Latest ArticlesConventional aromatic fluorophores in fluorescent probes can easily initiate molecular aggregation via π–π stacking, which drastically quenches fluorescence and hinders cellular permeability. To address this challenge, we developed an ingenious host-guest recognition strategy that converted detrimental π-π stacking into a relaxed molecular aggregation state, enabling the creation of a rhodamine-based supramolecular fluorescent probe called RAO@2CB[8]. This ternary conjugate, assembled by encapsulating adamantyl-modified rhodamine (RAO) with two cucurbit[8]uril (CB[8]), showcased enhanced fluorescence properties for the precise detection of salicylic acid (SA). Intriguingly, in intricate biological systems, RAO@2CB[8] demonstrated exceptional cell permeability, facilitating susceptible detection and imaging of SA in HEK-293 cells, radish roots, and salt-stressed white pea seedlings. This facile supramolecular strategy not only mitigates aggregation-induced quenching, but also provides profound insights for the precise modulation of molecular aggregation behavior.
The efficient design of novel macrocycles with enhanced properties over their parent scaffold represents a major challenge in supramolecular chemistry. Here, we exemplify imination as a purification-free method to develop novel pillar[n]arene-like macrocycles with partial-belt nitrogen functionalization. Compared to similarly sized pillar[n]arene-inspired arenes, the strategy provides an increased scalability and an up to 16-fold improvement in macrocyclization yield. X-ray crystallography and theoretical calculations reveal a similar electron density and cavity size as pillar[5]arene. The altered geometry and enhanced flexibility, however, permit complexing di-, tri- and tetrasubstituted cyanobenzenes, generating guest complementarity to all-carbon pillar[n]arenes. The suitable positioning of hydrogen bond acceptors facilitates binding based on endo-cavity hydrogen bonding, a feature largely unreported in peralkylated pillar[n]arenes. Reduction straightforwardly afforded a polyamine macrocycle of modified geometry.
The oxygen evolution reaction (OER) is crucial for renewable energy systems, such as water splitting and metal air batteries. However, the slow kinetics of OER significantly limits the overall energy conversion efficiency, necessitating effective catalysts. The multielement transition metal oxides offer a promising alternative compared to precious metal oxides, yet their composition optimization remains challenging due to the vastness of the combinatorial space. Traditional trial-and-error approaches are labor-intensive and inefficient. To address this challenge, we develop an innovative automated platform integrating machine learning (ML) with Bayesian optimization for rapid and cost-effective synthesis and evaluation of electrocatalysts. This platform allows the automation of the entire experimental process, from synthesis to evaluation, enabling real-time feedback and guiding subsequent experiments. In a continuous operation of 32 h, the platform conducted 96 experiments to optimize the composition of (Ni-Fe-Co-Mn-Mo)Ox, resulting in an electrocatalyst with an overpotential of 231 mV at 10 mA/cm2. This automated approach significantly reduces manual intervention and enhances efficiency, proving to be a valuable tool for optimizing materials in complex, multidimensional spaces.
The construction of quasi-solid-state sodium-air batteries (SABs) by replacing traditional liquid electrolytes with gel electrolytes has become one of the future focus areas in the SABs field. However, the currently developed quasi-solid-state SABs inevitably produce insoluble discharge products during the discharge process, which leads to limited rate capability and poor cycling stability. In this study, a hydrogel electrolyte (PANa-NCNT) containing nitrogen-doped carbon nanotubes (NCNT) and sodium polyacrylate (PANa) was designed, and a quasi-solid-state SAB with highly water-soluble NaOH as the main discharge product was constructed. The physical entanglement between NCNT and PANa in the PANa-NCNT hydrogel electrolyte leads to the heterogeneous structure of gel, which effectively enhances the thermodynamic stability of the hydrogel electrolyte. In addition, the aqueous components of electrolyte determine the reaction pathway of battery. During discharge, the oxygen reduction reaction proceeds via 2e- pathway to generate soluble NaOH, while during charging, the oxygen evolution reaction exhibits a mixed 2e-/4e- reaction pathway. Benefiting from the good thermodynamic stability of PANa-NCNT hydrogel electrolyte and the water-soluble discharge products, the fabricated quasi-solid-state SAB demonstrates stable cycling for 330 cycles (187 h) at 0.5 mA/cm2 in ambient air. These findings reveal the influence of the liquid-phase components in the gel electrolyte on the reaction pathways, which is conducive to promoting the application of hydrogels in quasi-solid-state SABs.
High-performance bifunctional oxygen electrocatalysts are urgently required for rechargeable zinc-air batteries (ZABs) due to sluggish kinetics of oxygen reduction/evolution reactions (ORR/OER) at the air cathode. In this study, an iron single-atom catalyst (Fe-SAC, FeTCPP@UiO-66–800) is synthesized by direct pyrolysis of a metalloporphyrin-incorporated multivariate MOF. The spatial separation effect of the framework linkers endows Fe-SAC with hierarchical porosity, improved metal utilization efficiency, and enhanced site accessibility by suppressing the metal agglomeration during pyrolysis. Moreover, the possible formation of di- or tri-atomic iron sites facilitates the OER activity via the oxide pathway mechanism (OPM), contributing to the excellent bifunctional ORR/OER performance with a ΔE of 0.59 V. Both liquid and flexible ZAB assembled with FeTCPP@UiO-66–800 demonstrate enhanced activity, long-term durability, and anti-deformation ability (340.5 mW/cm2 peak power density in liquid device). This study presents a novel strategy for preparing MOF-derived SACs with highly accessible single-atom sites, offering a promising route to high-performance energy conversion devices.
Mass spectrometry imaging (MSI) is a rapidly advancing field in omics research, offering spatially resolved localization of biomolecules such as metabolites, lipids, and proteins within tissue sections. Recent advancements in high-resolution MSI instrumentation have significantly enhanced the visualization of cellular structures, enabling molecular mapping at the single-cell level. Current single-cell MSI techniques can be broadly categorized into label-free approaches and multiplexed antibody-based strategies, both of which are continuously evolving to support comprehensive molecular profiling with subcellular precision. These technologies have become particularly valuable in cancer and neurodegenerative disease research, where they facilitate the characterization of cellular heterogeneity, metabolic reprogramming, and microenvironmental changes associated with disease progression. To meet the increasing demands of high-content spatial biology, multiple single-cell MSI platforms have been employed to detect low-abundance molecules, distinguish phenotypically distinct cell populations, and uncover region-specific molecular alterations in complex tissues. Moreover, emerging capabilities such as three-dimensional MSI are further extending the potential of this technology to reconstruct tissue biochemical architecture and capture spatially resolved molecular dynamics. In this review, we highlight pioneering advancements in single-cell MSI techniques and their applications in cancer and neurodegenerative disease research, with a particular emphasis on their role in elucidating disease mechanisms at the cellular level. We also discuss current challenges and future perspectives for expanding the utility of single-cell MSI in subcellular imaging and deeper biological discoveries.
Metal-free carbon materials are effective catalysts for electrochemical H2O2 synthesis. Here, we employ a hydrothermal-ball milling tandem strategy to convert nitrogen-doped carbon quantum dot (N-CQD) into N, B, O-codoped carbon nanosheets via mechanochemical crosslinking. The formation of covalent N–B–O linkages correlate with nanosheet thickness and boosts 2e− ORR performance. The optimized CN-B-3 catalyst achieves 98.4% selectivity at 0.68 V vs. RHE, a low Tafel slope of 73.5 mV/dec, and a high ring current density of 0.46 mA/cm2. It maintains 92.2% and 88.7% of initial ring and disk currents after 18 h, with exceptional long-term stability demonstrated over 50 h in both flow and solid-state electrolyte cells, yielding up to 213 mmol/L H2O2. DFT calculations reveal that covalent bonds formed by dehydration of two -OH groups (BO2HN-, B(OH)2-PyN- and B(OH)-PyN-) are key to nanosheet formation. Linkages between B and nitrogen atoms on the carbon ring favor H2O2 generation more than B–pyridinic-N connections. This study paves an avenue for converting 0D CQD to 2D carbon nanosheets and highlights the catalytic role of N–B–O linkers in sustainable H2O2 electrosynthesis.
Nitidine chloride (NC) exhibits potent antitumor activity through ferroptosis induction. However, its clinical application is limited by poor aqueous solubility and non-selective cytotoxicity. To overcome these challenges, we developed a pH-responsive delivery system (HD@NC@MOF), combining a hyaluronic acid (HA)-cloaked and mixed-valence iron-based metal-organic framework (Fe-MOF), enabling strategic targeting of lung squamous cell carcinoma (LUSC) cells via CD44 receptor recognition. Within the acidic intracellular microenvironment, HD@NC@MOF co-releases NC and iron ions, triggering a profound reactive oxygen species (ROS) surge, and ultimately inducing ferroptosis and necroptosis through the solute carrier family 7 member 11 (SLC7A11)/glutathione peroxidase 4 (GPX4) and receptor-interacting serine/threonine-protein kinase 1 (RIPK1)/receptor-interacting serine/threonine-protein kinase 3 (RIPK3)/mixed lineage kinase domain-like protein (MLKL) pathways. In vitro, HD@NC@MOF exhibited significantly enhanced selective cytotoxicity towards LUSC cells compared to free NC (selectivity index improved from 0.54 to 2.58). Mechanistic studies revealed that NC stimulated mitochondrial ROS production, synergizing with Fe-MOF-derived iron to amplify oxidative stress. In vivo, HD@NC@MOF achieved a 69.02% tumor inhibition rate (1.72-fold higher than free NC) with minimal systemic toxicity. This work highlighted the potential of HD@NC@MOF as an efficient and targeted carrier for NC in LUSC chemotherapy.
Photochromic materials have drawn considerable interest in chemical and material sciences, owing to their unique photo-responsive properties and transformative potential in smart material applications. Among these, ESIPT-triggered photochromic systems stand out as a particularly promising subclass because of their exceptional photochromic property. However, existing reviews have primarily concentrated on Schiff base derivatives within this category, largely overlooking critical advancements in three key dimensions: (1) The discovery of novel ESIPT-triggered structural frameworks beyond traditional systems, (2) innovative synthetic methodologies enabling precise control of photochromic behaviors in both solid and solution states, and (3) the emergence of unprecedented functional properties driving cutting-edge applications. These oversights have created a significant knowledge gap in comprehensively understanding the rapid evolution of ESIPT-triggered photochromic materials. Therefore, this review systematically summarizes recent breakthroughs through three analytical lenses: First, we establish a structural taxonomy of ESIPT photochromophores, elucidating design principles that govern their performance. Second, we summarize advanced construction strategies that can synthesize tailored ESIPT photochromophores in different phase states. Third, we summarize the expanding application landscape of ESIPT photochromic materials in various functional domains. By integrating fundamental understanding with application-oriented perspectives, this work is expected to inspire the development of smart materials and photoresponsive systems.
The strategic engineering of heterointerface architecture is demonstrating its critical pathway for optimizing charge dynamics in metal-organic framework (MOF)-based photo-Fenton systems. This work presents a novel ZIF-8@NH2−MIL-101(Fe) heterostructure with precisely controlled MOF-on-MOF configuration, which exhibits exceptional catalytic performance in the degradation of antibiotics. Experimental results revealed desired catalytic capacity with 91.4% tetracycline hydrochloride (TCH) degradation within a short time and satisfactory stability across pH 3.0–9.0 under visible light irradiation (λ ≥ 420 nm). Ecotoxicological assessment exhibits that the ecological risks of degradation intermediates diminish significantly when compared with those of the parent TCH. Comprehensive mechanistic investigation indicates that TCH decomposition is governed by superoxide radical (•O2−) and hydroxyl radical (•OH) as the primary reactive species. The proposed S-scheme charge transfer mechanism is verified by Mott–Schottky analysis and in X-ray photoelectron spectroscopy. Meanwhile, the enhanced interfacial charge separation efficiency is confirmed by electrochemical impedance spectroscopy. This work not only advances the development of Fe-based MOF heterojunctions for photo-Fenton catalysis but also provides critical insights into the relationship between heterostructure engineering and catalytic efficiency.
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