Aggregate (Hoboken, N.J.)最新文献

This study presents a new class of amphiphilic porous frameworks constructed through ion-dipole interactions between anionic silicate cages and K⁺ ions. These materials uniquely integrate solid-state porosity, demonstrated by selective gas adsorption, with molecular-scale solution processability. Remarkably, the materials preserve the discrete integrity of their cages in solution, enabling host–guest recognition. They can also be reversibly regenerated, offering a versatile strategy for designing multifunctional, amphibious porous materials (e70157).

Since Aggregate's inaugural issue in December 2020, we have embarked on the wonderful journey to advance aggregate science — a research field dedicated to exploring the science beyond molecules. The past five years have witnessed the remarkable flourishing of this discipline, alongside the growing academic recognition of Aggregate. As we celebrate the 5-year anniversary, let us reflect on the past journey and envision the promising future (e70234).

This study presents a fimbriae-targeted SeVB⊃PQ complex for enhanced photodynamic therapy of periodontitis. The selenoviologen cyclophane host encapsulates a P. gingivalis-specific peptide, enabling precise bacterial binding and ROS generation upon light activation. This selective delivery enhances antimicrobial efficacy, restores subgingival microbiome homeostasis, and outperforms methylene blue in reducing inflammation and promoting tissue regeneration (e70159).

This work introduces a scalable strategy for fabricating monodisperse cluster-luminescent polymer microspheres via functional group engineering. The microspheres exhibit broad emission (400–700 nm) and low fluorescence coefficient of variation (CV < 3%), fulfilling requirements for routine flow cytometer calibration. More importantly, kilogram-scale synthesis could be achieved facilely, demonstrating industrial potential (e70176).

Zhang et al. developed a novel direct deaminative functionalization strategy based on N-nitroamine intermediates, overcoming the explosiveness of traditional diazonium salts to achieve safe and efficient transformation. This method covers over 170 substrates, supports gram-scale preparation and one-pot cross-coupling, provides a new avenue for the synthesis of organic optoelectronic materials. And its N-nitroamine intermediate mechanism supplements the theoretical framework of deaminative reactions.

Agents to combine functions simultaneously are highly needed but still challenging in synergistic therapy. Particularly, capabilities to deplete glutathione (GSH) in tumors and monitor their process are also important. Therefore, platinum(II) metallacycles are prepared by using aggregation-induced emission active ligands. Despite their similar structures, high emission for Mh1 is obtained (PLQY = 49.2%) in solids, but a PLQY of only 6.8% is recorded for Mh2. NIR emission in Mh2 can be turned-on in depleting GSH by releasing emissive ligands. Also, both type I and type II reactive oxygen species (ROS) are obtained in Mh2 nanoparticles. Due to the depletion of GSH and generation of ROS, oxidative stress in immunogenic cell death can be induced. By combining chemotherapy and photoimmunotherapy, synergistic therapy in vivo is obtained for Mh2-NPs to well inhibit the tumor growth, also showing antitumor immune effects in distant tumors. The work here provides some guidelines in designing the multi-functional agents, showing the great potentials in efficient cancer therapy.

As environmental concerns and the transition to a carbon-neutral society gain importance, proton exchange membrane fuel cells (PEMFCs) using hydrogen as a fuel have attracted significant attention as eco-friendly energy technology. Although Pt is the primary catalyst for PEMFC anodes, its high cost and limited availability pose major barriers to commercialization. To address these challenges, non-Pt catalysts, alloy catalysts, and core-shell structured catalysts have been extensively studied; nevertheless, performance degradation and structural instability remain significant issues. In this study, we design Pt-lean Pt₁Co₄ alloy nanoparticles encapsulated with an ultrathin carbon shell derived from the carbon sources of the metal precursor ligands. Notably, after synthesizing the carbon-incorporated alloy nanoparticles, heat treatment under a carbon monoxide (CO) atmosphere induces selective surface segregation of Pt atoms due to their strong CO binding affinity, occurring before the carbonization temperature is reached for carbon shell formation, resulting in a Pt-enriched surface structure. The carbon shell imparts a nano-confinement effect that effectively suppresses particle growth and aggregation during heat treatment, thereby significantly enhancing electrochemical stability. Remarkably, despite a 55% reduction in Pt content, the combination of surface segregation and near-surface alloying allows the Pt-lean alloy catalyst to maintain hydrogen oxidation reaction activity comparable to a bare Pt catalyst while providing superior durability. Owing to this dual function of heat treatment, the design of the Pt-lean alloy catalyst structure offers a promising strategy for developing highly efficient and cost-effective anode catalysts for PEMFCs.

Confinement effect, by strengthening interactions between structural components, provides an effective strategy for precisely regulating functional units, which is critical for properties associated with microscopic accumulation effects, such as second harmonic generation (SHG) and ferroelectricity. Here, we propose a molecular dipole management strategy through confinement effect to enhance the SHG and ferroelectricity properties in a new hybrid germanium perovskite system. Utilizing the cyclohexylammonium (Cy) cation, we successfully synthesize three polar phases, including one-dimensional (1D) hexagonal (Cy)GeI₃, a step-like two-dimensional (2D) (Cy)₄Ge₃I₁₀ phase, and a 2D (CyF)₂GeI₄ phase (CyF = 4,4-difluorocyclohexanammonium). All three phases exhibit photoresponses, characteristic of semiconductors. The metastable 1D (Cy)GeI₃ phase has the highest local dipole moment (LDM) of 14.07 Debye along the c-axis, resulting in a strong SHG response, and a high octahedral distortion parameter (D_i = 0.10). The step-like 2D (Cy)₄Ge₃I₁₀ phase exhibits ferroelectric properties, where the remanent polarization of 0.34 µC/cm² has been confirmed by PFM and P-E hysteresis loop measurements. To achieve both high phase stability and SHG intensity, we introduce a fluorine group into the organic cation, forming strong C─H···F─C hydrogen bonds that align polar units uniformly, increasing D_i to 0.11. The 2D (CyF)₂GeI₄ phase achieves a high SHG of 4 × KH₂PO₄. Furthermore, its phase transition temperature also increases by 88 K compared to the (Cy)₄Ge₃I₁₀ phase. Raman spectra and DFT calculations further reveal intensified confinement effect in the (CyF)₂GeI₄ phases, consistent with its stronger structural rigidity. Our work provides comprehensive perspective and design strategies for tuning and optimizing hybrid perovskite-based nonlinear optical materials.

High-performance circularly polarized organic light-emitting diodes (CP-OLEDs) with ultraviolet and deep-blue circularly polarized electroluminescence (CP-EL) are important for 3D displays, but designing short-wavelength circularly polarized luminescence (CPL) materials remains a significant challenge. Herein, a series of ultraviolet and deep-blue CPL materials was developed, successfully integrating high photoluminescence quantum yields with efficient high-level reverse intersystem crossing (hRISC) properties. Efficient ultraviolet and deep-blue CP-OLEDs are created by utilizing these chiral materials as emitters, providing maximum external quantum efficiencies (η_ext,maxs) of 6.7% at 398 nm (full-width at half-maximum [FWHM] = 44 nm) and 10.8% at 454 nm (FWHM = 68 nm) with obvious CP-EL. Furthermore, by adopting these chiral materials as sensitizers or functional layers, well-developed achiral multi-resonance thermally activated delayed fluorescence green and yellow emitters are enabled to generate obvious CP-EL with large dissymmetry factors and excellent EL performance (η_exts = 34.5% and 35.3%, FWHM = 42 and 40 nm). These results demonstrate that the developed new ultraviolet and deep-blue chiral materials can be used not only as emitters for ultraviolet and deep-blue CP-OLEDs, but also as sensitizers and functional layers to furnish a simple and universal way of achieving efficient narrow-spectrum CP-OLEDs with achiral emitters.

Aggregation-induced emission luminogens (AIEgens) have become a vital class of functional materials for optoelectronic and biomedical applications. Extending AIE behavior from single-component to two-component systems opens a new avenue for modulating emission through intermolecular interactions, yet it also introduces substantial complexity in understanding and controlling the aggregation process. In particular, elucidating how multicomponent molecular packing governs macroscopic photophysical behavior remains a central challenge. Herein, we constructed four distinct charge-transfer (CT) cocrystals through the coassembly of electron-rich dibenzo-heterocyclic donors and electron-deficient 1,2,4,5-tetracyanobenzene (TCNB) acceptors. The cocrystallization process allows precise manipulation of the dynamic aggregation pathway by tuning the DMSO/H₂O ratio. Intriguingly, the morphology evolves from amorphous aggregates to rod-like and finally to needle-like microcrystals, showing a nonmonotonic size variation with increasing water content, accompanied by a gradual enhancement of fluorescence intensity. The four CT complexes exhibit wide emission tunability from green to orange-red, and notably, the AIE-active DBT/TCNB pair enables a practical demonstration in water-jet rewritable encryption paper. Overall, this work establishes a simple yet effective paradigm for designing high-performance solid-state emitters, while unveiling fundamental principles that govern the controllable molecular assembly in multicomponent luminescent systems.