Latest ArticlesThe elaborate regulation of heterostructure interface to accelerate the interfacial charge separation is one of practicable approaches to improve the photocatalytic CO2 reduction performance of halide perovskite (HP) materials. Herein, we report an in-situ growth strategy for the construction of 2D CsPbBr3 based heterostructure with perovskite oxide (SrTiO3) nanosheet as substrate (CsPbBr3/SrTiO3). Lattice matching and matchable energy band structures between CsPbBr3 and SrTiO3 endow CsPbBr3/SrTiO3 heterostructure with an efficient interfacial charge separation. Moreover, the interfacial charge transfer rate can be further accelerated by etching SrTiO3 with NH4F to form flat surface capped with Ti−O bonds. The resultant 2D/2D T-SrTiO3/CsPbBr3 heterostructure exhibits an impressive photocatalytic activity for CO2 conversion with a CO yield of 120.2 ± 4.9 µmol g−1 h−1 at the light intensity of 100 mW/cm2 and water as electron source, which is about 10 and 7 times higher than those of the pristine SrTiO3 and CsPbBr3 nanosheets, surpassing the reported halide perovskite-based photocatalysts under the same conditions.
Regulating flow direction of photo-excited electrons from interior to active sites in surface is critical to enhance the photocatalytic performance. Herein, photoinduced chemical reduction process was utilized to pinpoint deposit CdS and NiS nanodots sequentially onto g-C3N4 nanosheets. The resulted hybrid composite NiS/CdS/g-C3N4 was much more active under visible light, and eventually boosted the hydrogen evolution rate of 3015 µmol g−1 h−1, to be 2.4 folds better than that of g-C3N4. Because of the relative low content of CdS (around 3.0 wt%), the enhanced activity is due to the favoring band overlapping and promoting charge separation rather than increasing light absorption. Femto-second time-resolved transient absorption spectroscopy (fs-TAS) clearly reveals that the photo-excited electrons are from g-C3N4, and then migrate unidirectionally to CdS and finally to NiS, which is caused by the precisely regulate the position of CdS and NiS on g-C3N4 surface. This study elucidates the electron transfer kinetics and processes in multi-component system and affords a new avenue to construct stable photocatalysts with high activity.
Metallacycles hold great promise for fluorescence-based sensing due to their synthetic advantages and unique physicochemical properties. However, it remains highly challenging to develop a versatile methodology for constructing highly emissive metallacycles with targeted functionalities and therefore sought-after properties. Herein, we report a general strategy to construct a series of highly emissive perylene diimide-based metallacycles via the self-assembly of perylene diimide-based tetrapyridyl ligand with different dicarboxylic ligands featuring fixed angles and cis-Pt(PEt3)2(OTf)2. Single crystal X-ray diffraction analyses verify the formation of bowtie-like metallacycles with two triangular cavities. Notably, the fluorescence quantum yields of most assemblies exceed 98%, amongst the highest values for metallacycles. Additionally, such metallacycles exhibit sensitive fluorescence responses toward picric acid with a detection limit of 2.8 × 10−6 mol/L. This study not only provides a rational strategy for preparing highly emissive bowtie-shaped metallacycles, but also sheds light on their usage in the detection of picric acid and associated compounds.
Recently, hydrogen-bonding has attracted extensive attention in the design of chromophores. Here, a new class of hydrogen-bond locked purine chromophores (HOPs) were reported by introducing a hydroxyphenyl group into the C(6) position of purine. The intramolecular hydrogen bond plays a dominant role to light up these probes. As a bonus, HOPs show high photostability. Moreover, HOPs exhibit remarkable capability for the specific lipid droplets imaging in living cells with excellent biocompatibility and are also potential for diagnosing fatty liver diseases. These results bring important new insights into the photophysics of the purine-based chromophores and provide a new scaffold with high photostability for bioimaging.
Efficient oral delivery of drugs treating brain diseases has long been a challenging topic faced by the drug delivery community. Fortunately, polyester nanoparticles offer certain solutions to this problem. This review article firstly describes the main obstacles faced by oral administered brain targeting, including: (1) instability in the gastrointestinal tract; (2) poor penetration of the intestinal mucosa and epithelium; (3) blood clearance; and (4) restriction by the BBB. Then the key factors influencing brain-targeting efficiency of orally administered polyester nanoparticles are also discussed, such as size, shape and surface properties. Finally, recent brain-targeting delivery strategies using oral polyester nanoparticles as carriers and their effects on brain drugs transport are reviewed, and the delivery 'as a whole' strategy of polyester nanoparticles will provide new insight for oral brain-targeting delivery. And by combination of multiple strategies, both the stability and permeability of polyester nanoparticles can be greatly improved for oral brain drug delivery.
The transformation of a Palladium-based metal-organic cage to a structurally similar one by direct ligand replacement usually leads to unwanted ligand scrambling. In this work, an intermediate ligand with different shape and basicity from the initial/final ones was introduced to avoid ligand scrambling to achieve the efficient indirect cage-to-similar-cage transformation. Compared with the direct transformation, the stepwise conversion has the advantages of high efficiency (93%) and simple workup.
The first example of the microfluidic chips (MFCs) consisting of centimeter-level 3D channels with high-density and large-volume fabricated by femtosecond laser micromachining were utilized to develop a time-saving, economical and hazardless flow synthesis process, and its advantages have been proved by in situ formation of aryldiazonium salts and subsequent borylation with bis(pinacolato)diboron. There are several important advantages in our 3D MFC-based flow synthesis technology, including the following: (1) the reaction temperature was altered from ice bath to room temperature; (2) the residence time was reduced by 10 times; (3) the yield was greatly improved, that is, several arylboronates were successfully obtained with higher yield compared to traditional batch process. Therefore, it can be envisioned that a novel, simplified flow synthetic protocol will be developed toward green organic synthesis via MFCs.
Naphthalimide derivatives have good planarity and large conjugated structure and therefore possess photophysical properties and biological activities. Previously, our group discovered seven-membered heterocyclic derivatives via modifying 4- and 5-positions of naphthalimide skeleton and found the derivatives had good water solubility and showed large stokes shift and strong fluorescence in water. In this article, we designed and synthesized more seven-membered ring-fused naphthalimide derivatives (Y1-Y16) by introducing different substitutions on the imide group. Among them, Y1, Y5, Y9 were found to show similar cytotoxic activities with Amonafide against A549 and HL60 cells, with IC50 values at 10−6 mol/L. What is more, the asymmetry derivatives (Y1 and Y5) showed high fluorescent quantum yields in the aqueous phase (Ф = 0.47). Considering the great fluorescence quantum yields in water and the potent anti-tumor activities of the representative seven-membered ring-fused naphthalimides, they have potentials to be used as agents for cancer theranostics.
Sulfur mustard (SM) can be absorbed by skin quickly and cause serious system damage via reacting with nearly all cell constituents. Until now, there is still lack of effective antidotal therapy for SM and skin protection is highly important to defend SM. In this article, supramolecular liquid barrier based on pillar[5]arene with triethylene oxide substituents (EGP5) has been designed to impede the skin permeation of SM and further interaction with the skin tissue. EGP5 could encapsulate SM within its cavity, with a Ka value of (5.10 ± 0.47) × 102 L/mol. In vitro skin absorption test proved that EGP5 was capable to effectively prevent SM from penetrating through skin. This supramolecular liquid barrier was employed on rat models to systematically evaluate protective effect against SM intoxication. Pretreatment of EGP5 could alleviate skin and system damage induced by SM and improve survival rate of poisoned rat models from 10% to 90%. Additionally, EGP5 served as protective materials could be highly reused after recycling several times. Overall, these findings have provided the first insight into the construction of convenient liquid material for SM protection.
The effective materials and methods for detection and separation of pesticides are urgently needed because most of pesticides show very harmful influence on life and environment. As a new kind of macrocyclic host compound, pillar[n]arenes show very good performance in the detection and separation of pesticides, especially for paraquat (PQ). For the pesticide detection and separation materials, their structures determine performance. Therefore, this review summarizes the recent progress of pillar[n]arenes-based materials for detection and separation of pesticides covering single/multi-pillar[n]arenes, pillar[n]arenes-based polymers, frameworks, composites, nanomaterials, etc. The structure-performance relationships of these materials have been discussed according to the cavity size, the synergistic or collaboration effect, the structure of the polymer or framework, the substrate of the composites and the size of nanomaterials and so on. Based on these, we also look forward to the future and point out the possible way for improving the pesticides detection sensitivity and separation efficiency of this kind of materials.
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