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Dispersed Nano-MOFs via a Stimuli-Responsive Biohybrid-System with Enhanced Photocatalytic Performance
摘要： MOF-based heterogeneous catalysts with enhanced dispersibility in solution are highly promising for liquid-phase catalysis yet the preparation remains a great challenge. Herein, via introducing responsive polymer-functionalized hollow pollen pivots, a general strategy toward preparing MOF@Pollen composites with adjustable dispersibility, environment-responsive activity and significantly enhanced liquid-phase photocatalytic performance is presented.
关键词： switchable catalysis,nanoMOFs,stimuli responsive polymer,dispersion
更新于2025-09-19 17:15:36
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The construction and modulation of photoelectric functional hierarchical materials based on ionic self-assembly
摘要： The photoelectric functional hierarchical materials have been successfully prepared by the simple ionic self-assembly (ISA) strategy from the cationic ferrocenyl surfactant, 16-alkyl (ferrocenyl-methyl)ammonium bromide (Fc16AB) and the anionic alizarin red (AR). The obtained complexes exhibited multiple stimuli-responsive switching behaviour triggered by β-cyclodextrin (β-CD) inclusion, redox species, and pH. The switching mechanism corresponding to each stimulus was studied in detail. Moreover, the fluorescent intensity of binary complexes could be modulated by the concentration of Fc16AB and redox of ferrocene part. The fluorescence switching mechanism upon redox stimulus was studied in detail. Both the complexes fabrication and transition mechanisms were found to be controlled by the inclusion equilibrium and the cooperative binding of non-covalent interactions, including the electrostatic interactions, π-π stacking, and amphiphilic hydrophobic association. This work provides a deep understanding of electro-photo molecular switching device.
关键词： Hierarchical materials,pH,Redox species,Stimuli-responsive,β-Cyclodextrin (β-CD) inclusion,Ionic self-assembly
更新于2025-09-19 17:15:36
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Micelle-Assisted Formation of Nanoparticle Superlattices and Thermally Reversible Symmetry Transitions
摘要： Nanoparticle superlattices (NPSLs) are of great interests as materials with designed emerging properties depending on the lattice symmetry as well as composition. The symmetry transition of NPSLs depending on environmental conditions can be an excellent ground for making new stimuli-responsive functional materials. Here, we report a spherical micelle-assisted method to form exceptionally ordered NPSLs which are inherently sensitive to environmental conditions. Upon mixing functionalized gold nanoparticles (AuNPs) with a nonionic surfactant spherical micellar solution, NPSLs of different symmetries such as NaZn13, MgZn2, and AlB2-type are formed depending on the size ratio between micelles and functionalized AuNPs, and composition. The NPSLs formed by the spherical micelle-assisted method show thermally reversible order-order (NaZn13–AlB2) and order-disorder (MgZn2–isotropic) symmetry transitions, which are consistent with the Gibbs free energy calculations for binary hard-sphere model. This approach may open up new possibilities for NPSLs as stimuli-responsive functional materials.
关键词： small-angle x-ray scattering,nanoparticle superlattice,spherical micelle,stimuli-responsive symmetry transition
更新于2025-09-19 17:15:36
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Triple stimuli-responsive ZnO quantum dots-conjugated hollow mesoporous carbon nanoplatform for NIR-induced dual model antitumor therapy
摘要： Aiming at the inef?ciency and toxicity in traditional antitumor therapy, a novel multifunctional nanoplat-form was constructed based on hollow mesoporous carbon (HMC) to achieve triple stimuli response and dual model antitumor therapy via chemo-photothermal synergistic effect. HMC was used as an ideal nanovehicle with a high drug loading ef?ciency as well as a near-infrared (NIR) photothermal conversion agent for photothermal therapy. Acid-dissoluble, luminescent ZnO quantum dots (QDs) were used as the proper sealing agents for the mesopores of HMC, conjugated to HMC via disul?de linkage to prevent drug (doxorubicin, abbreviated as Dox) premature release from Dox/HMC-SS-ZnO. After cellular endocytosis, the Dox was released in a pH, GSH and NIR laser triple stimuli-responsive manner to realize accurate drug delivery. Moreover, the local hyperthermia effect induced by NIR irradiation could promote the drug release, enhance cell sensitivity to chemotherapeutic agents, and also directly kill cancer cells. As expected, Dox/HMC-SS-ZnO exhibited a high drug loading capacity of 43%, well response to triple stimuli and excellent photothermal conversion ef?ciency g of 29.7%. The therapeutic ef?cacy in 4T1 cells and multicellular tumor spheroids (MCTSs) demonstrated that Dox/HMC-SS-ZnO + NIR had satisfactory chemo-photothermal synergistic effect with a combination index (CI) of 0.532. The cell apoptosis rate of the combined treatment group was more than 95%. The biodistribution and pharmacodynamics studies showed its biosecurity to normal tissues and synergistic inhibition effect to tumor cells. These distinguished results indicated that the Dox/HMC-SS-ZnO nanoplatform is potential to realize ef?cient triple stimuli-responsive drug delivery and dual model chemo-photothermal synergistic antitumor therapy.
关键词： Chemo-photothermal synergistic therapy,Triple stimuli-responsive,Hollow mesoporous carbon nanoparticles,TEM-EDX mapping,ZnO quantum dots
更新于2025-09-19 17:13:59
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Bioinspired Simultaneous Changes in Fluorescence Color, Brightness, and Shape of Hydrogels Enabled by AIEgens
摘要： Development of stimuli-responsive materials with complex practical functions is significant for achieving bioinspired artificial intelligence. It is challenging to fabricate stimuli-responsive hydrogels showing simultaneous changes in fluorescence color, brightness, and shape in response to a single stimulus. Herein, a bilayer hydrogel strategy is designed by utilizing an aggregation-induced emission luminogen, tetra-(4-pyridylphenyl)ethylene (TPE-4Py), to fabricate hydrogels with the above capabilities. Bilayer hydrogel actuators with the ionomer of poly(acrylamide-r-sodium 4-styrenesulfonate) (PAS) as a matrix of both active and passive layers and TPE-4Py as the core function element in the active layer are prepared. At acidic pH, the protonation of TPE-4Py leads to fluorescence color and brightness changes of the actuators and the electrostatic interactions between the protonated TPE-4Py and benzenesulfonate groups of the PAS chains in the active layer cause the actuators to deform. The proposed TPE-4Py/PAS-based bilayer hydrogel actuators with such responsiveness to stimulus provide insights in the design of intelligent systems and are highly attractive material candidates in the fields of 3D/4D printing, soft robots, and smart wearable devices.
关键词： stimuli-responsive hydrogels,complex shape,simultaneous changes,fluorescence,aggregation-induced emission luminogens
更新于2025-09-19 17:13:59
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Self-Assembled Extended ??-Systems for Sensing and Security Applications
摘要： Molecules and materials derived from self-assembled extended π-systems have strong and reversible optical properties, which can be modulated with external stimuli such as temperature, mechanical stress, ions, the polarity of the medium, and so on. In many cases, absorption and emission responses of self-assembled supramolecular π-systems are manifested several times higher when compared with the individual molecular building blocks. These properties of molecular assemblies encourage scientists to have a deeper understanding of their design to explore them for suitable optoelectronic applications. Therefore, it is important to bring in highly responsive optical features in π-systems, for which it is necessary to modify their structures by varying the conjugation length and by introducing donor?acceptor functional groups. Using noncovalent forces, π-systems can be put together to form assemblies of different shapes and sizes with varied optical band gaps through controlling intermolecular electronic interactions. In addition, using directional forces, it is possible to bring anisotropy to the self-assembled nanostructures, facilitating efficient exciton migration, resulting in the modulation of optical and electron-transport properties. In this Account, we mainly summarize our findings with optically tunable self-assemblies of extended π-systems such as p-phenylenevinylenes (PVs), p-phenyleneethynylenes (PEs), and diketopyrrolopyrroles (DPPs) as different stimuli-responsive platforms to develop sensors and security materials. We start with how PV self-assemblies and their coassemblies with appropriate electron-deficient systems can be used for the sensing of analytes in contact mode or in the vapor phase. For example, whereas the PV having electron-deficient terminal groups has high sensitivity toward trinitrotoluene (TNT) in contact mode, the supercoiled fibers formed by the coassembly of self-sorted stacks of C3-symmetrical PV and C3-symmetrical electron-deficient perylene bisimide are capable of sensing vapors of nitrobenzene and o-toluidine. The power of different functional groups in combination with PVs has been further illustrated by attaching CO2-sensitive tertiary amine moieties to a cyano-substituted PV, which allowed the bimodal detection of CO2 using fluorescence and Raman spectroscopy. Interestingly, the functionalization of PVs with terminal amide groups and chiral alkoxy side chains provided a mechanochromic system that allows self-erasable imaging. Whereas PVs exhibit quenching of fluorescence in most cases during self-assembly, PE derivatives exhibit aggregation-induced emission. This property of PEs has been exploited for the development of stimuli-responsive security materials, especially for currency and documents. For instance, the blue fluorescence of a PE attached to hydrophilic oxyethylene side chains coated on a filter paper upon contact with water changes to cyan emission due to the change in the molecular packing. Interestingly, the molecular packing of a Bodipy-attached PE-based gelator allowed a stress-induced change in the emission behavior, resulting in strong near-infrared (NIR) emission upon the application of mechanical stress or gelation. Finally, the use of DPP-based π-systems for the development of NIR transparent optical filters that block UV?vis light and their security- and forensic-related applications are described. These selected examples of the π-system self-assemblies provide an idea of the current status and future opportunities for scientists interested in this field of self-assembly and soft materials research.
关键词： self-assembly,sensors,π-systems,NIR transparent optical filters,stimuli-responsive,mechanochromism,fluorescence,security materials,aggregation-induced emission
更新于2025-09-19 17:13:59
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Plasmonic Gold Nanorattle Impregnated Chitosan Nanocarrier for Stimulus Responsive Theranostics
摘要： Herein, a stimulus-responsive theranostic nanosystem comprising gold nanorattles (AuNRTs), having a solid octahedron core and thin porous cubic shell, encapsulated within chitosan nanocarriers (CS-AuNRT) has been reported. Due to the plasmonic AuNRTs, CS-AuNRT demonstrated unique features of near infrared (NIR) absorbance and accessible intrinsic electromagnetic “hot spots” arising due to coupling of inner solid core and outer porous shell. These properties enabled CS-AuNRTs to be used for NIR-responsive drug delivery, photothermal therapy, and surface enhanced Raman scattering (SERS) based bioimaging. Following loading of chemotherapeutic drug doxorubicin (DOX) within AuNRTs along with a phase changing material (PCM), application of NIR irradiation resulted in photothermal melting of the PCM and simultaneous payload release in the surrounding medium. Although being nontoxic themselves, CS-AuNRTs with or without loaded DOX could mount signi?cant cell death in breast cancer cell line (MCF-7) in the presence of NIR light as external stimulus. The oxidative stress generated by DOX-loaded and empty CS-AuNRTs upon NIR irradiation were con?rmed by ?ow-cytometric determination of intracellular reactive oxygen species (ROS). Further, the ROS-led induction of apoptosis in treated MCF-7 cells was established from characteristic nuclear fragmentation, morphological changes and membrane blebbing as observed through confocal ?uorescence and scanning electron microscopy. Thus, with NIR responsive chemo-photothermal therapy and SERS based bioimaging, the present nanocarrier system holds potential for cancer theranostics.
关键词： bioimaging,drug delivery,photothermal therapy,stimuli responsive,nanorattle,chitosan nanoparticle
更新于2025-09-19 17:13:59
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A Strongly Fluorescent Molecular Material Responsive to Physical/Chemical Stimuli and their Coupled Impact
摘要： Molecular materials with weak but extended and pliable supramolecular interactions are versatile candidates for eliciting stimuli-sensitive optical responses. A novel diaminodicyanoquinodimethane (DADQ) molecule, 7,7-bis(2-(2-pyridyl)ethylamino)-8,8-dicyanoquinodimethane (BPEDQ), has been synthesized and structurally characterized; it exhibits enhanced fluorescence emission in the aggregated and solid states, characteristic of DADQs. The pyridine moieties in the molecule, in addition to the amino and cyano groups of the strongly dipolar fluorophore moiety, induce extensive H-bonding interactions which can impart structural integrity to the solid material; this enables reversible crystalline-amorphous transformations triggered by mechanical grinding and solvent fuming. The concomitant fluorescence color and intensity switching are prominent and reversible. Protonation-deprotonation events induced by acidic and basic vapors also produce stark fluorescence response variations; the chemical stimuli also lead to amorphization of the solid. The full cycle of chemical and physical stimuli, and the consequence of their individual and coupled impact on the fluorescence emission, are illustrated using a BPEDQ-doped polymer thin film.
关键词： amorphous-crystalline transformation,stimuli-responsive,molecular crystal,protonation,fluorescence
更新于2025-09-11 14:15:04
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Design of Thermochromic Luminescent Dyes Based on the Bis(o-carborane)-Substituted Benzobithiophene Structure
摘要： To obtain solid-state emissive materials having stimuli-responsive luminescent chromic properties without phase transition, benzobithiophenes modified with two o-carborane units having various substituents in the adjacent phenyl ring in o-carborane were designed and synthesized. Their emission colors were strongly affected not only by the substituents at the para-position of the phenyl ring but also by molecular distribution in the solid state. In particular, the emission colors were changed by heating without crystal phase transition. It was proposed that their thermochromic properties were correlated not with isomerization but with the molecular motion at the distorted benzobithiophene moiety.
关键词： Thermochromic,Bis(o-carborane)-Substituted Benzobithiophene,Solid-State Emissive Materials,Stimuli-Responsive,Luminescent Dyes
更新于2025-09-10 09:29:36
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Construction of a Luminogen Exhibiting High Contrast and Multicolored Emission Switching through Combination of a Bulky Conjugation Core and Toly Groups
摘要： Stimuli responsive luminogens may find application in highly sensitive sensors, memories and security inks. However, few examples exhibiting both high contrast and multi-colored emission switching have been reported due to the absence of molecular design strategy. Through combination of large conjugation core and peripheral phenyl rings, we obtained ditolyldibenzofulvene (1). Luminogen 1 is AIE active and exhibits tetracolored emission depending on its morphology. Its three single crystals emit blue, yellow and dark orange light upon excitation, exhibiting a maximal emission of 461 nm, 545 nm and 586 nm, respectively, and its amorphous solid emits at 557 nm. All the four aggregates exhibit enhanced emission intensity at lower temperature, but only the orange emissive crystals exhibit blue-shifted emission. The emission of 1 can be switched reversibly between any two of the four states through morphology tuning. Finally, the potential application of 1 in optical data storage was also investigated.
关键词： AIE,fluorescence,sensor,mechanochromic luminescence,stimuli responsive luminogen
更新于2025-09-04 15:30:14