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- 实验方案
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Rhomboidal Pt(II) metallacycle-based NIR-II theranostic nanoprobe for tumor diagnosis and image-guided therapy
摘要： Fluorescent theranostics probes at the second near-IR region (NIR-II; 1.0–1.7 μm) are in high demand for precise theranostics that minimize autofluorescence, reduce photon scattering, and improve the penetration depth. Herein, we designed and synthesized an NIR-II theranostic nanoprobe 1 that incorporates a Pt(II) metallacycle 2 and an organic molecular dye 3 into DSPE-mPEG5000 (1,2-distearoyl-sn-glycero-3-phosphoethanolamine-N-[methoxy(polyethylene glycol)-5000]). This design endows 1 with good photostability and passive targeting ability. Our studies show that 1 accurately diagnoses cancer with high resolution and selectively delivers the Pt(II) metallacycle to tumor regions via an enhanced permeability and retention effect. In vivo studies reveal that 1 efficiently inhibits the growth of tumor with minimal side effects. At the same time, improved fluorescent imaging quality and signal-to-noise ratios are shown due to the long emission wavelengths. These studies demonstrate that 1 is a potential theranostic platform for tumor diagnosis and treatment in the NIR-II region.
关键词： metallacycle,image-guided therapy,supramolecular coordination complexes,second near-infrared region,theranostic
更新于2025-09-19 17:15:36
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A Supramolecular Gel of Oxalic Acid-Monoethanolamine for Potential Schottky Barrier Diode Application
摘要： A functional supramolecular gel of oxalic acid and monoethanolamine (OXMEA) has been achieved through direct instant mixing of N,N-dimethyl formamide (DMF) solution of oxalic acid and pure monoethanolamine at room temperature under ambient condition. The rheological analysis established the viscoelastic semi-solid type nature of mechanically stable OXMEA supramolecular gel. The morphological pattern, imaged through field emission scanning electron microscopic investigation, explores the bean-seed like hierarchical architecture of the gel network. The semiconducting property of the gel was verified from band gap energy and conductivity estimation. The electrical charge transport property was also analyzed in the form of OXMEA gel based metal-semiconductor junction thin film device. The obtained nonlinear current-voltage characteristics of the device signify Schottky barrier diode nature of the synthesized gel. Overall, this work has been proof of development of semiconducting electronic device by OXMEA gel based gel medium.
关键词： Semiconductor,Morphology,Supramolecular Gel,Rheology,Schottky barrier diode
更新于2025-09-19 17:15:36
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Formation of a supramolecular charge-transfer complex. Ultrafast excited state dynamics and quantum-chemical calculations
摘要： The formation of a supramolecular complex of bis(18-crown-6)stilbene (1) and 4,4’-bipyridine with two ammoniopropyl N-substituents (3) and the substitution reaction between 1·3 and alkali and alkaline-earth metal perchlorates have been studied using absorption, steady-state fluorescence, and femtosecond transient absorption spectroscopy. The formation of 1·(Mn+)2 complexes in acetonitrile was demonstrated. The weak long-wavelength charge-transfer absorption band of 1·3 completely vanishes upon complexation with metal cations because of disruption of the pseudocyclic structure. The spectroscopic and luminescence parameters, stability and substitution constants were calculated. The relaxation scheme of the 1·3 singlet state excited by a 25 fs laser pulse was proposed. It includes very fast vibrational relaxation and direct (τCT-d = 0.32 ps) and back (τCT-b = 0.51 ps) electron transfer resulting in complete fluorescence quenching. The quantum-chemistry calculations revealed the species taking part in the ET process and elucidated the mechanism of relaxation of the excited complex.
关键词： supramolecular complex,quantum-chemical calculations,femtosecond spectroscopy,charge-transfer,electron transfer
更新于2025-09-19 17:15:36
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Suppressing depolarization by tail substitution in an organic supramolecular ferroelectric
摘要： Despite being very well established in the field of electro-optics, ferroelectric liquid crystals so far lacked interest from a ferroelectric device perspective due to a typically high operating temperature, a modest remnant polarization and/or poor polarization retention. Here, we experimentally demonstrate how simple structural modification of a prototypical ferroelectric liquid-crystal benzene-1,3,5-trisamide (BTA) – introduction of branched-tail substituents – results in materials with a wide operating temperature range and a data retention time of more than 10 years in thin-film solution-processed capacitor devices at room temperature. The observed differences between linear- and branched-tail compounds are analyzed using density functional theory (DFT) and molecular dynamics (MD) simulations. We conclude that morphological factors like improved packing quality and reduced disorder, rather than electrostatic interactions or intra/inter-columnar steric hindrance, underlay the superior properties of the branched-tailed BTAs. Synergistic effects upon blending of compounds with branched and linear side-chains can be used to further improve the materials’ characteristics.
关键词： liquid crystal,BTA,DFT,molecular dynamics,supramolecular,ferroelectric,polarization retention
更新于2025-09-19 17:15:36
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Perylenetetracarboxylic Dianhydride and Aniline Assembled Supramolecular Nanomaterial with Multi-color Electrochemiluminescence for Highly Sensitive Label-free Immunoassay
摘要： Most electrochemiluminescence (ECL) studies were focused on the single emission of luminophore, which was severely limited the development of multi-color ECL fundamental theory and applications. Herein, we prepared a multi-color ECL supramolecular nanomaterial self-assembled by 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) and aniline (An) through hydrogen bonding. This PTCDA-An supramolecular nanomaterial simultaneously produced multi-color emission peaked at 486, 692 and 760 nm with K2S2O8 as coreactant. And the multi-emissions were assigned to excitated PTCDA monomer (486 nm), H-dimer (692 nm) and J-dimer (760 nm). The simultaneously increased dual-color ECL intensity significantly enhanced the total ECL intensity of PTCDA-An. And this high efficient ECL nanomaterial was further used as ECL platform to construct label-free immunosensor for tumor markers carcinoembryonic antigen (CEA) detection. The total ECL intensity of immunosensor exhibited a sensitive decrease due to the simultaneously decreased ECL of multi-emissions. And this immunosensor exhibited wide linear range from 1 pg mL-1 to 10 μg mL-1 with low detection limit of 0.23 pg mL-1. Multi-color ECL from the same luminophore PTCDA in this work also provided a new perspective for multi-color ECL biomaterial’s design.
关键词： supramolecular nanomaterial,multi-color ECL,electrochemiluminescence,aniline,PTCDA,CEA detection,label-free immunosensor
更新于2025-09-19 17:13:59
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Stereochemistry controlled supramolecular architectures of novel tetrahydroxy functionalized amphiphilic carbocyanine dye
摘要： The synthesis of novel amphiphilic 5,5',6,6'-tetrachlorobenzimidacarbocyanine (TBC) dye derivatives with amino-propanediol head groups differing in stereochemistry (chiral enantiomers, meso-form, and conformer) is reported. For the achiral meso-form, a new synthetic route towards asymmetric cyanine dyes was established. All compounds form J-aggregates in water whose optical properties were characterized by spectroscopic methods. The supramolecular structure of the aggregates was investigated by cryo-transmission electron microscopy (cryo-TEM), cryo-electron tomography (cryo-ET), and atomic force microscopy (AFM) revealing extended sheet-like aggregates for the chiral enantiomers and nanotubes for the mesomer, respectively, while the conformer forms predominately needle-like crystals. The experiments demonstrate that the aggregation behavior of compounds can be controlled solely by head group stereochemistry which in case of the enantiomers enables formation of extended hydrogen bond chains by the hydroxyl functionalities. In case of the achiral meso-form, however, such chains turned out to be sterically excluded.
关键词： Stereochemistry,cryo-TEM,supramolecular architectures,amphiphilic carbocyanine dye,cryo-ET,J-aggregates,AFM
更新于2025-09-19 17:13:59
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Semiconductor Quantum Dots as Components of Photoactive Supramolecular Architectures
摘要： Luminescent quantum dots (QDs) are colloidal semiconductor nanocrystals consisting of an inorganic core covered by a molecular layer of organic surfactants. Although QDs have been known for more than thirty years, they are still attracting the interest of researchers because of their unique size-tunable optical and electrical properties arising from quantum confinement. Moreover, the controlled decoration of the QD surface with suitable molecular species enables the rational design of inorganic-organic multicomponent architectures that can show a vast array of functionalities. This minireview highlights the recent progress in the use of surface-modified QDs – in particular, those based on cadmium chalcogenides – as supramolecular platforms for light-related applications such as optical sensing, triplet photosensitization, photocatalysis and phototherapy.
关键词： supramolecular chemistry,sensing,catalysis,triplet sensitization,quantum dots
更新于2025-09-19 17:13:59
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Supramolecular Valves Functionalized Rattle-Structured UCNPs@hm-SiO2 Nanoparticles with Controlled Drug Release Triggered by Quintuple Stimuli and Dual-modality Imaging Functions: A Potential Theranostic Nanomedicine
摘要： Integrating multimodality bioimaging and multiple stimuli-responsive controlled drug release properties into one single nanosystem for therapeutic application is highly desirable, but still remains a challenge. Herein, we coated a hollow mesoporous silica shell onto upconversion nanoparticles (UCNPs), conjugated pillarene-based supramolecular valves onto surface of UCNPs@hm-SiO2 using amine-coumarin phototriggers to obtain the multifunctional nanoparticles, UCNPs@hm-SiO2-Cou-Cys-DOX/WP[5]. Benefiting from the core-shell structured UCNPs, the UCNPs@hm-SiO2-Cou-Cys-DOX/WP[5] can serve as the efficient contrast agents for upconversion luminescence and T1-weighted magnetic resonance imaging in vitro/in vivo. More importantly, depending on exquisitely designed supramolecular valves, UCNPs@hm-SiO2-Cou-Cys-DOX/WP[5] can realize zero-premature release under normal physiological conditions (pH 7.4), which produces the minimal damage to normal tissue, whereas this nanosystem can respond to several disease-related signals including acid (most cancers), alkali (metabolic alkalosis), and Zn2+ (Alzheimer’s disease) along with two external stimuli including near infrared (NIR) light and reductive electrical potential via altering spatial structure of pseudorotaxanes, disassembling the molecular stalks, or undergoing photochemical reactions, ultimately resulting in opening of the gatekeepers and release of encapsulated drugs. The multifunctional UCNP-based nanoparticles were endowed with such quintuple stimuli-responsive controlled release characteristics. Specifically, in anticancer application, the rational utilization of the two of them, acid and NIR light, could regulate the release amount and rate of DOX from UCNPs@hm-SiO2-Cou-Cys-DOX/WP[5], accelerate the accumulation of DOX in cell nuclei and thereby promote the cancer cell apoptosis, indicating that the nanomaterials have promising application in cancer treatment. This study provides a novel design strategy for constructing multifunctional UCNP-based nanoparticles with multiple stimuli-responsive drug release features, which have great potential in diagnosis and therapy of relevant diseases as theranostic nanomedicines.
关键词： upconversion nanoparticles,Supramolecular nanovalve,theranostic nanoplatform,quintuple stimuli-responsiveness
更新于2025-09-19 17:13:59
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Selective fluorescence sensing of H <sub/>2</sub> PO <sub/>4</sub><sup>a??</sup> by the anion induced formation of self-assembled supramolecular polymers
摘要： The utilization of anions to induce the formation of self-assembled supramolecular polymers in solution is an undeveloped area of host–guest chemistry. We report in this manuscript a comparative study of two tripodal anion receptors by hydrogen or halogen bonding interactions to form self-assembled supramolecular structures induced by the presence of anions. DOSY NMR and DLS experiments provided evidence for the formation of supramolecular structures in solution in both halogen and hydrogen bond donors with H2PO4? anions. The nucleation and elongation constants obtained using the thermodynamic model indicate that the polymers grow following an isodesmic mechanism. Emission studies demonstrate that only the formation of the supramolecular polymer between the halogen bond donor receptor and H2PO4? anions results in the appearance of the excimer emission band.
关键词： halogen bonding,hydrogen bonding,DLS,anion receptors,DOSY NMR,excimer emission,supramolecular polymers
更新于2025-09-19 17:13:59
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The Power of Confocal Laser Scanning Microscopy in Supramolecular Chemistry: In situ Reala??time Imaging of Stimulia??Responsive Multicomponent Supramolecular Hydrogels
摘要： Multicomponent supramolecular hydrogels are promising scaffolds for applications in biosensors and controlled drug release due to their designer stimulus responsiveness. To achieve rational construction of multicomponent supramolecular hydrogel systems, their in-depth structural analysis is essential but still challenging. Confocal laser scanning microscopy (CLSM) has emerged as a powerful tool for structural analysis of multicomponent supramolecular hydrogels. CLSM imaging enables real-time observation of the hydrogels without the need of drying and/or freezing to elucidate their static and dynamic properties. Through multiple, selective fluorescent staining of materials in supramolecular hydrogels (e.g. inorganic materials and self-sorting nanofibers) can also be visualized. CLSM and the related microscopic techniques will be indispensable to investigate complex life-inspired supramolecular chemical systems.
关键词： confocal microscopy,gels,self-assembly,supramolecular chemistry,stimulus response
更新于2025-09-19 17:13:59