinding and vapor fuming, which provides a new platform for developing multi-stimuli functional materials.

Single-component ambipolar polymers are highly desirable for organic electrochemical transistors (OECTs) and integration into complementary logic circuits with reduced process complexity. However, they often suffer from imbalanced p-type and n-type characteristics and/or stability issues. Herein, a novel single-component ambipolar polymer, namely, gIDT–BBT is reported based on indacenodithiophene (IDT) as the electron donor, benzobisthiadiazole (BBT) as the electron acceptor and oligo ethylene glycol (OEG) as the side chain. Benefitting from the extended backbone planarity and rigidity of IDT, pronounced electron-withdrawing capability of BBT, favored ionic transport from OEG together with vertical OECT device structure, a nearly balanced ambipolar OECT performance is achieved for gIDT–BBT, revealing a high transconductance of 155.05 ± 1.58/27.28 ± 0.92 mS, a high current on/off ratio >10⁶ and an excellent operational stability under both p-type and n-type operation conditions. With gIDT–BBT in hand, furthermore, vertically stacked complementary inverters are successfully fabricated to show a maximum voltage gain of 28 V V⁻¹ (V_IN = 0.9 V) and stable operation over 1000 switching cycles, and then used for efficient electrooculogram recording. This work provides a new approach for the development of ambipolar single-component organic mixed ionic–electronic conductors and establishes a foundation for the manufacture of high-performance ambipolar OECTs and associated complementary circuits.

The exploration of antibiotic-independent phototherapy strategies for the treatment of bacterial biofilm infections has gained significant attention. However, efficient eradication of bacterial biofilms remains a challenge. Herein, a self-regulated phototheranostic nanosystem with single wavelength-triggered photothermal therapy (PTT)/photodynamic therapy (PDT) transformation and oxygen supply for multimodal synergistic therapy of bacterial biofilm infections is presented. This approach combines a eutectic mixture of natural phase-change materials (PCMs) and an aggregation-induced emission (AIE) phototheranostic agent TPA-ICN to form colloidally stable nanopartcicles (i.e. AIE@PCM NPs). The reversible solid−liquid phase transition of PCMs facilitates the adaptive regulation of the aggregation states of TPA-ICN, enabling a switch between the energy dissipation pathways for enhanced PDT in solid PCMs or enhanced PTT in liquid PCMs. Additionally, oxygen-carrying thermoresponsive nanoparticles are also introduced to alleviate the hypoxic microenvironment of biofilms by releasing oxygen upon heating by AIE@PCM NPs with enhanced PTT. The nanosystem exhibits outstanding therapeutic efficacy against bacterial biofilms both in vitro and in vivo, with an antibacterial efficiency of 99.99%. This study utilizes a self-regulated theranostic nanoplatform with adaptive PTT/PDT transformation via the phase transition of PCMs and heat-triggered oxygen release, holding great promise in the safe and efficient treatment of bacterial biofilm infections.

Developing the sensitive point-of-care testing (POCT) of oncogenic nucleic acids from human papillomavirus (HPV) infection is essential in preventing cervical cancer, especially in resource-limited settings. Rolling circle amplification (RCA) is attractive in achieving POCT via nucleic acid-based aggregation under isothermal conditions. However, the influence of RCA product structure on the aggregation remains unexplored resulting in limited sensitivity. Here, a minimum secondary structured RCA technique (MSS-RCA) is developed by designing a unique circular template, demonstrating significantly enhanced detection sensitivity with only one amplification step and one primer under isothermal conditions. The amplification efficiency of MSS-RCA could be kinetically manipulated by controlling the secondary structure of the circular template. Introducing the invertase probe to MSS-RCA, HPV16 E6/E7 nucleic acid target was detected with a personal glucose meter (PGM) with a sensitivity of 5 fm (50 zmol in 10 µL). This integrated MSS-RCA-PGM detection system was successfully applied to detect HPV16 E6/E7 mRNA extracted from 54 cervical swab samples reaching a positive predictive value of 100.00% and negative predictive values of 96.00% (77.77% to 99.40%, 95% CI). MSS-RCA-PGM provides a sensitive POCT platform for the detection of nucleic acid biomarkers for screening of cervical cancer or other diseases.

Organic light-emitting diodes (OLEDs) based on multiple resonance-thermally activated delayed fluorescence (MR-TADF) have the advantages of high exciton utilization and excellent color purity. However, the large conjugated planarity of general MR-TADF emitters makes them easily aggregate in the form of π–π stacking, resulting in aggregation-caused quenching (ACQ) and the formation of excimers, which reduce exciton utilization efficiency and color purity. To address these issues, large shielding units can be incorporated to prevent interchromophore interactions, whereas the majority of reported molecules are limited to blue-green light emissions. This work proposes a strategy of incorporating steric hindrance groups at different sites of the B/N core to suppress interactions between chromophore, contributing to blue MR-TADF emitters with high photo-luminance quantum yields (PLQYs ≥ 95%) and narrow full width at half maximum (FWHM), and importantly, great suppression of the ACQ effect. Therefore, blue OLEDs achieve high external quantum efficiencies up to 34.3% and high color purity with FWHM of about 27 nm and CIE around (0.12, 0.15), even at a high doping concentration of 20 wt%.

With the development of aggregation-induced emission (AIE) materials, the drawbacks of conventional fluorescence materials subjected to aggregation-caused quenching (ACQ) have been resolved. This has allowed for the improvement of novel AIE fluorescent materials that exhibit enhanced photostability, a higher signal-to-noise ratio, and better imaging quality. Meanwhile, the enhanced phototherapeutic effect of AIE materials has garnered widespread attention in the realm of tumor treatment. The distinct physiological and anatomical characteristics of the urinary system make it suitable for the use of AIE materials. Additionally, AIE-based phototherapy provides a superior solution to deal with the weaknesses of conventional treatments for urologic neoplasms. In this review, the scientific advancement on the use of AIE materials in urinary system diseases since the emergence of the AIE concept is reviewed in detail. The review highlights the promise of AIE materials for biomarkers detection, fluorescence imaging (FLI) in vivo and in vitro, AIE-based phototherapy, and synergistic therapy from both diagnostic and therapeutic viewpoints. It is firmly believed that AIE materials hold immense untapped potential for the diagnosis and treatment of urologic disease, as well as all diseases of the human body.

The energy dissipation pathways of a photosensitizer for phototherapies, including photodynamic therapy (PDT) and photothermal therapy (PTT), compete directly with that of its fluorescence (FL) emission. Enriching heavy atoms on the π-conjugated systems and aggregation-caused quenching are two effective methods to turn off the FL emission of photosensitizers, which is expected to boost the intersystem crossing (for PDT) and nonradiative transition (for PTT) of photosensitizers for maximized phototherapeutic efficacy. Following this approach, an all-iodine-substituted polydiacetylene aggregate poly(diiododiacetylene) (PIDA) has been developed, which shows a superior near infrared absorption (ε_808nm = 26.1 g⁻¹ cm⁻¹ L) with completely blocked FL, as well as high efficiency of reactive oxygen species generation (nearly 45 folds of indocyanine green) and photothermal conversion (33.4%). To make the insoluble fibrillar PIDA aggregates favorable for systemic administration, they are converted into nanospheres through a pre-polymerization morphology transformation strategy. The in vivo study on a 4T1 tumor-bearing mouse model demonstrates that PIDA nanospheres can almost eliminate the tumor entirely in 16 days and prolong the survival time of mice to over 60 days, validating their effective phototherapeutic response through the strategy of inhibiting FL for boosted intersystem crossing and nonradiative transition.

The prevention of blindness from glaucoma requires multiple treatments to lower intraocular pressure. Here, human contact lenses are modified with highly porous metal-organic frameworks with sustained release of brimonidine for prolonged glaucoma treatment. Various metal-organic frameworks were screened for their attachment to lenses, loading with brimonidine, and drug-release properties. Optimized therapeutic ocular lenses conjugated with MIL-101(Cr) frameworks maintain optical transparency and power. Coating of lenses with MIL-101(Cr) nanoparticles reduced brimonidine washout with tears and ensured a gradual and localized release of the drug into the eyeball through the cornea. The hybrid lenses provided a 4.5-fold better decrease in eye pressure, compared by area under the curve (AUC) value to a commercially available brimonidine tartrate solution. Therapeutic lenses did not induce any notable eye irritation or corneal damage in vivo. The newly developed hybrid lenses are expected to provide a robust platform for the therapy and prevention of various ocular diseases.

Metalated covalent organic frameworks (COFs) for 2D and 3D topologies are continuously being developed, whereas metalated COFs with 1D topologies are still in their infancy. Here, a novel 1D phenanthroline-based COF containing 4,4-(1,10-phenanthroline-2,9-diyl)bis[benzaldehyde] (PBA) is reported (PAD-COF). Subsequently, a metalated 1D COF, Co SAS/PAD-COF, is constructed using the bidentate ligand properties of PBA and anchoring the single Co atoms in PAD-COF through a post-synthetic modification strategy. This complex significantly improved the photocatalytic performance of PAD-COF, and the CO yield of the optimized Co SAS/PAD-COF was stable at 3091 µmol g⁻¹ h⁻¹ with a selectivity of 93%, which is approximately 43.7 times that of the original PAD-COF. Experimental and theoretical results demonstrate the excellent CO₂ photoreduction activity of Co SAS/PAD-COF owing to the synergistic effect of single Co catalytic sites and PAD-COF. Among them, PAD-COF, as the host, adsorbs CO₂ molecules and loads single Co atoms. Meanwhile, Co atoms function as catalytic sites and promote the adsorption and activation of CO₂, while reducing the reaction energy barrier formed by the *COOH intermediates. Therefore, this unique metalated 1D COF provides a fresh approach to photocatalytic CO₂ reduction.