Latest ArticlesHerein, we designed and constructed two metallacycles, 1 and 2, to illustrate the conformational effect of isomeric AIE fluorophores on the platform of supramolecular coordination complexes (SCCs). Specifically, the dangling phenyl rings in TPE units of the metallacycle 1 align completely outside the main cyclic structure, while in the metallacycle 2, these phenyl rings align half inside and half outside. The experimental results showed that two metallacycles exhibited different behaviors in terms of AIE fluorescence and chemical sensing, which could be attributed to the subtle structural difference of the TPE units. This work represents the unification of topics such as self-assembly, AIE, and chemical sensing, and further promotes the understanding for the structure-property relationship of isomeric AIE fluorophores.
The stimulator of interferon genes (STING) shows promising clinical activity in infectious diseases and tumors. However, the lack of targeting capability and intracellular stability of STING agonists severely limits the therapeutic efficacy. Recently, drug delivery systems (DDSs) overcome these delivery barriers of STING agonists via passive or active cell targeting, prolonged blood circulation and drug release, and lysosome escape, etc. In this review, we will describe in detail how existing DDSs are designed to overcome delivery barriers and activate the STING pathway, and the current biomedical applications of STING-activating DDSs in the treatments of infectious diseases and tumors. Finally, the prospects and challenges of DDSs in STING activation are discussed.
Due to their high specificity and affinity towards various targets, along with other unique advantages such as stability and low cost, aptamers are widely applied in analytical techniques. A typical aptamer-based electrochemical biosensor is composed of a aptamer as the biological recognition element and transducer converting the biologic interaction into electrical signals for the quantitative measurement of targets. Improvement of the sensitivity of a biosensor is significantly important in order to achieve the detection of biomolecules with low abundance, and different amplification strategies have been explored. The strategies either employ nanomaterials such as gold nanoparticles to construct electrodes which can transfer the biological reactions more efficiently, or attempt to obtain enhanced signal through multi-labeled carriers or utilize enzyme mimics to catalyze redox cycling. This review discusses recent advances in signal amplification methods and their applications. Critical assessment of each method is also considered.
A green tandem reaction, including insertion/aerobic oxidation/bisindolylation, starting from indoles and diazo compounds has been developed. The combination of water and fluorinated alcohol plays dual roles as solvent and promoter in this chemical transformation. Molecular oxygen in the air acts as an oxidant. 3, 3'-Bis(indolyl)methanes with quaternary carbon were produced under metal-free conditions. No any catalyst and additive were required. N2 and water were released as sole by-products. Absence of water and fluorinated alcohol resulted in Wolff rearrangement product.
A novel good water-soluble macrocycle containing two pyridinium moieties was synthesized in high yield. It could form 1:1 complexes with neutral guests containing naphthalene or phenyl units in water. The water-soluble macrocycle can selectively encapsulate naphthalene to form a 1:1 complex over a variety of polycyclic aromatic hydrocarbons.
Nowadays, the development of triplet-involved materials becomes a hot research topic in solid-state luminescence fields. However, the mechanism of triplet-involved emission still remains some mysteries to conquer. Here, we proposed a new concept of excited-state conformation capture for the constructions of different types of triplet-involved materials. Firstly, excited-state conformation could be trapped by supramolecular chains in crystal and form a new optimum excited-state structure which is different from that in solution or simple rigid environment, leading to bright thermally activated delayed fluorescence (TADF) emission. Based on excited-state conformation capture methodology, next, we obtained room-temperature phosphorescence (RTP) by introducing Br atoms for the enhancement of intersystem crossing. It could be concluded from experimental results that TADF may originate from aggregate effect while RTP may derive from monomers. Finally, heavy-atom free RTP and ultra RTP were achieved by eliminating aggregate effect. This work could not only extend the design methodology of triplet-involved materials but also set clear evidences for the mechanism of triplet-involved emissions.
Recently, stimuli-responsive DNA nanostructure-based nanodevices have been applied for cancer therapy. In this study, pH-responsive i-motif DNA was modified on gold nanoparticles (AuNPs) via a facile, time-saving freeze-thaw method and utilized to construct stimuli-responsive drug nanocarriers. When the environment pH changes from 7.4 to 5.0, the i-motif DNA would be folded into four-stranded (C-quadruplex) that could be characterized by circular dichroism, and the characteristic of acid stimulate was verified by fluorescence resonance energy transfer (FRET). To enhance specifical cellular uptake, MUC1 aptamer was employed as the targeting moiety. Doxorubicin (Dox) is an anticancer drug that can be efficiently intercalated into GC base pairs of DNA nanostructure to form drug-loaded nanovehicles (Dox@AuNP-MUC1). Additionally, owing to the excellent photothermal conversion efficiency of AuNPs, the synergistic effect between chemotherapy and PTT can be readily achieved by 808 nm near-infrared (NIR) irradiation, which exhibits specifically and efficiently anticancer efficiency. Hence, this multifunctional drug carrier shows the potential for synergistic photothermal-chemotherapy.
An unprecedented tunable hydrophobic effect in self-assembly of a small cationic organic fluorophore (NI-TPy+)-based with aggregation-induced emission (AIE) property was realized in aqueous solution. The amplification of hydrophobicity was found to be significantly dependent upon the increasing aggregates of NI-TPy+, which enabled the study of the hydrophobic binding of chaotropic anions with the Hofmeister series.
Despite of the promising achievements of immune checkpoints blockade therapy (ICB) in the clinic, which was often limited by low objective responses and severe side effects. Herein, we explored a synergistic strategy to combine in situ vaccination and gene-mediated anti-PD therapy, which was generated by unmethylated cytosine-phosphate-guanine (CpG) and pshPD-L1 gene co-delivery. PEI worked as the delivery carrier to co-deliver the CpG and pshPD-L1 genes, the formed PDC (PEI/DNA/CpG) nanoparticles were further shielded by aldehyde modified polyethylene glycol (OHC-PEG-CHO) via pH responsive Schiff base reaction for OHC-PEG-CHO-PEI/DNA/CpG nanoparticles (P(PDC) NPs) preparation. All steps could be finished within 30 min. Such simple nanoparticles achieved the synergistic antitumor efficacy in B16F10 tumor-bearing mice, and the amplified T cell responses, together with enhanced NK cells infiltration were observed after the combined treatments. In addition, the pH responsive delivery system reduced the side effects triggered by anti-PD therapy. The facile and effective combination strategy we presented here might provide a novel treatment for tumor inhibition.
Aggregation-induced emission luminogens (AIEgens) have been used in biomacromolecules detection. Herein, TPE-dC and TPE-dU acted as the nucleoside-based AIEgens sensors in the first case, which can be used to detect ctDNA and rRNA in vitro and light up the nucleus in vivo depending on the intermolecular binding affinity. This AIE process enables the quantitative analysis or visualization of nucleic acids in solution or gels state, respectively. Furthermore, confocal laser scanning microscopy (CLSM) images of L929 cells stained with TPE-dC or TPE-dU clearly shows that nucleoside-based AIEgens bio-probes can pass the cell membranes to reach the cell nucleus, without cytotoxicity at the imaging condition (incubation time > 12 h, and 10 μmol/L of concentration). Since the nucleus is rich in DNA/RNA, fluorescence turn-on mode has a great potential in nucleus imaging and clinical diagnosis.
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