Aggregate (Hoboken, N.J.)最新文献

Current phototherapeutic agents based on heptamethine cyanine dyes often rely on symmetric structures, limiting their photodynamic therapy (PDT) efficiency. Herein, we report a novel asymmetric heptamethine cyanine dye (Cyp-TPE) that features a twisted tetraphenylethylene moiety. This design facilitates the formation of stable aggregate nanoparticles (NPs) with a cross-arranged structure, as revealed by molecular dynamics simulations. This specific aggregation mode promotes exciton delocalization and dramatically enhances spin-orbit coupling, leading to an unprecedented ROS quantum yield of 154.54%. Under 808 nm laser irradiation, the Cyp-TPE NPs demonstrate potent synergistic photodynamic and photothermal activity, concurrently triggering ferroptosis and lysosomal dysfunction, thereby achieving multimodal death of cancer cells. Furthermore, the excellent NIR absorption and photothermal conversion of these aggregates enable precise photothermal imaging (PTI) and photoacoustic imaging (PAI). This work highlights the potential of asymmetric molecular design to overcome the limitations of conventional photosensitizers, offering a robust nanoplatform for imaging-guided cancer therapy.

Carbon dots (CDs), as an emerging class of zero-dimensional carbon-based nanomaterials, have attracted widespread attention owing to their remarkable optical properties, solution processability, and environmental friendliness, showing broad application prospects in optoelectronic devices. Nevertheless, although significant research progress has been achieved in recent years, a comprehensive theoretical framework is still absent for clarifying the correlations among the structure, optical properties, and performance of CDs in practical device applications. In this regard, the present review highlights recent developments in utilizing the distinctive optical features of CDs for various optoelectronic systems, including key examples such as photodetectors, optical memristors, lasers, electroluminescent diodes, and photovoltaic cells. Moreover, the current limitations and future research directions for CDs-based optoelectronic technologies are analyzed. The insights provided herein are expected to stimulate further research on enhancing the optical properties of CDs and promoting the rational design of high-performance devices from a new perspective.

The rise in pancreatic diseases, resulting from improved living quality and lifestyle habits changes, has imposed a serious social burden. To better understand the pancreatic functions during disease progression, constructing a bionic pancreas is vital yet challenging in tissue engineering. Herein, inspired by the physiological anatomy of the pancreas, we introduce core-shell microfibers with pancreatic stellate cells (PSCs) in the shell and pancreatic β-cells in the core. Compared to traditional plate culture, the β-cells encapsulated in the microfiber exhibit enhanced glucose-stimulated insulin secretion. Such microfibers also serve as a platform to study the progression of diabetes of the exocrine pancreas, where the PSCs are activated under conditions of pancreatic exocrine diseases such as chronic pancreatitis. The activated PSCs impede insulin synthesis and increase apoptosis in β-cells, resulting in elevated blood glucose. This high-glucose microenvironment further exacerbates the activation of PSCs, causing a vicious cycle of diabetes. Additionally, the bio-inspired pancreas also demonstrates its potential in drug screening, as evidenced by testing the glucagon-like peptide 1 receptor agonist, Exendin-4. Building upon such features, it is convincing that these multi-component microfibers hold promise for exploring the pancreatic exocrine and endocrine interactions, and showing potential in disease modeling, drug screening, and regenerative medicine.

Immunotherapy has emerged as one of the most promising strategies for achieving complete tumor eradication. However, its effectiveness against solid tumors remains limited due to the presence of an immunosuppressive tumor microenvironment. In addition, severe side effects such as cytokine storms further constrain its clinical application. Therefore, there is an urgent need to develop efficient and controllable immunotherapeutic approaches. Herein, we report the development of a novel mitochondrial DNA-releasing photosensitizer, MQ-PPy, which exhibits outstanding mitochondrial localization and robust reactive oxygen species generation. Upon light irradiation, MQ-PPy induces pronounced mitochondrial oxidative damage in tumor cells, triggering the release of immunogenic damage-associated molecular patterns and mitochondrial DNA, which activates the cGAS-STING signaling pathway. Meanwhile, MQ-PPy effectively induces immunogenic cell death, thereby remodeling the tumor immune microenvironment and enhancing antitumor immune responses. In vivo studies confirmed that MQ-PPy-mediated photodynamic therapy significantly inhibits tumor growth and notably increases the infiltration of cytotoxic T cells within the tumor. Moreover, we demonstrated that tumor cells treated with MQ-PPy-mediated PDT can function as a whole-cell vaccine, effectively establishing systemic immune memory and significantly suppressing tumor growth upon rechallenge. This study presents a promising and controllable strategy for advancing tumor immunotherapy through mitochondria-targeted photoactivation.

Mitochondria-targeted aggregation-induced emission (AIE) materials have emerged as promising candidates for precision medicine by enabling the controllable induction of oxidative stress within mitochondria. Yet, a comprehensive overview of the antitumor and other biological effects resulting from such oxidative stress remains lacking. This review summarizes the roles of both excessive and moderate oxidative stress triggered by mitochondria-targeted AIE materials across diverse applications, including: (1) direct induction of various forms of cancer cell death and degradation of cancer-associated proteins; (2) synergistic enhancement of chemo-, radio-, immune-, and other therapies; and (3) treatments beyond cancer. In addition, the challenges and key issues limiting their broader application are discussed. This review highlights the therapeutic potential of controllably induced oxidative stress by mitochondria-targeted AIE materials, aiming to accelerate their development for precise disease intervention and biological regulation.

Gliomas present a significant challenge in oncology due to their often subtle early symptoms and the insidious nature of their growth, which is compounded by the blood–brain barrier. Recent evidence has highlighted the diagnostic and therapeutic potential of monocytes, macrophages, and microglia in the context of glioma. This review focused on emerging evidence and hypotheses concerning the components and interrelationships within the mononuclear phagocyte system (MPS) in the central nervous system and its role in glioma development and invasion. By summarizing the involvement of the MPS in glioma biology, this paper offers a novel perspective for the integration of liquid biopsy and targeted therapies in oncology.

Apoptotic vesicles (ApoVs) are membrane structures formed during cell apoptosis and play crucial roles in homeostasis maintenance, signal transduction, and immune regulation. Importantly, ApoVs inherit the properties and contents of parental cells that show great potential in the diagnosis and treatment of diseases. Monitoring the formation process of ApoVs (such as quantity, morphological changes, release rules, etc.) can reveal the regulatory mechanism of apoptosis, and is also helpful for optimizing the preparation and application of ApoVs. However, due to the limitations of existing technologies, the formation processes of ApoVs have been challenging to precisely and entirely capture. Herein, we subtly constructed a versatile AIEgen (ADTP) that could induce ApoVs production and in situ monitor the formation process, and it was successfully applied to explore the formation mechanism of ApoVs. ADTP specifically targeted the plasma membrane, and it could effectively induce apoptosis under laser irradiation, so it was able to dynamically monitor the entire formation process of ApoVs and had validated ApoVs formation from membrane protrusions (including filopodia, tunneling nanotubes, and retraction fibers). Further investigation revealed that ApoVs derived from membrane protrusions with different components exhibited significant heterogeneity. Additionally, the near-infrared emission characteristic of ADTP was compatible with the stimulated emission depletion (STED) microscopy equipped with a 775 nm depletion laser, enabling high-resolution visualization of detailed dynamic changes in membrane protrusions during ApoVs formation. This work provided powerful tools for tracking the entire ApoVs formation process and also offered crucial scientific evidence for revealing the ApoVs formation mechanism.

Stacking angles played a decisive role in the coupling strength of the excited state, the overlap of electronic orbitals, and behavior of excitons, which further have ultimately affected the luminescent properties. However, developing effective strategies to precisely tailor molecular stacking anglets of chromophores still remains challenges. In this work, we constructed a series of figure-eight supramolecules S1–S3 through the coordination-driven self-assembly of anthracene-based 180° di-platinum(II) acceptor L and ditopic pyridyl ligands L1–L3, respectively. Variation in ligand length enabled regulation of intramolecular anthracene stacking angles in the assembled structures and photoluminescent properties. Photophysical studies revealed that larger stacking angles significantly enhance fluorescent intensities and photoluminescence quantum yields in both solution and solid states. Femtosecond transient absorption spectroscopy further demonstrated that the excited-state lifetimes of S1–S3 were extended due to suppressed non-radiative decay pathways. Moreover, density functional theory calculations showed that the increasing stacking angles weakened intramolecular anthracene interactions, leading to enhanced radiative transition rates. This study elucidated the relationship of molecular packing and luminescent properties, which will pave the way for construction of materials with excellent luminescent performance.

The rational design of aqueous-phase supramolecular catalysts that integrate substrate recognition, activation, reaction selectivity, and recyclability remains a significant challenge. This work presents a cucurbit[8]uril (Q[8])-based supramolecular photocatalyst, TMV⁸⁺@Q[8], which selectively encapsulates aromatic sulfide substrates via host-stabilized charge transfer (HSCT) interactions while markedly enhancing singlet oxygen (¹O₂) generation. Under visible-light irradiation, the substrate-TMV⁸⁺@Q[8] system facilitates the efficient catalytic oxidation of aromatic sulfides to sulfoxides. Competitive displacement experiments confirm that product desorption is substrate-driven, enabling catalyst regeneration. Crucially, the Q[8] cavity plays a multifaceted role by enhancing substrate activation through HSCT, promoting ¹O₂-mediated oxidation via confinement effects, and enforcing selectivity through size exclusion. These findings establish a new paradigm for supramolecular photocatalysis, wherein macrocyclic confinement concurrently enhances substrate recognition, catalytic efficiency, and recyclability. This study thereby provides a strategic blueprint for designing enzyme-inspired supramolecular photocatalysts operable in aqueous media.

The management of iodine species, notorious for their environmental persistence and health risks, requires innovative materials capable of efficient capture and conversion. Herein, we report the self-assembly and characterization of a Zr-based metal–organic tetrahedron (1) functionalized with redox-active triazatriangulenium (TATA⁺) panels. The cage exhibits a high binding affinity for triiodide (I₃⁻) (ca. 10⁶ M⁻¹) in methanol. The strong host–guest complexation significantly facilitates the disproportionation hydrolysis of I₂ to generate I₃⁻ and HOI. It also enables photocatalytic aerobic oxidation of I⁻ into I₃⁻ within its cavity. Mechanistic investigations revealed the key steps involving guest-to-host photoinduced electron transfer (ET) to generate radicals I^• and 1^• and ET from 1^• to dioxygen to generate superoxide. Solid-state adsorption experiments showed the rapid removal of I₂ and I₃⁻ from water by 1-NTf₂ because of the high affinity for polyiodides. Importantly, although solid-state 1-NTf₂ has no ability to directly adsorb I⁻ from water, we have for the first time developed a light-driven strategy that enables removal of I⁻ through coupled photooxidation and sequestration. This work highlights the significant potential of integrating photoredox-active moieties within stable metal–organic cages for controlling iodine binding and speciation and opens new avenues to address environmental and energy-related sequestration challenges.